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

Abstract

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.

Authors:
 [1];  [2];  [3]; ORCiD logo [4];  [1];  [5];  [4];  [6]; ORCiD logo [3]; ORCiD logo [5];  [4]; ORCiD logo [1]
  1. Univ. of Central Florida, Orlando, FL (United States)
  2. Indian Institute of Technology Indore, Madhya Pradesh (India); Florida A&M Univ. and Florida State Univ., Tallahassee, FL (United States)
  3. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
  4. Florida A&M Univ. and Florida State Univ., Tallahassee, FL (United States)
  5. Oregon State Univ., Corvallis, OR (United States)
  6. Argonne National Lab. (ANL), Argonne, IL (United States)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States); Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
University of Central Florida; Florida State University; USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1493917
Alternate Identifier(s):
OSTI ID: 1494911
Report Number(s):
PNNL-SA-139297
Journal ID: ISSN 2155-5435; 149193
Grant/Contract Number:  
AC02-06CH11357; AC05-76RL01830
Resource Type:
Accepted Manuscript
Journal Name:
ACS Catalysis
Additional Journal Information:
Journal Volume: 9; Journal Issue: 1; Journal ID: ISSN 2155-5435
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; S-doping; MoP; hydrogen evolution; nanoporous; pH-universal; MoP, S-doping, nanoporous, pH-universal, hydrogen evolution

Citation Formats

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., and Yang, Yang. S-Doped MoP Nanoporous Layer Toward High-Efficiency Hydrogen Evolution in pH-Universal Electrolyte. United States: N. p., 2018. Web. doi:10.1021/acscatal.8b04291.
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. S-Doped MoP Nanoporous Layer Toward High-Efficiency Hydrogen Evolution in pH-Universal Electrolyte. United States. doi:10.1021/acscatal.8b04291.
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., and Yang, Yang. Tue . "S-Doped MoP Nanoporous Layer Toward High-Efficiency Hydrogen Evolution in pH-Universal Electrolyte". United States. doi:10.1021/acscatal.8b04291. https://www.osti.gov/servlets/purl/1493917.
@article{osti_1493917,
title = {S-Doped MoP Nanoporous Layer Toward High-Efficiency Hydrogen Evolution in pH-Universal Electrolyte},
author = {Liang, Kun and Pakhira, Srimanta and Yang, Zhenzhong and Nijamudheen, A. and Ju, Licheng and Wang, Maoyu and Aguirre-Velez, Carlos I. and Sterbinsky, George E. and Du, Yingge and Feng, Zhenxing and Mendoza-Cortes, Jose L. and Yang, Yang},
abstractNote = {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.},
doi = {10.1021/acscatal.8b04291},
journal = {ACS Catalysis},
number = 1,
volume = 9,
place = {United States},
year = {2018},
month = {12}
}

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