Abstract

An overall carbon-neutral CO2 electroreduction requires enhanced conversion efficiency and intensified functionality of CO2-derived products to balance the carbon footprint from CO2 electroreduction against fixed CO2. A liquid Sn cathode is herein introduced into electrochemical reduction of CO2 in molten salts to fabricate core-shell Sn-C spheres (Sn@C). An in-situ generated Li2SnO3/C directs a self-template formation of Sn@C. Benefitting from the accelerated reaction kinetics from the liquid Sn cathode and the core-shell structure of Sn@C, a CO2-fixation current efficiency higher than 84% and a high reversible lithium-storage capacity of Sn@C are achieved. The versatility of this strategy is demonstrated by other low melting point metals, such as Zn and Bi. This process integrates energy-efficient CO2 conversion and template-free fabrication of value-added metal-carbon, achieving an overall carbon-neutral electrochemical reduction of CO2.

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