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Reaction Mechanism and Strategy for Optimizing the Hydrogen Evolution Reaction on Single-Layer 1T′ WSe2 and WTe2 Based on Grand Canonical Potential Kinetics

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    Surfaces, Interfaces, and Applications

    Reaction Mechanism and Strategy for Optimizing the Hydrogen Evolution Reaction on Single-Layer 1T′ WSe2 and WTe2 Based on Grand Canonical Potential Kinetics
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    • Jie Song
      Jie Song
      Materials and Process Simulation Center and Joint Center for Artificial Photosynthesis, California Institute of Technology, Pasadena, California 91125, United States
      Hefei National Laboratory for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, Anhui 230026, China
      More by Jie Song
      Orcidhttps://orcid.org/0000-0002-3936-8983
    • Soonho Kwon
      Soonho Kwon
      Materials and Process Simulation Center and Joint Center for Artificial Photosynthesis, California Institute of Technology, Pasadena, California 91125, United States
      More by Soonho Kwon
      Orcidhttps://orcid.org/0000-0002-9225-3018
    • Md Delowar Hossain
      Md Delowar Hossain
      Materials and Process Simulation Center and Joint Center for Artificial Photosynthesis, California Institute of Technology, Pasadena, California 91125, United States
      More by Md Delowar Hossain
    • Sheng Chen
      Sheng Chen
      Hefei National Laboratory for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, Anhui 230026, China
      More by Sheng Chen
    • Zhenyu Li*
      Zhenyu Li
      Hefei National Laboratory for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, Anhui 230026, China
      *Email: [email protected]
      More by Zhenyu Li
      Orcidhttps://orcid.org/0000-0003-2112-9834
    • William A. Goddard*
      William A. Goddard
      Materials and Process Simulation Center and Joint Center for Artificial Photosynthesis, California Institute of Technology, Pasadena, California 91125, United States
      *Email: [email protected]
      More by William A. Goddard
      Orcidhttps://orcid.org/0000-0003-0097-5716
    Other Access OptionsSupporting Information (1)

    ACS Applied Materials & Interfaces

    Cite this: ACS Appl. Mater. Interfaces 2021, 13, 46, 55611–55620
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    https://doi.org/10.1021/acsami.1c14234
    Published November 15, 2021
    Copyright © 2021 American Chemical Society
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    Abstract

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    Transition-metal dichalcogenides (TMDs) in the 1T′ phase are known high-performance catalysts for hydrogen evolution reaction (HER). Many experimental and some theoretical studies report that vacant sites play an important role in the HER on the basal plane. To provide benchmark calculations for comparison directly with future experiments on TMDs to obtain a validated detailed understanding that can be used to optimize the performance and material, we apply a recently developed grand canonical potential kinetics (GCP-K) formulation to predict the HER at vacant sites on the basal plane of the 1T′ structure of WSe2 and WTe2. The accuracy of GCP-K has recently been validated for single-crystal nanoparticles. Using the GCP-K formulation, we find that the transition-state structures and the concentrations of the four intermediates (0–3 H at the selenium or tellurium vacancy) change continuously as a function of the applied potential. The onset potential (at 10 mA/cm–2) is −0.53 V for WSe2 (experiment is −0.51 V) and −0.51 V for WTe2 (experiment is −0.57 V). We find multistep reaction mechanisms for H2 evolution from Volmer–Volmer–Tafel (VVT) to Volmer–Heyrovsky (VH) depending on the applied potential, leading to an unusual non-monotonic change in current density with the applied potential. For example, our detailed understanding of the reaction mechanism suggests a strategy to improve the catalytic performance significantly by alternating the applied potential periodically.

    Copyright © 2021 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsami.1c14234.

    • Fitted parameters of free energy and physical quantities for various WSe2 and WTe2 species; derivation of GCP (U) equation; quadratic behavior of GCP curves; validation that a doubled unit cell leads to negligible changes; changes in concentrations of WTe2 four intermediate states for the APS 6, explanation of why the free energy barrier of Tafel reaction increases as the applied potential becomes more negative; Python code used to analyze the data; and geometries (VASP POSCAR format) (PDF)

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    Cited By

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    This article is cited by 10 publications.

    1. Mohsen Tamtaji, Soonho Kwon, Charles B. Musgrave, III, William A. Goddard, III, GuanHua Chen. Reaction Mechanism of Rapid CO Electroreduction to Propylene and Cyclopropane (C3+) over Triple Atom Catalysts. ACS Applied Materials & Interfaces 2024, 16 (38) , 50567-50575. https://doi.org/10.1021/acsami.4c06257
    2. Bushra Rehman, K.M.M.D.K. Kimbulapitiya, Manisha Date, Chieh-Ting Chen, Ruei-Hong Cyu, Yu-Ren Peng, Mayur Chaudhary, Feng-Chuan Chuang, Yu-Lun Chueh. Rational Design of Phase-Engineered WS2/WSe2 Heterostructures by Low-Temperature Plasma-Assisted Sulfurization and Selenization toward Enhanced HER Performance. ACS Applied Materials & Interfaces 2024, 16 (25) , 32490-32502. https://doi.org/10.1021/acsami.4c03513
    3. Cooper R. Tezak, Nicholas R. Singstock, Abdulaziz W. Alherz, Derek Vigil-Fowler, Christopher A. Sutton, Ravishankar Sundararaman, Charles B. Musgrave. Revised Nitrogen Reduction Scaling Relations from Potential-Dependent Modeling of Chemical and Electrochemical Steps. ACS Catalysis 2023, 13 (19) , 12894-12903. https://doi.org/10.1021/acscatal.3c01978
    4. Silvio Osella, William A. Goddard III. CO2 Reduction to Methane and Ethylene on a Single-Atom Catalyst: A Grand Canonical Quantum Mechanics Study. Journal of the American Chemical Society 2023, 145 (39) , 21319-21329. https://doi.org/10.1021/jacs.3c05650
    5. William A. Goddard, Jie Song. Grand Canonical Quantum Mechanics with Applications to Mechanisms and Rates for Electrocatalysis. Topics in Catalysis 2023, 54 https://doi.org/10.1007/s11244-023-01794-8
    6. Faisal Rehman, Soonho Kwon, Md Delowar Hossain, Charles B. Musgrave III, William A. Goddard III, Zhengtang Luo. Reaction mechanism and kinetics for N 2 reduction to ammonia on the Fe–Ru based dual-atom catalyst. Journal of Materials Chemistry A 2022, 10 (43) , 23323-23331. https://doi.org/10.1039/D2TA06826E
    7. Fei Guo, Zhuo Liu, Jie Xiao, Xiaoyuan Zeng, Chengxu Zhang, Yan Lin, Peng Dong, Tingting Liu, Yingjie Zhang, Mian Li. Cobalt-embedded in ultrahigh boron and nitrogen codoped hierarchically porous carbon nanowires as excellent catalysts toward water splitting. Chemical Engineering Journal 2022, 446 , 137111. https://doi.org/10.1016/j.cej.2022.137111
    8. Haihua Huang, Guowei Hu, Chengchao Hu, Xiaofeng Fan. Enhanced Hydrogen Evolution Reactivity of T’-Phase Tungsten Dichalcogenides (WS2, WSe2, and WTe2) Materials: A DFT Study. International Journal of Molecular Sciences 2022, 23 (19) , 11727. https://doi.org/10.3390/ijms231911727
    9. Mamutjan Tursun, Chao Wu. Electrocatalytic Reduction of N 2 to NH 3 Over Defective 1T′‐WX 2 (X=S, Se, Te) Monolayers. ChemSusChem 2022, 15 (11) https://doi.org/10.1002/cssc.202200191
    10. Tadele Hunde Wondimu, Anteneh Wodaje Bayeh, Daniel Manaye Kabtamu, Qian Xu, Puiki Leung, Akeel Abbas Shah. Recent progress on tungsten oxide-based materials for the hydrogen and oxygen evolution reactions. International Journal of Hydrogen Energy 2022, 47 (47) , 20378-20397. https://doi.org/10.1016/j.ijhydene.2022.04.226
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    ACS Applied Materials & Interfaces

    Cite this: ACS Appl. Mater. Interfaces 2021, 13, 46, 55611–55620
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acsami.1c14234
    Published November 15, 2021
    Copyright © 2021 American Chemical Society
    Request reuse permissions

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