Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 58, Issue 36, Pages 12392-12397Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201906890
Keywords
CO2 photoreduction; covalent organic frameworks; electron transfer; H2O photooxidation
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Funding
- NSFC [21622104, 21701085, 21871141, 2187114]
- NSF of Jiangsu Province of China [BK20171032]
- Natural Science Research of Jiangsu Higher Education Institutions of China [17KJB150025]
- Priority Academic Program Development of Jiangsu Higher Education Institutions
- Foundation of Jiangsu Collaborative Innovation Center of Biomedical Functional Materials
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Solar energy-driven conversion of CO2 into fuels with H2O 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 H2O, 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 H2O oxidation. By adjusting the band structures of TTCOFs, TTCOF-Zn achieved the highest photocatalytic CO production of 12.33 mu mol with circa 100 % selectivity, along with H2O oxidation to O-2. 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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