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Promoting photocatalytic hydrogen evolution by modulating the electron-transfer in an ultrafast timescale through Mo-S6 configuration

Li, Yi ; Yu, Shan ; Cao, Yuehan ; Huang, Yue ; Wang, Qiaohao ; Duan, Yuangang ; Li, Lina ; Zheng, Kaibo LU and Zhou, Ying (2024) In Journal of Materials Science and Technology 193. p.73-80
Abstract

Maximizing ultrafast electron-transfer kinetics in semiconductor is pivotal but challenging for high-efficiency solar-to-energy during the photocatalytic reaction process due to the intrinsic property of photocatalysts with low surface electron density. Herein, a model photocatalyst CdS@Mo is synthesized through a typical hydrothermal method for modulating the ultrafast electron-transfer to enhance the surface electron density. X-ray absorption fine spectra (XAFS) reveal that Mo is coordinated with S atoms to form a Mo-S6 configuration which is different from common MoS2 and Mo foil structures. Based on the femtosecond transient absorption spectra (fs-TAS), it is found that the formation of Mo-S6... (More)

Maximizing ultrafast electron-transfer kinetics in semiconductor is pivotal but challenging for high-efficiency solar-to-energy during the photocatalytic reaction process due to the intrinsic property of photocatalysts with low surface electron density. Herein, a model photocatalyst CdS@Mo is synthesized through a typical hydrothermal method for modulating the ultrafast electron-transfer to enhance the surface electron density. X-ray absorption fine spectra (XAFS) reveal that Mo is coordinated with S atoms to form a Mo-S6 configuration which is different from common MoS2 and Mo foil structures. Based on the femtosecond transient absorption spectra (fs-TAS), it is found that the formation of Mo-S6 configuration contributes to the fast decay of CdS signal and Mo-S6 signal reactivation, illustrating the ultrafast electron-transfer (∼2.2 ps) from CdS to Mo-S6 configuration, which achieves the enhanced electron density of photocatalyst surface. Finally, a holistic photocatalytic performance evaluation discloses that the growing of Mo-S6 configuration obviously improves the photocatalytic hydrogen evolution (PHE) efficiency of CdS from 28.5 to 47.5 mmol g–1 h–1 with a solar-to-hydrogen (STH) efficiency of 0.10 % which is seldomly discussed in the system containing sacrificial agents. This work opens a new path to modulate the surface electron density by tuning the ultrafast electron-transfer for enhancing reaction efficiency in electron-density-dependent systems.

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author
; ; ; ; ; ; ; and
organization
publishing date
type
Contribution to journal
publication status
published
subject
keywords
CdS, Electron-transfer, Mo-S configuration, Photocatalytic hydrogen evolution
in
Journal of Materials Science and Technology
volume
193
pages
8 pages
publisher
Chinese Society of Metals
external identifiers
  • scopus:85188026281
ISSN
1005-0302
DOI
10.1016/j.jmst.2024.01.021
language
English
LU publication?
yes
id
0dec2026-0243-4b82-bb69-048b45c1c075
date added to LUP
2024-03-27 13:41:07
date last changed
2024-03-27 13:41:58
@article{0dec2026-0243-4b82-bb69-048b45c1c075,
  abstract     = {{<p>Maximizing ultrafast electron-transfer kinetics in semiconductor is pivotal but challenging for high-efficiency solar-to-energy during the photocatalytic reaction process due to the intrinsic property of photocatalysts with low surface electron density. Herein, a model photocatalyst CdS@Mo is synthesized through a typical hydrothermal method for modulating the ultrafast electron-transfer to enhance the surface electron density. X-ray absorption fine spectra (XAFS) reveal that Mo is coordinated with S atoms to form a Mo-S<sub>6</sub> configuration which is different from common MoS<sub>2</sub> and Mo foil structures. Based on the femtosecond transient absorption spectra (fs-TAS), it is found that the formation of Mo-S<sub>6</sub> configuration contributes to the fast decay of CdS signal and Mo-S<sub>6</sub> signal reactivation, illustrating the ultrafast electron-transfer (∼2.2 ps) from CdS to Mo-S<sub>6</sub> configuration, which achieves the enhanced electron density of photocatalyst surface. Finally, a holistic photocatalytic performance evaluation discloses that the growing of Mo-S<sub>6</sub> configuration obviously improves the photocatalytic hydrogen evolution (PHE) efficiency of CdS from 28.5 to 47.5 mmol g<sup>–1</sup> h<sup>–1</sup> with a solar-to-hydrogen (STH) efficiency of 0.10 % which is seldomly discussed in the system containing sacrificial agents. This work opens a new path to modulate the surface electron density by tuning the ultrafast electron-transfer for enhancing reaction efficiency in electron-density-dependent systems.</p>}},
  author       = {{Li, Yi and Yu, Shan and Cao, Yuehan and Huang, Yue and Wang, Qiaohao and Duan, Yuangang and Li, Lina and Zheng, Kaibo and Zhou, Ying}},
  issn         = {{1005-0302}},
  keywords     = {{CdS; Electron-transfer; Mo-S configuration; Photocatalytic hydrogen evolution}},
  language     = {{eng}},
  month        = {{09}},
  pages        = {{73--80}},
  publisher    = {{Chinese Society of Metals}},
  series       = {{Journal of Materials Science and Technology}},
  title        = {{Promoting photocatalytic hydrogen evolution by modulating the electron-transfer in an ultrafast timescale through Mo-S<sub>6</sub> configuration}},
  url          = {{http://dx.doi.org/10.1016/j.jmst.2024.01.021}},
  doi          = {{10.1016/j.jmst.2024.01.021}},
  volume       = {{193}},
  year         = {{2024}},
}