近日，中山大学吴明娒团队报道了强不对称局域电场促进NO高效深度氧化的供体-π-受体共轭聚合物光催化剂。该项研究成果发表在2025年10月13日出版的《德国应用化学》杂志上。

光催化低浓度NO_x转化为NO₃受强激子效应、光生载流子的快速重组以及催化剂中氧缺乏局部键合位点的限制。在活性位点上定向富集载流子和反应物（O₂和NO）是实现高效光催化去除NO的必要条件。

研究组通过将超薄氮化碳纳米片与供电子的π -芘-π分子共价结合，设计了一种供体-π -受体（D -π - a）共轭聚合物催化剂，该催化剂对NO的去除率高达82.2%，对离子产物NO₃选取。（75.9%），稳定运行超过1000分钟，优于先前报道的氮化碳光催化剂。在模拟环境室中，也实现了将NO水平迅速降低到安全浓度以下。

在D-π-A共轭聚合物催化剂中，通过接受电子的庚烷环和给予电子的芘单元之间的分子内电荷转移产生不对称局域电场，有利于激子解离，加速电荷转移动力学，并为捕获O₂和NO提供双重吸附位点，有利于O₂活化，使NO高选择性氧化为NO₃这项工作强调了不对称局部电场在D-π-A结构中促进高效光催化NO氧化的关键作用。

附：英文原文

Title: Donor−π−Acceptor Conjugated Polymeric Photocatalyst for Efficient Deep Oxidation of NO Facilitated by Strong Asymmetric Local Electric Field

Author: Kui Li, Zhijian Xiao, Jingling Yang, Jingnan Tu, Yangsen Xu, Mingshan Zhu, Mingmei Wu

Issue&Volume: 2025-10-13

Abstract: Photocatalytic conversion of low-concentration NOx into NO3 is limited by strong exciton effects, rapid recombination of photogenerated charge carriers, and lack of localized bonding sites of oxygen species in catalysts. Directed enrichment of charge carriers and reactants (O2 and NO) at active sites is essential for achieving high-performance photocatalytic NO removal. Herein, a donor–π–acceptor (D–π–A) conjugated polymeric catalyst was engineered by covalently incorporating ultrathin carbon nitride nanosheets with electron-donating π–pyrene–π molecules, which achieves an exceptional 82.2% NO elimination and 94.9% selectivity toward ionic products (NO3 sel. of 75.9%) with stable operation over 1000 mins, outperforming the previously reported carbon nitride photocatalysts. Rapidly reduces NO levels below safe concentration in a simulated environment chamber was also achieved. The generated asymmetric local electric field in D–π–A conjugated polymeric catalyst through intramolecular charge transfer between electron-accepting heptazine rings and electron-donating pyrene units facilitates exciton dissociation, accelerating charge transfer kinetics, and offer dual adsorption sites for capture O2 and NO, thus favoring the O2 activation for highly selective oxidization of NO to NO3. This work highlights the pivotal role of asymmetric local electric fields in D–π–A architectures for advancing efficient photocatalytic NO oxidation.

DOI: 10.1002/anie.202518300

Source: https://onlinelibrary.wiley.com/doi/10.1002/anie.202518300