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用于光催化产氢并耦合选择性苄胺氧化的核壳结构CdS@Cu-TCPP-Pt异质结中的超快电荷转移

Ultrafast Charge Transfer in a Core-shell CdS@Cu-TCPP-Pt Heterojunction for Photocatalytic Hydrogen Production Coupled with Selective Benzylamine Oxidation.

作者信息

Shi Manman, Luo Dian, Liu Rong, Wei Jieding, Guo Saiya, Lu Zhou, Ni Yonghong

机构信息

College of Chemistry and Materials Science, Key Laboratory of Functional Molecular Solids, Ministry of Education, Anhui Laboratory of Molecule-Based Materials, Anhui Key Laboratory of Functional Molecular Solids, Anhui Normal University, 189 Jiuhua Southern Road, Wuhu 241002, PR. China.

School of Physics and Electronic Information, Anhui Normal University, 189 Jiuhua Southern Road, Wuhu 241002, PR. China.

出版信息

Inorg Chem. 2024 Sep 30;63(39):18233-18241. doi: 10.1021/acs.inorgchem.4c03123. Epub 2024 Sep 18.

DOI:10.1021/acs.inorgchem.4c03123
PMID:39291763
Abstract

Photocatalytic selective oxidation of organic substances coupled with hydrogen production is believed to be one of the most favorable pathways to make full use of photogenerated charge carriers. However, this catalytic reaction is often discouraged due to the rapid recombination of photogenerated carriers in practical applications. In this work, a core-shell CdS@Cu-TCPP-Pt nanorod heterojunction was dexterously designed for boosting the photocatalytic dehydrogenation performance of benzylamine. The transient absorption results revealed that the photogenerated electron-holes could be effectively separated by properly matching the energy levels in CdS@Cu-TCPP. Surprisingly, Pt embedded in Cu-TCPP not only provided abundant hydrogen production active sites but also facilitated ultrafast charge transfer, which endowed CdS@Cu-TCPP-Pt with remarkable photocatalytic performances for the coproductions of -benzylidenebenzylamine (1 mL) with a conversion of 23.48% and H (20.75 mmol g h) under visible irradiation, far surpassing those of CdS and Cu-TCPP. Obviously, the present work verifies that designing and fabricating a hybrid photocatalyst with high separation efficiency of electron-hole pairs is also a significant avenue for other high-performance cooperative dual-functional photocatalytic reactions.

摘要

光催化选择性氧化有机物质并耦合产氢被认为是充分利用光生电荷载流子的最有利途径之一。然而,由于在实际应用中光生载流子的快速复合,这种催化反应常常受到阻碍。在这项工作中,巧妙地设计了一种核壳结构的CdS@Cu-TCPP-Pt纳米棒异质结,以提高苄胺的光催化脱氢性能。瞬态吸收结果表明,通过适当匹配CdS@Cu-TCPP中的能级,可以有效地分离光生电子-空穴。令人惊讶的是,嵌入Cu-TCPP中的Pt不仅提供了丰富的产氢活性位点,还促进了超快电荷转移,这赋予了CdS@Cu-TCPP-Pt在可见光照射下显著的光催化性能,用于共生产亚苄基苄胺(1 mL),转化率为23.48%,产氢量为(20.75 mmol g⁻¹ h⁻¹),远远超过了CdS和Cu-TCPP。显然,目前的工作证实了设计和制备具有高电子-空穴对分离效率的复合光催化剂也是实现其他高性能协同双功能光催化反应的重要途径。

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