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Self-optimizing, highly surface-active layered metal dichalcogenide catalysts for hydrogen evolution

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. (2017) Self-optimizing, highly surface-active layered metal dichalcogenide catalysts for hydrogen evolution. Nature Energy, 2 (9). Art. No. 17127. ISSN 2058-7546.

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Low-cost, layered transition-metal dichalcogenides (MX_2) 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 MX_2 surfaces, and leverage the understanding to report group-5 MX_2 (H-TaS_2 and H-NbS_2) 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. 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.

Item Type:Article
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URLURL TypeDescription ReadCube access
Liu, Yuanyue0000-0002-5880-8649
Vajtai, Robert0000-0002-3942-8827
Ajayan, Pulickel M.0000-0001-8323-7860
Additional Information:© 2017 Macmillan Publishers Limited, part of Springer Nature. We thank W. Zhou (ORNL), W. I. Choi (LLNL), A. Mohite and G. Gupta (LANL) for valuable discussions. B.C.W. and Y.L. acknowledge funding from LLNL LDRD Grant 12-ERD-053, with computing support from the LLNL Institutional Computing Grand Challenge Program. T.O. and B.C.W. acknowledge additional support from the US Department of Energy (DOE) Fuel Cell Technologies Office. Y.M.W. acknowledges the UCOP funding support on mesoscopic 2D materials. A portion of this work was performed under the auspices of the US DOE by LLNL under Contract DE-AC52-07NA27344. K.P.H. acknowledges funding from PIRE-2 Grant OISE-0968405. J.W. and K.K. acknowledge funding from MURI 2D Grant W911NF-11-1-0362. Y.Y., J.Z. and J.L. acknowledge support from the Welch Foundation grant C-1716. Y.L. and B.I.Y. acknowledge support from the Office of Naval Research Grant N00014-15-1-2372 and the Army Research Office Grant W911NF-16-1-0255. This work used computing resources sponsored by the DOE Office of EERE at NREL, and the NSF XSEDE Grant ACI-1053575. Author Contributions: Y.L. conceived the idea and performed the theory calculations with guidance from T.O., B.C.W. and B.I.Y. K.P.H. synthesized the samples. J.W. performed the electrochemical testing. J.W. and K.P.H. performed a majority of the materials characterization, under the guidance of R.V., J.L. and P.M.A. Other authors provided additional sample characterization. The authors declare no competing financial interests.
Funding AgencyGrant Number
Lawrence Livermore National Laboratory12-ERD-053
Department of Energy (DOE)UNSPECIFIED
University of CaliforniaUNSPECIFIED
Department of Energy (DOE)DE-AC52-07NA27344
Army Research Office (ARO)W911NF-11-1-0362
Robert A. Welch FoundationC-1716
Office of Naval Research (ONR)N00014-15-1-2372
Army Research Office (ARO)W911NF-16-1-0255
Issue or Number:9
Record Number:CaltechAUTHORS:20171130-125202641
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Official Citation:Liu, Y. et al. Self-optimizing, highly surface-active layered metal dichalcogenide catalysts for hydrogen evolution. Nat. Energy 2, 17127 (2017)
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:83602
Deposited By: Tony Diaz
Deposited On:30 Nov 2017 21:18
Last Modified:09 Mar 2020 13:19

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