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Title: Enhanced Electrocatalytic Hydrogen Evolution Activity in Single-Atom Pt-Decorated VS2 Nanosheets

Abstract

Enhancing catalytic activity by decorating noble metals in catalysts provides an opportunity for promoting the electrocatalytic hydrogen evolution reaction (HER) application. However, there are few systematic studies on regulating the structures of noble metals in catalytic materials and investigating their influence on HER. Herein, Pt catalysts with different structures including single atoms (SAs), clusters, and nanoparticles well-controllably anchored on VS2 nanosheets through a cost-effective optothermal method are reported, and their HER performance is studied. The most efficient Pt-decorated VS2 catalyst (with both Pt SAs and clusters) delivers an overpotential of 77 mV at 10 mA cm–2, close to that of Pt/C (48 mV). However, the optimal mass activity of Pt (normalizing to Pt content) is obtained from only SA Pt-decorated VS2 (i.e., 22.88 A mgPt–1 at 200 mV) and is 12 times greater than that of the Pt/C (1.87 A mgPt–1), attributed to the greatly enhanced Pt utilization. Additionally, the theoretical simulations reveal that Pt SA decoration makes the adsorption free energy of H* closer to the thermoneutral value and improves the charge-transfer kinetics, significantly enhancing HER activity. Furthermore, this work offers a pathway to prepare the desired catalyst based on synergy of Pt structures and VS2 and reveals themore » intrinsic mechanism for enhancing catalytic activity, which is important for HER applications.« less

Authors:
ORCiD logo [1];  [2]; ORCiD logo [3];  [1]; ORCiD logo [1];  [1];  [1];  [4];  [4]; ORCiD logo [3]; ORCiD logo [2]; ORCiD logo [1]
  1. Shenzhen Univ. (China)
  2. The Hong Kong Polytechnic Univ., Hong Kong (China)
  3. National Univ. of Singapore (Singapore)
  4. A*STAR (Singapore)
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1805236
Report Number(s):
BNL-221757-2021-JAAM
Journal ID: ISSN 1936-0851
Grant/Contract Number:  
SC0012704
Resource Type:
Accepted Manuscript
Journal Name:
ACS Nano
Additional Journal Information:
Journal Volume: 14; Journal Issue: 5; Journal ID: ISSN 1936-0851
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; single atom; platinum; vanadium disulfide; hydrogen evolution reaction; catalyst; cluster structure; evolution reactions; cluster chemistry

Citation Formats

Zhu, Jingting, Cai, Lejuan, Yin, Xinmao, Wang, Zhuo, Zhang, Linfei, Ma, Haibin, Ke, Yuxuan, Du, Yonghua, Xi, Shibo, Wee, Andrew T. S., Chai, Yang, and Zhang, Wenjing. Enhanced Electrocatalytic Hydrogen Evolution Activity in Single-Atom Pt-Decorated VS2 Nanosheets. United States: N. p., 2020. Web. doi:10.1021/acsnano.9b10048.
Zhu, Jingting, Cai, Lejuan, Yin, Xinmao, Wang, Zhuo, Zhang, Linfei, Ma, Haibin, Ke, Yuxuan, Du, Yonghua, Xi, Shibo, Wee, Andrew T. S., Chai, Yang, & Zhang, Wenjing. Enhanced Electrocatalytic Hydrogen Evolution Activity in Single-Atom Pt-Decorated VS2 Nanosheets. United States. https://doi.org/10.1021/acsnano.9b10048
Zhu, Jingting, Cai, Lejuan, Yin, Xinmao, Wang, Zhuo, Zhang, Linfei, Ma, Haibin, Ke, Yuxuan, Du, Yonghua, Xi, Shibo, Wee, Andrew T. S., Chai, Yang, and Zhang, Wenjing. Wed . "Enhanced Electrocatalytic Hydrogen Evolution Activity in Single-Atom Pt-Decorated VS2 Nanosheets". United States. https://doi.org/10.1021/acsnano.9b10048. https://www.osti.gov/servlets/purl/1805236.
@article{osti_1805236,
title = {Enhanced Electrocatalytic Hydrogen Evolution Activity in Single-Atom Pt-Decorated VS2 Nanosheets},
author = {Zhu, Jingting and Cai, Lejuan and Yin, Xinmao and Wang, Zhuo and Zhang, Linfei and Ma, Haibin and Ke, Yuxuan and Du, Yonghua and Xi, Shibo and Wee, Andrew T. S. and Chai, Yang and Zhang, Wenjing},
abstractNote = {Enhancing catalytic activity by decorating noble metals in catalysts provides an opportunity for promoting the electrocatalytic hydrogen evolution reaction (HER) application. However, there are few systematic studies on regulating the structures of noble metals in catalytic materials and investigating their influence on HER. Herein, Pt catalysts with different structures including single atoms (SAs), clusters, and nanoparticles well-controllably anchored on VS2 nanosheets through a cost-effective optothermal method are reported, and their HER performance is studied. The most efficient Pt-decorated VS2 catalyst (with both Pt SAs and clusters) delivers an overpotential of 77 mV at 10 mA cm–2, close to that of Pt/C (48 mV). However, the optimal mass activity of Pt (normalizing to Pt content) is obtained from only SA Pt-decorated VS2 (i.e., 22.88 A mgPt–1 at 200 mV) and is 12 times greater than that of the Pt/C (1.87 A mgPt–1), attributed to the greatly enhanced Pt utilization. Additionally, the theoretical simulations reveal that Pt SA decoration makes the adsorption free energy of H* closer to the thermoneutral value and improves the charge-transfer kinetics, significantly enhancing HER activity. Furthermore, this work offers a pathway to prepare the desired catalyst based on synergy of Pt structures and VS2 and reveals the intrinsic mechanism for enhancing catalytic activity, which is important for HER applications.},
doi = {10.1021/acsnano.9b10048},
journal = {ACS Nano},
number = 5,
volume = 14,
place = {United States},
year = {Wed Apr 22 00:00:00 EDT 2020},
month = {Wed Apr 22 00:00:00 EDT 2020}
}

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