Journal
CHEMISTRY OF MATERIALS
Volume 32, Issue 21, Pages 9107-9114Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.chemmater.0c01642
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Funding
- Engineering and Physical Sciences Research Council (EPSRC) [EP/N004884/1]
- Leverhulme Trust via the Leverhulme Research Centre for Functional Materials Design
- China Scholarship Council
- EPSRC [EP/N004884/1, EP/J019364/1] Funding Source: UKRI
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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 mu mol 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.
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