Self-optimizing, highly surface-active layered metal dichalcogenide catalysts for hydrogen evolution [Surface-active metal dichalcogenide electrocatalysts with self-improving performance for hydrogen evolution]
Abstract
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.
- Authors:
-
- 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
- Publication Date:
- Research Org.:
- Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)
- Sponsoring Org.:
- USDOE National Nuclear Security Administration (NNSA)
- OSTI Identifier:
- 1461742
- Report Number(s):
- LLNL-JRNL-659614
Journal ID: ISSN 2058-7546; 780651
- Grant/Contract Number:
- AC52-07NA27344
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nature Energy
- Additional Journal Information:
- Journal Volume: 2; Journal Issue: 9; Journal ID: ISSN 2058-7546
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 77 NANOSCIENCE AND NANOTECHNOLOGY; 36 MATERIALS SCIENCE; 30 DIRECT ENERGY CONVERSION
Citation Formats
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., and Yakobson, Boris I. Self-optimizing, highly surface-active layered metal dichalcogenide catalysts for hydrogen evolution [Surface-active metal dichalcogenide electrocatalysts with self-improving performance for hydrogen evolution]. United States: N. p., 2017.
Web. doi:10.1038/nenergy.2017.127.
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. Self-optimizing, highly surface-active layered metal dichalcogenide catalysts for hydrogen evolution [Surface-active metal dichalcogenide electrocatalysts with self-improving performance for hydrogen evolution]. United States. https://doi.org/10.1038/nenergy.2017.127
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., and Yakobson, Boris I. Mon .
"Self-optimizing, highly surface-active layered metal dichalcogenide catalysts for hydrogen evolution [Surface-active metal dichalcogenide electrocatalysts with self-improving performance for hydrogen evolution]". United States. https://doi.org/10.1038/nenergy.2017.127. https://www.osti.gov/servlets/purl/1461742.
@article{osti_1461742,
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]},
author = {Liu, Yuanyue and Wu, Jingjie and Hackenberg, Ken P. and Zhang, Jing and Wang, Y. Morris and Yang, Yingchao and Keyshar, Kunttal and Gu, Jing and Ogitsu, Tadashi and Vajtai, Robert and Lou, Jun and Ajayan, Pulickel M. and Wood, Brandon C. and Yakobson, Boris I.},
abstractNote = {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.},
doi = {10.1038/nenergy.2017.127},
journal = {Nature Energy},
number = 9,
volume = 2,
place = {United States},
year = {Mon Jul 31 00:00:00 EDT 2017},
month = {Mon Jul 31 00:00:00 EDT 2017}
}
Web of Science
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Niobium disulphide (NbS$_2$)-based (heterogeneous) electrocatalysts for an efficient hydrogen evolution reaction
text, January 2020
- Najafi, Leyla; Bellani, Sebastiano; Oropesa-Nuñez, Reinier
- arXiv
Extending the colloidal transition metal dichalcogenide library to ReS2 nanosheets for application in gas sensing and electrocatalysis
text, January 2020
- Martin-Garcia, Beatriz; Spirito, Davide; Bellani, Sebastiano
- arXiv