ELECTROCHIMICA ACTA
·
2021
·
IF 6.901
He-Qiang Chang,Guo-Hua Zhang,Kuo-Chih Chou
Electrochemical water splitting is considered a sustainable route for the hydrogen industry. In this work, Mo 2 C/MoC heterostructure supported on N -doped carbon (Mo 2 C/MoC@NC) was prepared via a carbonization strategy. For the product (Mo 2 C/MoC@NC-1-2) fabricated with a g-C 3 N 4 / ammonium molybdate tetrahydrate molar ratio of 1:2 at 700 °C under 10%CH 4 /H 2 atmosphere, a high stability and good HER activity with a η 10 of 113 mV in 1M KOH were achieved. To further enhance the catalytic performance of the synthesized Mo 2 C/MoC@NC, the phosphating strategy was proposed for the preparation of Mo 2 C/MoC/MoP heterostructure supported on N-doped carbon (Mo 2 C/MoC/MoP@NC). When the precursor Mo 2 C/MoC@NC-1-2 was phosphated at 650 °C with a heating rate of 5 °C min −1 and kept for 0 min, the as-synthesized Mo 2 C/MoC/MoP@NC-650-0 exhibits good HER catalytic activity with a pretty low η 10 of 78 mV, a j 0 of 0.398 mA cm −2 , and a Tafel slope of 52 mV dec −1 in 1M KOH. This good activity of HER can be ascribed to the N-doped carbon as substrate and the construction of transition metal-based heterostructures.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
FUEL
·
2022
·
IF 8.035
Qingtao Wang,Liqiu Huang,Huiping Liu,Yanxia Wu,Guofu Ma,Ziqiang Lei,Shufang Ren
As a sustainable and green technology for producing high-purity hydrogen, hydrogen evolution reaction (HER) has received extensive attention. The development of an electrocatalyst with good HER activity is the key to economic water electrolysis. Here, this work reports a defect-mediated successive ion layer adsorption and reaction method to construct Ag 2 S/irradiated Sb 2 Te 3 heterojunctions with good HER activity. First, ion irradiation is used to introduce a large number of defects into Sb 2 Te 3 . The defective Sb 2 Te 3 is continuously cyclically immersed in AgNO 3 solution and Na 2 S solution. Ag + and S 2- ions are adsorbed on the defect sites of Sb 2 Te 3 and deposited as Ag 2 S and the heterojunction of Ag 2 S/irradiated Sb 2 Te 3 is obtained. By this strategy, the electrochemical active surface area of the material is increased, reduces the charge transfer resistance, and improves the hydrophilicity of the material surface, thus exhibiting good HER activity. In this work, ion irradiation is used to regulate the surface defects of materials and then to regulate the growth of heterojunction to achieve the purpose of regulating the properties of material. The heterojunction growth method controlled by defect engineering can be widely used in the preparation of heterojunction materials in other energy and environmental fields.
研究领域:
材料科学
·
电催化
·
能源转换
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2024
·
IF 8.1
Guangxia Wang,Wenhui Wang,Xiuwei Sun,Liwen Zhou,Yongming Sui,Fuxin Wang,Dezhou Zheng,Zheng Liu,Qi Feng
Developing highly efficient catalysts for the hydrogen evolution reaction (HER) is crucial for advancing renewable hydrogen energy technologies. Heterophase nanomaterials have shown great promise in catalysis, owing to the synergistic effect among various phases and the abundance of active sites located at the phase boundaries or interfaces. However, achieving precise control over these phase structures during synthesis remains a significant challenge. In this work, we explored a one-pot synthesis method for amorphous/crystalline heterophase Rh nanoparticles, with crystallinity tunable by adjusting the quantity of urea and reaction duration. Due to the increased electrochemical active sites, enhanced electron transport, the resulting amorphous/crystalline heterophase Rh exhibits superior HER activities in both acidic (with an overpotential of 27 mV) and alkaline media (with an overpotential of 21 mV), surpassing that of commercial Pt/C and crystalline Rh. Theoretical calculations indicate that the amorphous/crystalline structure reduces the kinetic barrier for water splitting and optimizes adsorption free energy of hydrogen (ΔG H∗ ), thereby enabling the catalyst to exhibit significantly enhanced HER performance. This exploration offers a valuable reference for designing amorphous/crystalline heterophase structures and demonstrates the great potential of phase engineering strategy in the development of electrocatalysts.
研究领域:
材料科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
Materials Today Energy
·
2020
·
IF 5.604
L. Zheng,W. Zhang,B. Gao,H. Lu,X. Fan,Y. Zhang,Y. Wang,S. Wang,Q. Gao,Y. Tang
Transition metal dichalcogenides (TMDs) are regarded as the inexpensive and stable electrocatalysts for hydrogen evolution reaction (HER). Designing an electrocatalyst with few-layered molybdenum disulfide (MoS 2 ) is one of the most effective methods to enhance the activity and durability for HER due to its abundant exposed rim-sites, fast electron transfer and high chemical stability. Herein, a green and facile one-pot approach is developed to synthesize few-layered MoS 2 /nitrogen, sulfur codoped porous carbon (MoS 2 /NSPC) electrocatalyst via pyrolyzing the in-situ formed molybdate-melamine complex (MoO x -MEL) within the self-assembled networks of melamine-trithiocyanuric acid (MT). The optimal MoS 2 /NSPC electrocatalyst exhibits excellent HER stability and activity with overpotential of 114 mV at 10 mA cm −2 in 0.5 M H 2 SO 4 . Furthermore, few-layered tungsten disulfide anchored on N, S-codoped porous carbon (WS 2 /NSPC) with high HER activity can also be successfully synthesized by this strategy. It paves a universal way to design active sites–enriched few-layered dichalcogenides with high performance in the applications from energy conversion to storages.
研究领域:
材料科学
·
能源化学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Energy Chemistry
·
2025
·
IF 14.9
Shipeng Geng,Liming Chen,Yinlong Wu,Yi Wang,Shuqin Song
Designing efficient and durable hydrogen evolution reaction (HER) catalysts for seawater electrolysis is crucial for large-scale hydrogen production. Here, we introduce a theory-driven design of metal/WN electrocatalysts, with metal strongly coupled to lattice-matched WN. Theoretical calculations for Pt/WN reveal that W sites enhance H 2 O adsorption/dissociation, optimizing Pt’s H binding. The prepared Pt/WN@CP nanorod can catalyze HER with low overpotentials of 107 and 113 mV at 500 mA cm −2 in alkaline water/seawater, respectively, surpassing Pt/C. Extended calculations and experiments show that the optimized Ni/WN@CP-90 achieves an optimal Δ G H* and overpotential of 219 mV at 500 mA cm −2 in alkaline seawater, demonstrating the versatility of the WN support to promote HER activity. Notably, the anion exchange membrane water electrolyzer (AEMWE) constructed by Pt/WN@CP or Ni/WN@CP-90 with NiFe-LDH@NF demonstrates outstanding hydrogen production activity with excellent Faraday efficiency (∼100%) and durability (120 h), indicating the potential application of WN-supported catalysts for efficient, stable seawater electrolysis.
研究领域:
材料科学
·
电化学
·
可再生能源
✓ 已验证
产品关联
DOI
高影响因子
Particuology
·
2022
·
IF 3.251
Chao Song,Yuhua Liu,Chengxiang Huang,Miao Liu,Nailin Yue,Zunhao Zhang,Zizhun Wang,Xu Zou,Wei Zhang,Weitao Zheng
Through inverted-design rather than modifying the generally-assumed S active sites in popular MoS 2 , we unlock the potential of Mo sites and successfully prepared novel MoS 2 @Ni 3 S 2 /NF core-shell nanospheres as a catalyst for the high-performance hydrogen evolution reaction (HER). The ΔG H at the Mo site is optimized via Ni 3 S 2 to achieve excellent HER activity. At low current densities, it has similar activity to the Pt/C. However, its performance is better than Pt/C at high density. Moreover, our catalyst shows a considerable stability at a variety of current densities for 50 h, promising to substitute noble metal catalysts in application of commercial alkaline electrocatalysts .
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Materials Chemistry A
·
2021
·Vol. 9
·期 30
·16427-16435
·
IF 12.732
Xue Zhao,Mai Zheng,Zhenyang Zhang,Yufeng Wang,Yingtang Zhou,Xiaohai Zhou,Haibo Zhang
Electrochemical hydrogen evolution reaction (HER) is a green and convenient way to produce hydrogen with high calorific value and zero environmental pollution, but the precious metal Pt, which catalyzes its efficient operation, faces the dilemma of resource scarcity. Before finding an HER catalyst to replace platinum-based materials, morphology control engineering can achieve high-efficiency hydrogen production with a lower platinum input. Here, we used a supramolecular assembly (host: cucurbituril[7]; guest: closo-[B12H12]2−) with weak reducibility as a carrier to convert Pt4+ into ultrafine and highly dispersed Pt nanoparticles (BOPs@Pt) in situ, and the supported Pt-based catalyst (BC3N@Pt) obtained after pyrolysis had the ability to very efficiently catalyze HER. BC3N@Pt exhibited excellent performance in catalyzing HER in the full pH range. Among them, the overpotentials to achieve a current density of 10 mA cm−2 in the media of pH = 14, pH = 7 and pH = 1 were only 26.1 mV, 38.5 mV and 23.1 mV, respectively, and the corresponding Tafel slopes were as low as 41.59 mV dec−1, 59.05 mV dec−1, and 61.07 mV dec−1, respectively. In terms of mass activity, the rate of HER driven by BC3N@Pt was at least three times than that achieved with the commercial 20 wt% Pt/C. The density functional theory (DFT) calculations verified that B doped on CN changes the local electronic distribution, facilitates water dissociation and hydrogen adsorption, and hence enhances the HER activity. The annealing treatment converts the organic polymer into an inorganic BC3N matrix, which not only accelerates the electron transfer rate in HER, but also ensures the stability of BCN@Pt when catalyzing HER in the entire pH range.
研究领域:
材料科学
·
电化学
·
理论计算
✓ 已验证
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2021
·
IF 19.503
Jiadong Chen,Minkai Qin,Shuangxiu Ma,Ruxue Fan,Xiaozhong Zheng,Shanjun Mao,Chunhong Chen,Yong Wang
Increasing OH* adsorption to promote water dissociation while reducing H* adsorption to accelerate hydrogen generation kinetics is an effective solution to further improve the HER activity of Pt-based catalysts. Herein, we have successfully constructed a Pt/PtTe x heterogeneous catalysis interface by electrochemical activation of PtTe 2 nanorods (NRs). The reduction of H* adsorption and significant increase of OH* adsorption was observed on Pt/PtTe x heterojunction via cyclic voltammetry method. Theoretical calculations indicate that Gibbs free energy change (ΔG) of H* is closer to 0.00 eV and ΔG of OH* decreased from 1.36 eV of Pt (111) to −0.40 eV of Pt/PtTe x , which reinforces the experimental results. The rational modulation of adsorbed intermediates endows Pt/PtTe x NRs with exceptionally lower Tafel slopes of 16 and 23 mV dec −1 in 0.5 M H 2 SO 4 and 1.0 M KOH electrolytes, which is among the best reported HER electrocatalysts.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Hongqiang Xin,Lan Sun,Yiwei Zhao,Yuanjiang Lv,Qiaomei Luo,Shengwu Guo,Danyang Li,Ce Mu,Bo Huang,Fei Ma
Abundant of defective regions and oxygen-containing groups on graphene oxide (GO) could promote the nucleation and growth of metallic nanoparticles . In this work, the composite catalyst is synthesized by pyrolysis of the mixture powder of GO and rhodium organometallic reactant at 900 °C, Ar atmosphere and low pressure, in which dispersive Rh 2 P nanoparticles are uniformly attached on reduced graphene oxide (Rh 2 P/RGO). The sizes of Rh 2 P nanoparticles are controllable by adjusting the mass proportion of reactants. For the optimized size of Rh 2 P nanoparticles at 6.0 nm, only 11.7 and 10.3 mV of the overpotentials are required at the current density of 10 mA cm −2 in 0.5 M H 2 SO 4 and 1 M KOH electrolytes, respectively, exhibiting superior HER activity over the commercial Pt/C. Theoretical calculations indicate that the hydrogen adsorption free energy of Rh 2 P/RGO composites is close to zero, and Bede charge analysis confirms the accelerated electron transport between the RGO and Rh 2 P. Therefore, the introduction of RGO substrate could not only promote a uniform distribution and tunable size of Rh 2 P NPs, but also be advantageous to the electron transport from RGO to Rh 2 P NPs, and a favorable H 2 evolution during the HER process. This work provides a facile strategy to control the size of metal phosphide nanoparticles on RGO for the design of advanced HER electrocatalysts .
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Energy Materials
·
2018
·
IF 0
Xiaorong Gan,Lawrence Yoon Suk Lee,Kwok-yin Wong,Tsz Wing Lo,Kwun Hei Ho,Dang Yuan Lei,Huimin Zhao
The phase transition of multilayer MoS2 nanosheets from semiconducting 2H to metallic 1T (2H/1T) has been realized mainly by chemical methods (e.g., Li intercalation). Here, we develop a simple yet effective method, cyclic voltammetry, to successfully tune the 2H/1T phase transition of multilayer MoS2 nanosheets without using intercalation species. The phase transition is triggered by the electrochemical incorporation of S vacancies (obtained by electrochemical etching), which on the one hand injects electrons into the framework of S–Mo–S and on the other hand facilitates the sliding of S planes. Density functional theory calculations show that O doping in the framework of S–Mo–S decreases the energy barrier for forming S vacancies and stabilizes the 1T-phase by occupying the 4d orbital of Mo. Our calculations further show that the presence of S vacancies and O incorporation not only reduces the bandgap of MoS2, indicating an increased conductivity, but also decreases the hydrogen adsorption free energy, implying significant improvement of hydrogen evolution reaction (HER) activity. Indeed, the overpotential and Tafel plot of the electrochemically treated MoS2 nanosheets are decreased respectively by 174 mV and 25 mV/dec at a cathodic current density of 10 mA cm–2 compared with pristine 2H-MoS2 nanosheets. The HER experiment also reveals the order of catalytical activity for the studied phases and structural defects: 1T-MoS2 > S vacancies > O doping >2H-MoS2. Our study has provided a new route to control the phase transition of multilayer MoS2 nanosheets with promising applications potentially in catalysis and optoelectronics.
研究领域:
材料科学
·
电化学
·
催化
·
纳米技术
·
理论化学
✓ 已验证
产品关联
DOI
JOURNAL OF ALLOYS AND COMPOUNDS
·
2021
·
IF 5.316
Yuxiao Gong,Lian-Hua Xu,Junji Li,Dan Shan
Research of highly dispersed transition metal phosphides (TMPs)-based catalysts for electrocatalytic hydrogen evolution is of great significance in the area of renewable energy. Herein, the high dispersion of FeNiP nanoparticles on N, P-doped electrospun carbon fibers was realized via the confinement effect induced by phytic acid (PA) and polyacrylonitrile (PAN), as well as electrospinning technique. PA and PAN were used as ligand for coordinating transition metal (TM) ions and carbon sources, respectively. In addition, the nucleophilic addition reaction between PA and PAN resulted in the cyclization of PAN and the further formation of a supramolecular network. Besides, the chelating ability of PA to TM ions was also modulated. Benefitting from the confinement effect, the optimized FeNiP/NPC800 exhibit good hydrogen evolution reaction (HER) activities for achieving a current density of 10 mA cm −2 at an overpotential of 277 mV in 0.5 M H 2 SO 4 .
研究领域:
材料科学
·
电化学
·
可再生能源
✓ 已验证
产品关联
DOI
高影响因子
Advanced Materials Interfaces
·
2017
·Vol. 4
·期 12
·1700005
·
IF 4.279
Juan Wang,Jia Wei Chen,Jia Dong Chen,Han Zhu,Ming Zhang,Ming Liang Du
Well-dispersed Pt Cu alloy nanoparticles (NPs) with a diameter of only ≈2 nm encapsulated in carbon nanofibers (CNFs) are synthesized using electrospinning technology followed by a graphitization process in a chemical vapor deposition furnace. Distinctly, even with a small amount of Pt, the Pt Cu/CNFs-1:2 catalyst possesses outstanding hydrogen evolution reaction (HER) activity, including small overpotential, long-term stability, and a high exchange current density as well as large double layer capacitance ( C dl ). The excellent HER performance of the Pt Cu/CNFs-1:2 catalyst is attributed to the synergistic interaction between Pt and Cu, the uniform distribution of the alloy NPs and the use of CNFs with 3D architectures. This development may provide a simple, efficient, and green synthesis method to design bi- or multimetal alloys for use as the cathode electrocatalysts for the HER or other electrocatalytic devices.
研究领域:
材料科学
·
电化学
·
纳米技术
·
催化
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）