Covalent Organic Framework Nanosheets Embedding Single Cobalt Sites for Photocatalytic Reduction of Carbon Dioxide



Wang, Xiaoyan, Fu, Zhiwei ORCID: 0000-0002-6428-8504, Zheng, Lirong, Zhao, Chengxi, Wang, Xue, Chong, Samantha Y ORCID: 0000-0002-3095-875X, McBride, Fiona ORCID: 0000-0003-2985-3173, Raval, Rasmita, Bilton, Matthew ORCID: 0000-0002-0475-2942, Liu, Lunjie
et al (show 4 more authors) (2020) Covalent Organic Framework Nanosheets Embedding Single Cobalt Sites for Photocatalytic Reduction of Carbon Dioxide. CHEMISTRY OF MATERIALS, 32 (21). pp. 9107-9114.

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Abstract

Covalent organic framework nanosheets (CONs), fabricated from two-dimensional covalent organic frameworks (COFs), present a promising strategy for incorporating atomically distributed catalytic metal centers into well-defined pore structures with desirable chemical environments. Here, a series of CONs was synthesized by embedding single cobalt sites that were then evaluated for photocatalytic carbon dioxide reduction. A partially fluorinated, cobalt-loaded CON produced 10.1 μmol carbon monoxide with a selectivity of 76%, over 6 hours irradiation under visible light (TON = 28.1), and a high external quantum efficiency (EQE) of 6.6% under 420 nm irradiation in the presence of an iridium dye. The CONs appear to act as a semiconducting support, facilitating charge carrier transfer between the dye and the cobalt centers, and this results in a performance comparable with that of the state-of-the-art heterogeneous catalysts in the literature under similar conditions. The ultrathin CONs outperformed their bulk counterparts in all cases, suggesting a general strategy to enhance the photocatalytic activities of COF materials.

Item Type: Article
Depositing User: Symplectic Admin
Date Deposited: 15 Dec 2020 10:40
Last Modified: 18 Jan 2023 23:17
DOI: 10.1021/acs.chemmater.0c01642
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URI: https://livrepository.liverpool.ac.uk/id/eprint/3110222