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A dual-interfacial system with well-defined spatially separated redox-sites for boosting photocatalytic overall H2S splitting

Dan, Meng LU ; Wu, Fan LU ; Xiang, Jianglai ; Cao, Yuehan ; Zhong, Yunqian ; Zheng, Kaibo LU ; Liu, Yang LU ; Liu, Zhao Qing ; Yu, Shan and Zhou, Ying (2021) In Chemical Engineering Journal 423.
Abstract

Integration of high activity, selectivity, and stability is urgently desired to achieve more ideal photocatalysts. Herein, we reported the rational design of MoS2-MnS@(InxCu1-x)2S3 (M-M@IC) catalysts with dual interface to integrate separated redox sites for boosting photocatalytic hydrogen sulphide (H2S) splitting and the resource utilization of sacrificial reagents (Na2S/Na2SO3). The spatially separated reduction (MnS) and oxidation (In2S3) sites in MnS/In2S3 heterojunction, on which MoS2 and Cu were selectively loaded, can drive electrons and holes near the surface to flow along... (More)

Integration of high activity, selectivity, and stability is urgently desired to achieve more ideal photocatalysts. Herein, we reported the rational design of MoS2-MnS@(InxCu1-x)2S3 (M-M@IC) catalysts with dual interface to integrate separated redox sites for boosting photocatalytic hydrogen sulphide (H2S) splitting and the resource utilization of sacrificial reagents (Na2S/Na2SO3). The spatially separated reduction (MnS) and oxidation (In2S3) sites in MnS/In2S3 heterojunction, on which MoS2 and Cu were selectively loaded, can drive electrons and holes near the surface to flow along opposite directions, while the heterojunction between MnS and In2S3 inhibits the bulk charge recombination. Furthermore, the introduction of Cu atoms creates a d-band center, which favours mass diffusion of reactants/products species and greatly facilitates sunlight response. The MoS2 serves to provide abundant sites for proton reduction due to the unsaturated-sulfur-edge-rich (US-rich) nature. As a result, the M−M@IC shows a state-of-the-art visible-light photocatalytic H2 evolution rate (126.5 mmol g-1h−1), inspiring stability of >50 h, and nearly 100% selectivity toward value-added Na2S2O3 production under optimized condition. This work opens up new opportunities for the construction and design of spatially separated catalytic site in photocatalysts.

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author
; ; ; ; ; ; ; ; and
organization
publishing date
type
Contribution to journal
publication status
published
subject
keywords
Dual-interfacial system, H evolution, Sacrificial reagent conversion, Spatially separated reaction sites
in
Chemical Engineering Journal
volume
423
article number
130201
publisher
Elsevier
external identifiers
  • scopus:85108114474
ISSN
1385-8947
DOI
10.1016/j.cej.2021.130201
language
English
LU publication?
yes
id
49da9537-5279-4b99-95ed-6f63bdcbe93f
date added to LUP
2021-08-11 10:30:28
date last changed
2023-11-08 17:04:27
@article{49da9537-5279-4b99-95ed-6f63bdcbe93f,
  abstract     = {{<p>Integration of high activity, selectivity, and stability is urgently desired to achieve more ideal photocatalysts. Herein, we reported the rational design of MoS<sub>2</sub>-MnS@(In<sub>x</sub>Cu<sub>1-x</sub>)<sub>2</sub>S<sub>3</sub> (M-M@IC) catalysts with dual interface to integrate separated redox sites for boosting photocatalytic hydrogen sulphide (H<sub>2</sub>S) splitting and the resource utilization of sacrificial reagents (Na<sub>2</sub>S/Na<sub>2</sub>SO<sub>3</sub>). The spatially separated reduction (MnS) and oxidation (In<sub>2</sub>S<sub>3</sub>) sites in MnS/In<sub>2</sub>S<sub>3</sub> heterojunction, on which MoS<sub>2</sub> and Cu were selectively loaded, can drive electrons and holes near the surface to flow along opposite directions, while the heterojunction between MnS and In<sub>2</sub>S<sub>3</sub> inhibits the bulk charge recombination. Furthermore, the introduction of Cu atoms creates a d-band center, which favours mass diffusion of reactants/products species and greatly facilitates sunlight response. The MoS<sub>2</sub> serves to provide abundant sites for proton reduction due to the unsaturated-sulfur-edge-rich (US-rich) nature. As a result, the M−M@IC shows a state-of-the-art visible-light photocatalytic H<sub>2</sub> evolution rate (126.5 mmol g<sup>-1</sup>h<sup>−1</sup>), inspiring stability of &gt;50 h, and nearly 100% selectivity toward value-added Na<sub>2</sub>S<sub>2</sub>O<sub>3</sub> production under optimized condition. This work opens up new opportunities for the construction and design of spatially separated catalytic site in photocatalysts.</p>}},
  author       = {{Dan, Meng and Wu, Fan and Xiang, Jianglai and Cao, Yuehan and Zhong, Yunqian and Zheng, Kaibo and Liu, Yang and Liu, Zhao Qing and Yu, Shan and Zhou, Ying}},
  issn         = {{1385-8947}},
  keywords     = {{Dual-interfacial system; H evolution; Sacrificial reagent conversion; Spatially separated reaction sites}},
  language     = {{eng}},
  publisher    = {{Elsevier}},
  series       = {{Chemical Engineering Journal}},
  title        = {{A dual-interfacial system with well-defined spatially separated redox-sites for boosting photocatalytic overall H<sub>2</sub>S splitting}},
  url          = {{http://dx.doi.org/10.1016/j.cej.2021.130201}},
  doi          = {{10.1016/j.cej.2021.130201}},
  volume       = {{423}},
  year         = {{2021}},
}