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231225s2022 xx |||||o 00| ||eng c |
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|a 10.1002/adma.202108475
|2 doi
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|a pubmed24n1111.xml
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|a (DE-627)NLM333490991
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|a (NLM)34811811
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|a DE-627
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|e rakwb
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|a eng
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1 |
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|a Gao, Duoduo
|e verfasserin
|4 aut
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|a Optimizing Atomic Hydrogen Desorption of Sulfur-Rich NiS1+ x Cocatalyst for Boosting Photocatalytic H2 Evolution
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|c 2022
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|a Text
|b txt
|2 rdacontent
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|a ƒaComputermedien
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|2 rdamedia
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|a ƒa Online-Ressource
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|2 rdacarrier
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|a Date Revised 10.02.2022
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|a published: Print-Electronic
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|a Citation Status PubMed-not-MEDLINE
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|a © 2021 Wiley-VCH GmbH.
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|a Low-cost transition-metal chalcogenides (MSx ) are demonstrated to be potential candidate cocatalyst for photocatalytic H2 generation. However, their H2 -generation performance is limited by insufficient quantities of exposed sulfur (S) sites and their strong bonding with adsorbed hydrogen atoms (SHads ). To address these issues, an efficient coupling strategy of active-site-enriched regulation and electronic structure modification of active S sites is developed by rational design of core-shell AuNiS1+ x nanostructured cocatalyst. In this case, the Au@NiS1+ x cocatalyst can be skillfully fabricated to synthesize the Au@NiS1+ x modified TiO2 (denoted as TiO2 /Au@NiS1+ x ) by a two-step route. Photocatalytic experiments exhibit that the resulting TiO2 /Au@NiS1+ x (1.7:1.3) displays a boosted H2 -generation rate of 9616 µmol h-1 g-1 with an apparent quantum efficiency of 46.0% at 365 nm, which is 2.9 and 1.7 times the rate over TiO2 /NiS1+ x and TiO2 /Au, respectively. In situ/ex situ XPS characterization and density functional theory calculations reveal that the free-electrons of Au can transfer to sulfur-enriched NiS1+ x to induce the generation of electron-enriched Sδ - active centers, which boosts the desorption of Hads for rapid hydrogen formation via weakening the strong SHads bonds. Hence, an electron-enriched Sδ - -mediated mechanism is proposed. This work delivers a universal strategy for simultaneously increasing the active site number and optimizing the binding strength between the active sites and hydrogen adsorbates
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|a Journal Article
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|a H2 evolution
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|a cocatalysts
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|a electron-enriched S atoms
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|a photocatalysis
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|a rich-active sites
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|a Xu, Jiachao
|e verfasserin
|4 aut
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1 |
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|a Wang, Linxi
|e verfasserin
|4 aut
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|a Zhu, Bicheng
|e verfasserin
|4 aut
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| 700 |
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|a Yu, Huogen
|e verfasserin
|4 aut
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| 700 |
1 |
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|a Yu, Jiaguo
|e verfasserin
|4 aut
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| 773 |
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|i Enthalten in
|t Advanced materials (Deerfield Beach, Fla.)
|d 1998
|g 34(2022), 6 vom: 10. Feb., Seite e2108475
|w (DE-627)NLM098206397
|x 1521-4095
|7 nnns
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| 773 |
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|g volume:34
|g year:2022
|g number:6
|g day:10
|g month:02
|g pages:e2108475
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|u http://dx.doi.org/10.1002/adma.202108475
|3 Volltext
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