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1.
ChemSusChem ; : e202301881, 2024 Mar 11.
Artigo em Inglês | MEDLINE | ID: mdl-38467567

RESUMO

Conversion of CO2 into high-value chemicals using solar energy is one of promising approaches to achieve carbon neutrality. However, the oxidation of water in the photocatalytic CO2 reduction is kinetically unfavorable due to multi-electron and proton transfer processes, along with the difficulty in generating O-O bonds. To tackle these challenges, this study investigated the coupling reaction of photocatalytic CO2 reduction and selective propane oxidation using the Pd/P25 (1 wt%) catalyst. Our findings reveal a significant improvement in CO2 reduction, nearly fivefold higher, achieved by substituting water oxidation with selective propane oxidation. This substitution not only accelerates the process of CO2 reduction but also yields valuable propylene. The relative ease of propane oxidation, compared to water, appears to increase the density of photogenerated electrons, ultimately enhancing the efficiency of CO2 reduction. We further found that hydroxyl radicals and reduced intermediate (carboxylate species) played important roles in the photocatalytic reaction. These findings not only propose a potential approach for the efficient utilization of CO2 through the coupling of selective propane oxidation into propylene, but also provide insights into the mechanistic understanding of the coupling reaction.

2.
ChemSusChem ; 15(10): e202200216, 2022 May 20.
Artigo em Inglês | MEDLINE | ID: mdl-35301825

RESUMO

The photocatalytic conversion of CO2 into solar fuels or chemicals is a sustainable approach to relieve the immediate problems related to global warming and the energy crisis. This study concerns the effects of morphological control on a Cu/Cu2 O-based photocatalyst for CO2 reduction. The as-synthesized spherical Cu/Cu2 O photocatalyst exhibits higher activity than the octahedral one under visible light irradiation. The difference in photocatalytic performance between these two catalysts could be attributed to the following two factors: (1) The multifaceted structure of spherical Cu/Cu2 O favors charge separation; (2) octahedral Cu/Cu2 O only contains more positively charged (111) facets, which are unfavorable for CO2 photoreduction. The results further highlight the importance of utilizing crystal facet engineering to further improve the performance of CO2 reduction photocatalysts.

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