Long Cheng, Rong Wang, Wenzhe Si, Yanxi Deng*, Junhua Li and Yue Peng*,
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引用次数: 0
Abstract
Cu-based catalysts leveraging Cu+/Cu0 active sites have emerged as pivotal for synthesizing essential hydrocarbons and alcohols in electrochemical CO2 reduction, such as ethylene and ethanol (C2 products). However, the dynamic reduction of Cu+ to Cu0 during electroreduction leads to site instability, resulting in diminished efficiency for CO2 conversion to C2 products. Herein, we introduced Si into CuO by the selective dissolution method, engendering Cu–O–Si units to stabilize the Cu+/Cu0 sites. The catalyst manifested good activity in CO2 electroreduction with an elevated Faradaic efficiency for C2 products reaching 81.9% at −100 mA/cm2. After ten cycles of electrochemical testing, the Cu+/Cu0 sites and performance exhibited no signs of degradation. The Si incorporation significantly improved the hybridization of O 2p and Cu 3d orbitals, thereby reinforcing the Cu–O bonds and stabilizing the Cu+/Cu0 sites, which was critical in promoting C–C coupling via decreasing the energy barriers for *OCCO formation and enhancing C2 product selection. The active Cu+ cations with unsaturated coordination contributed to the reaction stabilization, thereby improving the preservation of Cu2O metastable state.
期刊介绍:
ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels.
The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.