A dual-interfacial system with well-defined spatially separated redox-sites for boosting photocatalytic overall H2S splitting
(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
- 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
- organization
- publishing date
- 2021
- 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 >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}}, }