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

Journal Article · · Nature Materials
DOI:https://doi.org/10.1038/NMAT4465· OSTI ID:1257223
 [1]; ORCiD logo [2];  [1];  [1];  [3];  [3];  [1];  [1];  [3];  [4];  [2];  [1]
  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)

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.

Research Organization:
Energy Frontier Research Centers (EFRC) (United States). Center on Nanostructuring for Efficient Energy Conversion (CNEEC); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
Sponsoring Organization:
USDOE
Grant/Contract Number:
AC02-76SF00515
OSTI ID:
1257223
Journal Information:
Nature Materials, Vol. 15, Issue 1; ISSN 1476-1122
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 4 works
Citation information provided by
Web of Science

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Strain and defect engineered monolayer Ni-MoS 2 for pH-universal hydrogen evolution catalysis journal January 2019
Activated basal planes of WS 2 by intrinsic defects as catalysts for the electrocatalytic nitrogen reduction reaction journal January 2019
Mo 2 C/graphene heterostructures: low temperature chemical vapor deposition on liquid bimetallic Sn–Cu and hydrogen evolution reaction electrocatalytic properties journal January 2019
Size-dependent optical properties of MoS 2 nanoparticles and their photo-catalytic applications journal January 2020
Post Graphene 2D Chemistry: The Emerging Field of Molybdenum Disulfide and Black Phosphorus Functionalization text January 2019
General approach for preparing sandwich-structured metal sulfide@reduced graphene oxide as highly reversible Li-ion battery anode text January 2018