S-Doped MoP Nanoporous Layer Toward High-Efficiency Hydrogen Evolution in pH-Universal Electrolyte

Liang, Kun; Pakhira, Srimanta; Yang, Zhenzhong; Nijamudheen, A.; Ju, Licheng; Wang, Maoyu; Aguirre-Velez, Carlos I.; Sterbinsky, George E.; Du, Yingge; Feng, Zhenxing; Mendoza-Cortes, Jose L.; Yang, Yang

doi:10.1021/acscatal.8b04291

Title: S-Doped MoP Nanoporous Layer Toward High-Efficiency Hydrogen Evolution in pH-Universal Electrolyte

Journal Article · Tue Dec 18 00:00:00 EST 2018 · ACS Catalysis

DOI:https://doi.org/10.1021/acscatal.8b04291· OSTI ID:1493917

Liang, Kun ^[1]; Pakhira, Srimanta ^[2]; Yang, Zhenzhong ^[3];

^[4]; Ju, Licheng ^[1]; Wang, Maoyu ^[5]; Aguirre-Velez, Carlos I. ^[4]; Sterbinsky, George E. ^[6];

^[3];

^[5]; Mendoza-Cortes, Jose L. ^[4];

^[1]

Univ. of Central Florida, Orlando, FL (United States)
Indian Institute of Technology Indore, Madhya Pradesh (India); Florida A&M Univ. and Florida State Univ., Tallahassee, FL (United States)
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Florida A&M Univ. and Florida State Univ., Tallahassee, FL (United States)
Oregon State Univ., Corvallis, OR (United States)
Argonne National Lab. (ANL), Argonne, IL (United States)

In this study, we report a non-precious metal catalyst for high-efficiency hydrogen evolution reaction (HER). A self-organized S-doped MoP nanoporous layer (S-MoP NPL) is achieved through a facile electrochemical anodic treatment and a two-step chemical vapor deposition process, which can be directly used as a binder-free catalyst for HER in pH-universal electrolytes. S-MoP NPL exhibits excellent HER activity with a low overpotential of 86 mV at 10 mA cm-1 and low Tafel slope of 34 mV dec-1 in 0.5 M H₂SO₄ electrolyte. Moreover, S-MoP NPL also shows high HER performance in basic and neutral electrolytes. First principle based density functional theory (DFT) calculations were performed to support our experiment. The present DFT calculations show that the H₂ formation (via Volmer-Heyrovsky mechanism) from the reaction of a metal (Mo) absorbed hydride with a solvated proton is favored over S-MoP than MoS₂. Both experimental and computational studies demonstrate that the extraordinary HER activity and stability performance displayed by a MoP catalyst can be enhanced by S-doping, opening up a promising paradigm for the rational design of high-performance non-precious metal catalyst for hydrogen generation.

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Research Organization:: Argonne National Lab. (ANL), Argonne, IL (United States); Pacific Northwest National Lab. (PNNL), Richland, WA (United States)

Sponsoring Organization:: University of Central Florida; Florida State University; USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-06CH11357; AC05-76RL01830

OSTI ID:: 1493917

Alternate ID(s):: OSTI ID: 1494911

Report Number(s):: PNNL-SA-139297; 149193

Journal Information:: ACS Catalysis, Vol. 9, Issue 1; ISSN 2155-5435

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 131 works

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
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Title: S-Doped MoP Nanoporous Layer Toward High-Efficiency Hydrogen Evolution in pH-Universal Electrolyte

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