English

• 0.   Introduction

  Amidst rapid global economic development and the depletion of fossil fuels, energy shortages and environmental pollution have emerged as urgent worldwide challenges requiring immediate solutions^[1-3]. Consequently, the development of large-scale new energy storage technologies has become increasingly critical^[4-6]. Among these, electrochemical energy storage stands out due to its high efficiency and flexibility, making it a key pathway to addressing these issues^[7-8]. Lithium-ion batteries (LIBs) represent a breakthrough in electrochemical energy storage, offering high energy density, long cycle life, and high operating voltage^[9-11]. A typical LIB comprises four primary components: a cathode (e.g., lithium metal oxides such as LiCoO₂, LiFePO₄, or LiNi_xMn_yCo₂O₂), an anode (commonly graphite), a separator, and an electrolyte (typically a lithium salt such as LiPF₆ dissolved in organic solvents). The electrochemical performance of LIBs is evaluated based on several key metrics, including specific capacity (mAh·g^-1), energy density (Wh·kg^-1 or Wh·L^-1), power density (W·kg^-1), rate capability (i.e., the electrochemical performance under varying charge/discharge rates), Coulombic efficiency, and cycling stability (capacity retention over extended cycling). However, the widespread adoption of electric vehicles and growing demand for portable electronics have imposed stringent requirements for fast-charging capabilities^[12-14]. Traditional LIBs remain constrained by their inherent material limitations, struggling to meet escalating energy storage demands^[15-17]. For example, in widely used graphite anodes, solvent molecules from the electrolyte can co-intercalate with lithium ions (Li⁺) during deintercalation^[18-19]. This leads to gradual degradation of the graphite layered structure, flaking, and a decline in reversible specific capacity and cycle stability. Furthermore, repeated Li⁺ intercalation and deintercalation damage the solid electrolyte interphase (SEI) film, triggering continuous electrolyte decomposition and progressive SEI thickening^[20-21]. An excessively thick SEI film not only lengthens the Li⁺ diffusion pathway but also increases interfacial charge-transfer resistance, severely impairing the cycling performance at high rates (i.e., fast-charging capability)^[22-23]. Therefore, developing novel electrode materials with high energy density, excellent fast-charging capability, and long cycle life is crucial for advancing LIB technology toward large-scale industrial applications^[24].

  Metal-organic frameworks (MOFs), crystalline porous materials assembled from metal nodes and organic ligands via coordination bonds, exhibit outstanding characteristics such as high specific surface area, tunable pore structure, and controllable chemical composition and morphology^[25-27]. They have demonstrated promising applications in gas adsorption and separation, drug delivery, and energy storage and conversion^[28-32]. Although intrinsic MOFs typically exhibit poor electrical conductivity (generally < 10^-10 S·cm^-1), which limits their direct application as bulk electrode materials^[33-35], significant progress has been made in overcoming this limitation through various strategies. These approaches include: (1) developing intrinsically conductive MOFs by designing π-conjugated frameworks that enable charge delocalization (e.g., MOFs based on tetrathiafulvalene, triphenylene, or hexaaminobenzene ligands); (2) incorporating conductive additives (such as carbon nanotubes, graphene, or conductive polymers) to form MOF composites; (3) partial carbonization or pyrolysis to generate MOF-derived carbon composites that retain the structural characteristics of the parent MOF; (4) fabricating ultrathin MOF coatings on conductive substrates, keeping the coating thickness below the electron tunneling distance. These strategies have enabled the development of MOF-based electrodes as composites, derivatives, or ultrathin coatings that achieve significantly enhanced conductivity while preserving the structural and porosity advantages of MOFs. This provides new insights for the design of high-performance energy storage materials. Notably, the high specific surface area and tunable porosity of MOFs lay a strong foundation for their use in fast-charging batteries, facilitating electrolyte wetting and ion transport, while their mechanical strength helps buffer volume changes^[36]. Their abundant active sites further contribute to enhanced battery capacity^[37]. Additionally, MOF-based separator materials show excellent structural stability and ionic conductivity^[38]. Currently, MOF applications in fast-charging batteries have expanded from ion-conductive materials to functionalized separators, Li-metal anode interface control materials, and further into quasi-solid/solid electrolyte domains^[39-41].

  This review systematically summarizes recent advances, core mechanisms, and optimization strategies for MOFs and their derivatives as fast-charging battery electrode materials. It analyzes key challenges facing MOF-based electrodes and elaborates on their roles in critical battery components-anodes, cathodes, separators, and electrolytes (Fig.1). Specifically, we discuss how MOF-based materials address the fundamental fast-charging bottlenecks outlined above, including their roles as anode materials or coatings that mitigate Li⁺ desolvation sluggishness and suppress dendrite growth through spatial confinement and ion-flux homogenization; as cathode modifiers that stabilize electrode/electrolyte interfaces and inhibit transition metal dissolution; as functional separators that enhance ion-transport uniformity and thermal stability; and as solid-state electrolyte components that improve ionic conductivity and interfacial contact while mechanically suppressing dendrite penetration. Finally, the review discusses current limitations and future directions for MOFs in fast-charging batteries, aiming to provide insights and guidance for ongoing research and material design in this field.

  Figure 1

  

  Figure 1.  Mechanisms and applications of MOFs in enhancing the fast-charging performance of LIBs

  下载: 全尺寸图片 幻灯片

  1.   Fundamental mechanisms of MOFs in fast-charging batteries

  To address severe challenges associated with fast-charging of batteries—such as sluggish Li⁺ transport, exacerbated interfacial side reactions, and lithium dendrite growth—the structural tunability of MOF materials offers a distinctive molecular-level toolbox^[42]. Their core mechanisms of application revolve around three dimensions: ion-transport regulation, interface stabilization, and conductive-network construction^[43-45]. Through precise pore-size engineering, surface chemical modification, and multifunctional integration, MOFs fundamentally optimize the kinetic processes and stability of batteries.

  1.1   Mechanism of selective ion sieving and transport

  A primary bottleneck in achieving fast-charging performance is the need for rapid and selective Li⁺ conduction within the electrolyte. MOF materials, with their highly ordered and size-tunable nanochannels, present an ideal platform as "intelligent ion sieves" to address this challenge^[46-47]. Their mechanism of action extends beyond simple size exclusion, integrating multiple effects such as pore size matching, surface chemical regulation, and specific recognition^[48]. Various modification strategies based on MOF materials have been applied to LIB systems. For example, Zhang et al.^[49] employed an in-situ growth method to fabricate a fluorine-functionalized UiO-66-4F MOF membrane on a PET substrate (Fig.2a), offering an innovative approach to ion sieving and selective transport. This membrane leverages the strong electronegativity of fluorine groups to enhance affinity for Li⁺ while precisely tuning pore sizes to the sub-nanometer scale, creating steric hindrance that inhibits the migration of hydrated magnesium ions (Fig.2b-2e). This synergistic mechanism, combining size-based screening and chemical affinity, achieved a Mg²⁺/Li⁺ separation factor of 283 while maintaining a Li⁺ permeation flux of 0.16 mol·m^-2·h^-1 (Fig.2f). The study demonstrates that functionalization of MOF membranes can simultaneously enhance both ion transport selectivity and flux. Beyond pore channel functionalization, the inherent channel architecture itself can be precisely designed to achieve selective ion recognition. Zhao et al.^[50] designed and synthesized a novel MOF material, TYUST-8, through the coordination of CrO₆ clusters with 1,2,4,5-benzenetetracarboxylic acid (Fig.2g). The material features nanoscale 4-O tetrahedral pockets along the walls of its one-dimensional channels, which serve as core adsorption sites. This design prevents pore blockage while enabling preferential Li⁺ adsorption via strong chelation and size-matching effects. TYUST-8 exhibited a Li⁺ adsorption capacity of 76.1 mg·g^-1 with an equilibrium time of only 30 min (Fig.2h, 2i). It also showed remarkable separation selectivity toward coexisting ions such as Na⁺ and K⁺, along with outstanding stability in both acidic and alkaline environments. This study elucidates the synergistic mechanism between channel structure and ionic pockets, confirming that the precise design of the site structure in MOF materials can effectively optimize their ion-sieving performance.

  Figure 2

  

  Figure 2.  (a) Schematic of the preparation and structure regulation of the UiO-66-4F membrane for ion separation; SEM images of (b) UiO-66 and (c) UiO-66-4F membrane surfaces; Pore sizes of (d) UiO-66 and (e) UiO-66-4F powders; (f) Ion selectivity of the UiO-66-4F membrane (Copyrighted from Ref.^[49] with a license); (g) Schematic diagrams for the framework structure of TYUST-8; Adsorption amounts of Li⁺ at various (h) initial concentrations and (i) contact times (c₀=100 and 500 mg·L^-1; pH=6.5±0.2) (Copyrighted from Ref.^[50] with a license)

  下载: 全尺寸图片 幻灯片

  Furthermore, the trade-off between ion selectivity and conductivity can be addressed through structural modulation and defect repair of MOF membranes. Cao et al.^[51] fabricated polycrystalline MOF-801 membranes on α-Al₂O₃ substrates via secondary hydrothermal growth (Fig.3a). By applying a sub-10 nm thick sPEEK polymer coating to seal membrane defects, they opened new avenues for ion-sieving research (Fig.3b). Owing to its precisely tuned sub-nanometer pores (0.35 nm) and hydrogen-bonded networks within the channels, this membrane achieved an exceptional H⁺/V selectivity of 194 and an ionic conductivity of 0.028 S·cm^-1, significantly surpassing the performance of commercial Nafion-117 membranes. In vanadium flow battery (VFB) tests, it delivered a Coulombic efficiency (CE) of 96.1% and an energy efficiency (EE) of 83.2% (Fig.3c-3e).

  Figure 3

  

  Figure 3.  (a) Structure diagram of MOF-801 polycrystalline membrane with sub-10 nm polymer protective coating applied to the VFB system; (b) Cross-section SEM images of MOF-801 membrane; (c) Ion permeation of metal salts through MOF-801 and s-MOF-801 membrane; (d) Ion selectivity of MOF-801 and s-MOF-801 membrane; (e) CEs, VEs, and EEs of VFB cells equipped with s-MOF-801 membrane at 20-80 mA·cm^-2 (Copyrighted from Ref.^[51] with a license); (f) Schematic representation of the synthesis process for the formation of the Ag/MOFs membrane and Ag/PSS@MOFs composite membrane; (g, h) Output current and power of PSS@MOFs-3 with different external resistances for different concentration gradients; (i) Maximum output powers of PSS@MOFs-3 with different concentration gradients (Copyrighted from Ref.^[52] with a license)

  下载: 全尺寸图片 幻灯片

  In-situ functional doping of MOF membranes offers another effective route to simultaneously enhance ion selectivity and permeability. Yao et al.^[52] employed anodic electrodeposition to fabricate PSS@MOFs composite membranes with in-situ polystyrene sulfonate (PSS) doping on anodic aluminum oxide (AAO) substrates. The incorporated sulfonate groups strengthen ionic electrostatic interactions, creating negatively charged nanoconductors that promote preferential cation transport. Under a 100-fold salinity gradient, this composite membrane with a thickness of only 860 nm demonstrated a high cation mobility of 0.993, an energy conversion efficiency of 48.8%, an output power of 2.90 μW, and an internal resistance of merely 999 Ω (Fig.3f-3i).

  Consequently, the key advantage of MOF materials in ion sieving and selective transport stems from their structural tailorability and synergistic multi-mechanism operation. By engineering pore dimensions, functionalizing surfaces, and precisely constructing specific recognition sites, MOFs can concurrently modulate ion-size exclusion, electrostatic interactions, and chemical affinity. This integrated approach allows for efficient, high-speed screening of target ions, such as Li⁺, at the molecular scale.

  1.2   Mechanism of interfacial regulation and dendrite inhibition

  The growth of Li dendrites poses a significant safety challenge that hinders the development of fast-charging batteries, primarily due to the uneven distribution of Li⁺ flux at the electrode/electrolyte interface^[53-55]. MOFs, with their tunable porous structures and high specific surface areas, act as ideal "ion redistributors" and "physical barriers". They synergistically inhibit dendrite growth through kinetic mechanisms (regulating ion transport) and thermodynamic mechanisms (stabilizing interfaces)^[47,56]. The microporous structure of MOFs provides a spatial confinement effect, which helps reduce local current density and thereby enhances interfacial stability. For pore sizes below 1 nm (typically < 0.5 nm), such as the 0.293 nm glassy MOF coating reported by Xu et al.^[57] spatial confinement primarily functions through size exclusion and desolvation effects (Fig.4a). These sub-nanometer channels are smaller than the solvated Li⁺ radius ([Li(PC)₃]⁺ complex: ca. 0.48 nm), forcing Li⁺ to undergo partial or complete desolvation prior to intercalation. This desolvation process reduces solvent co-intercalation and associated graphite exfoliation, while the uniform pore size ensures homogeneous ion flux, collectively suppressing dendrite nucleation (Fig.4b). This anode delivered a capacity exceeding 250 mAh·g^-1 at a 5C rate, five times that of pristine graphite, and maintained a dendrite-free structure even after 200 fast-charging cycles (Fig.4c). The assembled NCM811//glass@graphite full cell achieved an energy density of 283 Wh·kg^-1 and retained 80% of its capacity after 300 cycles (Fig.4d). For pore sizes in the range of 2-5 nm, such as the ca. 4 nm pores in the MXene/Ni-MOF heterojunction reported by Zhu et al.^[58], spatial confinement operates through a different mechanism. These mesoporous channels are too large for size exclusion effects but serve as an ion redistribution layer, guiding uniform Li⁺ nucleation and promoting lateral diffusion to prevent localized ion aggregation-induced dendrite formation. Concurrently, the MOF monolayer functions as an artificial SEI film (Fig.4e). MOFs exhibited a high binding energy of -3.78 eV (Fig.4f), which was higher than that of Cu (-2.57 eV), indicating the strong interaction between Li and MOFs. The spatial confinement effect of the microporous structure markedly reduces local current density, enabling controlled Li deposition. Even at a high deposition rate of 5 mAh·cm^-2, the electrode surface exhibited no significant dendrites, forming a uniform nanosheet structure. Furthermore, chemical bonding between MOF and MXene enhances interfacial stability, enabling symmetric cells based on this heterojunction substrate to achieve a cycle life of 500 h at a current density of 1 mA·cm^-2 (Fig.4g). The assembled Li||LiFePO₄ full cell maintained a capacity retention of 91% after 600 cycles (Fig.4h).

  Figure 4

  

  Figure 4.  (a) Schematic illustration of the preparation process and the benefits of coating commercial graphite with 0.293 nm MOF glass containing P elements; (b) HRTEM images of glass@graphite coated with uniform and ultra-thin MOF glass featuring subnanochannels; (c) Cycling performance of assembled NCM-811//graphite and NCM-811//glass@graphite full cells; (d) Cycling performance of NCM-811//glass@graphite pouch cell (inset: schematic illustration of the pouch cell) (Copyrighted from Ref.^[57] with a license); (e) Schematic illustrating the self-assembly process of MXene/MOFs heterojunction; (f) Lithium adsorption energy at the surface of MOFs; (g) Cycling performances of Li symmetrical cells with MXene/MOFs, MXene, MOFs, and Cu substrates; (h) Long-term cycling performances of Li||LiFePO₄ cells with MXene/MOFs, MXene, MOFs, and Cu substrates at 1C (Copyrighted from Ref.^[58] with a license)

  下载: 全尺寸图片 幻灯片

  MOFs can effectively mitigate Li dendrite formation in fast-charging batteries through synergistic mechanisms such as ion flux homogenization, spatial confinement, and interfacial reinforcement. Similarly, Xu et al.^[59] developed an MOF808@PAN@PEO composite electrolyte that employed a comparable suppression strategy (Fig.5a). The microporous structure of the MOF induces a spatial confinement effect, regulating the local current density within an optimized range (Fig.5b-5d). Concurrently, it adsorbs TFSI^- anions via Lewis acid-base interactions, promoting Li⁺ dissociation and uniform migration, thereby increasing the Li⁺ transference number to 0.42. This composite structure also enhances the mechanical stability and elastic recovery of the interface, facilitating the formation of a stable SEI layer that effectively impedes dendrite penetration. Experiments demonstrated that symmetric cells using this composite electrolyte could cycle stably for 1 800 h at 0.1 mA·cm^-2 (Fig.5e). Moreover, the Li metal anode remained smooth and dense even after 100 cycles, further confirming that efficient Li dendrite suppression can be achieved through MOF-mediated interface regulation (Fig.5f-5h).

  Figure 5

  

  Figure 5.  Material design flowchart and morphological structural characterization of 3D MOF@PAN network: (a) schematic of the process; SEM images of (b) electrostatically spun PAN fiber and (c, d) MOF808 network on loaded PAN fiber at different magnifications; (e) Cycling performance of Li|PEO-LiTFSI|Li and Li|MOF808@PAN@PEO-LiTFSI|Li lithium symmetric batteries at 0.1 mA·cm^-2 at 60 ℃; (f) SEM image of the lithium anode surface of Li|PEO-LiTFSI|Li symmetric cell after 100 cycles; (g) optical photographs of PEO-LiTFSI and MOF808@PAN@PEO-LiTFSI polymer electrolyte films; (h) SEM image of the lithium anode surface after 100 cycles of Li|MOF808@PAN@PEO-LiTFSI|Li symmetric cell (Copyrighted from Ref.^[59] with a license)

  下载: 全尺寸图片 幻灯片

  MOF materials possess an "active design" nature that surpasses traditional materials in regulating lithium metal interfaces. Their significance extends beyond the physical confinement offered by porous structures to encompass multidimensional synergistic control of ion transport, nucleation behavior, and interface stability, achieved through precise coupling of pore engineering and surface chemistry. This represents a paradigm shift from "passive protection" toward "active guidance", providing a fundamental material design strategy to address core safety challenges in fast-charging batteries. However, current research remains largely focused on validating performance at the material level. Future efforts should prioritize the deep integration of these smart interface materials into practical battery systems and systematically assess their long-term effectiveness and scalability under realistic fast-charging conditions.

  1.3   Mechanism of electrolyte confinement and ionic conductivity enhancement

  The development of solid-state or quasi-solid-state electrolytes that simultaneously achieve high ionic conductivity and interfacial stability represents a fundamental challenge in building safe, fast-charging battery systems. Capitalizing on their tunable structures, abundant pore channels, and modifiable active sites, MOF materials have been incorporated as key functional components into polymer matrices, offering innovative strategies to overcome the typical limitations of conventional solid-state electrolytes, such as low ionic conductivity, low Li⁺ transference numbers, and high interfacial impedance^[39-40]. The introduction of MOFs not only establishes continuous ion transport pathways but also exploits their open metal sites or specific functional groups (e.g., amino or fluoro groups) to effectively facilitate Li salt dissociation and anion immobilization through Lewis acid-base interactions^[60]. This dual effect concurrently enhances Li⁺ mobility and improves the overall ionic conduction kinetics^[41].

  Research indicates that rationally designed structures can effectively incorporate MOFs into high-performance ionic conduction networks. For instance, Wang et al.^[61] adopted an in-situ growth approach to create continuous three-dimensional ZIF-8 channels inside a polymer matrix (Fig.6a-6d). By utilizing the inherent porosity of MOFs to improve electrolyte infiltration, a continuous ion-permeable pathway was established, yielding a composite electrolyte with an ionic conductivity of 0.46 mS·cm^-1 and raising the Li⁺ transference number to 0.74.

  Figure 6

  

  Figure 6.  (a) Schematic diagram of MOF/polymer composite electrolytes that promote ion transport; (b) SEM image of ZCP; (c) Infrared thermal images of prepared matrices; (d) DFT calculation of the coordination bond length in single LiTFSI and ZIF-8 adsorbed LiTFSI (Copyrighted from Ref.^[61] with a license); (e) Synthetic strategy and structure illustration of Li-IL@UIOF; (f) Lewis acid-base interaction with lithium salt and fast ion channel of Li-IL@UIOF filler; (g) Adsorption energies of TFSI^- on VEC, UIO, and UIOF; (h) Schematic of the mechanism to inhibit the growth of lithium dendrites by incorporating Li-IL@UIOF fillers; (i) Long-term cycling performance at 0.5C of Li|VP20UFI/CL|LFP cells after being subjected to 2C (Copyrighted from Ref.^[62] with a license)

  下载: 全尺寸图片 幻灯片

  Functionalization strategies can further enhance the ion-regulating properties of MOFs. Niu et al.^[62] leveraged the strong electronegativity of fluorinated UiO-66 to trap TFSI^- anions, which facilitated Li salt dissociation and increased the concentration of free Li⁺ (Fig.6e-6i). Similarly, Zhang et al.^[63] synergistically improved anion binding ability and Li⁺ transport efficiency using an iodine-and amino-co-modified MOF (CuBTC-NH-I), achieving ionic conductivities of 5.68×10^-4 and 6.6×10^-4 S·cm^-1, respectively (Fig.7a-7e). These cases collectively illustrate how the combined pore confinement effect and tailored surface chemistry of MOFs create low-resistance pathways for Li⁺ transport.

  Figure 7

  

  Figure 7.  (a) Schematic illustration of CuBTC, CuBTC-NH₂, and CuBTC-NH₂-I₃; (b) Adsorption models of CuBTC-TFSI, CuBTC-NH₂-TFSI, and CuBTC-NH₂-I₃-TFSI; (c) Binding energies of CuBTC, CuBTC-NH₂, and CuBTC-NH₂-I₃ for TFSI^-; (d) Ionic conductivities of CuBTC-PVDF, CuBTC-NH₂-PVDF, and CuBTC-NH₂-I₃-PVDF at 25 ℃; (e) Li plating/stripping cycle curves of Li//Li symmetric cells assembled with CuBTC-PVDF, CuBTC-NH₂-PVDF, and CuBTC-NH₂-I₃-PVDF electrolytes at a current density of 1 mA·cm^-2 (Copyrighted from Ref.^[63] with a license); (f) Pore apertures and pore volumes of Zn-MOF-74, HKUST-1, and MOF-5; (g) Uptake of LiTFSI and total uptake of LiTFSI+DME together in Li-doped MOFs measured by quantitative NMR; (h) Comparison of activation energy and Li⁺ transference number of MOF electrolytes in this work with other reported works (Copyrighted from Ref.^[64] with a license)

  下载: 全尺寸图片 幻灯片

  Moreover, the structural features of MOFs, such as pore size and open metal sites, directly influence their electrochemical performance. Dong et al.^[64] demonstrated that MOFs with larger pores enable high-capacity adsorption of Li salts, while open metal sites (e.g., in Zn-MOF-74) can markedly promote Li salt dissociation, attaining a Li⁺ transference number as high as 0.47 in ionic liquid-based composite systems (Fig.7f-7h).

  In terms of interfacial stability, integrating MOFs (e.g., UiO-66-NH₂) into polymer networks via chemical crosslinking not only constructs continuous Li⁺-enriched conduction channels but also enhances mechanical robustness, inhibits Li dendrite penetration, and helps form a stable electrode/electrolyte interface.

  Therefore, as multifunctional fillers or ion-conducting matrices, MOFs systematically enhance the ionic conductivity and electrochemical stability of solid or quasi-solid electrolytes through various mechanisms. These include constructing continuous conduction pathways, promoting lithium salt dissociation, immobilizing anions, and stabilizing interfaces. This underscores their significant potential for enabling safe, high-performance batteries capable of fast charging.

  2.   Applications of MOFs in key battery components

  Based on the fundamental mechanisms of MOFs in regulating ion transport, stabilizing interfaces, and constructing conductive networks discussed above, research into their application for fast-charging batteries has progressed toward the precise design and performance optimization of key battery components. This section systematically elaborates on the specific application strategies and recent progress of MOFs and their derivatives in core components, including anodes, cathodes, separators, and solid-state electrolytes (Table 1)^[59,65-78]. By analyzing the structure-property relationships between material design and electrochemical performance, it reveals how MOFs can systematically enhance the fast-charging capability, cycling stability, and safety of batteries from an integrated device-level perspective.

  Table 1

  

  Table 1.  Performance comparison of MOFs for fast-charging lithium-ion batteries

  下载: 导出CSV

  Material	Conductivity /(mS·cm-1)	Temperature /℃	$ {t}_{\text{Li}^{+}} $ /(cm2·s-1)a	Initial capacity /(mAh·g-1)	Cyclic performance	Ref.
  10%Co-SIM-1/PAN	2.38	25	0.74	166.3 (5C)	135.2 mAh·g-1 (250th/5C)	[65]
  PI@ZIF-8	2.4	25	0.88	n.d.	97.4% retention rate (300th/2C)	[66]
  Li-IL@HKUST-1/PAN	2.4	25	0.698	71.7 (5C)	67.5 mAh·g-1 (100th/5C)	[67]
  PP@ZIF-67	0.718	25	0.3	142.2 (0.5C)	84.6% retention rate (500th/2C)	[68]
  Si/CoMo@NCP	n.d.b	n.d.	0.44	1 615 (0.1C)	745 mAh·g-1 (400th/1C)	[69]
  MOFs-SN-FEC	0.704	25	n.d.	n.d.	691 mAh·g-1 (500th/1C)	[70]
  MOF808@PAN@PEO-LiTFSI	2.83	30	0.42	136 (0.5C)	102 mAh·g-1 (1 000th/1C)	[59]
  P/Ni@C	0.4	n.d.	n.d.	1 131 (200C)	1 184.6 mAh·g-1 (400th/200 mA·g-1); 579.4 mAh·g-1(2 500th/2C)	[71]
  VN-GC@PDA-C-50	1.6	n.d.	n.d.	1 012 (0.1C)	351 mAh·g-1 (2 200th/2C); 453 mAh·g-1 (1 100th/1C)	[72]
  GZ-62-QSSE	3.32	25	0.74	132.1 (1C)	72.6% retention rate(3 000th/1C)	[73]
  HSiOx@N-GA	0.871	25	0.697	1 363 (0.1C)	86% retention rate, 133.2 mAh·g-1 (500th/10C); 453 mAh·g-1 (1 100th/1C)	[74]
  Co3O4@CNTs	0.508	25	n.d.	1 043.5 (0.1C)	1 037.6 mAh·g-1 (200th/1C); 581 mAh·g-1 (200th/5C)	[75]
  ZIF-8@nylon 6, 6 separators	3.6	25	n.d.	160 (0.2C)	140 mAh·g-1 at 3C	[76]
  SPE2-PI-ZIF8	0.638	25	0.68	135 (0.5C)	95.6% retention rate, 129.1mAh·g-1 (100th/1C)	[77]
  CuS(70wt%)@Cu-BTC	17	30	1.95	1 185 (0.1C)	80% retention rate, 480 mAh·g-1 at 1C	[78]
  a tLi+: lithium ion transference number; b n.d.: not described.

  2.1   Engineering stable anode interfaces

  Under fast-charging conditions, sluggish interfacial kinetics and thermodynamic instability at the anode represent a fundamental bottleneck limiting battery performance^[57]. During high-rate charging, conventional graphite anodes suffer from slow Li⁺ desolvation, which readily triggers metallic lithium plating and unstable SEI growth, leading to capacity degradation and safety risks. MOFs and their derivatives offer innovative solutions for precise anode interface engineering, owing to their structural tunability, high specific surface area, and abundant active sites^[48]. By optimizing ion transport pathways, alleviating electrode strain, and regulating SEI formation, they significantly enhance the reversibility and stability of anodes during high-speed Li insertion/extraction cycles^[79-80].

  As precursors, MOFs can be transformed into functional carbon materials with precisely engineered pore structures, effectively optimizing ion transport pathways and interface stability. Zheng et al.^[81] utilized porous carbon derived from two-dimensional Cu-BDC MOF (Fig.8a). By controlling pyrolysis temperature, they formed abundant mesoporous structures that not only provided efficient transport pathways for Li⁺/K⁺ but also facilitated stable SEI film formation through surface characteristics (Fig.8b). Specifically, C₅₀₀ maintained a capacity of 210.3 mAh·g^-1 after 500 cycles at 5.0 A·g^-1 as a LIB anode. When used for K⁺-ion batteries, C₇₀₀ achieved a capacity retention rate of 71.6% after 500 cycles at 1.0 A·g^-1, demonstrating excellent fast-charging tolerance and interfacial stability (Fig.8c). For high-capacity anode materials like silicon with significant volume expansion, MOF-derived encapsulation structures offer distinct advantages. Ruan et al.^[69] prepared a composite material featuring nitrogen-doped carbon polyhedra encapsulating silicon particles using a cobalt-molybdenum bimetallic MOF precursor (Fig.8d). This structure not only effectively buffered silicon's volumetric expansion rate during cycling to 12.4%, but also its porous framework and bimetallic doping synergistically enhanced electronic conductivity and ionic transport efficiency. This facilitated rapid Li⁺ desolvation and the formation of a stable thin SEI film, enabling the electrode to maintain a capacity of 745 mAh·g^-1 after 400 cycles at 1.0 A·g^-1 (Fig.8e, 8f).

  Figure 8

  

  Figure 8.  (a) Schematic of the formation process of C₅₀₀ and C₇₀₀ from 2D Cu-BDC; (b) SEM images of Cu@C₅₀₀; (c) Cycling performance of two samples at 5.0 A·g^-1 (Copyrighted from Ref.^[81] with a license); (d) Schematic representation of the procedure of synthesis of Si/CoMo@NCP from the feed solution from Si@CoMo-MOF and the final product Si/CoMo@NCP; (e) Charge/ discharge curves of Si/CoMo@NCP electrode at different current densities; (f) Cycling performances of Si/CoMo@NCP and Si/Co@NCP at 1.0 A·g^-1 (Copyrighted from Ref.^[69] with a license)

  下载: 全尺寸图片 幻灯片

  Directly employing MOFs or their derivatives as anode active materials can also significantly improve fast-charging performance through synthetic control and interfacial engineering. Gaber et al.^[82] developed a three-dimensional conjugated MOF material (Fe-Tp) based on ortho-hydroxybenzaldehyde. Via precise interface engineering (Fig.9a), this material effectively addresses the interfacial kinetic limitations of conventional graphite anodes in fast-charging batteries. Fe-Tp possessed a hierarchically porous structure and a high density of lithiophilic sites, which greatly facilitate Li⁺ desolvation and bulk diffusion. It delivered a high specific capacity of 1 447 mAh·g^-1 at 0.1 A·g^-1 and retained 89% of its capacity after 500 cycles at 1.0 A·g^-1 (Fig.9b). Moreover, an anode prepared by compositing 10% Fe-Tp with commercial graphite showed a doubled specific capacity after 400 cycles, with an average Coulombic efficiency approaching 100% (Fig.9c, 9d).

  Figure 9

  

  Figure 9.  (a) Synthetic scheme of Fe-Tp; (b) Specific capacity analysis of MOFite and graphite for 800 cycles at 2.0 A·g^-1; (c) Performance graph of MOFite and graphite at 0th, 400th and 800th cycles; (d) Diagrammatic representation of Li⁺ ion diffusion through the hierarchically porous Fe-Tp and possible sites of interactions (Copyrighted from Ref.^[82] with a license); (e) Hydrothermal synthesis process of CoBPDCA products; (f) SEM and (g) TEM images of CoBPDCA; (h) Cycle stability and the corresponding Coulombic efficiency at 0.2C of CoBPDCA electrode; (i) Long-term cycling performance at 10C of CoBPDCA electrode (Copyrighted from Ref.^[83] with a license)

  下载: 全尺寸图片 幻灯片

  Su et al.^[83] designed and synthesized a novel cobalt-based MOF (CoBPDCA) using cobalt(Ⅱ) nitrate as the metal source and an organic small molecule as a ligand (Fig.9e). SEM revealed that CoBPDCA exhibited a distinct hexagonal-like morphology (Fig.9f), while TEM further confirmed its typical hexagonal structure with side lengths of about 60 nm (Fig.9g). The material possesses dual Li⁺ active centers located on the cobalt cations and the BPDCA ligand (—C=O and —C=N groups), respectively, together with abundant Li⁺ migration pathways, which significantly enhance reversible capacity and reaction kinetics. Electrochemical tests demonstrated that the CoBPDCA electrode delivered a high specific capacity of 1 112.9 mAh·g^-1 at 0.05C (Fig.9h) and exhibited excellent long-term cycling stability (84.5% capacity retention rate after 2 500 cycles at 10C, Fig.9i) as well as outstanding rate capability (184.9 mAh·g^-1 at 10C). Its overall performance was markedly superior to that of the pure BPDCA electrode. Chen et al.^[84] prepared HA₂₀-Mn-MOF anode materials by in-situ hydrothermal compositing of humic acid (HA) with Mn-MOF, offering an innovative solution for optimizing fast-charging battery interfaces (Fig.10a). Utilizing the oxygen-containing functional groups of HA to build a stable interface and form an ultra-thin nanosheet structure, this material enhanced conductivity and shortened ion diffusion paths, achieving a Li⁺ diffusion coefficient of 1.32×10^-12 cm²·s^-1. The interface design promoted Li⁺ desolvation, inhibited Mn²⁺ dissolution and volume expansion (expansion rate of only 8.82%), and facilitated the formation of a stable SEI (Fig.10b, 10c). This material retained a capacity of 657 mAh·g^-1 after 1 000 cycles at 1 A·g^-1 and delivered 197.7 mAh·g^-1 at 10 A·g^-1 (Fig.10d-10f). Thus, in-situ compositing of MOFs enables synergistic optimization of interface components and structure, effectively addressing challenges like Li plating and unstable SEI during fast charging, and provides key technical support for developing high-stability fast-charging anodes.

  Figure 10

  

  Figure 10.  (a) Schematic diagram of the synthesis of Mn-MOF and HA₂₀-Mn-MOF; Cross-sectional SEM images of the electrodes of (b) Mn-MOF and (c) HA₂₀-Mn-MOF before and after 500 cycles at 1 A·g^-1; (d) Nyquist plots of Mn-MOF and HA₂₀-Mn-MOF electrodes after 0, 5, and 35 cycles (inset: equivalent circuit diagram); (e) Electrochemistry diffusion coefficient of Li⁺ in Mn-MOF and HA₂₀-Mn-MOF electrodes during discharge and charge; (f) Cyclic performance of HA, Mn-MOF, and HA₂₀-Mn-MOF electrodes at 0.1 A·g^-1 (Copyrighted from Ref.^[84] with a license)

  下载: 全尺寸图片 幻灯片

  MOF-based materials enhance fast-charging anode performance by establishing conductive networks for rapid ion transport, buffering volume change to inhibit Li plating, and optimizing interfacial structures for SEI stabilization.

  2.2   Enhancing cathode performance and stability

  The cathode materials of LIBs are critical components that determine overall energy density, operating voltage, and cycle life. However, traditional cathodes, such as Li-rich Mn-based oxides or high-nickel materials, often face multiple challenges, including low initial Coulombic efficiency, rapid voltage decay during cycling, dissolution of transition metal ions, and interfacial side reactions. These issues significantly limit their performance in fast-charging applications. MOFs offer promising opportunities to construct high-performance cathodes and optimize electrode/electrolyte interfaces, owing to their high porosity, large specific surface area, tunable redox-active sites, and adaptable surface chemistry^[85].

  MOFs can function as effective coatings or precursors to stabilize cathode structures and mitigate side reactions. Yang et al.^[86] reported a one-dimensional copper-based MOF (DDA-Cu), synthesized from 1,5-diamino-4, 8-dihydroxy-9, 10-anthraquinone ligands and Cu²⁺ ions, and employed it as a cathode material for LIBs. The material contains Cu-O₃N units with π-d conjugated structures, which provide a high density of redox-active sites (Fig.11a). Its distinctive ribbon-like architecture exhibited a specific surface area of 110 m²·g^-1 and microporous channels of 0.92 nm, improving electrolyte wettability and enabling rapid Li⁺ transport (Fig.11b, 11c). Electrochemical tests reveal that the cathode retained 78% of its capacity after 1 000 cycles at a high current density of 2 A·g^-1 (Fig.11d).

  Figure 11

  

  Figure 11.  (a) Synthetic schematic diagram of DDA; (b) N₂ adsorption-desorption isotherm, (c) pore diameter distribution, and (d) electrochemical performance of DDA-Cu as LIBs cathode at 2 A·g^-1 (Copyrighted from Ref.^[86] with a license); (e) Schematic of chelation-type MOF-modified cathodes offering a highly promising passivation strategy for high-performance LIBs by suppressing transition metal cross-interference and enhancing Li⁺ transport; (f) Scheme of decreasing activation energy from desolvation by MOF pore; (g) Li⁺ ion diffusion coefficient of NCM while discharging after cycling process; (h) Cycle test of NCM half-cell at 1C (Copyrighted from Ref.^[87] with a license)

  下载: 全尺寸图片 幻灯片

  To address performance degradation caused by transition metal dissolution and migration from high-nickel cathodes to the anode, Ahn's team innovatively applied chelation-functionalized MOF (MOF-CA) as an additive to NCM cathodes (Fig.11e)^[87]. This MOF-CA layer effectively traps transition metal ions dissolved from the cathode, significantly reducing their deposition at the anode. Furthermore, the pores of the MOF facilitate partial desolvation of Li⁺, while its metal sites can immobilize electrolyte anions. These synergistic effects lower the charge-transfer resistance and increase the Li⁺ diffusion coefficient (Fig.11f). Consequently, the cathode with the MOF-CA additive maintained a discharge capacity of 180.4 mAh·g^-1 after 100 cycles, with a capacity retention rate of 86.6%. After 200 cycles, its capacity (156.5 mAh·g^-1) remained significantly higher than that of the untreated NCM cathode (105.4 mAh·g^-1) (Fig.11g, 11h).

  Additionally, MOFs can be used directly as intrinsically active coating materials. The Shin team pioneered the application of an imidazole-functionalized MOF (i-MOF) as a coating on LiNi_0.9Co_0.085Mn_0.015O₂ (i-NCM), forming a uniform, ultra-thin coating layer (ca. 5 nm) (Fig.12a)^[88]. This coating effectively suppresses microcracking, harmful phase transformations, and interfacial side reactions during cycling, significantly enhancing the structural stability of the cathode material. The i-NCM cathode exhibited an initial discharge capacity of up to 219.70 mAh·g^-1, with capacity retention rates of 71.10% and 46.84% after 100 cycles at 25 and 50 ℃, respectively (Fig.12b, 12c). Another significant approach involves deriving composite cathode materials from MOFs as precursors. Lin et al.^[89] successfully synthesized fluorine-oxygen co-doped carbon-matrix-encapsulated LiFePO₄ (LFP@OFC) via solid-state sintering using Fe-MOF as the precursor (Fig.12d). The carbon matrix derived from MOF not only serves as a structural template and protective layer, facilitating the formation of hierarchical charge diffusion pathways to accelerate reaction kinetics, but also provides additional active sites for Li storage and buffers volumetric stress during charging and discharging. Consequently, the LFP@OFC cathode exhibited a high specific capacity of 169.9 mAh·g^-1 at 0.1C, excellent rate performance (85.6 mAh·g^-1 at 16.2C), and remarkable long-term cycling stability (160.9 mAh·g^-1 after 500 cycles at 1C) (Fig.12e-12i).

  Figure 12

  

  Figure 12.  (a) Synthesis process of i-NCM; (b) Long-term cycling performance over 400 cycles with Coulombic efficiency at 1C and room temperature; (c) SEM images of NCM and i-NCM in the cross-sectional view before and after 100 cycles at room temperature and 50 ℃ (scale bar: 5 μm) (Copyrighted from Ref.^[88] with a license); (d) Illustration of the synthesis procedure for MOF-derived LiFePO₄ microparticles encapsulated in O, F-codoped carbon matrix; (e) Long-term cyclability at 1C of the LFP, LFP@OC, and LFP@OFC electrodes; (f) Rate capability at different current densities; Total and orbital-resolved partial DOS plots of (g) LFP bulk and (h) LFP@OFC (the Fermi levels were set to be 0 eV); (i) Differential charge density distribution of LFP@OFC, where the electronic accumulation is indicated by yellow regions and the electronic depletion is depicted by aquamarine regions (Copyrighted from Ref.^[89] with a license)

  下载: 全尺寸图片 幻灯片

  By serving as multifunctional coatings, active additives, or structural precursors, MOFs effectively enhance the electrochemical performance and structural stability of cathode materials under fast-charging conditions. This is achieved through multiple dimensions, including suppressing transition metal dissolution, stabilizing the interface structure, promoting ion transport, and buffering volumetric strain.

  2.3   Designing functional MOF-based separators

  As a critical component of LIBs, separators not only prevent electrode short circuits but also directly influence the uniformity of Li⁺ transport and the stability of the electrode/electrolyte interface. Traditional polyolefin separators suffer from low ionic conductivity, poor electrolyte wettability, and insufficient thermal stability. These shortcomings can easily lead to uneven ion migration, aggravated concentration polarization, and consequently, induce non-uniform Li deposition and dendrite growth. To overcome this bottleneck, functionalized separators based on MOFs have emerged as a significant research direction. Leveraging their tunable nanochannels, high specific surface area, and rich surface chemistry, MOFs can significantly enhance the ion-sieving capability, electrolyte affinity, and thermomechanical stability of separators, thereby optimizing the fast-charging performance and safety window of the battery^[65,90].

  Incorporating MOFs into polymers is an effective strategy to enhance the overall performance of separators. Huang et al.^[91] fabricated a ZIF-8/PAN composite separator via electrospinning. Its high porosity and excellent electrolyte wettability synergistically promoted rapid ion transport through the electrolyte-filled membrane, achieving a high Li⁺ transference number of 0.68 and an ionic conductivity of 2.11 mS·cm^-1 (Fig.13a). This effectively suppressed Li dendrite growth, enabling the matched battery to maintain a capacity of 104 mAh·g^-1 after 2 000 cycles at a high rate of 5C (Fig.13b-13d). Similarly, an electrospun composite separator constructed from Co-SIM-1/PAN featured a three-dimensional nanofiber network and a high porosity of up to 85%^[65]. This structure led to an electrolyte uptake of 794%, far surpassing that of commercial PP separators (Fig.13e). The unsaturated metal sites in the MOF could immobilize anions, raising the Li⁺ transference number to 0.74 and significantly suppressing concentration polarization (Fig.13f). As a result, symmetric cells using this separator remained stable for over 1 000 h at 5 mA·cm^-2. This separator also exhibited a broad electrochemical window of 5.2 V and excellent thermal stability. When paired with an NCM811 cathode, it maintained 81.3% capacity retention rate after 250 cycles at 5C (Fig.13g, 13h).

  Figure 13

  

  Figure 13.  (a) TGA curves of PAN, ZIF-8, and ZIF-8/PAN fiber composite membranes; (b) Thermal stability tests of commercialized Celgard 2400 separator, PAN nanofiber membrane, and ZIF-8/PAN fiber composite membrane; (c) Rate performance and (d) cycle performance at 5C of LiFePO₄-Li cells with the ZIF-8/PAN composite fibrous separator (Copyrighted from Ref.^[91] with a license); (e) Thermal shrinkage of the PP, PAN, and MOF/PAN membranes; (f) Ionic conduction process and anion adsorption process of the MOF in the Co-SIM-1/PAN separator; (g) Rate performance of the NCM811||separator||Li batteries with different separators; (h) Charge/discharge cycling and Columbic efficiency of the NCM811||separator||Li batteries with different separators at 5C (Copyrighted from Ref.^[65] with a license)

  下载: 全尺寸图片 幻灯片

  These results collectively confirm that this MOF-based separator effectively enhances ion transport uniformity and interfacial stability. To further enhance ion transport and mechanical properties, multiscale MOF network structures were incorporated into the separator design. Lan et al.^[66] reported a PI@ZIF-8 nanofiber separator constructed via electrospinning-assisted in-situ self-assembly, forming a three-dimensional multiscale MOF network (Fig.14a). The synergistic effect between the sub-nanochannels and Lewis acid sites of ZIF-8 created an efficient ion-sieving network. This endowed the separator with a remarkably high Li⁺ transference number of 0.88, an ionic conductivity of 2.40 mS·cm^-1, and an exceptional electrolyte uptake of 1 298% (Fig. 14b, 14c). The separator exhibited negligible thermal shrinkage below 280 ℃ while maintaining good mechanical strength and flexibility (Fig.14d). A Li||Li symmetric cell using this separator demonstrated stable cycling for 2 000 h. Furthermore, an assembled LFP||Li full cell achieved a high capacity retention of 94.5% after 250 cycles, fully confirming its outstanding efficacy in homogenizing ion flux and stabilizing interfaces (Fig. 14e, 14f).

  Figure 14

  

  Figure 14.  (a) Schematic diagram for the detailed fabrication procedures of PI@ZIF-8 nanofiber separators; (b) Current-time curves and the relevant Nyquist plots of PI@ZIF-8 nanofiber separators in symmetric Li-Li cells; (c) Electrolyte uptakes of PE, PI, and PI@ZIF-8; (d) Thermal shrinkage photographs of the three separators from 100 to 200 ℃; (e) Cycling performance of Li‖Li cells at a current density of 1.0 mA·cm^-2 with an area capacity of 1.0 mAh·cm^-2; (f) Cycling performance of NCM811‖Li cell at 0.5C (Copyrighted from Ref.^[66] with a license); (g) Mechanism of action of the separator inside the cell; (h) 200-cycle charge/discharge cycle curves of the LiFePO₄ half-cells assembled with PP, OPBI, OPBI@M-H5, and OPBI@M-H10 separators (Copyrighted from Ref.^[92] with a license)

  下载: 全尺寸图片 幻灯片

  Beyond enhancing ion transport kinetics, MOF-functionalized separators also exhibit unique advantages in improving battery thermal safety. A notable example is the OPBI@M-H10 composite separator developed by Zhou et al.^[92], which exhibited significantly superior high-temperature resistance compared to traditional separators (Fig.14g). This separator maintained its original shape at 200 ℃ and retained 80.03% of its weight at 650 ℃, whereas a conventional PP separator underwent severe shrinkage at 150 ℃. In high-temperature cycling tests at 90 ℃, a LiFePO₄ half-cell using this separator retained 76.18% of its capacity after 100 cycles, far outperforming the 18.39% retention of the cell with a PP separator (Fig.14h). This excellent thermal stability originates from the synergistic effect between the MOF and other nanomaterials (such as halloysite nanotubes), providing an effective material solution for mitigating thermal accumulation and runaway risks under demanding conditions like fast charging.

  By constructing a highly porous conductive network, introducing ion-selective sites, and enhancing thermomechanical stability, MOF-functionalized separators simultaneously address multiple limitations of conventional separators, including low ionic conductivity, poor wettability, and elevated thermal safety risks.

  2.4   Constructing solid-state electrolytes and ideal interfaces

  With increasing demands for battery safety, solid-state batteries are regarded as a crucial direction for next-generation energy storage technologies. However, their development faces a core challenge of poor solid-solid interfacial contact between the electrode and the solid-state electrolyte, leading to high interfacial impedance and sluggish ion transport^[93-94]. MOF materials, with their highly tunable pore structures, high specific surface area, and versatile surface chemistry, offer innovative material solutions for optimizing interfacial contact and ion transport in solid-state batteries^[95-97]. MOFs are primarily applied in solid-state electrolyte systems through three approaches. Firstly, incorporating MOFs as functional fillers into polymer matrices can significantly enhance the overall performance of composite electrolytes. Zhang et al.^[63] added amino-iodine co-modified CuBTC-NH₂-I₃ MOF as a filler to PVDF-HFP polymer (Fig.15a). The —NH₂ groups effectively promoted LiTFSI dissociation (free TFSI^- reached 82.56%), while iodine groups modulated the local electron distribution. Their synergistic effect increased the room-temperature ionic conductivity of the composite electrolyte to 6.6×10^-4 S·cm^-1 and raised the Li⁺ transference number to 0.94, far surpassing the unmodified control group (Fig.15b-15d). A LiFePO₄||Li battery assembled with this electrolyte exhibited a capacity retention close to 100% after 400 cycles at a 2C rate, demonstrating excellent long-term cycling stability (Fig.15e). Secondly, MOFs can serve as self-supporting solid-state electrolyte membranes. Xiong et al.^[98] synthesized a Cu-TTBT MOF featuring ordered one-dimensional channels with a central pore diameter of approximately 0.63 nm. This material achieved ion conduction without any polymer support, exhibiting an ionic conductivity of 1.83×10^-4 S·cm^-1 at 298 K and a Li⁺ transference number of 0.67 (Fig.15f, 15g). A LiFePO₄|SSEs|Li battery assembled with this membrane retained 96% of its capacity after 200 cycles at a 1.0C rate (Fig.15h). The material also demonstrated similarly high performance in sodium-ion systems, confirming its versatility as a standalone electrolyte membrane.

  Figure 15

  

  Figure 15.  (a) Schematic illustration of the preparation of CuBTC-NH₂-I₃-PVDF; (b) Ionic conductivities of CuBTC-PVDF, CuBTC-NH₂-PVDF, and CuBTC-NH₂-I₃-PVDF at 25 ℃; (c) Ion mobility numbers of CuBTC-PVDF, CuBTC-NH₂-PVDF, and CuBTC-NH₂-I₃-PVDF; (d) Raman spectra of CuBTC-NH₂-I₃-PVDF and the corresponding quantification results of the TFSI^- anion states; (e) Cycling stabilities of the LiFePO₄||Li solid-state batteries at 2C (Copyrighted from Ref.^[63] with a license); (f) Ionic conductivities of Cu-TTBT-X (X=Li, Na, and Mg); (g) t_Li⁺ of Cu-TTBT-Li; (h) Cycling performance of the LMB (Copyrighted from Ref.^[98] with a license)

  下载: 全尺寸图片 幻灯片

  Addressing the common challenges of low ionic conductivity and high interfacial resistance in MOF-based solid-state electrolytes, Zhou et al.^[99] demonstrated the potential of MOF materials as functional interlayers for optimizing solid-solid interface contact (Fig.16a, 16b). To address the issues of high interfacial resistance and uneven lithium-ion transport between electrodes and solid-state electrolytes, they designed a polymer-composite electrolyte based on a three-dimensional cross-linked MOF. In this system, the MOF component-featuring imidazole sites with strong cationic character-effectively traps anions from the electrolyte, thereby promoting uniform Li⁺ migration across the interface and raising the Li⁺ transference number to 0.54 (Fig.16c). Simultaneously, the 3D network constructed by the MOF not only provides continuous transport pathways for Li⁺ but also enhances mechanical strength, helping to maintain the physical stability of the interface and suppress lithium-dendrite penetration. When assembled into a Li/LiFePO₄ full cell, this material exhibited excellent cycling stability and rate capability, confirming its effectiveness in reducing interfacial resistance and improving interfacial contact (Fig.16d, 16e). This work offers a practical strategy for utilizing MOFs as interface modifiers to enhance ion transport and stability at solid-solid interfaces in solid-state batteries.

  Figure 16

  

  Figure 16.  (a) Main chemicals for the synthesis of cross-linked polymers; (b) Temperature dependence of ionic conductivity for MCPEs; (c) Current-time curves of DC polarization and Nyquist plots (inset) before and after polarization of P-PETEA-MOF; (d) Rate capability of Li/P-PETEA-MOF/LiFePO₄ battery from 0.05C to 3C; (e) Cycling performance of Li/P-PETEA-MOF/LiFePO₄ battery at 1C (Copyrighted from Ref.^[99] with a license); (f) Chronoamperometric curve and EIS of PDMML before and after polarization; (g) Cycling performance of LFP|PDMML|Li full cell at a current density of 1.0C; (h) Charge/discharge profiles of the cell (Copyrighted from Ref.^[100] with a license)

  下载: 全尺寸图片 幻灯片

  The ion conduction mechanism in MOF-based solid-state electrolytes primarily relies on continuous transport through their internally ordered pore channels, ion hopping migration at interfaces, and transport via defects or grain boundaries. By precisely engineering the pore size, surface functional groups (such as introducing Lewis acid sites), and topological structure of MOFs, these transport pathways can be optimized. This approach enhances ionic conductivity while increasing the Li⁺ transference number and strengthening mechanical integrity to suppress dendrite formation. In the MOF-808-SLi composite electrolyte studied by Luo et al.^[100], the Zr⁴⁺ Lewis acid sites exhibited strong coordination with TFSI^- anions, effectively immobilizing the anions and leading to a Li⁺ transference number as high as 0.77. Correspondingly, the Li metal surface remained smooth after symmetric cell cycling, and the LiFePO₄//Li full cell exhibited stable cycling at 1C without capacity drop, fully validating its dendrite growth inhibition and interfacial stabilization effects (Fig.16f-16h).

  MOFs, serving as high-performance fillers, standalone electrolyte membranes, or interfacial modification layers, can systematically address critical interface challenges in solid-state batteries by reducing interfacial impedance, enhancing ionic conductivity and migration number, and mechanically suppressing dendrite growth.

  3.   Future directions and challenges for MOF-based fast-charging batteries

  3.1   Current technical challenges

  MOFs hold transformative potential for advancing fast-charging battery technology. Integrating advanced techniques is crucial for enhancing the electrochemical performance of next-generation MOF-based fast-charging batteries. Despite their renowned high activity and stability, MOF materials remain an emerging research field and face several significant challenges for practical application:

  (1) Scalability challenges for industrial energy storage applications: the commercialization of MOF materials continues to face scalability limitations due to economic constraints and underdeveloped supply chains, hindering their practical adoption in energy storage systems. Typical MOF synthesis routes depend on costly organic ligands and multi-step procedures, often accompanied by prolonged reaction times that elevate production expenses. Furthermore, comprehensive evaluation frameworks for assessing critical fast-charging properties that include structural integrity and ion-transport dynamics remain insufficiently established, demanding further experimental and computational validation before scalable manufacturing becomes feasible. While certain MOF architectures can now be controllably synthesized, and their corresponding electrodes demonstrate promising electrochemical behavior, the absence of affordable, sustainable precursor alternatives and streamlined synthetic protocols limits their suitability for mass-produced fast-charging batteries.

  (2) Electrochemical stability concerns in fast-charging operations: Repeated high-rate cycling subjects electrode materials to severe ionic fluxes and complex electrochemical stress, imposing stringent durability requirements on MOF frameworks. Although the inherent porosity and mechanical resilience of MOFs could theoretically enhance stability, many MOF materials undergo gradual degradation, phase changes, or pore collapse during extended cycling. Such deterioration not only reduces the accessible surface area and compromises pore functionality but also promotes electrode swelling and disrupts the solid-electrolyte interphase. These effects collectively accelerate capacity fade and limit cycle life, directly relating to the fundamental fast-charging issues of interfacial instability and electrode expansion highlighted in the abstract.

  (3) Inherently low conductivity as a rate-limiting factor: efficient electron and ion mobility is essential for high-power battery electrodes, yet most MOFs exhibit poor intrinsic electronic conductivity, which restricts charge transfer kinetics and rate performance under fast-charging conditions. Common approaches to enhance conductivity involve blending MOFs with conductive additives (e.g., carbon materials) to form hybrid composites. However, the weak interfacial interactions in such mixtures often lead to insufficient electronic coupling and inefficient charge percolation pathways. Moreover, physical blending can partially block the ordered porous network of MOFs, counteracting their innate ability to facilitate rapid ion diffusion. Thus, achieving high electronic conductivity without sacrificing structural integrity and ion-accessibility remains a pivotal research challenge for MOF-based fast-charging electrodes.

  Advancing MOF materials for fast-charging batteries requires targeted strategies that address the fundamental limitations currently faced by high-power lithium-ion systems. By refining MOF composition, tailoring pore architecture, engineering stable interfaces, and developing cost-effective scale-up routes, the above hurdles can be systematically overcome. Such efforts would enable MOFs to fully exploit their unique structural attributes in mitigating key degradation modes, including lithium dendrite formation, particle fracture, and interfacial degradation, thereby paving the way for their integration into next-generation fast-charging energy.

  3.2   Future development directions and outlook

  To address existing challenges, future research and development of MOFs in fast-charging batteries may focus on the following cutting-edge directions:

  (1) Multifunctional collaborative design for targeted solutions: future developments call for an integrated multifunctional design of MOF materials that collectively address the essential requirements of rapid ion transport, efficient electron conduction, interfacial stabilization, and suppression of lithium dendrite formation. For instance, precisely embedding lithophilic sites or ion-conductive dopants within the MOF pores could leverage their ordered channel structure for selective ion sieving and fast transport while simultaneously inhibiting dendritic lithium growth. Meanwhile, constructing continuous conductive networks through in-situ polymerization or chemical bonding with conductive components would improve electron transport efficiency, enhance structural stability, and alleviate electrode swelling. The key lies in achieving synergistic effects between the inherent advantages of MOFs and functional additives, ensuring that enhanced conductivity and stability do not compromise their high surface area and tunable porosity.

  (2) Green and scalable synthesis to support industrialization: to overcome the high cost, complex processing, and environmental concerns associated with MOF synthesis, future efforts should prioritize developing green and sustainable fabrication routes. This includes adopting aqueous-phase synthesis, mechanochemical methods, and microwave-or ultrasound-assisted processes to shorten synthesis times and reduce energy consumption. In parallel, exploring low-cost and readily available ligand and metal sources will help diminish reliance on precious metals and expensive organic linkers. Coupled with theoretical simulations and advanced characterization, establishing clear structure-property-performance relationships will provide a rational basis for designing cost-effective, high-performance MOFs and accelerate their scalable production and supply chain maturation.

  (3) Integration of machine learning and advanced characterization for accelerated development: the use of machine learning and high-throughput computational screening can rapidly predict MOF composition, structure, and key electrochemical properties such as stability and ionic conductivity, substantially shortening the material discovery cycle. Complemented with in-situ characterization techniques, such as XRD and TEM under operating conditions, this approach can enable deep insights into structural evolution, interfacial processes, and lithium dendrite dynamics during fast-charging cycles. Such an integrated approach will shift MOF-based material development from trial-and-error experimentation toward rational design, allowing precise structural and performance optimization and expediting the realization of high-performance materials for fast-charging batteries.

  Overall, MOF research for fast-charging batteries remains in a rapid development phase, facing multiple challenges from material design to large-scale production. This review systematically outlines the mechanisms and applications of MOFs in ion sieving, interfacial regulation, and electrolyte enhancement, summarizes current technical bottlenecks, and explores potential future development pathways. Through interdisciplinary collaboration and deep integration of industry, academia, and research, it is anticipated that MOF materials with high ionic conductivity, excellent stability, and low cost can be scaled up for mass production and application. This will lay a solid material foundation for constructing next-generation high-performance, high-safety fast-charging battery systems.

  
  
• 1. [1]

     HOLECHEK J L, GELI H M E, SAWALHAH M N, VALDEZ R. A global assessment: can renewable energy replace fossil fuels by 2050?[J]. Sustainability, 2022, 14(8): 4792 doi: 10.3390/su14084792

  2. [2]

     YANG M, PANG M Y, ZHANG H H, AN J, WANG Z F, YE J J, KONG Z, DU Y Y, QU J Y, LI C X, SONG J B. Synthesis strategies, characterization techniques, and prospects of defect-engineered single-atom catalysts for electrocatalysis[J]. Fuel, 2026, 407: 137384 doi: 10.1016/j.fuel.2025.137384

  3. [3]

     LV T T, ZHU G Y, DONG S Y, KONG Q Q, PENG Y, JIANG S, ZHANG G X, YANG Z L, YANG S Y, DONG X C, PANG H, ZHANG Y Z. Co-intercalation of dual charge carriers in metal-ion-confining layered vanadium oxide nanobelts for aqueous zinc-ion batteries[J]. Angew. Chem.‒Int. Edit., 2023, 62(5): e202216089 doi: 10.1002/anie.202216089

  4. [4]

     WILLIAMS J H, DEBENEDICTIS A, GHANADAN R, MAHONE A, MOORE J, MORROW W R, PRICE S, TORN M S. The technology path to deep greenhouse gas emissions cuts by 2050: The pivotal role of electricity[J]. Science, 2012, 335(6064): 53-59 doi: 10.1126/science.1208365

  5. [5]

     AN J, ZHANG H H, WANG Y J, KONG Z, LI W S, GAO X, SONG J B, YAO Y C. Application and prospects of interface engineering in energy storage and conversion of graphdiyne-based materials[J]. EcoEnergy, 2025, 3(1): 77-104 doi: 10.1002/ece2.76

  6. [6]

     LIU C L, BAI Y, LI W T, YANG F Y, ZHANG G, X, PANG H. In situ growth of three-dimensional MXene/metal-organic framework composites for high-performance supercapacitors[J]. Angew. Chem.‒Int. Edit., 2022, 61(11): e202116282 doi: 10.1002/anie.202116282

  7. [7]

     CHEN T T, WANG F F, CAO S, BAI Y, ZHENG S S, LI W T, ZHANG S T, HU S X, PANG H. In situ synthesis of MOF-74 family for high areal energy density of aqueous nickel-zinc batteries[J]. Adv. Mater., 2022, 34(30): 2201779 doi: 10.1002/adma.202201779

  8. [8]

     BAI Y, LIU C L, CHEN T T, LI W T, ZHENG S S, PI Y C, LUO Y S, PANG H. MXene-copper/ccobalt hhybrids via Lewis acidic molten salts etching for high performance symmetric supercapacitors[J]. Angew. Chem.‒Int. Edit., 2021, 60(48): 25318-25322 doi: 10.1002/anie.202112381

  9. [9]

     LIN S N, ZHANG T G. NiCo-MOFs porous nanomaterials prepared by different organic frameworks as anodes for Li-ion batteries[J]. J. Energy Storage, 2023, 72: 108492 doi: 10.1016/j.est.2023.108492

  10. [10]

      CHENG H, SHAPTER J G, LI Y Y, GAO G. Recent progress of advanced anode materials of lithium-ion batteries[J]. J. Energy Chem., 2021, 57: 451-468 doi: 10.1016/j.jechem.2020.08.056

  11. [11]

      GENG J R, NI Y X, ZHU Z, WU Q, GAO S N, HUA W B, INDRIS S, CHEN J, LI F. Reversible metal and ligand redox chemistry in two-dimensional iron-organic framework for sustainable lithium-ion batteries[J]. J. Am. Chem. Soc., 2023, 145(3): 1564-1571 doi: 10.1021/jacs.2c08273

  12. [12]

      WANG R, WANG L, LIU R, LI, X Y, WU Y Z, RAN F. "Fast-charging" anode materials for lithium-ion batteries from perspective of ion diffusion in crystal structure[J]. ACS Nano, 2024, 18(4): 2611-2648 doi: 10.1021/acsnano.3c08712

  13. [13]

      ZHAO F S, WANG J, JIANG T Y, SI Y L, ZHU X Y, ZHANG S T, LI K, MENG W J, ZHANG H M, CAO G P, MING H, ZHANG W F, QIU J Y. Internal resistance reduction strategies for high-power and fast-charging lithium-ion batteries[J]. Mater. Sci. Eng. R‒Rep., 2025, 166: 101076 doi: 10.1016/j.mser.2025.101076

  14. [14]

      LI J W, GUO C Y, TAO L J, MENG J S, XU X M, LIU F, WANG X P. Electrode and electrolyte design strategies toward fast-charging lithium-ion batteries[J]. Adv. Funct. Mater., 2024, 34(49): 2409097 doi: 10.1002/adfm.202409097

  15. [15]

      ZENG Q H, DONG Y T, CHEN Y M, YUE X Y, LIANG Z. Recent advancements and perspectives of fast-charging composite anodes for lithium-ion batteries[J]. Sci. China Chem., 2024, 67(12): 3952-3963 doi: 10.1007/s11426-024-2265-9

  16. [16]

      WANG R, LI Y, LI G Y, FU Y H, WU Y Z, RAN F. "Fast-charging" mechanism of Li₃VO₄ from the perspective of material science for lithium-ion battery[J]. Chem. Eng. J., 2024, 498: 155371 doi: 10.1016/j.cej.2024.155371

  17. [17]

      KANG S, MA G, LIU Y X, WANG D M, ZHANG Y, LI J J, XU C, LI Y F. Progress in fast-charging graphite anodes for lithium-ion batteries: reaction kinetics[J]. Energy Storage Mater., 2025, 81: 104531 doi: 10.1016/j.ensm.2025.104531

  18. [18]

      ZHU X T, CAO B, YAN C, TANG C, CHEN A B, ZHANG Q. Advances in coating strategies for graphite anodes in lithium-ion batteries[J]. Acta Phys.‒Chim. Sin., 2025, 41(9): 100096 doi: 10.1016/j.actphy.2025.100096

  19. [19]

      DONG Y, LIU C, RUI M X, ZHANG X Y, GUAN Y B, CHEN L, HUANG Q, WANG M, SU Y F, WU F, LI N. Review on graphite anodes for fast-charging lithium-ion batteries: Mechanism, modification and characterizations[J]. Adv. Funct. Mater., 2025, 35(45): 2506190 doi: 10.1002/adfm.202506190

  20. [20]

      MA D, KIM D H, YU M CHO Y E, KIM H S. Porous silicon layer overlaid graphite anode materials for fast-charging of lithium-ion batteries[J]. J. Power Sources, 2025, 645: 237199 doi: 10.1016/j.jpowsour.2025.237199

  21. [21]

      ZHAO H L, ZUO H B, WANG J X, JIAO S Q. Practical application of graphite in lithium-ion batteries: Modification, composite, and sustainable recycling[J]. J. Energy Storage, 2024, 98: 113125 doi: 10.1016/j.est.2024.113125

  22. [22]

      MATSUO Y, FUMITA K, FUKUTSUKA T, SUGIE Y, KOYAMA H, INOUE K. Butyrolactone derivatives as electrolyte additives for lithium-ion batteries with graphite anodes[J]. J. Power Sources, 2003, 119-121: 373-377 doi: 10.1016/S0378-7753(03)00271-4

  23. [23]

      QUAN Z H, LU A B, WANG F, LIU Z D, WANG S, ZHOU Y D, ZHANG C Z, YE C, LIU J S, TAN J. Soft carbon filled in expanded graphite layer pores for superior fast-charging lithium-ion batteries[J]. Carbon, 2024, 229: 119500 doi: 10.1016/j.carbon.2024.119500

  24. [24]

      ZHANG H H, PANG M Y, YANG M, KONG Z, YE J J, SUN C Y, HE W, LI W S, PAK Y L, AN J, GAO X, SONG J B. Constructing three-dimensional porous SnS₂/RGO as superior-rate and long-life anodes for lithium-ion batteries[J]. Langmuir, 2025, 41(1): 876-884 doi: 10.1021/acs.langmuir.4c04214

  25. [25]

      ZHENG S S, SUN Y, XUE H G, BRAUNSTEIN P, HUANG W, PANG H. Dual-ligand and hard-soft-acid-base strategies to optimize metal-organic framework nanocrystals for stable electrochemical cycling performance[J]. Natl. Sci Rev., 2022, 9(7): nwab197 doi: 10.1093/nsr/nwab197

  26. [26]

      TANG J Y, WANG D H, QIN W, FANG S Y, XU T, HUANG J M, TANG M, WANG Z B. In-situ solvent-free preparation of MOF/polymer composite electrolytes with highly dispersed and defected MOF nanoparticles for lithium-metal batteries[J]. Chem. Eng. J., 2025, 513: 163082 doi: 10.1016/j.cej.2025.163082

  27. [27]

      NIU Y W, WANG Y H, ZHANG H J. MOF in catalysis, sensing and energy storage applications[J]. Nano Energy, 2026, 147: 111598 doi: 10.1016/j.nanoen.2025.111598

  28. [28]

      ZHENG H Q, ZHANG Y N, LIU L F, WAN W, GUO P, NYSTRÖM A M, ZOU X D. One-pot synthesis of metal-organic frameworks with encapsulated target molecules and their applications for controlled drug delivery[J]. J. Am. Chem. Soc., 2016, 138(3): 962-968 doi: 10.1021/jacs.5b11720

  29. [29]

      TEPLENSKY M H, FANTHAM M, POUDEL C, HOCKINGS C, LU M, GUNA A, ARAGONES-ANGLADA M, MOGHADAM P Z, LI P, FARHA O K, FERNÁNDEZ S B D, RICHARDS F M, JODRELL D I, SCHIERLE G K, KAMINSKI C F, FAIREN-JIMENEZ D. A highly porous metal-organic framework system to deliver payloads for gene knockdown[J]. Chem, 2019, 5(11): 2926-2941 doi: 10.1016/j.chempr.2019.08.015

  30. [30]

      HOU C C, XU Q. Metal-organic frameworks for energy[J]. Adv. Energy Mater., 2019, 9(23): 1801307 doi: 10.1002/aenm.201801307

  31. [31]

      LI Z Q, GE X L, LI C X, DONG S H, TANG R, WANG C X, ZHANG Z W, YIN L W. Rational microstructure design on metal-organic framework composites for better electrochemical performances: Design principle, synthetic strategy, and promotion mechanism[J]. Small Methods, 2020, 4(3): 1900756 doi: 10.1002/smtd.201900756

  32. [32]

      YANG H Z, LI X K, TIAN L Y, LIU J G, LI Z S, WANG Y, ZOU, Z G. Boosting photocatalytic performance of MOF-on-MOF heterostructures by constructing rigid charge channels[J]. Small, 2025, 22(2): e10060

  33. [33]

      JIANG H Q, LIU X C, WU Y S, SHU Y F, GONG X, KE F S, DENG H X. Metal-organic frameworks for high charge-discharge rates in lithium-sulfur batteries[J]. Angew. Chem.‒Int. Edit. 2018, 57(15): 3916-3921 doi: 10.1002/anie.201712872

  34. [34]

      SAMMAWIPAWEKUL N, KAEOSAMUT N, AUTTHAWONG T, WATWIANGKHAM A, SUTHIRAKUN S, WANNAPAIBOON S, MAHAMAI N, SARAKONSRI T, CHIMUPALA Y, YIMKLAN S. Isostructural dual-ligand-based MOFs with different metal centers in response to diverse capacity lithium-ion battery anode[J]. Chem. Eng. J., 2024, 482: 148904 doi: 10.1016/j.cej.2024.148904

  35. [35]

      HU Q, HAN G G, WANG A P, GAO K D, LIAO J Y, DING M L, ZHOU Y C, DOMINKO R, WANG H T, YAO J F. Functionalized MOF enables stable cycling of nickel-rich layered oxides for lithium-ion batteries[J]. Chem. Eng. J. 2024, 497: 154608 doi: 10.1016/j.cej.2024.154608

  36. [36]

      MWIZERWA J P, LI J, NSENGIYUMVA W, LI C, XU K, RASAKI S A, LIU C. Thick 3D-printed hierarchical Li₄Ti₅O₁₂@MOF anode and grid-lined micropores for high-performance lithium-ion batteries[J]. J. Colloid Interface Sci., 2025, 696: 137883 doi: 10.1016/j.jcis.2025.137883

  37. [37]

      LIU M W, LI A, LIN H A, LI Z J, WANG L, DENG Y R, WANG Y F, LIU R P, HE X M. Architectural engineering of metal-organic frameworks in lithium-ion batteries: Multifunctional roles, challenges, and future perspectives[J]. Nano Energy, 2025, 143: 111310 doi: 10.1016/j.nanoen.2025.111310

  38. [38]

      YANG J C, LIU Q, SONG Z X, LIU Z H, WANG K H, HAO J H, WANG X, XU L F, WANG Z Z, SHEN B X. Research progress in the application of metal-organic framework materials as anodes for lithium-ion batteries[J]. Coord. Chem. Rev. 2026, 549: 217343 doi: 10.1016/j.ccr.2025.217343

  39. [39]

      LUO B Q, WANG Z R, ZHU X T, LI J Y, YANG H X, GUO B, WANG K. Linker fluorinated metal-organic frameworks enhancing ion conduction for fast-charging lithium metal batteries[J]. J. Energy Chem., 2026, 113: 749-760 doi: 10.1016/j.jechem.2025.09.063

  40. [40]

      LI L C, JIANG G S, WANG K, YANG A P, CAO T F, KONG O, LI J J, ZHU J P, ZHENG J G, SUN C G, LI L X, XU F, AN B G. Engineering electronic inductive effect of linker in metal-organic framework glass toward fast-charging and stable-cycling quasi-solid-state lithium metal batteries[J]. Adv. Funct. Mater., 2025, 35(46): 2505700 doi: 10.1002/adfm.202505700

  41. [41]

      WANG Z R, XU Z, MU Y B, SLATER B, LI J Y, ZENG L, GUO B, WANG K. Defect-tailoring metal-organic frameworks for highly fast-charging quasi-solid-state electrolytes lithium metal batteries[J]. ACS Appl. Mater. Interfaces, 2025, 17(17): 25223-25236 doi: 10.1021/acsami.4c22902

  42. [42]

      CHENG L, ZHANG Y X, LI D D, LI R, OUYANG H, HE H G, CHEN S, ZHENG S Y, LI H. Cu-MOF functionalized hydroxyapatite/bacterial cellulose composite separator enabling dendrite-free fast charging and enhanced thermal safety for high-loading graphite anode[J]. Adv. Funct. Mater., 2025, 36(3): e15523

  43. [43]

      XIANG J H, LI M J, LI M R, HUANG L Z, LIU S C, LIANG J H, DU L, CUI Z M, SONG H Y, LIANG Z X. Durable 4.5 V sodium metal batteries stabilized by negatively charged metal-organic frameworks in gel polymer electrolyte[J]. J. Energy Chem., 2025, 111: 886-895 doi: 10.1016/j.jechem.2025.07.089

  44. [44]

      MA Y T, QIU Y, YANG K, LV S, LI Y H, AN X F, XIAO G Y, HAN Z, MA Y T, CHEN L K, ZHANG D F, LV W, TIAN Y, HOU T Z, LIU M, ZHOU Z, KANG F Y, HE Y B. Competitive Li-ion coordination for constructing a three-dimensional transport network to achieve ultra-high ionic conductivity of a composite solid-state electrolyte[J]. Energy Environ. Sci., 2024, 17(21): 8274-8283 doi: 10.1039/D4EE03134B

  45. [45]

      XU Z, WANG Z R, LI J Y, ZHU X T, REN H X, GUO B, WANG K. Engineering 3D lattice oxygen metal-organic frameworks for fast-charging quasi-solid-state lithium metal batteries[J]. Small, 2025, 21(29): 2501103 doi: 10.1002/smll.202501103

  46. [46]

      YANG Z H, WENG C C, GAO X Y, MENG F Y, JI Y Y, LI J B, LU T, LI J L, WANG J C, PAN L K. In situ construction of Sn-based metal-organic frameworks on MXene achieving fast electron transfer for rapid lithium storage[J]. Chem. Eng. J., 2024, 486: 150299 doi: 10.1016/j.cej.2024.150299

  47. [47]

      HAN X, WU T T, GU L H, CHEN M F, SONG J Z, TIAN D, CHEN J Z. Li-MOF-based ions regulator enabling fast-charging and dendrite-free lithium metal anode[J]. Chin. Chem. Lett., 2023, 34(2): 107594 doi: 10.1016/j.cclet.2022.06.017

  48. [48]

      XU L Q, XIAO X H, TU H Y, ZHU F J, WANG J, LIU H X, HUANG W Y, DENG W T, HOU H S, LIU T C, JI X B, AMINE K, ZOU G Q. Engineering functionalized 2D metal-organic frameworks nanosheets with fast Li⁺ conduction for advanced solid Li batteries[J]. Adv. Mater., 2023, 35(38): 2303193 doi: 10.1002/adma.202303193

  49. [49]

      ZHANG Y J, SUN S, WANG M, LUO X, JIA Z H, PENG J Y, CONG S Z, HE T, PANG H. Rationally engineered metal-organic framework membrane structure for effective Mg²⁺/Li⁺ separation[J]. Chem. Eng. J., 2025, 525: 170104 doi: 10.1016/j.cej.2025.170104

  50. [50]

      ZHAO X D, ZHANG X Y, XING X X, BIAN F L, GAO X L, LIU B S, SONG S F, ZHANG Y Z, HUANG H L. Constructing angstrom-level ion pocket array in 1D channel wall for efficient lithium ion sieving[J]. Adv. Funct. Mater., 2025, 35(10): 2416628 doi: 10.1002/adfm.202416628

  51. [51]

      CAO H Y, XIA Y, LU Y Q, WU Y L, XIA Y S, HOU X X, WANG Y X, LIU G P, HUANG K, XU Z. MOF-801 polycrystalline membrane with sub-10 nm polymeric assembly layer for ion sieving and flow battery storage[J]. AIChE J., 2022, 68(6): e17657 doi: 10.1002/aic.17657

  52. [52]

      YAO B, HUSSAIN S, YE Z Z, PENG X S. Electrodeposited MOFs membrane with in situ incorporation of charged molecules for osmotic energy harvesting[J]. Small, 2023, 19(18): 2207559 doi: 10.1002/smll.202207559

  53. [53]

      LIU Y C, LI Y, FU X, XUE Z A, WANG J J. Lithium dendrite growth, evolution, inhibition in lithium-ion batteries[J]. J. Energy Storage, 2025, 138: 118559 doi: 10.1016/j.est.2025.118559

  54. [54]

      LI J Y, MEI B A, FENG H H, ZUO Z X, XIONG R. Lithium dendrite deposition kinetics and its dynamic impact on capacity fading of lithium-ion batteries[J]. J. Power Sources, 2025, 654: 237753 doi: 10.1016/j.jpowsour.2025.237753

  55. [55]

      XU Y J, WANG B, WAN Y, SUN Y, WANG W L, SUN K, YANG L J, HU H, WU M B. Understanding the process of lithium deposition on a graphite anode for better lithium-ion batteries[J]. New Carbon Mater., 2023, 38(4): 678-693 doi: 10.1016/S1872-5805(23)60747-4

  56. [56]

      YANG L Y, CAO J H, LIANG W H, WANG Y K, WU D Y. Effects of the separator MOF-Al₂O₃ coating on battery rate performance and solid-electrolyte interphase formation[J]. ACS Appl. Mater. Interfaces, 2022, 14(11): 13722-13732 doi: 10.1021/acsami.2c00390

  57. [57]

      XU Y, ZHANG D N, ZHANG S B, BAI L S, LIU Y, ZHAO J W, CHANG Z, ZHOU H S. Accelerating lithium-ion pre-desolvation and transport via glassy MOF for fast-charging and high-energy-density lithium-ion batteries[J]. Natl. Sci Rev., 2025, 12(11): nwaf349 doi: 10.1093/nsr/nwaf349

  58. [58]

      ZHU M Q, HAN D Y, CAI C Y, ZHONG J Y, WENG J Z, TANG C G, GAO F, ZHANG J D. Two-dimensional MXene/MOFs heterojunction nanosheets as confinement hosts for dendrite-free lithium metal anodes[J]. Carbon, 2024, 227: 119248 doi: 10.1016/j.carbon.2024.119248

  59. [59]

      XU M, LIANG S T, SHI H T, MIAO J P, TIAN F, CUI W H, SHAO R Q, XU Z W. High-strength MOF-based polymer electrolytes with uniform ionic flow for lithium dendrite suppression[J]. Small, 2024, 20(46): 2406007 doi: 10.1002/smll.202406007

  60. [60]

      SONG C, HAN S H, MOON H, CHOI N S. Unlocking fast-charging capabilities of lithium-ion batteries through liquid electrolyte engineering[J]. EcoMat, 2024, 6(7): e12476 doi: 10.1002/eom2.12476

  61. [61]

      WANG M X, TONG L J, LV S W, LI M X, ZHAO J Y, LI X, LI C P, CHEN X C, WU J X, LI X Y, CHEN Q H, CHEN Y M. In situ-engineered MOF/polymer hybrid electrolyte with 3D continuous ion channels for high-voltage and thermal-resistant lithium metal batteries[J]. Interd. Mater., 2025, 4(5): 763-774

  62. [62]

      NIU X Y, JU C J, XU D, WANG T T, FU N, YANG Z L. Fluorine-rich MOFs-based composite solid electrolytes realizing fast Li⁺ transportation kinetics and dendrite-free interface[J]. Chem. Eng. J., 2025, 519: 165463 doi: 10.1016/j.cej.2025.165463

  63. [63]

      ZHANG X X, SU Q M, ZHANG F, LV Y J, SHI W H, WANG L M, HUANG W H, ZHANG J, ZHAO W Q, ZHANG M, DING S K, DU G H, XU B S. Realizing high-flux Li⁺ conduction and stable solid electrolyte interface by iodine- and amino-functionalized MOFs doping in solid-state electrolytes[J]. Chem. Eng. J., 2024, 500: 157242 doi: 10.1016/j.cej.2024.157242

  64. [64]

      DONG P P, ZHANG X H, HISCOX W, LIU J J, ZAMORA J, LI X Y, SU M Q, ZHANG Q, GUO X F, MCCLOY J, SONG M K. Toward high-performance metal-organic-framework-based quasi-solid-state electrolytes: Tunable structures and electrochemical properties[J]. Adv. Mater., 2023, 35(32): 2211841 doi: 10.1002/adma.202211841

  65. [65]

      YANG L Y, CAO J H, CAI B R, LIANG T, WU D Y. Electrospun MOF/PAN composite separator with superior electrochemical performances for high energy density lithium batteries[J]. Electrochim. Acta, 2021, 382: 138346 doi: 10.1016/j.electacta.2021.138346

  66. [66]

      LAN F F, ZHAO H J, JIANG Y, JIN C C, ZHAO G D, LI L. A thermomechanically stable nanofiber separator with multiscale MOF networks towards high-efficiency ion transport[J]. J. Mater. Chem. A, 2025, 13(10): 7357-7370 doi: 10.1039/D4TA07790C

  67. [67]

      REN Z P, CONG B, XU F, OUYANG S, ZHAO J H, YANG H J, GUO S, WU D, DUAN X, ZHANG X M. Construction of excellent solid-state electrolyte by incorporating Li-IL into open-pore MOF/polymer-based materials[J]. Mater. Chem. Front., 2024, 8(19): 3166-3174 doi: 10.1039/D4QM00436A

  68. [68]

      HAN G M, HU Q, XIA Y, GAO K D, WANG Y, YAO J F. Stabilizing dendrite-free lithium metal batteries via an anionphilic ZIF-67 modified separator[J]. J. Alloy. Compd., 2025, 1036: 181713 doi: 10.1016/j.jallcom.2025.181713

  69. [69]

      RUAN H, ZHANG L F, LI S, WANG K, HUANG W H, GUO S W. Carbon polyhedra encapsulated Si derived from Co-Mo bimetal MOFs as anode materials for lithium-ion batteries[J]. J. Mater. Sci. Technol., 2023, 159: 91-98 doi: 10.1016/j.jmst.2023.03.009

  70. [70]

      JIANG S, LV T T, PENG Y, PANG H. MOFs containing solid-state electrolytes for batteries[J]. Adv. Sci., 2023, 10(10): 2206887 doi: 10.1002/advs.202206887

  71. [71]

      KONG W Q, ZHAO L Z, GUO J C, ZHU H Y, LI W R, HAN X, LIU S, YU W H, CUI L Y, WEN Z S. Phosphorus decorated MOF-derived microflower-like carbon as a superior anode for lithium-ion batteries[J]. Carbon, 2023, 215: 118439 doi: 10.1016/j.carbon.2023.118439

  72. [72]

      KITCHAMSETTI N, NARSIMULU D, PAYYAVULA S, CHAKRA C S, DE BARROS A L F. V-MOF derived porous nanorods comprising polydopamine-derived C coated VN quantum dots composited with graphitic C as electrodes for long-lasting and high-rate lithium-ion batteries and hybrid supercapacitors[J]. J. Energy Storage, 2025, 109: 115144 doi: 10.1016/j.est.2024.115144

  73. [73]

      KONG O, JIANG G S, WANG K, YANG A P, ZHENG J G, WU S, HAN W C, LI J J, LI L C, AN X L, WANG J, SUN C G, LI L X, XU F, AN B G. Elucidation of Li⁺ conduction behavior in MOF glass electrolyte toward long-cycling and high C-rate lithium metal batteries[J]. Adv. Energy Mater., 2025, 15(22): 2405593 doi: 10.1002/aenm.202405593

  74. [74]

      GUO C F, XIE Y, PAN K, LI L. MOF-derived hollow SiO_x nanoparticles wrapped in 3D porous nitrogen-doped graphene aerogel and their superior performance as the anode for lithium-ion batteries[J]. Nanoscale, 2020, 12(24): 13017-13027 doi: 10.1039/D0NR02453H

  75. [75]

      LI Z A, WANG S G, CHEN P P, LEI J T, HOU Y L, CHEN J Z, ZHAO D L. Interface engineering of MOF-derived Co₃O₄@CNT and CoS₂@CNT anodes with long cycle life and high-rate properties in lithium/sodium-ion batteries[J]. ACS Appl. Mater. Interfaces, 2024, 16(15): 19730-19741 doi: 10.1021/acsami.3c19361

  76. [76]

      YANILMAZ M, ATIK A, TOSUN M, ZHANG X W. MOF@nanofiber separators for lithium-ion batteries[J]. J. Appl. Polym. Sci., 2025, 142(10): e56562 doi: 10.1002/app.56562

  77. [77]

      WANG G X, HE P G, FAN L Z. Asymmetric polymer electrolyte constructed by metal-organic framework for solid-state, dendrite-free lithium metal battery[J]. Adv. Funct. Mater., 2021, 31(3): 2007198 doi: 10.1002/adfm.202007198

  78. [78]

      WANG P, SHEN M Q, ZHOU H, MENG C F, YUAN A H. MOF-derived CuS@Cu-BTC composites as high-performance anodes for lithium-ion batteries[J]. Small, 2019, 15(47): 1903522 doi: 10.1002/smll.201903522

  79. [79]

      ZHANG C L, LI H, ZHANG Q, CAO F H, XIE Y, LU B R, ZHANG W D, CONG H P, LI H. Core-shell structured porous carbon nanofibers integrated with ultra-small SnO₂ nanocrystals for fast and stable lithium storage[J]. Chem. Eng. J., 2021, 420: 127705 doi: 10.1016/j.cej.2020.127705

  80. [80]

      LI J S, XU N N, HAN Q, ZHU L M, CAO X Y. Spherical NiCo₂S₄ wrapped with nitrogen-doped carbon as ultra-fast/high lithium storage materials[J]. J. Alloy. Compd., 2022, 927: 167067 doi: 10.1016/j.jallcom.2022.167067

  81. [81]

      ZHENG G J, XING Z, GAO X R, NIE C H, XU Z H, JU Z C. Fabrication of 2D Cu-BDC MOF and its derived porous carbon as anode material for high-performance Li/K-ion batteries[J]. Appl. Surf. Sci., 2021, 559: 149701 doi: 10.1016/j.apsusc.2021.149701

  82. [82]

      GABER S, MOHAMMED A K, JAVAREGOWDA B H, MARTÍNEZ J I, SÁNCHEZ P P, GÁNDARA F, KRISHNAMOORTHY K, SHETTY D. MOFite: A high-density lithiophilic and scalable metal-organic framework anode for rechargeable lithium-ion battery[J]. Angew. Chem.‒Int. Edit., 2024, 63(44): e202409256 doi: 10.1002/anie.202409256

  83. [83]

      SU L H, CHEN J, ZHOU J Z, LIU J J, HU Z L, LI S, HU X B, XU L L, ZHANG L. Co-based metal-organic frameworks with dual redox active centers for lithium-ion batteries with high capacity and excellent rate capability[J]. Adv. Energy Mater., 2024, 14(48): 2402489 doi: 10.1002/aenm.202402489

  84. [84]

      CHEN Z, HUA Y N, CHEN B, FENG J W, LIU G, JIANG B. In-situ compositing HA significantly enhancing electrochemical performance of Mn-MOF anode materials[J]. Chem. Eng. J., 2025, 506: 160004 doi: 10.1016/j.cej.2025.160004

  85. [85]

      BAI L S, XU Y, LIU Y, ZHANG D N, ZHANG S B, YANG W J, CHANG Z, ZHOU H S. Metal-organic framework glass stabilizes high-voltage cathodes for efficient lithium-metal batteries[J]. Nat. Commun., 2025, 16(1): 3484 doi: 10.1038/s41467-025-58639-z

  86. [86]

      YANG M H, WANG Y, HUANG Y F, XIAO J M, ZHU G Y, FANG Y, ZHOU X C, LONG J H, XIE M, BIN D S, LI D. A conductive Cu-based metal-organic framework ribbon with high-density redox-active centers as cathode for stable high-capacity lithium-ion batteries[J]. Angew. Chem.‒Int. Edit., 2025, 64: e202421008 doi: 10.1002/anie.202421008

  87. [87]

      AHN H, PARK Y, NAM K W. Chelated metal-organic frameworks for improved the performance of high-nickel cathodes in lithium-ion batteries[J]. ChemSusChem, 2025, 18(2): e202400823 doi: 10.1002/cssc.202400823

  88. [88]

      SHIN S, YOON Y, PARK S, SHIN M W. Metal-organic framework coating layer with inherent self-reactivity toward lithium ions to enhance both structural stability and electrochemical performance of LiNi_0.9Co_0.085Mn_0.015O₂ cathodes[J]. Appl. Surf. Sci., 2024, 643: 158735 doi: 10.1016/j.apsusc.2023.158735

  89. [89]

      LIN J, SUN Y H, LIN X M. Metal-organic framework-derived LiFePO₄ cathode encapsulated in O, F-codoped carbon matrix towards superior lithium storage[J]. Nano Energy, 2022, 91: 106655 doi: 10.1016/j.nanoen.2021.106655

  90. [90]

      CHU Z H, GAO X C, WANG C Y, WANG T Y, WANG G X. Metal-organic frameworks as separators and electrolytes for lithium-sulfur batteries[J]. J. Mater. Chem. A, 2021, 9(12): 7301-7316 doi: 10.1039/D0TA11624F

  91. [91]

      HUANG D, LIANG C, CHEN L N, TANG M, ZHENG Z J, WANG Z B. MOF composite fibrous separators for high-rate lithium-ion batteries[J]. J. Mater. Sci., 2021, 56(9): 5868-5877 doi: 10.1007/s10853-020-05559-6

  92. [92]

      ZHOU Q, HUSSAIN S, HU J S, ZHANG G H, ZHANG W X, ZHANG B, WANG L. Polybenzimidazole composite separators engineered from MOFs-HNTs composites applicated in lithium-ion batteries[J]. Small, 2025, 21(19): 2502051 doi: 10.1002/smll.202502051

  93. [93]

      SUN N, LIU Q S, CAO Y, LOU S F, GE M Y, XIAO X H, LEE W K, GAO Y Z, YIN G P, WANG J J, SUN X L. Anisotropically electrochemical-mechanical evolution in solid-state batteries and interfacial tailored strategy[J]. Angew. Chem.‒Int. Edit., 2019, 58(51): 18647-18653 doi: 10.1002/anie.201910993

  94. [94]

      KIM K O, PARK S H, CHUN H B, LEE W Y, JANG B Y, KIM D, YU J H, YUN K S, KIM J, LI O. L, HAN, Y J. Design and optimization of composite cathodes for solid-state batteries using hybrid carbon networks with facile electronic and ionic percolation pathways[J]. ACS Appl. Mater. Interfaces, 2023, 15(30): 36748-36758 doi: 10.1021/acsami.3c04394

  95. [95]

      HAN D D, WANG P F, LI P, SHI J, LIU J, CHEN P J, ZHAI L P, MI L W, FU Y Z. Homogeneous and fast Li-ion transport enabled by a novel metal-organic-framework-based succinonitrile electrolyte for dendrite-free Li deposition[J]. ACS Appl. Mater. Interfaces, 2021, 13(44): 52688-52696 doi: 10.1021/acsami.1c16498

  96. [96]

      LIU Y X, WANG S Q, CHEN W C, KONG W H, WANG S P, LIU H X, DING L, DING L X, WANG H H. 5.1 µm ion-regulated rigid quasi-solid electrolyte constructed by bridging fast Li-ion transfer channels for lithium metal batteries[J]. Adv. Mater., 2024, 36(28): 2401837 doi: 10.1002/adma.202401837

  97. [97]

      LI S, CHEN Y N, LENG X L, YANG M D, ARIFEEN W U, KO T J. Rapid Li⁺ transport within the MOF-based composite solid electrolyte enables high-performance solid-state lithium-ion batteries[J]. Chem. Eng. J., 2024, 500: 157209 doi: 10.1016/j.cej.2024.157209

  98. [98]

      XIONG Z Y, WU S T, GU L, ZHAI M Y, PAN Y K, MA Y H, CHEN Z J. The assembly of a high-efficiency tris-benzotriazolate-based metal-organic framework solid-state electrolyte[J]. ACS Cent. Sci., 2025, 11(7): 1199-1206 doi: 10.1021/acscentsci.5c00567

  99. [99]

      ZHOU J, WANG X, FU J F, CHEN L Y, WEI X R, JIA R R, SHI L Y. A 3D cross-linked metal-organic framework (MOF)-derived polymer electrolyte for dendrite-free solid-state lithium-ion batteries[J]. Small, 2024, 20(18): 2309317 doi: 10.1002/smll.202309317

  100. [100]

       LUO H B, CHEN W Z, MO Y H, GAO J L, ZHANG G Q, TONG Y B, REN X M. In situ polymer‒Integrated metal-organic framework for solid-state electrolyte membrane. inorganic chemistry[J]. Inorg. Chem., 2025, 64(42): 21255-21262 doi: 10.1021/acs.inorgchem.5c04173

• 

  Figure 1  Mechanisms and applications of MOFs in enhancing the fast-charging performance of LIBs

  下载: 全尺寸图片 幻灯片
  

  Figure 2  (a) Schematic of the preparation and structure regulation of the UiO-66-4F membrane for ion separation; SEM images of (b) UiO-66 and (c) UiO-66-4F membrane surfaces; Pore sizes of (d) UiO-66 and (e) UiO-66-4F powders; (f) Ion selectivity of the UiO-66-4F membrane (Copyrighted from Ref.^[49] with a license); (g) Schematic diagrams for the framework structure of TYUST-8; Adsorption amounts of Li⁺ at various (h) initial concentrations and (i) contact times (c₀=100 and 500 mg·L^-1; pH=6.5±0.2) (Copyrighted from Ref.^[50] with a license)

  下载: 全尺寸图片 幻灯片
  

  Figure 3  (a) Structure diagram of MOF-801 polycrystalline membrane with sub-10 nm polymer protective coating applied to the VFB system; (b) Cross-section SEM images of MOF-801 membrane; (c) Ion permeation of metal salts through MOF-801 and s-MOF-801 membrane; (d) Ion selectivity of MOF-801 and s-MOF-801 membrane; (e) CEs, VEs, and EEs of VFB cells equipped with s-MOF-801 membrane at 20-80 mA·cm^-2 (Copyrighted from Ref.^[51] with a license); (f) Schematic representation of the synthesis process for the formation of the Ag/MOFs membrane and Ag/PSS@MOFs composite membrane; (g, h) Output current and power of PSS@MOFs-3 with different external resistances for different concentration gradients; (i) Maximum output powers of PSS@MOFs-3 with different concentration gradients (Copyrighted from Ref.^[52] with a license)

  下载: 全尺寸图片 幻灯片
  

  Figure 4  (a) Schematic illustration of the preparation process and the benefits of coating commercial graphite with 0.293 nm MOF glass containing P elements; (b) HRTEM images of glass@graphite coated with uniform and ultra-thin MOF glass featuring subnanochannels; (c) Cycling performance of assembled NCM-811//graphite and NCM-811//glass@graphite full cells; (d) Cycling performance of NCM-811//glass@graphite pouch cell (inset: schematic illustration of the pouch cell) (Copyrighted from Ref.^[57] with a license); (e) Schematic illustrating the self-assembly process of MXene/MOFs heterojunction; (f) Lithium adsorption energy at the surface of MOFs; (g) Cycling performances of Li symmetrical cells with MXene/MOFs, MXene, MOFs, and Cu substrates; (h) Long-term cycling performances of Li||LiFePO₄ cells with MXene/MOFs, MXene, MOFs, and Cu substrates at 1C (Copyrighted from Ref.^[58] with a license)

  下载: 全尺寸图片 幻灯片
  

  Figure 5  Material design flowchart and morphological structural characterization of 3D MOF@PAN network: (a) schematic of the process; SEM images of (b) electrostatically spun PAN fiber and (c, d) MOF808 network on loaded PAN fiber at different magnifications; (e) Cycling performance of Li|PEO-LiTFSI|Li and Li|MOF808@PAN@PEO-LiTFSI|Li lithium symmetric batteries at 0.1 mA·cm^-2 at 60 ℃; (f) SEM image of the lithium anode surface of Li|PEO-LiTFSI|Li symmetric cell after 100 cycles; (g) optical photographs of PEO-LiTFSI and MOF808@PAN@PEO-LiTFSI polymer electrolyte films; (h) SEM image of the lithium anode surface after 100 cycles of Li|MOF808@PAN@PEO-LiTFSI|Li symmetric cell (Copyrighted from Ref.^[59] with a license)

  下载: 全尺寸图片 幻灯片
  

  Figure 6  (a) Schematic diagram of MOF/polymer composite electrolytes that promote ion transport; (b) SEM image of ZCP; (c) Infrared thermal images of prepared matrices; (d) DFT calculation of the coordination bond length in single LiTFSI and ZIF-8 adsorbed LiTFSI (Copyrighted from Ref.^[61] with a license); (e) Synthetic strategy and structure illustration of Li-IL@UIOF; (f) Lewis acid-base interaction with lithium salt and fast ion channel of Li-IL@UIOF filler; (g) Adsorption energies of TFSI^- on VEC, UIO, and UIOF; (h) Schematic of the mechanism to inhibit the growth of lithium dendrites by incorporating Li-IL@UIOF fillers; (i) Long-term cycling performance at 0.5C of Li|VP20UFI/CL|LFP cells after being subjected to 2C (Copyrighted from Ref.^[62] with a license)

  下载: 全尺寸图片 幻灯片
  

  Figure 7  (a) Schematic illustration of CuBTC, CuBTC-NH₂, and CuBTC-NH₂-I₃; (b) Adsorption models of CuBTC-TFSI, CuBTC-NH₂-TFSI, and CuBTC-NH₂-I₃-TFSI; (c) Binding energies of CuBTC, CuBTC-NH₂, and CuBTC-NH₂-I₃ for TFSI^-; (d) Ionic conductivities of CuBTC-PVDF, CuBTC-NH₂-PVDF, and CuBTC-NH₂-I₃-PVDF at 25 ℃; (e) Li plating/stripping cycle curves of Li//Li symmetric cells assembled with CuBTC-PVDF, CuBTC-NH₂-PVDF, and CuBTC-NH₂-I₃-PVDF electrolytes at a current density of 1 mA·cm^-2 (Copyrighted from Ref.^[63] with a license); (f) Pore apertures and pore volumes of Zn-MOF-74, HKUST-1, and MOF-5; (g) Uptake of LiTFSI and total uptake of LiTFSI+DME together in Li-doped MOFs measured by quantitative NMR; (h) Comparison of activation energy and Li⁺ transference number of MOF electrolytes in this work with other reported works (Copyrighted from Ref.^[64] with a license)

  下载: 全尺寸图片 幻灯片
  

  Figure 8  (a) Schematic of the formation process of C₅₀₀ and C₇₀₀ from 2D Cu-BDC; (b) SEM images of Cu@C₅₀₀; (c) Cycling performance of two samples at 5.0 A·g^-1 (Copyrighted from Ref.^[81] with a license); (d) Schematic representation of the procedure of synthesis of Si/CoMo@NCP from the feed solution from Si@CoMo-MOF and the final product Si/CoMo@NCP; (e) Charge/ discharge curves of Si/CoMo@NCP electrode at different current densities; (f) Cycling performances of Si/CoMo@NCP and Si/Co@NCP at 1.0 A·g^-1 (Copyrighted from Ref.^[69] with a license)

  下载: 全尺寸图片 幻灯片
  

  Figure 9  (a) Synthetic scheme of Fe-Tp; (b) Specific capacity analysis of MOFite and graphite for 800 cycles at 2.0 A·g^-1; (c) Performance graph of MOFite and graphite at 0th, 400th and 800th cycles; (d) Diagrammatic representation of Li⁺ ion diffusion through the hierarchically porous Fe-Tp and possible sites of interactions (Copyrighted from Ref.^[82] with a license); (e) Hydrothermal synthesis process of CoBPDCA products; (f) SEM and (g) TEM images of CoBPDCA; (h) Cycle stability and the corresponding Coulombic efficiency at 0.2C of CoBPDCA electrode; (i) Long-term cycling performance at 10C of CoBPDCA electrode (Copyrighted from Ref.^[83] with a license)

  下载: 全尺寸图片 幻灯片
  

  Figure 10  (a) Schematic diagram of the synthesis of Mn-MOF and HA₂₀-Mn-MOF; Cross-sectional SEM images of the electrodes of (b) Mn-MOF and (c) HA₂₀-Mn-MOF before and after 500 cycles at 1 A·g^-1; (d) Nyquist plots of Mn-MOF and HA₂₀-Mn-MOF electrodes after 0, 5, and 35 cycles (inset: equivalent circuit diagram); (e) Electrochemistry diffusion coefficient of Li⁺ in Mn-MOF and HA₂₀-Mn-MOF electrodes during discharge and charge; (f) Cyclic performance of HA, Mn-MOF, and HA₂₀-Mn-MOF electrodes at 0.1 A·g^-1 (Copyrighted from Ref.^[84] with a license)

  下载: 全尺寸图片 幻灯片
  

  Figure 11  (a) Synthetic schematic diagram of DDA; (b) N₂ adsorption-desorption isotherm, (c) pore diameter distribution, and (d) electrochemical performance of DDA-Cu as LIBs cathode at 2 A·g^-1 (Copyrighted from Ref.^[86] with a license); (e) Schematic of chelation-type MOF-modified cathodes offering a highly promising passivation strategy for high-performance LIBs by suppressing transition metal cross-interference and enhancing Li⁺ transport; (f) Scheme of decreasing activation energy from desolvation by MOF pore; (g) Li⁺ ion diffusion coefficient of NCM while discharging after cycling process; (h) Cycle test of NCM half-cell at 1C (Copyrighted from Ref.^[87] with a license)

  下载: 全尺寸图片 幻灯片
  

  Figure 12  (a) Synthesis process of i-NCM; (b) Long-term cycling performance over 400 cycles with Coulombic efficiency at 1C and room temperature; (c) SEM images of NCM and i-NCM in the cross-sectional view before and after 100 cycles at room temperature and 50 ℃ (scale bar: 5 μm) (Copyrighted from Ref.^[88] with a license); (d) Illustration of the synthesis procedure for MOF-derived LiFePO₄ microparticles encapsulated in O, F-codoped carbon matrix; (e) Long-term cyclability at 1C of the LFP, LFP@OC, and LFP@OFC electrodes; (f) Rate capability at different current densities; Total and orbital-resolved partial DOS plots of (g) LFP bulk and (h) LFP@OFC (the Fermi levels were set to be 0 eV); (i) Differential charge density distribution of LFP@OFC, where the electronic accumulation is indicated by yellow regions and the electronic depletion is depicted by aquamarine regions (Copyrighted from Ref.^[89] with a license)

  下载: 全尺寸图片 幻灯片
  

  Figure 13  (a) TGA curves of PAN, ZIF-8, and ZIF-8/PAN fiber composite membranes; (b) Thermal stability tests of commercialized Celgard 2400 separator, PAN nanofiber membrane, and ZIF-8/PAN fiber composite membrane; (c) Rate performance and (d) cycle performance at 5C of LiFePO₄-Li cells with the ZIF-8/PAN composite fibrous separator (Copyrighted from Ref.^[91] with a license); (e) Thermal shrinkage of the PP, PAN, and MOF/PAN membranes; (f) Ionic conduction process and anion adsorption process of the MOF in the Co-SIM-1/PAN separator; (g) Rate performance of the NCM811||separator||Li batteries with different separators; (h) Charge/discharge cycling and Columbic efficiency of the NCM811||separator||Li batteries with different separators at 5C (Copyrighted from Ref.^[65] with a license)

  下载: 全尺寸图片 幻灯片
  

  Figure 14  (a) Schematic diagram for the detailed fabrication procedures of PI@ZIF-8 nanofiber separators; (b) Current-time curves and the relevant Nyquist plots of PI@ZIF-8 nanofiber separators in symmetric Li-Li cells; (c) Electrolyte uptakes of PE, PI, and PI@ZIF-8; (d) Thermal shrinkage photographs of the three separators from 100 to 200 ℃; (e) Cycling performance of Li‖Li cells at a current density of 1.0 mA·cm^-2 with an area capacity of 1.0 mAh·cm^-2; (f) Cycling performance of NCM811‖Li cell at 0.5C (Copyrighted from Ref.^[66] with a license); (g) Mechanism of action of the separator inside the cell; (h) 200-cycle charge/discharge cycle curves of the LiFePO₄ half-cells assembled with PP, OPBI, OPBI@M-H5, and OPBI@M-H10 separators (Copyrighted from Ref.^[92] with a license)

  下载: 全尺寸图片 幻灯片
  

  Figure 15  (a) Schematic illustration of the preparation of CuBTC-NH₂-I₃-PVDF; (b) Ionic conductivities of CuBTC-PVDF, CuBTC-NH₂-PVDF, and CuBTC-NH₂-I₃-PVDF at 25 ℃; (c) Ion mobility numbers of CuBTC-PVDF, CuBTC-NH₂-PVDF, and CuBTC-NH₂-I₃-PVDF; (d) Raman spectra of CuBTC-NH₂-I₃-PVDF and the corresponding quantification results of the TFSI^- anion states; (e) Cycling stabilities of the LiFePO₄||Li solid-state batteries at 2C (Copyrighted from Ref.^[63] with a license); (f) Ionic conductivities of Cu-TTBT-X (X=Li, Na, and Mg); (g) t_Li⁺ of Cu-TTBT-Li; (h) Cycling performance of the LMB (Copyrighted from Ref.^[98] with a license)

  下载: 全尺寸图片 幻灯片
  

  Figure 16  (a) Main chemicals for the synthesis of cross-linked polymers; (b) Temperature dependence of ionic conductivity for MCPEs; (c) Current-time curves of DC polarization and Nyquist plots (inset) before and after polarization of P-PETEA-MOF; (d) Rate capability of Li/P-PETEA-MOF/LiFePO₄ battery from 0.05C to 3C; (e) Cycling performance of Li/P-PETEA-MOF/LiFePO₄ battery at 1C (Copyrighted from Ref.^[99] with a license); (f) Chronoamperometric curve and EIS of PDMML before and after polarization; (g) Cycling performance of LFP|PDMML|Li full cell at a current density of 1.0C; (h) Charge/discharge profiles of the cell (Copyrighted from Ref.^[100] with a license)

  下载: 全尺寸图片 幻灯片

  Table 1.  Performance comparison of MOFs for fast-charging lithium-ion batteries

  Material	Conductivity /(mS·cm-1)	Temperature /℃	$ {t}_{\text{Li}^{+}} $ /(cm2·s-1)a	Initial capacity /(mAh·g-1)	Cyclic performance	Ref.
  10%Co-SIM-1/PAN	2.38	25	0.74	166.3 (5C)	135.2 mAh·g-1 (250th/5C)	[65]
  PI@ZIF-8	2.4	25	0.88	n.d.	97.4% retention rate (300th/2C)	[66]
  Li-IL@HKUST-1/PAN	2.4	25	0.698	71.7 (5C)	67.5 mAh·g-1 (100th/5C)	[67]
  PP@ZIF-67	0.718	25	0.3	142.2 (0.5C)	84.6% retention rate (500th/2C)	[68]
  Si/CoMo@NCP	n.d.b	n.d.	0.44	1 615 (0.1C)	745 mAh·g-1 (400th/1C)	[69]
  MOFs-SN-FEC	0.704	25	n.d.	n.d.	691 mAh·g-1 (500th/1C)	[70]
  MOF808@PAN@PEO-LiTFSI	2.83	30	0.42	136 (0.5C)	102 mAh·g-1 (1 000th/1C)	[59]
  P/Ni@C	0.4	n.d.	n.d.	1 131 (200C)	1 184.6 mAh·g-1 (400th/200 mA·g-1); 579.4 mAh·g-1(2 500th/2C)	[71]
  VN-GC@PDA-C-50	1.6	n.d.	n.d.	1 012 (0.1C)	351 mAh·g-1 (2 200th/2C); 453 mAh·g-1 (1 100th/1C)	[72]
  GZ-62-QSSE	3.32	25	0.74	132.1 (1C)	72.6% retention rate(3 000th/1C)	[73]
  HSiOx@N-GA	0.871	25	0.697	1 363 (0.1C)	86% retention rate, 133.2 mAh·g-1 (500th/10C); 453 mAh·g-1 (1 100th/1C)	[74]
  Co3O4@CNTs	0.508	25	n.d.	1 043.5 (0.1C)	1 037.6 mAh·g-1 (200th/1C); 581 mAh·g-1 (200th/5C)	[75]
  ZIF-8@nylon 6, 6 separators	3.6	25	n.d.	160 (0.2C)	140 mAh·g-1 at 3C	[76]
  SPE2-PI-ZIF8	0.638	25	0.68	135 (0.5C)	95.6% retention rate, 129.1mAh·g-1 (100th/1C)	[77]
  CuS(70wt%)@Cu-BTC	17	30	1.95	1 185 (0.1C)	80% retention rate, 480 mAh·g-1 at 1C	[78]
  a tLi+: lithium ion transference number; b n.d.: not described.

  下载: 导出CSV
•