Wang Shengdong, Xie Zhipeng, Zhu Da, Fu Shuai, Wu Yishi, Yu Hongling, Lu Chuangye, Zhou Panke, Bonn Mischa, Wang Hai I, Liao Qing, Xu Hong, Chen Xiong, Gu Cheng
College of Polymer Science and Engineering, State Key Laboratory of Polymer Materials Engineering, Sichuan University, 610065, Chengdu, People's Republic of China.
State Key Laboratory of Luminescent Materials and Devices, Institute of Polymer Optoelectronic Materials and Devices, South China University of Technology, 510640, Guangzhou, People's Republic of China.
Nat Commun. 2023 Oct 28;14(1):6891. doi: 10.1038/s41467-023-42720-6.
Developing efficient artificial photocatalysts for the biomimetic photocatalytic production of molecular materials, including medicines and clean energy carriers, remains a fundamentally and technologically essential challenge. Hydrogen peroxide is widely used in chemical synthesis, medical disinfection, and clean energy. However, the current industrial production, predominantly by anthraquinone oxidation, suffers from hefty energy penalties and toxic byproducts. Herein, we report the efficient photocatalytic production of hydrogen peroxide by protonation-induced dispersible porous polymers with good charge-carrier transport properties. Significant photocatalytic hydrogen peroxide generation occurs under ambient conditions at an unprecedented rate of 23.7 mmol g h and an apparent quantum efficiency of 11.3% at 450 nm. Combined simulations and spectroscopies indicate that sub-picosecond ultrafast electron "localization" from both free carriers and exciton states at the catalytic reaction centers underlie the remarkable photocatalytic performance of the dispersible porous polymers.
开发用于仿生光催化生产分子材料(包括药物和清洁能源载体)的高效人工光催化剂,仍然是一项在基础和技术层面都至关重要的挑战。过氧化氢广泛应用于化学合成、医学消毒和清洁能源领域。然而,目前主要通过蒽醌氧化法进行的工业生产,存在能源消耗大以及产生有毒副产物的问题。在此,我们报道了通过质子化诱导的具有良好电荷载流子传输性能的可分散多孔聚合物高效光催化生产过氧化氢。在环境条件下,以空前的速率23.7 mmol g h以及在450 nm处11.3%的表观量子效率实现了显著的光催化过氧化氢生成。结合模拟和光谱分析表明,在催化反应中心,来自自由载流子和激子态的亚皮秒超快电子“局域化”是可分散多孔聚合物卓越光催化性能的基础。