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用金-二氧化铈杂化物修饰聚合氮化碳以提高光催化析氢活性。

Modification of Polymeric Carbon Nitride with Au-CeO Hybrids to Improve Photocatalytic Activity for Hydrogen Evolution.

作者信息

Zhang Linzhu, Chen Lu, Xia Yuzhou, Liang Zhiyu, Huang Renkun, Liang Ruowen, Yan Guiyang

机构信息

Province University Key Laboratory of Green Energy and Environment Catalysis, Ningde Normal University, Ningde 352100, China.

Fujian Provincial Key Laboratory of Featured Materials in Biochemical Industry, Ningde Normal University, Ningde 352100, China.

出版信息

Molecules. 2022 Nov 3;27(21):7489. doi: 10.3390/molecules27217489.

Abstract

The construction of a multi-component heterostructure for promoting the exciton splitting and charge separation of conjugated polymer semiconductors has attracted increasing attention in view of improving their photocatalytic activity. Here, we integrated Au nanoparticles (NPs) decorated CeO (Au-CeO) with polymeric carbon nitride (PCN) via a modified thermal polymerization method. The combination of the interfacial interaction between PCN and CeO via N-O or C-O bonds, with the interior electronic transmission channel built by the decoration of Au NPs at the interface between CeO and PCN, endows CeAu-CN with excellent efficiency in the transfer and separation of photo-induced carriers, leading to the enhancement of photochemical activity. The amount-optimized CeAu-CN nanocomposites are capable of producing ca. 80 μmol· H per hour under visible light irradiation, which is higher than that of pristine CN, Ce-CN and physical mixed CeAu and PCN systems. In addition, the photocatalytic activity of CeAu-CN remains unchanged for four runs in 4 h. The present work not only provides a sample and feasible strategy to synthesize highly efficient organic polymer composites containing metal-assisted heterojunction photocatalysts, but also opens up a new avenue for the rational design and synthesis of potentially efficient PCN-based materials for efficient hydrogen evolution.

摘要

鉴于提高共轭聚合物半导体的光催化活性,构建用于促进其激子分裂和电荷分离的多组分异质结构已引起越来越多的关注。在此,我们通过改进的热聚合方法将金纳米颗粒(NPs)修饰的CeO(Au-CeO)与聚合氮化碳(PCN)集成在一起。PCN与CeO之间通过N-O或C-O键的界面相互作用,与在CeO和PCN界面处通过金纳米颗粒修饰构建的内部电子传输通道相结合,赋予CeAu-CN在光生载流子转移和分离方面的优异效率,从而导致光化学活性增强。经过量优化的CeAu-CN纳米复合材料在可见光照射下每小时能够产生约80 μmol·H,高于原始CN、Ce-CN以及物理混合的CeAu和PCN体系。此外,CeAu-CN的光催化活性在4小时内进行四次循环后保持不变。本工作不仅为合成包含金属辅助异质结光催化剂的高效有机聚合物复合材料提供了一个示例和可行的策略,而且为合理设计和合成潜在高效的用于高效析氢的基于PCN的材料开辟了一条新途径。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5455/9656339/24ac8ba47276/molecules-27-07489-g001.jpg

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