Auto-optimizing hydrogen evolution catalytic activity of ReS2 through intrinsic charge engineering

Optimizing active electronic states responding to catalysis is of paramount importance for developing high-activity catalysts because thermodynamics itself may not favor forming an optimal electronic state. Setting the monolayer transition metal dichalcogenide (TMD) ReS2 as a model for the hydrogen...

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Main Authors: Zhou, Yao, Song, Erhong, Zhou, Jiadong, Lin, Junhao, Ma, Ruguang, Wang, Youwei, Qiu, Wujie, Shen, Ruxiang, Suenaga, Kazutomo, Liu, Qian, Wang, Jiacheng, Liu, Zheng, Liu, Jianjun
Other Authors: School of Materials Science and Engineering
Format: Article
Language:English
Published: 2020
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Online Access:https://hdl.handle.net/10356/143597
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Institution: Nanyang Technological University
Language: English
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spelling sg-ntu-dr.10356-1435972020-09-14T01:53:06Z Auto-optimizing hydrogen evolution catalytic activity of ReS2 through intrinsic charge engineering Zhou, Yao Song, Erhong Zhou, Jiadong Lin, Junhao Ma, Ruguang Wang, Youwei Qiu, Wujie Shen, Ruxiang Suenaga, Kazutomo Liu, Qian Wang, Jiacheng Liu, Zheng Liu, Jianjun School of Materials Science and Engineering Engineering::Materials Monolayer Transition Metal Dichalcogenides Optimizing active electronic states responding to catalysis is of paramount importance for developing high-activity catalysts because thermodynamics itself may not favor forming an optimal electronic state. Setting the monolayer transition metal dichalcogenide (TMD) ReS2 as a model for the hydrogen evolution reaction (HER), we uncover that intrinsic charge engineering has an auto-optimizing effect on enhancing catalytic activity through regulating active electronic states. The experimental and theoretical results show that intrinsic charge compensation from S to Re-Re bonds could manipulate the active electronic states, allowing hydrogen to absorb the active sites neither strongly nor weakly. Two types of S sites exhibit the optimal hydrogen adsorption free energies (Δ GH*) of 0.016 and 0.061 eV, which are the closest to zero corresponding to the highest HER activity. This auto-optimization via charge engineering is further demonstrated by higher turnover frequency per sulfur atom of 1-10 s-1 and lower overpotential of -147 mV at 10 mA cm-2 than those of other TMDs through multiscale activation and optimization. This work opens an avenue in designing extensive active catalysts through intrinsic charge engineering strategy. 2020-09-14T01:53:06Z 2020-09-14T01:53:06Z 2018 Journal Article Zhou, Y., Song, E., Zhou, J., Lin, J., Ma, R., Wang, Y., ... Liu, J. (2018). Auto-optimizing hydrogen evolution catalytic activity of ReS2 through intrinsic charge engineering. ACS Nano, 12(5), 4486-4493. doi:10.1021/acsnano.8b00693 1936-086X https://hdl.handle.net/10356/143597 10.1021/acsnano.8b00693 29697961 5 12 4486 4493 en ACS Nano © 2018 American Chemical Society. All rights reserved.
institution Nanyang Technological University
building NTU Library
country Singapore
collection DR-NTU
language English
topic Engineering::Materials
Monolayer
Transition Metal Dichalcogenides
spellingShingle Engineering::Materials
Monolayer
Transition Metal Dichalcogenides
Zhou, Yao
Song, Erhong
Zhou, Jiadong
Lin, Junhao
Ma, Ruguang
Wang, Youwei
Qiu, Wujie
Shen, Ruxiang
Suenaga, Kazutomo
Liu, Qian
Wang, Jiacheng
Liu, Zheng
Liu, Jianjun
Auto-optimizing hydrogen evolution catalytic activity of ReS2 through intrinsic charge engineering
description Optimizing active electronic states responding to catalysis is of paramount importance for developing high-activity catalysts because thermodynamics itself may not favor forming an optimal electronic state. Setting the monolayer transition metal dichalcogenide (TMD) ReS2 as a model for the hydrogen evolution reaction (HER), we uncover that intrinsic charge engineering has an auto-optimizing effect on enhancing catalytic activity through regulating active electronic states. The experimental and theoretical results show that intrinsic charge compensation from S to Re-Re bonds could manipulate the active electronic states, allowing hydrogen to absorb the active sites neither strongly nor weakly. Two types of S sites exhibit the optimal hydrogen adsorption free energies (Δ GH*) of 0.016 and 0.061 eV, which are the closest to zero corresponding to the highest HER activity. This auto-optimization via charge engineering is further demonstrated by higher turnover frequency per sulfur atom of 1-10 s-1 and lower overpotential of -147 mV at 10 mA cm-2 than those of other TMDs through multiscale activation and optimization. This work opens an avenue in designing extensive active catalysts through intrinsic charge engineering strategy.
author2 School of Materials Science and Engineering
author_facet School of Materials Science and Engineering
Zhou, Yao
Song, Erhong
Zhou, Jiadong
Lin, Junhao
Ma, Ruguang
Wang, Youwei
Qiu, Wujie
Shen, Ruxiang
Suenaga, Kazutomo
Liu, Qian
Wang, Jiacheng
Liu, Zheng
Liu, Jianjun
format Article
author Zhou, Yao
Song, Erhong
Zhou, Jiadong
Lin, Junhao
Ma, Ruguang
Wang, Youwei
Qiu, Wujie
Shen, Ruxiang
Suenaga, Kazutomo
Liu, Qian
Wang, Jiacheng
Liu, Zheng
Liu, Jianjun
author_sort Zhou, Yao
title Auto-optimizing hydrogen evolution catalytic activity of ReS2 through intrinsic charge engineering
title_short Auto-optimizing hydrogen evolution catalytic activity of ReS2 through intrinsic charge engineering
title_full Auto-optimizing hydrogen evolution catalytic activity of ReS2 through intrinsic charge engineering
title_fullStr Auto-optimizing hydrogen evolution catalytic activity of ReS2 through intrinsic charge engineering
title_full_unstemmed Auto-optimizing hydrogen evolution catalytic activity of ReS2 through intrinsic charge engineering
title_sort auto-optimizing hydrogen evolution catalytic activity of res2 through intrinsic charge engineering
publishDate 2020
url https://hdl.handle.net/10356/143597
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