卟啉
四硫富瓦烯
共价键
人工光合作用
光化学
光敏剂
化学
晶体结构
光催化
催化作用
材料科学
电子转移
共价有机骨架
纳米技术
分子
结晶学
有机化学
作者
Meng Lu,Jiang Liu,Qiang Li,Mi Zhang,Ming Liu,Jinlan Wang,Daqiang Yuan,Ya‐Qian Lan
标识
DOI:10.1002/anie.201906890
摘要
Solar energy-driven conversion of CO2 into fuels with H2 O as a sacrificial agent is a challenging research field in photosynthesis. Herein, a series of crystalline porphyrin-tetrathiafulvalene covalent organic frameworks (COFs) are synthesized and used as photocatalysts for reducing CO2 with H2 O, in the absence of additional photosensitizer, sacrificial agents, and noble metal co-catalysts. The effective photogenerated electrons transfer from tetrathiafulvalene to porphyrin by covalent bonding, resulting in the separated electrons and holes, respectively, for CO2 reduction and H2 O oxidation. By adjusting the band structures of TTCOFs, TTCOF-Zn achieved the highest photocatalytic CO production of 12.33 μmol with circa 100 % selectivity, along with H2 O oxidation to O2 . Furthermore, DFT calculations combined with a crystal structure model confirmed the structure-function relationship. Our work provides a new sight for designing more efficient artificial crystalline photocatalysts.
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