Synergistic Modulation at Atomically Dispersed Fe/Au Interface for Selective CO<sub>2</sub> Electroreduction.

Shen, Xinyi; Liu, Xiaokang; Wang, Sicong; Chen, Tao; Zhang, Wei; Cao, Linlin; Ding, Tao; Lin, Yue et al. · Nano Lett · 2021

basic_science · Level V

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Abstract

The electrocatalytic carbon dioxide reduction reaction (CO<sub>2</sub>RR) offers an attractive route to fuels and feedstocks from renewable energy. Gold is active for the electrochemical CO<sub>2</sub>RR to CO, while the competing hydrogen evolution reaction is unavoidable. Here, we report a synergistic strategy, via introducing atomically dispersed Fe to tune the electronic structure of the Au nanoparticle, to improve the CO selectivity. By using operando X-ray absorption and infrared spectroscopies, we reveal the dynamic structural evolution and the adsorption of reactant intermediates at the single-atom Fe<sub>1</sub>/Au interface. During the reaction, the interaction between Fe and Au atoms becomes stronger, and the Fe<sub>1</sub>/Au synergies affect the adsorption of reaction intermediates, thus improving the selectivity of CO up to 96.3% with a mass activity of 399 mA mg<sup>-1</sup>. These results highlight the significant importance of synergistic modulation for advancing the single-atom decorated nanoparticle catalysis.