首页|Enhancing *CO coverage on Sm-Cu2O via 4f-3d orbital hybridization for highly efficient electrochemical CO2 reduction to C2H4
Enhancing *CO coverage on Sm-Cu2O via 4f-3d orbital hybridization for highly efficient electrochemical CO2 reduction to C2H4
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The electrocatalytic conversion of CO2 into valuable chemical feedstocks using renewable electricity offers a compelling strategy for closing the carbon loop.While copper-based materials are effective in catalyzing CO2 to C2+products,the instability of Cu+species,which tend to reduce to Cu0 at cathodic potentials during CO2 reduction,poses a significant challenge.Here,we report the development of Sm-Cu2O and investigate the influence of f-d orbital hybridization on the CO2 reduction reaction(CO2RR).Supported by density functional theory(DFT)calculations,our experimental results demonstrate that hybridization between Sm3+4f and Cu+3d orbitals not only improves the adsorption of*CO intermediates and increases CO coverage to stabilize Cu+but also facilitates CO2 activation and lowers the energy bar-riers for C—C coupling.Notably,Sm-Cu2O achieves a Faradaic efficiency for C2H4 that is 38％higher than that of undoped Cu2O.Additionally,it sustains its catalytic activity over an extended operational period exceeding 7 h,compared to merely 2 h for the undoped sample.This research highlights the potential off-d orbital hybridization in enhancing the efficacy of copper-based catalysts for CO2RR,pointing towards a promising direction for the development of durable,high-performance electrocatalysts for sustainable chemical synthesis.
Electrochemical CO2 reductionF-d orbital hybridizationAdsorption of *COCO coverageC2+products
State Key Laboratory of Organic-Inorganic Composites,Beijing Advanced Innovation Center for Soft Matter Science and Engineering,Beijing University of Chemical Technology,Beijing 100029,China
Zolix Instruments Company Limited,Beijing 101102,China
School of Mechanical and Manufacturing Engineering,University of New South Wales,Sydney 2052,New South Wales,Australia
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