State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, 116023, China.
Center of Materials Science and Optoelectronics Engineering, University of Chinese Academy of Sciences, Beijing, 100049, P. R. China.
Angew Chem Int Ed Engl. 2023 Jun 5;62(23):e202302829. doi: 10.1002/anie.202302829. Epub 2023 Apr 20.
Rational design of polymer structures at the molecular level promotes the iteration of high-performance photocatalyst for sustainable photocatalytic hydrogen peroxide (H O ) production from oxygen and water, which also lays the basis for revealing the reaction mechanism. Here we report a benzoxazine-based m-aminophenol-formaldehyde resin (APFac) polymerized at ambient conditions, exhibiting superior H O yield and long-term stability to most polymeric photocatalysts. Benzoxazine structure was identified as the crucial photocatalytic active segment in APFac. Favorable adsorption of oxygen/intermediates on benzoxazine structure and commendable product selectivity accelerated the reaction kinetically in stepwise single-electron oxygen reduction reaction. The proposed benzoxazine-based phenolic resin provides the possibility of production in batches and industrial application, and sheds light on the de novo design and analysis of metal-free polymeric photocatalysts.
在分子水平上对聚合物结构进行合理设计，促进了高性能光催化剂的迭代，从而实现了从氧气和水中可持续生产过氧化氢（H2O2），这也为揭示反应机制奠定了基础。在这里，我们报道了一种在环境条件下聚合的苯并恶嗪基间氨基酚-甲醛树脂（APFac），该树脂表现出优于大多数聚合光催化剂的 H2O2 产率和长期稳定性。苯并恶嗪结构被确定为 APFac 中关键的光催化活性片段。苯并恶嗪结构对氧气/中间体的有利吸附和出色的产物选择性在逐步单电子氧还原反应中加速了反应动力学。所提出的基于苯并恶嗪的酚醛树脂为批量生产和工业应用提供了可能性，并为无金属聚合型光催化剂的全新设计和分析提供了思路。
