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Title: Activating and optimizing MoS2 basal planes for hydrogen evolution through the formation of strained sulphur vacancies

Abstract

As a promising non-precious catalyst for the hydrogen evolution reaction, molybdenum disulphide (MoS2) is known to contain active edge sites and an inert basal plane. Activating the MoS2 basal plane could further enhance its HER activity but is not often a strategy for doing so. Herein, we report the first activation and optimization of the basal plane of monolayer 2H-MoS2 for HER by introducing sulphur (S) vacancies and strain. Our theoretical and experimental results show that the S-vacancies are new catalytic sites in the basal plane, where gap states around the Fermi level allow hydrogen to bind directly to exposed Mo atoms. The hydrogen adsorption free energy (ΔGH) can be further manipulated by straining the surface with S-vacancies, which fine-tunes the catalytic activity. Furthermore, proper combinations of S-vacancy and strain yield the optimal ΔGH = 0 eV, which allows us to achieve the highest intrinsic HER activity among molybdenum-sulphide-based catalysts.

Authors:
 [1]; ORCiD logo [2];  [1];  [1];  [3];  [3];  [1];  [1];  [3];  [4];  [2];  [1]
+ Show Author Affiliations
  1. Stanford Univ., Stanford, CA (United States)
  2. Stanford Univ., Stanford, CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
  3. SLAC National Accelerator Lab., Menlo Park, CA (United States); Stanford Univ., Stanford, CA (United States)
  4. SLAC National Accelerator Lab., Menlo Park, CA (United States)
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Center on Nanostructuring for Efficient Energy Conversion (CNEEC); SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1257223
Grant/Contract Number:  
AC02-76SF00515
Resource Type:
Accepted Manuscript
Journal Name:
Nature Materials
Additional Journal Information:
Journal Volume: 15; Journal Issue: 1; Journal ID: ISSN 1476-1122
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; chemical engineering; electrocatalysis; two-dimensional materials

Citation Formats

Li, Hong, Tsai, Charlie, Koh, Ai Leen, Cai, Lili, Contryman, Alex W., Fragapane, Alex H., Zhao, Jiheng, Han, Hyun Soon, Manoharan, Hari C., Abild-Pedersen, Frank, Nørskov, Jens K., and Zheng, Xiaolin. Activating and optimizing MoS2 basal planes for hydrogen evolution through the formation of strained sulphur vacancies. United States: N. p., 2015. Web. doi:10.1038/NMAT4465.
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Li, Hong, Tsai, Charlie, Koh, Ai Leen, Cai, Lili, Contryman, Alex W., Fragapane, Alex H., Zhao, Jiheng, Han, Hyun Soon, Manoharan, Hari C., Abild-Pedersen, Frank, Nørskov, Jens K., & Zheng, Xiaolin. Activating and optimizing MoS2 basal planes for hydrogen evolution through the formation of strained sulphur vacancies. United States. doi:https://doi.org/10.1038/NMAT4465
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Li, Hong, Tsai, Charlie, Koh, Ai Leen, Cai, Lili, Contryman, Alex W., Fragapane, Alex H., Zhao, Jiheng, Han, Hyun Soon, Manoharan, Hari C., Abild-Pedersen, Frank, Nørskov, Jens K., and Zheng, Xiaolin. Mon . "Activating and optimizing MoS2 basal planes for hydrogen evolution through the formation of strained sulphur vacancies". United States. doi:https://doi.org/10.1038/NMAT4465. https://www.osti.gov/servlets/purl/1257223.
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@article{osti_1257223,
title = {Activating and optimizing MoS2 basal planes for hydrogen evolution through the formation of strained sulphur vacancies},
author = {Li, Hong and Tsai, Charlie and Koh, Ai Leen and Cai, Lili and Contryman, Alex W. and Fragapane, Alex H. and Zhao, Jiheng and Han, Hyun Soon and Manoharan, Hari C. and Abild-Pedersen, Frank and Nørskov, Jens K. and Zheng, Xiaolin},
abstractNote = {As a promising non-precious catalyst for the hydrogen evolution reaction, molybdenum disulphide (MoS2) is known to contain active edge sites and an inert basal plane. Activating the MoS2 basal plane could further enhance its HER activity but is not often a strategy for doing so. Herein, we report the first activation and optimization of the basal plane of monolayer 2H-MoS2 for HER by introducing sulphur (S) vacancies and strain. Our theoretical and experimental results show that the S-vacancies are new catalytic sites in the basal plane, where gap states around the Fermi level allow hydrogen to bind directly to exposed Mo atoms. The hydrogen adsorption free energy (ΔGH) can be further manipulated by straining the surface with S-vacancies, which fine-tunes the catalytic activity. Furthermore, proper combinations of S-vacancy and strain yield the optimal ΔGH = 0 eV, which allows us to achieve the highest intrinsic HER activity among molybdenum-sulphide-based catalysts.},
doi = {10.1038/NMAT4465},
journal = {Nature Materials},
number = 1,
volume = 15,
place = {United States},
year = {2015},
month = {11}
}
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    Defective MoS2 electrocatalyst for highly efficient hydrogen evolution through a simple ball-milling method
    journal, September 2017

    Two-dimensional Mo1.33C MXene with divacancy ordering prepared from parent 3D laminate with in-plane chemical ordering
    journal, April 2017

    • Tao, Quanzheng; Dahlqvist, Martin; Lu, Jun
    • Nature Communications, Vol. 8, Issue 1
    • DOI: 10.1038/ncomms14949

    Efficient hydrogen production on MoNi4 electrocatalysts with fast water dissociation kinetics
    journal, May 2017

    • Zhang, Jian; Wang, Tao; Liu, Pan
    • Nature Communications, Vol. 8, Issue 1
    • DOI: 10.1038/ncomms15437

    Activating cobalt(II) oxide nanorods for efficient electrocatalysis by strain engineering
    journal, November 2017

    Demonstration of chemistry at a point through restructuring and catalytic activation at anchored nanoparticles
    journal, November 2017

    • Neagu, Dragos; Papaioannou, Evangelos I.; Ramli, Wan K. W.
    • Nature Communications, Vol. 8, Issue 1
    • DOI: 10.1038/s41467-017-01880-y

    Photoinduced semiconductor-metal transition in ultrathin troilite FeS nanosheets to trigger efficient hydrogen evolution
    journal, January 2019

    Asymmetric MXene/monolayer transition metal dichalcogenide heterostructures for functional applications
    journal, February 2019

    Earth-abundant catalysts for electrochemical and photoelectrochemical water splitting
    journal, January 2017

    • Roger, Isolda; Shipman, Michael A.; Symes, Mark D.
    • Nature Reviews Chemistry, Vol. 1, Issue 1
    • DOI: 10.1038/s41570-016-0003

    Three-dimensional carbon foam/N-doped graphene@MoS 2 hybrid nanostructures as effective electrocatalysts for the hydrogen evolution reaction
    journal, January 2016

    • Park, Seung-Keun; Chung, Dong Young; Ko, Dongjin
    • Journal of Materials Chemistry A, Vol. 4, Issue 33
    • DOI: 10.1039/c6ta03458f

    Single-layer MoS 2 formation by sulfidation of molybdenum oxides in different oxidation states on Au(111)
    journal, January 2017

    • Salazar, Norberto; Beinik, Igor; Lauritsen, Jeppe V.
    • Physical Chemistry Chemical Physics, Vol. 19, Issue 21
    • DOI: 10.1039/c7cp00958e

    TMD-based highly efficient electrocatalysts developed by combined computational and experimental approaches
    journal, January 2018

    • Zhu, Changrong (Rose); Gao, Daqiang; Ding, Jun
    • Chemical Society Reviews, Vol. 47, Issue 12
    • DOI: 10.1039/c7cs00705a

    Nanostructured materials on 3D nickel foam as electrocatalysts for water splitting
    journal, January 2017

    • Chaudhari, Nitin K.; Jin, Haneul; Kim, Byeongyoon
    • Nanoscale, Vol. 9, Issue 34
    • DOI: 10.1039/c7nr04187j

    Electrochemical maps and movies of the hydrogen evolution reaction on natural crystals of molybdenite (MoS 2 ): basal vs. edge plane activity
    journal, January 2017

    • Bentley, Cameron L.; Kang, Minkyung; Maddar, Faduma M.
    • Chemical Science, Vol. 8, Issue 9
    • DOI: 10.1039/c7sc02545a

    Understanding the high-electrocatalytic performance of two-dimensional MoS 2 nanosheets and their composite materials
    journal, January 2017

    • Jayabal, Subramaniam; Saranya, Govindarajan; Wu, Jian
    • Journal of Materials Chemistry A, Vol. 5, Issue 47
    • DOI: 10.1039/c7ta08327k

    The atomic origin of nickel-doping-induced catalytic enhancement in MoS 2 for electrochemical hydrogen production
    journal, January 2019

    • Luo, Ruichun; Luo, Min; Wang, Ziqian
    • Nanoscale, Vol. 11, Issue 15
    • DOI: 10.1039/c8nr10023c

    Atomic (single, double, and triple atoms) catalysis: frontiers, opportunities, and challenges
    journal, January 2019

    • Chen, Z. W.; Chen, L. X.; Yang, C. C.
    • Journal of Materials Chemistry A, Vol. 7, Issue 8
    • DOI: 10.1039/c8ta11416a

    A computational study on Pt and Ru dimers supported on graphene for the hydrogen evolution reaction: new insight into the alkaline mechanism
    journal, January 2019

    • Liu, Xin; Jiao, Yan; Zheng, Yao
    • Journal of Materials Chemistry A, Vol. 7, Issue 8
    • DOI: 10.1039/c8ta11626a

    Strain engineering in functional 2-dimensional materials
    journal, February 2019

    • Sun, Yufei; Liu, Kai
    • Journal of Applied Physics, Vol. 125, Issue 8
    • DOI: 10.1063/1.5053795

    Strain-Enhanced p Doping in Monolayer MoS 2
    journal, February 2018

    Substrate screening effects on the quasiparticle band gap and defect charge transition levels in MoS 2
    journal, August 2018

    Key role of antibonding electron transfer in bonding on solid surfaces
    journal, September 2019

    Combining theory and experiment in electrocatalysis: Insights into materials design
    journal, January 2017

    Earth-Abundant Electrocatalysts in Proton Exchange Membrane Electrolyzers
    journal, December 2018

    • Sun, Xinwei; Xu, Kaiqi; Fleischer, Christian
    • Catalysts, Vol. 8, Issue 12
    • DOI: 10.3390/catal8120657
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