Lan Zhi-An, Wu Meng, Fang Zhongpu, Chi Xu, Chen Xiong, Zhang Yongfan, Wang Xinchen
State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou, 350116, P. R. China.
College of Chemical Engineering, Fuzhou University, Fuzhou, 350116, P. R. China.
Angew Chem Int Ed Engl. 2021 Jul 19;60(30):16355-16359. doi: 10.1002/anie.202103992. Epub 2021 Jun 17.
Charge generation and separation are regarded as the major constraints limiting the photocatalytic activity of polymeric photocatalysts. Herein, two new linear polyarylether-based polymers (PAE-CPs) with distinct linking patterns between their donor and acceptor motifs were tailor-made to investigate the influence of different linking patterns on the charge generation and separation process. Theoretical and experimental results revealed that compared to the traditional single-stranded linker, the double-stranded linking pattern strengthens donor-acceptor interactions in PAE-CPs and generates a coplanar structure, facilitating charge generation and separation, and enabling red-shifted light absorption. With these prominent advantages, the PAE-CP interlinked with a double-stranded linker exhibits markedly enhanced photocatalytic activity compared to that of its single-strand-linked analogue. Such findings can facilitate the rational design and modification of organic semiconductors for charge-induced reactions.
电荷产生与分离被视为限制聚合物光催化剂光催化活性的主要因素。在此，定制了两种新型的基于线性聚芳醚的聚合物（PAE-CPs），其供体和受体基序之间具有不同的连接模式，以研究不同连接模式对电荷产生与分离过程的影响。理论和实验结果表明，与传统的单链连接体相比，双链连接模式增强了PAE-CPs中供体-受体相互作用，并产生了共面结构，促进了电荷产生与分离，并使光吸收发生红移。具有这些突出优势，与双链连接体互连的PAE-CP与其单链连接类似物相比，表现出显著增强的光催化活性。这些发现有助于合理设计和修饰用于电荷诱导反应的有机半导体。
