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• W4383313797 abstract "Efficient conversion of carbon dioxide (CO2) into value-added materials and feedstocks, powered by renewable electricity, presents a promising strategy to reduce greenhouse gas emissions and close the anthropogenic carbon loop. Recently, there has been intense interest in Cu2O-based catalysts for the CO2 reduction reaction (CO2RR), owing to their capabilities in enhancing C-C coupling. However, the electrochemical instability of Cu+ in Cu2O leads to its inevitable reduction to Cu0, resulting in poor selectivity for C2+ products. Herein, we propose an unconventional and feasible strategy for stabilizing Cu+ through the construction of a Ce4+ 4f-O 2p-Cu+ 3d network structure in Ce-Cu2O. Experimental results and theoretical calculations confirm that the unconventional orbital hybridization near Ef based on the high-order Ce4+ 4f and 2p can more effectively inhibit the leaching of lattice oxygen, thereby stabilizing Cu+ in Ce-Cu2O, compared with traditional d-p hybridization. Compared to pure Cu2O, the Ce-Cu2O catalyst increased the ratio of C2H4/CO by 1.69-fold during the CO2RR at -1.3 V. Furthermore, in situ and ex situ spectroscopic techniques were utilized to track the oxidation valency of copper under CO2RR conditions with time resolution, identifying the well-maintained Cu+ species in the Ce-Cu2O catalyst. This work not only presents an avenue to CO2RR catalyst design involving the high-order 4f and 2p orbital hybridization but also provides deep insights into the metal-oxidation-state-dependent selectivity of catalysts." @default.
• W4383313797 created "2023-07-07" @default.
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• W4383313797 date "2023-07-06" @default.
• W4383313797 modified "2023-10-10" @default.
• W4383313797 title "Boosting CO₂ Electroreduction to C₂H₄ <i>via</i> Unconventional Hybridization: High-Order Ce⁴⁺ 4f and O 2p Interaction in Ce-Cu₂O for Stabilizing Cu⁺" @default.
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• W4383313797 doi "https://doi.org/10.1021/acsnano.3c03952" @default.
• W4383313797 hasPubMedId "https://pubmed.ncbi.nlm.nih.gov/37410800" @default.
• W4383313797 hasPublicationYear "2023" @default.
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