Abstract

As a potential approach to mitigate greenhouse effect meanwhile produce value-added chemical, electrochemical reduction reaction of CO2 (eCO2RR) to formate has gained increasing popularity recently, while its development is impeded by lack of electrocatalyst with satisfying selectivity and activity and low toxicity. Herein, we develop bimetallic Zn3Sn2 catalyst in-situ originated from the hetero-structured ZnxSnyOz nanoparticles supported on CNTs. With an optimized composition, the Zn3Sn2 catalyst (YSn = 39.1 %) achieves higher selectivity for formate by suppressing CO adsorption and reducing the energy barrier of formate intermediate *OCHO compared to its pristine counterparts, which is supported by DFT calculation. It enables a remarkably high Faradic efficiency (FE)formate of 96.7 %, formate yield (924 ppm h−1 mg−1), 26.0 mA cm−2 partial current density of formate (jformate), and better durability in flow cell at −1.1 V vs. reversible hydrogen electrode (RHE), which outperforms most of the reported electrocatalysts for CO2-to-formate conversion. The enhanced formate production from eCO2RR is unlocked for the synergistic effect between Zn-Sn system, implicating vast possibility to improve the electrocatalytic reactivity utilizing metal-metal interaction.

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