Journal
APPLIED CATALYSIS B-ENVIRONMENTAL
Volume 274, Issue -, Pages -Publisher
ELSEVIER
DOI: 10.1016/j.apcatb.2020.119096
Keywords
CO2 photoreduction; COFs; Electron delocalization; Olefin-based; Single atom
Funding
- National Natural Science Foundation of China [51872107, 21975090, 51902121, 51802107, 21633004, 21633015, 11721404]
- World Premier International Research Center Initiative (WPI Initiative) on Materials Nanoarchitectonics (MANA), MEXT (Japan)
- Photoexcitonix Project in Hokkaido Univerisity, Japan
- Natural Science Foundation of Hubei Province [2019CFB322]
- Ministry of Science and Technology [2018YFA0208701]
- Fundamental Research Funds for the Central Universities [2662018QD011, 2662017JC021, 2662016PY088, 2662018QD041]
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The photocatalytic conversion of CO2 into chemical fuels represents a promising approach for solving the future energy crisis. However, the construction of a photocatalyst simultaneously integrating a photosensitizer and molecular cocatalyst with intramolecular electron delivery is challenging. Herein, we designed covalent organic frameworks (COFs) with excellent extended conjugation and potential embedded redox active sites. The full -C = C- bridging in sp(2)c-COFdpy creates and dredges the donor-acceptor channel for intramolecular electron delocalization and a cascade effect. Interestingly, CO2 photoreduction can be carried out in water, and the optimized sp(2)c-COFdpy-Co exhibits the highest activity and stability among COFs without noble metal involvement achieving up to 17.93 mmol g(-1) CO with 81.4 % selectivity in a long-range reaction. Theoretical calculations and experimental data suggest that the structural advantages enable excitons to facilely reach single Co sites via the electron cascade, which provides a new concept in the nanoarchitecture of COFs for efficient CO2 photoreduction.
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