Login In
2025 Volume 41 Issue 10
Applications of Generative Artificial Intelligence in Battery Research: Current Status and Prospects
2025, 41(10): 100115
doi: 10.1016/j.actphy.2025.100115
Abstract:
With the rapid development of renewable energy and electric vehicles, batteries, as the core components of electrochemical energy storage systems, have become a global focus in both scientific research and industrial sectors due to their critical impact on system efficiency and safety. However, the complex multi-physics reactions within batteries make traditional mathematical models inadequate for comprehensively revealing their mechanisms. The key to solving this problem lies in introducing data-driven approaches, which have laid a solid foundation for battery research and development through extensive accumulation of experimental data and extraction of effective information. Generative artificial intelligence (GAI), leveraging its powerful latent pattern learning and data generation capabilities, has already found widespread applications in protein structure prediction, material inverse design, and data augmentation, demonstrating its broad application prospects. Applying GAI to battery research workflows with diverse battery data resources could provide innovative solutions to challenges in battery research. In this perspective, we introduce the core principles and latest advancements of generative models (GMs), including Generative Adversarial Network (GAN), Variational Auto-Encoder (VAE), and Diffusion Model (DM), which can learn the latent distribution of the input samples to generate new data by sampling from it. Applications of GAI in battery research are then reviewed. For battery materials design, by learning material compositions, structures, and properties, GM can generate novel candidate materials with desired properties through conditional constraints, significantly extending the chemical space to be explored. For electrode microstructure characterization, GM can serve as a bridge for interconversion and integration of different image data, enhance the quality of microscopic characterization, and generate realistic synthetic data. For battery state estimation, GM can perform data augmentation and feature extraction on battery datasets, which benefits the model performance for battery state estimation. Lastly, we discuss the challenges and future development directions in terms of data governance and model design, including data quality and diversity, data standardization and sharing, usability of synthetic data, interpretability of GM, and foundational models for battery research. For the innovation and advancement of battery technology, this perspective offers theoretical references and practical guidelines for implementing GAI as an effective tool in battery research workflows by discussing its status and prospects in this field.![]()
With the rapid development of renewable energy and electric vehicles, batteries, as the core components of electrochemical energy storage systems, have become a global focus in both scientific research and industrial sectors due to their critical impact on system efficiency and safety. However, the complex multi-physics reactions within batteries make traditional mathematical models inadequate for comprehensively revealing their mechanisms. The key to solving this problem lies in introducing data-driven approaches, which have laid a solid foundation for battery research and development through extensive accumulation of experimental data and extraction of effective information. Generative artificial intelligence (GAI), leveraging its powerful latent pattern learning and data generation capabilities, has already found widespread applications in protein structure prediction, material inverse design, and data augmentation, demonstrating its broad application prospects. Applying GAI to battery research workflows with diverse battery data resources could provide innovative solutions to challenges in battery research. In this perspective, we introduce the core principles and latest advancements of generative models (GMs), including Generative Adversarial Network (GAN), Variational Auto-Encoder (VAE), and Diffusion Model (DM), which can learn the latent distribution of the input samples to generate new data by sampling from it. Applications of GAI in battery research are then reviewed. For battery materials design, by learning material compositions, structures, and properties, GM can generate novel candidate materials with desired properties through conditional constraints, significantly extending the chemical space to be explored. For electrode microstructure characterization, GM can serve as a bridge for interconversion and integration of different image data, enhance the quality of microscopic characterization, and generate realistic synthetic data. For battery state estimation, GM can perform data augmentation and feature extraction on battery datasets, which benefits the model performance for battery state estimation. Lastly, we discuss the challenges and future development directions in terms of data governance and model design, including data quality and diversity, data standardization and sharing, usability of synthetic data, interpretability of GM, and foundational models for battery research. For the innovation and advancement of battery technology, this perspective offers theoretical references and practical guidelines for implementing GAI as an effective tool in battery research workflows by discussing its status and prospects in this field.
2025, 41(10): 100112
doi: 10.1016/j.actphy.2025.100112
Abstract:
Hydrogen peroxide (H2O2) is an eco-friendly oxidant vital for chemical synthesis, water treatment, and disinfection. However, the conventional anthraquinone production method is energy-intensive, generates waste, and requires hazardous transport of concentrated H2O2. Electrochemical H2O2 synthesis via a two-electron oxygen reduction reaction (2e− ORR) has emerged as a sustainable alternative, enabling renewable-powered, decentralized production under mild conditions. Noble metal catalysts outperform alternatives in acidic media, demonstrating superior stability and selectivity. Despite these advantages, several technical challenges must be addressed to enable industrial-scale implementation. The primary challenge lies in optimizing catalyst performance to achieve both high activity and selectivity for the 2e− pathway while suppressing the competing 4e− pathway that produces water. This requires precise control of the catalyst's electronic and surface structures. Additionally, the development of cost-effective reactor systems that can maintain high performance at scale presents another significant hurdle. Current research focuses on improving mass transport, current distribution, and product separation while minimizing energy consumption.This review provides a comprehensive examination of recent progress in the 2e− ORR, with particular emphasis on noble metal catalysts and reactor engineering. We begin by discussing the fundamental principles and reaction mechanisms underlying the 2e− ORR, emphasizing the role of material design in optimizing catalytic performance. Noble-metal catalysts are categorized into four types, namely, pure metals, alloys, compounds, and single-atom catalysts, with a critical evaluation of their performance based on theoretical and experimental findings. The second part of the review focuses on reactor design strategies for practical applications. We evaluate reactor designs, including H-cells, flow cells, membrane electrode assemblies, and solid-state electrolyte cells, with a focus on their mass transport and scalability characteristics. Particular emphasis is placed on gas diffusion electrodes for improved oxygen accessibility and innovative in situ product separation methods. Finally, we discuss the remaining challenges and future directions, including the need for reduced noble metal loading, improved long-term stability, and system integration with renewable energy sources. The review concludes by highlighting the tremendous potential of electrochemical H2O2 production to transform industrial oxidation processes while contributing to the development of sustainable chemical manufacturing.![]()
Hydrogen peroxide (H2O2) is an eco-friendly oxidant vital for chemical synthesis, water treatment, and disinfection. However, the conventional anthraquinone production method is energy-intensive, generates waste, and requires hazardous transport of concentrated H2O2. Electrochemical H2O2 synthesis via a two-electron oxygen reduction reaction (2e− ORR) has emerged as a sustainable alternative, enabling renewable-powered, decentralized production under mild conditions. Noble metal catalysts outperform alternatives in acidic media, demonstrating superior stability and selectivity. Despite these advantages, several technical challenges must be addressed to enable industrial-scale implementation. The primary challenge lies in optimizing catalyst performance to achieve both high activity and selectivity for the 2e− pathway while suppressing the competing 4e− pathway that produces water. This requires precise control of the catalyst's electronic and surface structures. Additionally, the development of cost-effective reactor systems that can maintain high performance at scale presents another significant hurdle. Current research focuses on improving mass transport, current distribution, and product separation while minimizing energy consumption.This review provides a comprehensive examination of recent progress in the 2e− ORR, with particular emphasis on noble metal catalysts and reactor engineering. We begin by discussing the fundamental principles and reaction mechanisms underlying the 2e− ORR, emphasizing the role of material design in optimizing catalytic performance. Noble-metal catalysts are categorized into four types, namely, pure metals, alloys, compounds, and single-atom catalysts, with a critical evaluation of their performance based on theoretical and experimental findings. The second part of the review focuses on reactor design strategies for practical applications. We evaluate reactor designs, including H-cells, flow cells, membrane electrode assemblies, and solid-state electrolyte cells, with a focus on their mass transport and scalability characteristics. Particular emphasis is placed on gas diffusion electrodes for improved oxygen accessibility and innovative in situ product separation methods. Finally, we discuss the remaining challenges and future directions, including the need for reduced noble metal loading, improved long-term stability, and system integration with renewable energy sources. The review concludes by highlighting the tremendous potential of electrochemical H2O2 production to transform industrial oxidation processes while contributing to the development of sustainable chemical manufacturing.
2025, 41(10): 100120
doi: 10.1016/j.actphy.2025.100120
Abstract:
Electrocatalytic hydrodechlorination (EHDC) is a promising technology for degrading chlorinated aromatic hydrocarbons (CAHs), offering high efficiency, minimal secondary pollution, and mild operating conditions. Its effectiveness relies on three critical steps: atomic hydrogen (H*) generation, C―Cl bond cleavage, and adsorption/desorption of CAHs/products. Developing high-performance electrocatalysts is essential to optimize energy efficiency and cost-effectiveness. It is urgent to summarize research progress on design strategies for catalysts and establish fundamental principles. In this review, we first summarize commonly deployed measurement methods and metrics for assessing catalyst activity and stability in EHDC. Then, a series of strategies for enhancing the production of H*, facilitating the cleavage of C―Cl bonds, and optimizing the adsorption and desorption kinetics of CAHs and their intermediates/products on the catalyst surface are summarized. These strategies include the loading of catalysts on carbon-based/transition-based support to enhance the dispersion of Pd; constructing heterostructures or forming alloys to modulate the electronic structure of active metal nanocatalysts and optimize its binding affinities with reactants and intermediates; and modulating the microenvironment to modify the interface hydrophilicity/hydrophobicity of catalyst to increase reaction rates or improve stability of catalysts. Additionally, the applications of electrocatalysts for EHDC in recent years, such as Pd-based supported electrocatalysts, Pd-based heterostructure electrocatalysts, Pd-based alloy electrocatalysts, and noble-metal-free electrocatalysts are discussed, as well as the influence of catalyst composition on performance. It is noted that the EHDC efficiency of CAHs is influenced not only by the catalyst but also significantly correlated with the structure of CAHs. Thus, the effects of CAHs structures on EHDC performance are also discussed. Studies demonstrate that weak adsorption between the electrode and CAHs is more conducive to EHDC reactions. The number and position of chlorine functional groups, steric hindrance, and the properties of other functional groups in the substrate molecule can also influence EHDC performance. Finally, the challenges and future prospects of EHDC are highlighted, including improving the catalytic performance of non-noble catalysts, employing advanced in situ and operando characterization techniques, and optimizing DFT calculations to more closely align with real catalytic conditions, all aiming to inspire new investigations and advancements in the field of EHDC of CAHs.![]()
Electrocatalytic hydrodechlorination (EHDC) is a promising technology for degrading chlorinated aromatic hydrocarbons (CAHs), offering high efficiency, minimal secondary pollution, and mild operating conditions. Its effectiveness relies on three critical steps: atomic hydrogen (H*) generation, C―Cl bond cleavage, and adsorption/desorption of CAHs/products. Developing high-performance electrocatalysts is essential to optimize energy efficiency and cost-effectiveness. It is urgent to summarize research progress on design strategies for catalysts and establish fundamental principles. In this review, we first summarize commonly deployed measurement methods and metrics for assessing catalyst activity and stability in EHDC. Then, a series of strategies for enhancing the production of H*, facilitating the cleavage of C―Cl bonds, and optimizing the adsorption and desorption kinetics of CAHs and their intermediates/products on the catalyst surface are summarized. These strategies include the loading of catalysts on carbon-based/transition-based support to enhance the dispersion of Pd; constructing heterostructures or forming alloys to modulate the electronic structure of active metal nanocatalysts and optimize its binding affinities with reactants and intermediates; and modulating the microenvironment to modify the interface hydrophilicity/hydrophobicity of catalyst to increase reaction rates or improve stability of catalysts. Additionally, the applications of electrocatalysts for EHDC in recent years, such as Pd-based supported electrocatalysts, Pd-based heterostructure electrocatalysts, Pd-based alloy electrocatalysts, and noble-metal-free electrocatalysts are discussed, as well as the influence of catalyst composition on performance. It is noted that the EHDC efficiency of CAHs is influenced not only by the catalyst but also significantly correlated with the structure of CAHs. Thus, the effects of CAHs structures on EHDC performance are also discussed. Studies demonstrate that weak adsorption between the electrode and CAHs is more conducive to EHDC reactions. The number and position of chlorine functional groups, steric hindrance, and the properties of other functional groups in the substrate molecule can also influence EHDC performance. Finally, the challenges and future prospects of EHDC are highlighted, including improving the catalytic performance of non-noble catalysts, employing advanced in situ and operando characterization techniques, and optimizing DFT calculations to more closely align with real catalytic conditions, all aiming to inspire new investigations and advancements in the field of EHDC of CAHs.
2025, 41(10): 100113
doi: 10.1016/j.actphy.2025.100113
Abstract:
Photodynamic therapy (PDT), as a Food and Drug Administration (FDA)-approved therapeutic modality, has witnessed substantial advancements in the field of oncology. However, the conventional PDT may suffer poor prognosis due to the transient nature of (Reactive Oxygen Species) ROS, excessive phototoxicity, and inducing traditional apoptosis. In this study, a nanoengineered carbon dots (NCDs) was constructed through electrostatic interaction between a positive-charged carbon dots photosensitizers (PCDs) and new indocyanine green (IR820). The introduction of IR820 at variable ratios could change the surface charge and amphiphilic characteristics of NCDs, thereby modulating the membrane-anchoring capability of NCDs. Besides, the J-aggregation of IR820 led to a redshift of fluorescence from NIR-Ⅰ to NIR-Ⅱ region, thereby achieving NIR-Ⅱ imaging. Furthermore, the photoactivity of PCDs was quenched by IR820, with subsequent restoration of PDT occurring contingent on the photobleaching of IR820 via 750 nm laser irradiation. Finally, both in vitro and in vivo studies had demonstrated that under a cascaded laser irradiation, the membrane-targeted NCDs could effectively induce cell pyroptosis, thereby eradicating tumors with minimal side effects while simultaneously activating immune responses to inhibit tumor lung metastasis. This study developed a multifunctional nanoengieering carbon dots and offered novel perspectives for tumor photodynamic-immunotherapy with enhanced controllability, improved efficacy and high security.![]()
Photodynamic therapy (PDT), as a Food and Drug Administration (FDA)-approved therapeutic modality, has witnessed substantial advancements in the field of oncology. However, the conventional PDT may suffer poor prognosis due to the transient nature of (Reactive Oxygen Species) ROS, excessive phototoxicity, and inducing traditional apoptosis. In this study, a nanoengineered carbon dots (NCDs) was constructed through electrostatic interaction between a positive-charged carbon dots photosensitizers (PCDs) and new indocyanine green (IR820). The introduction of IR820 at variable ratios could change the surface charge and amphiphilic characteristics of NCDs, thereby modulating the membrane-anchoring capability of NCDs. Besides, the J-aggregation of IR820 led to a redshift of fluorescence from NIR-Ⅰ to NIR-Ⅱ region, thereby achieving NIR-Ⅱ imaging. Furthermore, the photoactivity of PCDs was quenched by IR820, with subsequent restoration of PDT occurring contingent on the photobleaching of IR820 via 750 nm laser irradiation. Finally, both in vitro and in vivo studies had demonstrated that under a cascaded laser irradiation, the membrane-targeted NCDs could effectively induce cell pyroptosis, thereby eradicating tumors with minimal side effects while simultaneously activating immune responses to inhibit tumor lung metastasis. This study developed a multifunctional nanoengieering carbon dots and offered novel perspectives for tumor photodynamic-immunotherapy with enhanced controllability, improved efficacy and high security.
2025, 41(10): 100114
doi: 10.1016/j.actphy.2025.100114
Abstract:
Activated carbons are widely used as the electrode material for supercapacitors owing to its large surface area, good electric conductivity, and outstanding electrochemical stability. Improving the electric conductivity of activated carbon is crucial for promoting its electrochemical energy storage, but hard to achieve because well-developed pores usually break the continuous conductive network. To solve this problem, researchers have developed several methods, such as selection of highly-conjugated carbon precursors, high-temperature post-treatment, compositing with highly conductive nanocarbons, and local catalytic graphitization. However, these methods generally suffer from high cost, low efficiency, and sacrifice of specific surface area. Herein, we propose a selective chemical etching strategy to prepare activated carbon with both high surface area and electric conductivity using a mixture of pitch and polyacrylonitrile (PAN) as the precursor. Through systematic investigation of the activation behavior of pure pitch, pure PAN, and the composite precursors, we demonstrate that the PAN-derived carbon contains amorphous and crystallized components. During activation, the amorphous carbon is primarily etched away due to its high reactivity, leading to the in-situ formation of less-defective carbon as the entire conductive network. The optimized sample shows a surface area of 2773 m2·g−1 and 2.6 times increased electric conductivity of 912 S·m−1, outperforming most of the reported activated carbons. Furthermore, the strong cross-linking between pitch and PAN molecules through pre-oxidation leads to a higher activated carbon yield of 58% than the pure pitch-derived activated carbon (34%). The optimized cross-linking structure also allows the activator K+ to be adsorbed more easily in the carbon precursor, which enhances the activation efficiency. As a result, the embedded PAN simultaneously construct conductive network and promote activation efficiency, leading to the integration of high electric conductivity and surface area of the activated carbon. For aqueous supercapacitor application, at the high electrode mass loading of 10 mg·cm−2, the optimized material shows remarkable areal capacitance (2.8 F·cm−2 at 1 A·g−1) and good rate performance (41% retention at 50 A·g−1). The corresponding device shows high energy densities (10.9 Wh·kg−1) and remarkable cycle stability (100% retention after 50000 cycles). The reason is that good electric conductivity enables high surface area utilization, significantly improved electric double-layer formation and ion transport kinetics. This work demonstrates the significant potential of highly conductive activated carbon for practical applications, and provides novel insights into the design of conductive activated carbon for advanced energy storage.![]()
Activated carbons are widely used as the electrode material for supercapacitors owing to its large surface area, good electric conductivity, and outstanding electrochemical stability. Improving the electric conductivity of activated carbon is crucial for promoting its electrochemical energy storage, but hard to achieve because well-developed pores usually break the continuous conductive network. To solve this problem, researchers have developed several methods, such as selection of highly-conjugated carbon precursors, high-temperature post-treatment, compositing with highly conductive nanocarbons, and local catalytic graphitization. However, these methods generally suffer from high cost, low efficiency, and sacrifice of specific surface area. Herein, we propose a selective chemical etching strategy to prepare activated carbon with both high surface area and electric conductivity using a mixture of pitch and polyacrylonitrile (PAN) as the precursor. Through systematic investigation of the activation behavior of pure pitch, pure PAN, and the composite precursors, we demonstrate that the PAN-derived carbon contains amorphous and crystallized components. During activation, the amorphous carbon is primarily etched away due to its high reactivity, leading to the in-situ formation of less-defective carbon as the entire conductive network. The optimized sample shows a surface area of 2773 m2·g−1 and 2.6 times increased electric conductivity of 912 S·m−1, outperforming most of the reported activated carbons. Furthermore, the strong cross-linking between pitch and PAN molecules through pre-oxidation leads to a higher activated carbon yield of 58% than the pure pitch-derived activated carbon (34%). The optimized cross-linking structure also allows the activator K+ to be adsorbed more easily in the carbon precursor, which enhances the activation efficiency. As a result, the embedded PAN simultaneously construct conductive network and promote activation efficiency, leading to the integration of high electric conductivity and surface area of the activated carbon. For aqueous supercapacitor application, at the high electrode mass loading of 10 mg·cm−2, the optimized material shows remarkable areal capacitance (2.8 F·cm−2 at 1 A·g−1) and good rate performance (41% retention at 50 A·g−1). The corresponding device shows high energy densities (10.9 Wh·kg−1) and remarkable cycle stability (100% retention after 50000 cycles). The reason is that good electric conductivity enables high surface area utilization, significantly improved electric double-layer formation and ion transport kinetics. This work demonstrates the significant potential of highly conductive activated carbon for practical applications, and provides novel insights into the design of conductive activated carbon for advanced energy storage.
2025, 41(10): 100119
doi: 10.1016/j.actphy.2025.100119
Abstract:
The development of high-performance and low-cost hard carbon plays a crucial role in the commercialization of sodium-ion batteries (SIBs). Asphalt is considered a suitable hard carbon precursor due to its wide distribution, abundance, and cost-effectiveness. However, its low capacity and poor electrochemical reaction kinetics limit its further application. Herein, we have successfully synthesized asphalt-based hard carbon nanosheets through a process of intramolecular oxidation, facilitated by the synergistic action of mixed acids. The introduction of sulfuric acid plays a crucial role in expanding the tightly packed asphalt molecules, which in turn allows for the intramolecular oxidation of asphalt molecules by nitric acid. This oxidation process effectively introduces oxygen-containing functional groups (OFGs), leading to an increase in interlayer spacing and the formation of a more nanoporous structure, resulting in both enhanced capacity and improved rate performance. The optimized asphalt-based hard carbon boosts reversible capacity from 115.0 to 304.4 mAh∙g−1 at 0.03 A∙g−1, and the plateau capacity is increased by 5.5 times. This work provides a profound understanding of the impact of liquid-phase acid oxidation on the structure and composition of sodium-storage hard carbon, and further unveils an effective method for obtaining low-cost and high-performance asphalt-based hard carbon.![]()
The development of high-performance and low-cost hard carbon plays a crucial role in the commercialization of sodium-ion batteries (SIBs). Asphalt is considered a suitable hard carbon precursor due to its wide distribution, abundance, and cost-effectiveness. However, its low capacity and poor electrochemical reaction kinetics limit its further application. Herein, we have successfully synthesized asphalt-based hard carbon nanosheets through a process of intramolecular oxidation, facilitated by the synergistic action of mixed acids. The introduction of sulfuric acid plays a crucial role in expanding the tightly packed asphalt molecules, which in turn allows for the intramolecular oxidation of asphalt molecules by nitric acid. This oxidation process effectively introduces oxygen-containing functional groups (OFGs), leading to an increase in interlayer spacing and the formation of a more nanoporous structure, resulting in both enhanced capacity and improved rate performance. The optimized asphalt-based hard carbon boosts reversible capacity from 115.0 to 304.4 mAh∙g−1 at 0.03 A∙g−1, and the plateau capacity is increased by 5.5 times. This work provides a profound understanding of the impact of liquid-phase acid oxidation on the structure and composition of sodium-storage hard carbon, and further unveils an effective method for obtaining low-cost and high-performance asphalt-based hard carbon.
2025, 41(10): 100121
doi: 10.1016/j.actphy.2025.100121
Abstract:
Complete mineralization of persistent organic pollutants in wastewater remains a formidable challenge. Here, we report the rational design of a ZIF-8-derived ZnO/polyaniline (PANI) S-scheme heterojunction synthesized via in situ oxidative polymerization. Advanced characterizations confirm the S-scheme charge transfer mechanism within the ZnO/PANI heterojunction. The optimized composite achieves complete phenol mineralization within 60 min while concurrently generating H2O2 at a rate of 0.75 mmol∙L−1·h–1 under simulated solar irradiation. Mechanistic studies verify that the S-scheme heterojunction retains strong redox potentials, driving the formation of reactive oxygen species for H2O2 production and phenol degradation. This work establishes a universal design paradigm for MOF-derived inorganic/organic S-scheme heterojunctions, effectively coupling solar-driven energy conversion with environmental remediation.![]()
Complete mineralization of persistent organic pollutants in wastewater remains a formidable challenge. Here, we report the rational design of a ZIF-8-derived ZnO/polyaniline (PANI) S-scheme heterojunction synthesized via in situ oxidative polymerization. Advanced characterizations confirm the S-scheme charge transfer mechanism within the ZnO/PANI heterojunction. The optimized composite achieves complete phenol mineralization within 60 min while concurrently generating H2O2 at a rate of 0.75 mmol∙L−1·h–1 under simulated solar irradiation. Mechanistic studies verify that the S-scheme heterojunction retains strong redox potentials, driving the formation of reactive oxygen species for H2O2 production and phenol degradation. This work establishes a universal design paradigm for MOF-derived inorganic/organic S-scheme heterojunctions, effectively coupling solar-driven energy conversion with environmental remediation.
2025, 41(10): 100122
doi: 10.1016/j.actphy.2025.100122
Abstract:
Modulating the internal electric field (IEF) remains a critical challenge for S-scheme heterojunction photocatalysts. The BiVO4/WO3-x S-scheme heterojunctions were successfully prepared to purify the wastewater environment where tetracycline (TC) and Cr(Ⅵ) coexist under visible light illumination. The BiVO4/WO3-x with 10% (wt) WO3-x (BVO/WO3-x-10) demonstrated superior photocatalytic efficiency, which could degrade 78.5% of TC and reduce 85.3% of Cr(Ⅵ) in 60 min. The photocatalytic activity of BVO/WO3-x-10 displayed enhanced removal efficiency in the mixed system. The removal ability of TC and Cr(Ⅵ) was increased by 1.29 and 1.32 times, respectively. Based on infrared thermography (IR) thermography measurements, the elevated reaction system temperatures were ascribed to the photothermal effect of WO3-x. Oxygen vacancies (OVs) could amplify the energy band difference between WO3-x and BiVO4, which strengthens the IEF and accelerates the separation of carriers. A detailed degradation pathway and intermediate toxicity were carried out using the mung bean experiment and the results of the Liquid Chromatograph Mass Spectrometer (LC-MS). In general, this work provided new insights for regulating IEF to enhance the degradation efficiency in mixed wastewater and the carriers separation in the S-scheme heterojunction of the photothermal-catalytic system. ![]()
Modulating the internal electric field (IEF) remains a critical challenge for S-scheme heterojunction photocatalysts. The BiVO4/WO3-x S-scheme heterojunctions were successfully prepared to purify the wastewater environment where tetracycline (TC) and Cr(Ⅵ) coexist under visible light illumination. The BiVO4/WO3-x with 10% (wt) WO3-x (BVO/WO3-x-10) demonstrated superior photocatalytic efficiency, which could degrade 78.5% of TC and reduce 85.3% of Cr(Ⅵ) in 60 min. The photocatalytic activity of BVO/WO3-x-10 displayed enhanced removal efficiency in the mixed system. The removal ability of TC and Cr(Ⅵ) was increased by 1.29 and 1.32 times, respectively. Based on infrared thermography (IR) thermography measurements, the elevated reaction system temperatures were ascribed to the photothermal effect of WO3-x. Oxygen vacancies (OVs) could amplify the energy band difference between WO3-x and BiVO4, which strengthens the IEF and accelerates the separation of carriers. A detailed degradation pathway and intermediate toxicity were carried out using the mung bean experiment and the results of the Liquid Chromatograph Mass Spectrometer (LC-MS). In general, this work provided new insights for regulating IEF to enhance the degradation efficiency in mixed wastewater and the carriers separation in the S-scheme heterojunction of the photothermal-catalytic system.
2025, 41(10): 100126
doi: 10.1016/j.actphy.2025.100126
Abstract:
The reaction of CO2 catalytic hydrogenation to dimethyl ether (DME) usually relies on a Cu-containing metal oxide/molecular sieve system; however, the migration of copper species to molecular sieves is unavoidable during the reaction, leading to the loss of Cu0 sites and acidic sites. In this work, a Cu/x%Ga-γ-Al2O3 bifunctional catalyst was synthesized via the coprecipitation method. Ga was doped into the γ-Al2O3 lattice at a low concentration, forming interfacial active sites with surface Cu0 species to achieve the hydrogenation of CO2 to DME. Experimental studies combined with Density functional theory (DFT) calculations demonstrate that the catalyst remains stable for 180 h and that the Ga-doped Cu/γ-Al2O3 interface sites exhibit catalytic effects on CO2 hydrogenation to CH3OH and CH3OH dehydration to produce DME. The doping of Ga increases the specific surface area of the catalyst, reduces the particle size of Cu0, enhances the number of acidic and basic sites on the catalyst, and promotes the adsorption of H2 and CO2. In addition, a new reaction pathway for DME synthesis was proposed. This work removes the dehydrated component of a traditional Cu-based bifunctional catalyst, enabling two reactions to occur at the same active sites, thus providing a new strategy for the design of novel dimethyl ether synthesis bifunctional catalysts. ![]()
The reaction of CO2 catalytic hydrogenation to dimethyl ether (DME) usually relies on a Cu-containing metal oxide/molecular sieve system; however, the migration of copper species to molecular sieves is unavoidable during the reaction, leading to the loss of Cu0 sites and acidic sites. In this work, a Cu/x%Ga-γ-Al2O3 bifunctional catalyst was synthesized via the coprecipitation method. Ga was doped into the γ-Al2O3 lattice at a low concentration, forming interfacial active sites with surface Cu0 species to achieve the hydrogenation of CO2 to DME. Experimental studies combined with Density functional theory (DFT) calculations demonstrate that the catalyst remains stable for 180 h and that the Ga-doped Cu/γ-Al2O3 interface sites exhibit catalytic effects on CO2 hydrogenation to CH3OH and CH3OH dehydration to produce DME. The doping of Ga increases the specific surface area of the catalyst, reduces the particle size of Cu0, enhances the number of acidic and basic sites on the catalyst, and promotes the adsorption of H2 and CO2. In addition, a new reaction pathway for DME synthesis was proposed. This work removes the dehydrated component of a traditional Cu-based bifunctional catalyst, enabling two reactions to occur at the same active sites, thus providing a new strategy for the design of novel dimethyl ether synthesis bifunctional catalysts.
2025, 41(10): 100131
doi: 10.1016/j.actphy.2025.100131
Abstract:
The rational construction of step-scheme (S-scheme) heterojunctions has been demonstrated as an effective strategy to optimize interfacial charge carrier separation dynamics in semiconductor photocatalysts. In this work, a hierarchical ReSe2/ZnCdS S-scheme heterojunction with well-defined architectures was successfully synthesized via an ultrasonication-assisted synthetic strategy, achieving precise nanostructure control and enhanced interfacial coupling for optimized photogenerated charge dynamics. The disordered nanoflower-like ReSe2 architecture enhances light-harvesting efficiency and the density of surface reaction sites, and significantly suppresses ZnCdS nanoparticle aggregation. The optimized 5%ReSe2/ZnCdS composite exhibits an exceptional hydrogen evolution rate of 13.96 mmol∙g−1∙h−1 under visible light irradiation, representing a 5.91-fold enhancement over pristine ZnCdS (2.36 mmol∙g−1∙h−1) and outperforming most conventional heterojunction systems. The outstanding photocatalytic performance is attributed to the formation of the ReSe2/ZnCdS S-scheme heterojunction, which promotes the separation of photogenerated electrons and holes, enhancing the photo-redox capacity. Combining in situ X-ray photoelectron spectroscopy (XPS) analysis and density functional theory (DFT) calculations further conform the S-scheme charge transfer mechanism at the heterointerface of ReSe2/ZnCdS. Furthermore, Gibbs free energy calculations of hydrogen adsorption confirm that ReSe2 as the predominant catalytic center provides more favorable hydrogen adsorption kinetics than ZnCdS. This work provides a universal framework to design ZnCdS-based S-scheme heterojunctions for high-efficiency photocatalytic hydrogen evolution. ![]()
The rational construction of step-scheme (S-scheme) heterojunctions has been demonstrated as an effective strategy to optimize interfacial charge carrier separation dynamics in semiconductor photocatalysts. In this work, a hierarchical ReSe2/ZnCdS S-scheme heterojunction with well-defined architectures was successfully synthesized via an ultrasonication-assisted synthetic strategy, achieving precise nanostructure control and enhanced interfacial coupling for optimized photogenerated charge dynamics. The disordered nanoflower-like ReSe2 architecture enhances light-harvesting efficiency and the density of surface reaction sites, and significantly suppresses ZnCdS nanoparticle aggregation. The optimized 5%ReSe2/ZnCdS composite exhibits an exceptional hydrogen evolution rate of 13.96 mmol∙g−1∙h−1 under visible light irradiation, representing a 5.91-fold enhancement over pristine ZnCdS (2.36 mmol∙g−1∙h−1) and outperforming most conventional heterojunction systems. The outstanding photocatalytic performance is attributed to the formation of the ReSe2/ZnCdS S-scheme heterojunction, which promotes the separation of photogenerated electrons and holes, enhancing the photo-redox capacity. Combining in situ X-ray photoelectron spectroscopy (XPS) analysis and density functional theory (DFT) calculations further conform the S-scheme charge transfer mechanism at the heterointerface of ReSe2/ZnCdS. Furthermore, Gibbs free energy calculations of hydrogen adsorption confirm that ReSe2 as the predominant catalytic center provides more favorable hydrogen adsorption kinetics than ZnCdS. This work provides a universal framework to design ZnCdS-based S-scheme heterojunctions for high-efficiency photocatalytic hydrogen evolution.
