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稳定的超小 Au 团簇以增强光氧化还原催化。

Stabilizing ultrasmall Au clusters for enhanced photoredox catalysis.

机构信息

State Key Laboratory of Photocatalysis on Energy and Environment College of Chemistry, Fuzhou University, 350116, Fuzhou, People's Republic of China.

College of Chemistry, New Campus, Fuzhou University, 350116, Fuzhou, People's Republic of China.

出版信息

Nat Commun. 2018 Apr 18;9(1):1543. doi: 10.1038/s41467-018-04020-2.

Abstract

Recently, loading ligand-protected gold (Au) clusters as visible light photosensitizers onto various supports for photoredox catalysis has attracted considerable attention. However, the efficient control of long-term photostability of Au clusters on the metal-support interface remains challenging. Herein, we report a simple and efficient method for enhancing the photostability of glutathione-protected Au clusters (Au GSH clusters) loaded on the surface of SiO sphere by utilizing multifunctional branched poly-ethylenimine (BPEI) as a surface charge modifying, reducing and stabilizing agent. The sequential coating of thickness controlled TiO shells can further significantly improve the photocatalytic efficiency, while such structurally designed core-shell SiO-Au GSH clusters-BPEI@TiO composites maintain high photostability during longtime light illumination conditions. This joint strategy via interfacial modification and composition engineering provides a facile guideline for stabilizing ultrasmall Au clusters and rational design of Au clusters-based composites with improved activity toward targeting applications in photoredox catalysis.

摘要

最近,将负载配体保护的金(Au)簇作为可见光光敏剂负载到各种载体上用于光氧化还原催化引起了相当大的关注。然而,有效地控制 Au 簇在金属-载体界面上的长期光稳定性仍然具有挑战性。在此,我们报道了一种简单有效的方法,通过利用多功能支化聚乙烯亚胺(BPEI)作为表面电荷修饰、还原和稳定剂,来提高负载在 SiO2球表面的谷胱甘肽保护的 Au 簇(AuGSH 簇)的光稳定性。通过控制厚度的 TiO2壳的顺序涂层可以进一步显著提高光催化效率,而这种结构设计的核壳 SiO2-AuGSH 簇-BPEI@TiO2复合材料在长时间光照条件下仍保持高的光稳定性。这种通过界面修饰和组成工程的联合策略为稳定超小 Au 簇以及合理设计基于 Au 簇的复合材料提供了一个简便的指导原则,这些复合材料在光氧化还原催化中的靶向应用中具有更高的活性。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/0723/5906565/bdffd071adee/41467_2018_4020_Fig1_HTML.jpg

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