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| 2024-01-06 11:55:15 | onclick： | Scientists Build Multi-Cluster Assembly Catalyst for Series Conversion Reactions |
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Recently, Professor Liu Jiang/Lan Yagan of the School of Chemistry of South China Normal University made important progress in the field of photocatalysis, designed and constructed two multi-functional cluster catalysts.The results were published in Nature Synthesis.
Solar-powered carbon dioxide reduction reactions (CO2RR) that directly convert CO2 into useful chemicals have become a promising technology for carbon dioxide recycling.As a common side reaction, hydrogen precipitation reaction (HER) not only reduces the product selectivity of CO2 light reduction, but also leads to the production of hydrogen (H2), carbon-based reduced gaseous products and unconverted CO2 mixture.Although some specific proportions of CO and H2 mixtures can be industrial converted as syngas, a mixture of low concentrations of CO, H2 and remaining untransformed CO2 is not suitable for Feto synthesis in low-selective CO2 photo reduction systems.Therefore, the reduction of CO2 light to syngas for conversion is only proposed as a conceptual work, but it has not been realized at present.
Based on this, the Lanagan team designed and constructed two highly active, multifunctional cluster-based catalysts formed from W10 polymetallic hydrochloride assemblies (Ni5W10 and Ni6W10) with reducing activity and rapid electron transfer capability.The H2 and CO hybrid reduction products can be transformed into high-value olefin and carbonyl compounds, and the atomic utilization efficiency of the reduction products can reach 94%.
The low selective CO2 photo-reduction reaction coupled with the in-situ one-pot method can greatly improve the overall photo-conversion efficiency (from 935 μmol g-1h-1 to 1425.0 μmol g-1h-1), CO-selectivity (from 50% to 80.0%) and alkyne to olefin (Conv). > 86.0%, Sel. ≈100.0%）。More importantly, Ni6W10 with co-active region can reduce the energy barrier of hydrogenation process by Volmer-Tafel mechanism compared with the Volmer-Heyrovsky reaction path of Ni5W10 with independent active site.
In short, the three-series system can not only inhibit the formation of H2 by-products, but also control the selectivity of photocatalytic CO2RRR, and can appreciate and separate low-value H2 and CO in turn.At the same time, 13C-labeled antidepressant molecules and deuterolefin compounds can be easily synthesized by triple series reaction.This series system with high atomic utilization provides a broad prospect for the practical application of low selective photocatalytic CO2RRR in the future.
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