Title: Activating MoS₂ for pH-Universal Hydrogen Evolution Catalysis

Abstract

MoS₂ presents a promising catalyst for the hydrogen evolution reaction (HER) in water splitting, but its worse catalytic performance in neutral and alkaline media than in acidic environment may be problematic for practical application. This is because the other half reaction of water splitting, i.e., oxygen evolution reaction, often needs to be implemented in alkaline environment. Here we demonstrate a universal strategy that may be used to significantly improve the HER catalysis of MoS₂ in all kinds of environments from acidic to alkaline, proton intercalation. Protons may be enabled to intercalate between monolayer MoS₂ and underlying substrates or in the interlayer space of thicker MoS₂ by two processes: electrochemically polarizing MoS₂ at negative potentials (vs RHE) in acidic media or immersing MoS2 into certain acid solutions like TFSI. The improvement in catalytic performance is due to the activity enhancement of the active sites in MoS₂ by the intercalated protons, which might be related with the effect of the intercalated protons on electrical conductance and the adsorption energy of hydrogen atoms. The enhancement in catalytic activity by the intercalated proton is very stable even in neutral and alkaline electrolytes.

Authors:

Li, Guoqing ^[1]; Zhang, Du ^[2]; Yu, Yifei ^[1]; Huang, Shengyang ^[3]; Yang, Weitao  ^[4];

• Search DOE PAGES for author "Yang, Weitao"
• Search DOE PAGES for ORCID "0000-0001-5576-2828"

Cao, Linyou  ^[5]

• Search DOE PAGES for author "Cao, Linyou"
• Search DOE PAGES for ORCID "0000-0002-7834-8336"

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+ Show Author Affiliations

1. North Carolina State Univ., Raleigh, NC (United States). Dept. of Materials Science and Engineering
2. Duke Univ., Durham, NC (United States). Dept. of Chemistry
3. North Carolina State Univ., Raleigh, NC (United States). Dept. of Chemical and Biomolecular Engineering
4. Duke Univ., Durham, NC (United States). Dept. of Chemistry
5. North Carolina State Univ., Raleigh, NC (United States). Dept. of Materials Science and Engineering, Dept. of Physics, and Dept. of Electrical and Computer Engineering

Publication Date:

Wed Oct 25 00:00:00 EDT 2017

Research Org.:

Energy Frontier Research Centers (EFRC) (United States). Center for the Computational Design of Functional Layered Materials (CCDM)

Sponsoring Org.:

USDOE Office of Science (SC), Basic Energy Sciences (BES)

OSTI Identifier:

1470022

Grant/Contract Number:  

SC0012575

Resource Type:

Accepted Manuscript

Journal Name:

Journal of the American Chemical Society

Additional Journal Information:

Journal Volume: 139; Journal Issue: 45; Related Information: CCDM partners with Temple University (lead); Brookhaven National Laboratory; Drexel University; Duke University; North Carolina State University; Northeastern University; Princeton University; Rice University; University of Pennsylvania; Journal ID: ISSN 0002-7863

Publisher:

American Chemical Society (ACS)

Country of Publication:

United States

Language:

English

Subject:

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; catalysis (heterogeneous); solar (photovoltaic); energy storage (including batteries and capacitors); hydrogen and fuel cells; defect; , mechanical behavior; materials and chemistry by design; synthesis (novel materials)