2024 Volume 40 Issue 4

Constructing a one-dimensional Cu-coordination polymer-based cathode material for Li-ion batteries
Qingyan JIANG , Yanyong SHA , Chen CHEN , Xiaojuan CHEN , Wenlong LIU , Hao HUANG , Hongjiang LIU , Qi LIU
2024, 40(4): 657-668  doi: 10.11862/CJIC.20240004
[Abstract](80) [FullText HTML] [PDF 11821KB](0)
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A novel one-dimensional (1D) polycarbonyl coordination polymer [Cu(BGPD)(DMA)(H2O)]·DMA (named Cu-BD, H2BGPD=N, N′-bis(glycinyl)pyromellitic diimide; DMA=dimethylacetamide) was synthesized, and evaluated as a cathode material for lithium - ion batteries (LIBs) for the first time. The electrochemical performance study revealed that the Cu-BD cathode exhibited better cycling stability and a specific capacity of 50 mAh·g-1 after 100 cycles at a current density of 50 mA·g-1. The study of the reaction mechanism for the Cu-BD electrode discloses that both BGPD2- ligands and Cu(Ⅱ) ions may take part in the electron-transfer process during charging and discharging.
Preparation of high-performance supercapacitor based on bimetallic high nuclearity titanium-oxo-cluster based electrodes
Wen LUO , Lin JIN , Palanisamy Kannan , Jinle HOU , Peng HUO , Jinzhong YAO , Peng WANG
2024, 40(4): 782-790  doi: 10.11862/CJIC.20230418
[Abstract](112) [FullText HTML] [PDF 6231KB](1)
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A series of novel titanium-oxo-clusters (TOCs, including Zn-Ti11 and Cd-Ti11) was designed for supercapacitors, expanding the potential application of TOCs. These materials demonstrate the benefits of titanium-based materials through their excellent pseudocapacitive energy storage capabilities. The prepared supercapacitor exhibited impressive performance, with a maximum power density of 9.5 W·kg-1 and an energy density of 463 Wh·kg-1.
Synthesis, structures, and catalytic activity of aluminum and zinc complexes chelated by 2-((2,6-dimethylphenyl)amino)ethanolate
Anqiu LIU , Long LIN , Dezhi ZHANG , Junyu LEI , Kefeng WANG , Wei ZHANG , Junpeng ZHUANG , Haijun HAO
2024, 40(4): 791-798  doi: 10.11862/CJIC.20230424
[Abstract](59) [FullText HTML] [PDF 2499KB](0)
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Treatment of ArNHCH2CH2OH (HL, Ar=2,6-Me2C6H3) with AlMe3 and ZnEt2 resulted in the formation of a bi-aluminum complex, [(Me2Al)(L)]2 (1), and a tetra-zinc complex, [EtZn2(L)3]2 (2), respectively. They were characterized by elemental analysis, NMR, and single-crystal X-ray diffraction analysis. Complex 1 is a crystallographically centrosymmetric dimer with an Al2O2 core in the solid state, while a Zn4O6 core is observed in 2, which can be viewed as two side-by-side cubes missing a pair of opposite vertices. Preliminary catalytic activity tests indicated that the aluminum complex 1 was inactive for the ring-opening polymerization (ROP) of ε-caprolactone, while the zinc complex 2 was a highly active initiator for the ROP of ε-caprolactone and could control the molecular weight distribution of the resulted polymers in narrow ranges.
Preparation and efficient catalysis for olefins epoxidation of a polyoxovanadate-based hybrid
Ning LI , Siyu DU , Xueyi WANG , Hui YANG , Tao ZHOU , Zhimin GUAN , Peng FEI , Hongfang MA , Shang JIANG
2024, 40(4): 799-808  doi: 10.11862/CJIC.20230372
[Abstract](68) [FullText HTML] [PDF 3554KB](0)
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A new polyoxovanadate compound [Co(pIM)V2O6] (1) was hydrothermally synthesized, where pIM stands for 2-(2-pyridyl)imidazole. For its characterizations, an integration of X-ray single crystal diffraction, powder X-ray diffraction, Fourier transform infrared spectra, and elemental analysis was accomplished. The compound exhibited a 2D architecture composed of VO4 tetrahedra and CoO3N2 square pyramids via both edge - and corner - sharing. Considering the excellent catalytic oxidation features of polyoxovanadate, compound 1 was used as an efficient heterogeneous catalyst for the epoxidation of olefins with H2O2 as an oxidant, and could be reused without consuming activity. Besides, the magnetic studies indicated the antiferromagnetic interactions in 1.
Waste biomass-derived carbon modified porous graphite carbon nitride heterojunction for efficient photodegradation of oxytetracycline in seawater
Wenda WANG , Jinku MA , Yuzhu WEI , Shuaishuai MA
2024, 40(4): 809-822  doi: 10.11862/CJIC.20230353
[Abstract](81) [FullText HTML] [PDF 14987KB](0)
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A metal - free photocatalyst was developed and synthesized through a single - step thermal treatment process involving banana peel (BP) and urea. The close interfacial connection between biomass-derived carbon (BC) and porous graphite carbon nitride (pg - C3N4) resulted in an increased specific surface area, expanded photo-response range, effective migration of photo-induced electrons, and enhanced stability. The reaction rate constant of pg-C3N4/BC for degradation oxytetracycline (OTC) in artificial seawater was 9.4 times higher than that of pristine pg-C3N4 after 70 min of visible-light illumination, and pg-C3N4/BC also performed better photocatalytic degradation on OTC in the continuous flow reaction process owing to facilitated photogenerated charge separation and transfer. Additionally, a potential photocatalytic mechanism was proposed to explain the enhanced performance of pg-C3N4/BC composites.
Assembling a luminescence silencing system based on post-synthetic modification strategy: A highly sensitive and selective turn-on metal-organic framework probe for ascorbic acid detection
Jie ZHANG , Xin LIU , Zhixin LI , Yuting PEI , Yuqi YANG , Huimin LI , Zhiqiang LIU
2024, 40(4): 823-833  doi: 10.11862/CJIC.20230310
[Abstract](84) [FullText HTML] [PDF 14239KB](0)
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A unique 3D luminescent metal-organic framework, namely [Cd(L)(H2O)0.5]·DMF·2.5H2O (1), where H2L=3-(tetrazol-5-yl)triazole, has been successfully prepared and characterized. The framework has demonstrated excellent luminescence properties and structural stability in the water system. Notably, the luminescence intensity of 1 was significantly quenched by Cr(Ⅵ) (1 mL of Cr2O72- or 150 μL of CrO42-, 1 mmol·L-1), leading to the formation of an "on-off" luminescence silencing system (Cr2O72-@1), which was capable of accurately detecting Cr(Ⅵ) in the water system. The primary mechanism responsible for luminescence quenching was the Forster resonance energy transfer (FRET) process. Additionally, by removing the involvement of the FRET process, the luminescence intensity of the Cr2O72-@1 system could be restored, allowing for the highly selective and sensitive detection of ascorbic acid (AA) in water systems. Moreover, it has been demonstrated that 1 can successfully detect AA in vitamin C tablets, yielding recovery rates ranging from 98.20% to 103.33% and relative standard deviations (RSDs) ranging from 1.78% to 3.42%. Based on the findings of this experiment, a luminescent "IMPLICATION" molecular logic gate has been constructed utilizing AA and Cr(Ⅵ) as the chemical inputs, respectively.
Design, synthesis, and fluorescence sensing performance of highly sensitive and multi-response lanthanide metal-organic frameworks
Ruikui YAN , Xiaoli CHEN , Miao CAI , Jing REN , Huali CUI , Hua YANG , Jijiang WANG
2024, 40(4): 834-848  doi: 10.11862/CJIC.20230301
[Abstract](85) [FullText HTML] [PDF 7409KB](0)
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Based on the 5-(3, 4-dicarboxyphenoxy) isophthalic acid (H4dppa) ligand, two lanthanide metal-organic frameworks (Ln-MOFs) were designed and synthesized by hydrothermal synthesis: {(dima)[Dy(dppa)(H2O)2]·2.5H2O}n (Dy - MOF) and {(dima) [Eu(dppa) (H2O)2]·1.5H2O}n (Eu - MOF) (dima=dimethylamine cation). The structures were characterized by elemental analysis, infrared spectroscopy, single-crystal X-ray diffraction, etc. Dy-MOF and Eu- MOF are hetero-isomorphic 2D network structures, and adjacent 2D networks further form 3D supramolecular network structures through hydrogen bonding. Fluorescence analysis shows that Dy-MOF and Eu-MOF have excellent fluorescence properties at room temperature, and Dy-MOF has excellent fluorescence sensing properties, which can efficiently and high-sensitively detect a variety of pollutants in water: aniline (ANI), nitrobenzene (NB), tetracycline (TC), pyrimethanil (PTH), and tryptophan (Trp). The fluorescence quenching mechanism of Dy-MOF in detecting pollutants was also investigated.
Preparation and in vivo tracing of 68Ga-labeled PM2.5 mimetic particles for positron emission tomography imaging
Donghui PAN , Yuping XU , Xinyu WANG , Lizhen WANG , Junjie YAN , Dongjian SHI , Min YANG , Mingqing CHEN
2024, 40(4): 669-676  doi: 10.11862/CJIC.20230468
[Abstract](53) [FullText HTML] [PDF 12303KB](0)
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Melanin nanoparticle (MNP) was modified by polyethylene glycols (PEG), and the resulting compound (PEG-MNP) was obtained. The 68Ga labeled PEG-MNP was prepared by chelating radioactive 68Ga3+ ions with high labeling yield (95.6%±1.9%) and radiochemical purity (>95%). The stability of the labeling compound as well. Then 68Ga-PEG-MNP for simulating PM2.5 particles (particulate matter 2.5, size < 2.5 μm) was obtained through nebulization. After inhaling the nebulized particles, whole-body positron emission tomography (PET) in mice was performed. It revealed that nebulized 68Ga - PEG - MNP diffused from the trachea to the bilateral lobe area of the lungs and retained in the lungs. Quantification of PET images showed that the uptakes of the trachea and lung were (7.20±2.44)%·g-1, (4.46±1.04)%·g-1, (4.91±2.48)%·g-1, (4.71±2.39)%·g-1, (3.34±1.14)%·g-1, and (17.90±3.75)%·g-1, (18.10±4.52)%·g-1, (19.49±6.11)%·g-1, (19.19±2.83)%·g-1, (20.87±2.40)%·g-1 at 0 min, 30 min, 1 h, 2 h, 4 h after administration of the nebulized 68Ga-PEG-MNP, respectively. The results were highly consistent with the findings of ex-vivo radiographic autoradiography.
Preparation of nitrogen-doped porous carbons with ultra-high surface areas for high-performance supercapacitors
Zhaomei LIU , Wenshi ZHONG , Jiaxin LI , Gengshen HU
2024, 40(4): 677-685  doi: 10.11862/CJIC.20230404
[Abstract](55) [FullText HTML] [PDF 13334KB](0)
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N-doped porous carbons with ultra-high surface area was prepared by simple grinding and carbonization using sucrose as the carbon source, urea as the nitrogen source, and potassium oxalate as the activator. The effects of potassium oxalate and urea at different temperatures on the specific surface area, nitrogen content, and capacitive performance of carbons were investigated. The results showed that the specific surface area of KC- 800 prepared using only potassium oxalate as an activation agent was 1 114 m2·g-1, while the specific surface area of KNC-800 prepared using both potassium oxalate and urea was as high as 3 033 m2·g-1. In a three-electrode system, the specific capacitance of KNC-800 was 405 F·g-1 at the current density of 0.5 A·g-1, while the specific capacitance of KC-800 was only 248 F·g-1, indicating that the synergistic effect of potassium oxalate and urea can significantly improve the specific surface area and capacitive performance. The capacitance contribution analysis showed that both the electrical double-layer capacitance and pseudocapacitance values of KNC-800 were higher than those of KC-800. KNC-800 maintained an initial specific capacitance of 98.3% after 10 000 cycles at 0.5 A·g-1, demonstrating excellent cycling performance.
Energy storage and photoluminescence properties of Sm3+-doped Ba0.85Ca0.15Ti0.90Zr0.10O3 lead-free multifunctional ferroelectric ceramics
Ming ZHENG , Yixiao ZHANG , Jian YANG , Pengfei GUAN , Xiudong LI
2024, 40(4): 686-692  doi: 10.11862/CJIC.20230388
[Abstract](51) [FullText HTML] [PDF 10495KB](0)
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Sm3+-doped Ba0.85Ca0.15Ti0.90Zr0.10O3 (BCTZ∶xSm3+, x=0.0%, 0.2%, 0.4%, 0.6%, 0.8%, 1.0%, mole fraction) ceramics were synthesized using the conventional solid state reaction method, and their microstructure, ferroelectricity, energy storage performance, and photoluminescence (PL) properties were systematically investigated. The results showed that the mean grain size of the ceramics decreased obviously and the density increased significantly after the addition of Sm3+. All ceramics exhibited typical ferroelectric properties. Moreover, with the further increase of doping amount, the remanent polarization (Pr) gradually decreased to 8.432 μC·cm-2 (BCTZ: 1.0%Sm3+), and the ferroelectricity was suppressed. The energy storage density of BCTZ∶1.0%Sm3+ ceramic was improved by ca. 49.0% compared with that of pure BCTZ ceramic. In addition, BCTZ∶xSm3+ceramics exhibit strong orange-red luminescence at about 596 nm under light excitation at 408 nm, and the PL intensity can be adjusted by 449%.
Preparation and performance of N-doped carbon nanotubes composite Co3O4 as oxygen reduction reaction electrocatalysts
Hailang JIA , Hongcheng LI , Pengcheng JI , Yang TENG , Mingyun GUAN
2024, 40(4): 693-700  doi: 10.11862/CJIC.20230402
[Abstract](81) [FullText HTML] [PDF 16852KB](0)
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Carbon nanotube (CNT) was used as raw materials, loaded with vitamin B12, and then subjected to simple pyrolysis to obtain a nitrogen doped carbon nanotube (N/CNT) and loaded with low content Co3O4 nanoparticles (Co3O4@N/CNT) as an oxygen reduction reaction electrocatalyst. Due to the uniformly dispersed Co3O4 nanoparticles and N-doped effect, Co3O4@N/CNT exhibited excellent oxygen reduction reaction catalytic performance, with a half wave potential of 0.844 V (vs RHE), surpassing the performance of commercial Pt/C (0.820 V vs RHE). Compared to Pt/C, the zinc-air battery based on Co3O4@N/CNT exhibited better discharge performance and cycle stability.
Synthesis and photoelectric properties of fluorescence materials with electron donor-acceptor structures based on quinoxaline and pyridinopyrazine, carbazole, and diphenylamine derivatives
Yonghui ZHOU , Rujun HUANG , Dongchao YAO , Aiwei ZHANG , Yuhang SUN , Zhujun CHEN , Baisong ZHU , Youxuan ZHENG
2024, 40(4): 701-712  doi: 10.11862/CJIC.20230373
[Abstract](99) [FullText HTML] [PDF 9253KB](2)
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Four nitrogen heterocyclic fluorescent materials F1 - F4 with electron donor - acceptor structures were synthesized based on quinoxaline and pyridinopyrazine derivatives, which were constructed by the condensation reaction of α-diketone with o-phenylenediamine and pyridine diamine. Their photophysical properties were studied in detail. By testing of the fluorescence lifetimes and low-temperature fluorescence/phosphorescence spectra of F1-F4, combined with density functional theory calculations, it can be concluded that all four molecules are fluorescent small materials. Compounds F1-F4 showed photoluminescence spectra with peaks at 529, 464, 568, and 507 nm, respectively, with photoluminescence quantum efficiencies (PLQYs) of up to 98.2% in toluene. Additionally, positive solvatochromism was recorded from the emission spectra of four compounds in solvents with different polarities, further confirming their intramolecular charge transfer nature. Furthermore, the lifetimes of four compounds were 12.21, 2.61, 9.76, and 6.03 ns, respectively. To further explore the functionalized applications of these fluorescent molecules, they were doped as luminescent materials in organic light- emitting diodes (DF1 - DF4). Among them, devices DF1 and DF3 achieved maximum current efficiencies of 13.38 and 11.98 cd·A-1 and maximum external quantum efficiencies of 4.8% and 4.5% with low-efficiency roll-off, which are related to the high PLQYs of molecules F1 and F3.
A functionalized Eu3+ metal-organic framework for selective fluorescent detection of pyrene
Peiran ZHAO , Yuqian LIU , Cheng HE , Chunying DUAN
2024, 40(4): 713-724  doi: 10.11862/CJIC.20230355
[Abstract](80) [FullText HTML] [PDF 11493KB](1)
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A functional 3D lanthanide metal-organic framework (Eu-4L) was successfully designed and synthesized by solvothermal method. The ligand of Eu-4L is a kind of diphenylamine tetracarboxylic acid derivative (named H4L). The specific surface area of Eu-4L was high, which made Eu-4L have an excellent 3D structure. Eu-4L had good thermostability and can remain stable in water of pH from 3 to 11. Eu-4L can be used as a fluorescent probe for sensing pyrene. The limit of detection of Eu-4L for sensing pyrene was 5 μmol·L-1, which displays high sensitivity. Eu-4L is also a kind of recyclable material. The fluorescence sensing mechanism of Eu-4L for sensing pyrene belongs to the static mechanism. Moreover, the selectivity and competition of Eu-4L are also discussed.
Methyl-functionalized Cd-based metal-organic framework for highly sensitive electrochemical sensing of dopamine
Tiantian MA , Sumei LI , Chengyu ZHANG , Lu XU , Yiyan BAI , Yunlong FU , Wenjuan JI , Haiying YANG
2024, 40(4): 725-735  doi: 10.11862/CJIC.20230351
[Abstract](80) [FullText HTML] [PDF 7319KB](0)
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A Cd-based metal-organic framework (MOF) [Cd(BDC)(BPZ)(H2O)]n (1), where BPZ=3,3′,5,5′-tetramethyl-1H,1′H-4,4′-bipyrazole and H2BDC=terephthalic acid, was designed and synthesized. Compound 1 possesses a 3D pore structure with —CH3 groups and free carboxyl oxygen atoms on the pore walls. The presence of methyl groups significantly enhances the hydrophobicity and stability of MOF. Moreover, the methyl group and uncoordinated carboxyl oxygen atoms can interact with dopamine (DA) molecules through hydrogen bonding or van der Waals interactions, endowing in 1 with sensitive electrochemical sensing properties for DA. The differential pulse voltammetry (DPV) test of the prepared 1/GCE electrode showed that it had a wide linear range of 0.4 to 764.7 μmol·L-1 for detecting DA, and the detection limit was as low as 56.8 nmol·L-1. The DPV response current of the electrode remained unchanged in the presence of common interferents. When the electrode was applied for real sample analysis, the recovery rates ranged from 95.23% to 100.90%.
Nickel phosphide modified phosphorus doped gallium oxide for visible light photocatalytic water splitting to hydrogen
Bo YANG , Gongxuan LÜ , Jiantai MA
2024, 40(4): 736-750  doi: 10.11862/CJIC.20230346
[Abstract](72) [FullText HTML] [PDF 51277KB](0)
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Nickel phosphide (Ni2P) modified phosphorus doped gallium oxide (Ga2O3) (x-Ni2P/Ga2O3-Py, x represents the molar ratio of Ni2+ and Ga2O3, y represents the molar ratio of NaH2PO·H2O and Ga2O3) photocatalyst was prepared by impregnation and low temperature phosphating method using Ga2O3 semiconductor as a precursor. 5%-Ni2P/Ga2O3-P6 exhibits excellent photocatalytic hydrogen evolution activity in pure water and has a photo quantum efficiency of 0.22% under 430 nm monochromatic light irradiation. The mechanism study shows that phosphorus doping and Ni2P cocatalyst modification extend the photo-response range and promote carrier separation and migration efficiency. The long-term photocatalytic stability is better than that of a non-phosphating catalyst.
Effect of heterogeneous dual carbon sources on electrochemical properties of LiMn0.8Fe0.2PO4/C composites
Yuanchao LI , Weifeng HUANG , Pengchao LIANG , Zifang ZHAO , Baoyan XING , Dongliang YAN , Li YANG , Songlin WANG
2024, 40(4): 751-760  doi: 10.11862/CJIC.20230252
[Abstract](98) [FullText HTML] [PDF 24902KB](0)
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LiMn0.8Fe0.2PO4/C composite was synthesized using sucrose and graphite as heterogeneous carbon sources through a solid-state method assisted by aqueous rheological phase. The effect of different addition methods of graphite on electrochemical performances was studied. The LiMn0.8Fe0.2PO4/C composite was characterized by the X-ray diffraction (XRD), N2 adsorption-desorption, scanning electron microscopy (SEM), and transmission electron microscopy (TEM). The results showed that different graphite coating processes had obvious effects on the structure and electrochemical properties of the materials. The sample, which the graphite was added after the precursor was calcined, showed a high purity and uniform elliptic morphology. And its specific discharge capacity was 149 mAh·g-1 (87% of the theoretical specific capacity) at 0.1C. The specific discharge capacity was 133 mAh·g-1 at 5C. After 300 cycles at 2C, its capacity was maintained at 127 mAh·g-1, whose decay rate was 1.9%, showing excellent electrochemical performances.
Synthesis and antibacterial properties of silver-loaded sod-based zeolite
Yuhao SUN , Qingzhe DONG , Lei ZHAO , Xiaodan JIANG , Hailing GUO , Xianglong MENG , Yongmei GUO
2024, 40(4): 761-770  doi: 10.11862/CJIC.20230169
[Abstract](100) [FullText HTML] [PDF 14282KB](0)
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A series of sod-based zeolites (EMT, FAU, SOD) were synthesized by two-step method, and Ag+ was introduced by ion exchange method to obtain silver-loaded zeolite. X-ray diffraction (XRD) and scanning electron microscope (SEM) showed that the structure and grain size of the zeolite did not change significantly before and after ion exchange. It was proved by infrared (IR) and thermogravimetry (TG) that the silver bearing zeolite had good stability. The Ag+ release experiment and antibacterial activity test were carried out on the prepared silver-loaded zeolite, and the effects of zeolite type and grain size on antibacterial performance were investigated. The results showed that the cage structure of FAU and EMT zeolite had better antibacterial properties because they could store more Ag+, and the super cage structure of FAU zeolite had the best antibacterial properties. By comparing the antibacterial data of FAU zeolite with different grain sizes, it was found that the FAU zeolite with grain size of 100 nm had the best antibacterial performance and antibacterial life because of the abundant antibacterial active sites on the outer surface and the Ag+ could be stored and released continuously inside. The silver-loaded FAU zeolite with grain size of 10 nm had the fastest Ag+ release rate and the highest antibacterial efficiency due to its small grain size, large external specific surface area and short diffusion path. The factors affecting the antibacterial properties of silver-loaded zeolite were summarized.
C60-MoP-C nanoflowers van der Waals heterojunctions and its electrocatalytic hydrogen evolution performance
Wenjiang LI , Pingli GUAN , Rui YU , Yuansheng CHENG , Xianwen WEI
2024, 40(4): 771-781  doi: 10.11862/CJIC.20230289
[Abstract](99) [FullText HTML] [PDF 27022KB](0)
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Molybdenum phosphide-carbon nanoflowers (MoP-CFs) were prepared by the gas-solidification method, and C60 was modified on the surface of MoP-CFs to form van der Waals heterojunctions by simple ultrasonic self-assembly. It is found that the modification of C60 can effectively reduce the overpotential of electrocatalytic hydrogen evolution. Among all samples, 10% C60-MoP-CFs (10% was the mass fraction of C60) exhibited the best catalytic activity with overpotentials of 158 and 157 mV to achieve a current density of 10 mA·cm-2 in acidic and alkaline conditions, respectively. Moreover, this sample also showed good stability which could work stably for more than 20 h. The strong electron coupling between C60 and MoP-CFs promotes electron migration from C60 to the surface of MoP-CFs, reduces the charge transport resistance, and accelerates the electrocatalytic hydrogen evolution interface reaction kinetics process.
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