Self-optimizing, highly surface-active layered metal dichalcogenide catalysts for hydrogen evolution [Surface-active metal dichalcogenide electrocatalysts with self-improving performance for hydrogen evolution]

Liu, Yuanyue; Wu, Jingjie; Hackenberg, Ken P.; Zhang, Jing; Wang, Y. Morris; Yang, Yingchao; Keyshar, Kunttal; Gu, Jing; Ogitsu, Tadashi; Vajtai, Robert; Lou, Jun; Ajayan, Pulickel M.; Wood, Brandon C.; Yakobson, Boris I.

doi:10.1038/nenergy.2017.127

Title: Self-optimizing, highly surface-active layered metal dichalcogenide catalysts for hydrogen evolution [Surface-active metal dichalcogenide electrocatalysts with self-improving performance for hydrogen evolution]

Journal Article · Mon Jul 31 00:00:00 EDT 2017 · Nature Energy

DOI:https://doi.org/10.1038/nenergy.2017.127· OSTI ID:1461742

^[1]; Wu, Jingjie ^[2]; Hackenberg, Ken P. ^[2];

^[2]; Wang, Y. Morris ^[3]; Yang, Yingchao ^[2]; Keyshar, Kunttal ^[2]; Gu, Jing ^[4]; Ogitsu, Tadashi ^[3];

^[2]; Lou, Jun ^[2]; Ajayan, Pulickel M. ^[2]; Wood, Brandon C. ^[3]; Yakobson, Boris I. ^[5]

Rice Univ., Houston, TX (United States); California Inst. of Technology (CalTech), Pasadena, CA (United States)
Rice Univ., Houston, TX (United States)
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
San Diego State Univ., San Diego, CA (United State)
Rice Univ., Houston, TX (United States

Low-cost, layered transition-metal dichalcogenides (MX₂) based on molybdenum and tungsten have attracted substantial interest as alternative catalysts for the hydrogen evolution reaction (HER). These materials have high intrinsic per-site HER activity; however, a significant challenge is the limited density of active sites, which are concentrated at the layer edges. Here we unravel electronic factors underlying catalytic activity on MX₂ surfaces, and leverage the understanding to report group-5 MX₂ (H-TaS₂ and H-NbS₂) electrocatalysts whose performance instead mainly derives from highly active basal-plane sites, as suggested by our first-principles calculations and performance comparisons with edge-active counterparts. Beyond high catalytic activity, they are found to exhibit an unusual ability to optimize their morphology for enhanced charge transfer and accessibility of active sites as the HER proceeds, offering a practical advantage for scalable processing. In conclusion, the catalysts reach 10 mA cm^–2 current density at an overpotential of ~50–60 mV with a loading of 10–55 μg cm^–2, surpassing other reported MX₂ candidates without any performance-enhancing additives.

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Research Organization:: Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: AC52-07NA27344

OSTI ID:: 1461742

Report Number(s):: LLNL-JRNL-659614; 780651

Journal Information:: Nature Energy, Vol. 2, Issue 9; ISSN 2058-7546

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 296 works

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One-step synthesis of a hierarchical self-supported WS ₂ film for efficient electrocatalytic hydrogen evolution Wang, Min; Zhang, Li; Huang, Meirong Journal of Materials Chemistry A, Vol. 7, Issue 39 https://doi.org/10.1039/c9ta07868a	journal	January 2019
Recent progress in the controlled synthesis of 2D metallic transition metal dichalcogenides Zhang, Zhepeng; Yang, Pengfei; Hong, Min Nanotechnology, Vol. 30, Issue 18 https://doi.org/10.1088/1361-6528/aaff19	journal	February 2019
Preparation and Physical and Photocatalytic Activity of a New Niobate Oxide Material Containing NbO ₄ Tetrahedra Pan, Hengkai; Wang, Bei; Zhang, Feng International Journal of Photoenergy, Vol. 2018 https://doi.org/10.1155/2018/8516356	journal	September 2018
Activation of MoS ₂ Basal Planes for Hydrogen Evolution by Zinc Wu, Wenzhuo; Niu, Chunyao; Wei, Cong Angewandte Chemie, Vol. 131, Issue 7 https://doi.org/10.1002/ange.201812475	journal	January 2019
Doping‐Induced Amorphization, Vacancy, and Gradient Energy Band in SnS ₂ Nanosheet Arrays for Improved Photoelectrochemical Water Splitting Meng, Linxing; Wang, Siyu; Cao, Fengren Angewandte Chemie International Edition, Vol. 58, Issue 20 https://doi.org/10.1002/anie.201902411	journal	May 2019
Niobium disulphide (NbS$_2$)-based (heterogeneous) electrocatalysts for an efficient hydrogen evolution reaction Najafi, Leyla; Bellani, Sebastiano; Oropesa-Nuñez, Reinier arXiv https://doi.org/10.48550/arxiv.2003.03257	text	January 2020
Extending the colloidal transition metal dichalcogenide library to ReS2 nanosheets for application in gas sensing and electrocatalysis Martin-Garcia, Beatriz; Spirito, Davide; Bellani, Sebastiano arXiv https://doi.org/10.48550/arxiv.2005.13022	text	January 2020

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