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...
| Main Authors: | , , , , , , , , , , , , |
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| Other Authors: | |
| Format: | Journal Article |
| Language: | English |
| Published: |
2020
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| Subjects: | |
| Online Access: | https://hdl.handle.net/10356/143597 |
| _version_ | 1826124036098228224 |
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| 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 |
| 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 |
| author_sort | Zhou, Yao |
| collection | NTU |
| 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. |
| first_indexed | 2024-10-01T06:14:26Z |
| format | Journal Article |
| id | ntu-10356/143597 |
| institution | Nanyang Technological University |
| language | English |
| last_indexed | 2024-10-01T06:14:26Z |
| publishDate | 2020 |
| record_format | dspace |
| spelling | ntu-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. |
| 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 |
| title | 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_short | 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 |
| topic | Engineering::Materials Monolayer Transition Metal Dichalcogenides |
| url | https://hdl.handle.net/10356/143597 |
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