journal article Aug 08, 2019

Rational Design of Crystalline Covalent Organic Frameworks for Efficient CO2 Photoreduction with H2O

Angewandte Chemie International Edition Vol. 58 No. 36 pp. 12392-12397 · Wiley
View at Publisher Save 10.1002/anie.201906890
Abstract
AbstractSolar 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 μmol with circa 100 % selectivity, along with H2O 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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535
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40
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Details
Published
Aug 08, 2019
Vol/Issue
58(36)
Pages
12392-12397
License
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Funding
National Natural Science Foundation of China Award: 21622104
Natural Science Research of Jiangsu Higher Education Institutions of China Award: 17KJB150025
Cite This Article
Meng Lu, Jiang Liu, Qiang Li, et al. (2019). Rational Design of Crystalline Covalent Organic Frameworks for Efficient CO2 Photoreduction with H2O. Angewandte Chemie International Edition, 58(36), 12392-12397. https://doi.org/10.1002/anie.201906890
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