Linking oxidative and reductive clusters to prepare crystalline porous catalysts for photocatalytic CO<sub>2</sub> reduction with H<sub>2</sub>O.
basic_science · Level V
Where this comes from
- Record sourced from PubMed, PMID 35948601.
- Also identified by DOI 10.1038/s41467-022-32449-z and PMC identifier 9365760.
- Licence recorded as CC BY.
- The licence permits redistribution, so the abstract is shown in full and the full text is available from the publisher.
Abstract
Mimicking natural photosynthesis to convert CO<sub>2</sub> with H<sub>2</sub>O into value-added fuels achieving overall reaction is a promising way to reduce the atmospheric CO<sub>2</sub> level. Casting the catalyst of two or more catalytic sites with rapid electron transfer and interaction may be an effective strategy for coupling photocatalytic CO<sub>2</sub> reduction and H<sub>2</sub>O oxidation. Herein, based on the MOF ∪ COF collaboration, we have carefully designed and synthesized a crystalline hetero-metallic cluster catalyst denoted MCOF-Ti<sub>6</sub>Cu<sub>3</sub> with spatial separation and functional cooperation between oxidative and reductive clusters. It utilizes dynamic covalent bonds between clusters to promote photo-induced charge separation and transfer efficiency, to drive both the photocatalytic oxidative and reductive reactions. MCOF-Ti<sub>6</sub>Cu<sub>3</sub> exhibits fine activity in the conversion of CO<sub>2</sub> with water into HCOOH (169.8 μmol g<sup>-1</sup>h<sup>-1</sup>). Remarkably, experiments and theoretical calculations reveal that photo-excited electrons are transferred from Ti to Cu, indicating that the Cu cluster is the catalytic reduction center.