Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 61, Issue 6, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202115854
Keywords
Hydrogen-bonded organic frameworks; Metallization; Photocatalytic CO2 reduction; Porphyrin; Structural stability
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Funding
- National Key Research and Development Program of China [2018YFA020860]
- Key Research Program of the Chinese Academy of Sciences [ZDRW-CN-2016-1]
- National Natural Science Foundation of China (NSFC) [21520102001, 21871267, 22005305]
- Key Research Program of Frontier Science, CAS [QYZDJ-SSW-SLH045]
- China Postdoctoral Science Foundation [2020M671955]
- Russian Science Foundation [18-73-10116]
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This study successfully prepared a series of metalloporphyrinic hydrogen-bonded organic frameworks (HOFs) with high surface area and excellent stability by introducing a transition metal which caused noticeable changes on noncovalent interaction, orbital overlap, and molecular geometry. These metalloporphyrinic HOFs were then used as photocatalysts for the photoreduction of CO2 to CO.
Under topological guidance, the self-assembly process based on a tetratopic porphyrin synthon results in a hydrogen-bonded organic framework (HOF) with the predicted square layers topology (sql) but unsatisfied stability. Strikingly, simply introducing a transition metal in the porphyrin center does not change the network topology but drastically causes noticeable change on noncovalent interaction, orbital overlap, and molecular geometry, therefore ultimately giving rise to a series of metalloporphyrinic HOFs with high surface area, and excellent stability (intact after being soaked in boiling water, concentrated HCl, and heated to 270 degrees C). On integrating both photosensitizers and catalytic sites into robust backbones, this series of HOFs can effectively catalyze the photoreduction of CO2 to CO, and their catalytic performances greatly depend on the chelated metal species in the porphyrin centers. This work enriches the library of stable functional HOFs and expands their applications in photocatalytic CO2 reduction.
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