The active sites of 0.5Cu@CeO2 exhibit atomic level dispersion with abundant FLPs.
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The photothermal methanol yield of 0.5Cu@CeO2 reached 1896.02 μmol·gcat–1·mL–1.
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The new FLPs resulting from Cu2+ replacing Ce3+ promote the upward shift of CB.
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The FLPs of 0.5Cu@CeO2 promote the parallel adsorption of CO2 and *CO species.
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Ov can inhibit the dissociation of oxygen species and boost methanol synthesis.
Abstract
Photothermal CO2 into methanol is an effective approach to address energy and environmental challenges, but the low conversion and poor selectivity limit its large-scale application. Here, 0.5Cu@CeO2 with atomically dispersed active sites and abundant Frustrated-Lewis-pairs (FLPs) was synthesized using coordination complex precipitation reaction. The substitution of Cu2+ with Ce3+ results in the formation of new FLPs, which promotes the upward shift of conduction band (CB) and enhances the reducing capability of catalyst. Moreover, the more sensitive and stronger capability of photogenerated carriers also endows 0.5Cu@CeO2 with stronger CO2 reduction capability. The photothermal methanol yield of 0.5Cu@CeO2 reached 1896.02 μmol·gcat–1·h–1. The DFT results demonstrate the FLPs structure of 0.5Cu@CeO2 promotes parallel adsorption of CO2 and *CO species. Meanwhile, the presence of Ov inhibits the dissociation of oxygen species, consequently boosting the methanol synthesis. The construction of FLPs structure introduces a novel method to enhance CO2 conversion utilizing photothermal catalysis.
