Zhang Jieping, Lei Hang, Li Zhijia, Jiang Feilong, Chen Lian, Hong Maochun
Department of Chemistry, School of Chemistry and Materials Science, University of Science and Technology of China, Hefei, Anhui, 230026, P. R. China.
State Key Laboratory of Structure Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, Fujian, 350002, P. R. China.
Angew Chem Int Ed Engl. 2024 Jan 15;63(3):e202316998. doi: 10.1002/anie.202316998. Epub 2023 Dec 8.
H O is a widely used eco-friendly oxidant and a potential energy carrier. Photocatalytic H O production from water and O is an ideal approach with the potential to address the current energy crisis and environmental issues. Three zig-zag two-dimensional coordination polymers (2D CPs), named CuX-dptz, were synthesized by a rapid and facile method at room temperature, showing preeminent H O photoproduction performance under pure water and open air without any additives. CuBr-dptz exhibits a H O production rate high up to 1874 μmol g h , exceeding most reported photocatalysts under this condition, even comparable to those supported by sacrificial agents and O . The coordination environment of Cu can be modulated by halogen atoms (X=Cl, Br, I), which in turn affects the electron transfer process and finally determines the reaction activity. This is the first time that 2D CPs have been used for photocatalytic H O production in such challenging conditions, which provides a new pathway for the development of portable in situ H O photosynthesis devices.
过氧化氢是一种广泛使用的环保型氧化剂和潜在的能量载体。由水和氧气光催化产生过氧化氢是一种理想的方法，有潜力解决当前的能源危机和环境问题。通过一种快速简便的方法在室温下合成了三种名为CuX-dptz的之字形二维配位聚合物（2D CP），在纯水和露天环境下无任何添加剂时表现出卓越的过氧化氢光生成性能。CuBr-dptz的过氧化氢生成速率高达1874 μmol g h ，超过了在此条件下大多数报道的光催化剂，甚至与那些由牺牲剂和氧气支持的光催化剂相当。铜的配位环境可由卤素原子（X = Cl、Br、I）调节，这反过来又影响电子转移过程并最终决定反应活性。这是首次在如此具有挑战性的条件下将二维配位聚合物用于光催化过氧化氢生成，为便携式原位过氧化氢光合作用装置的开发提供了一条新途径。
