Synergistic Modulation at Atomically Dispersed Fe/Au Interface for Selective CO2 Electroreduction

Xinyi Shen; Xiaokang Liu; Sicong Wang; Tao Chen; Wei Zhang; Linlin Cao; Tao Ding; Yue Lin; Dong Liu; Lan Wang; Wei Zhang; Tao Yao

doi:10.1021/acs.nanolett.0c04291

Synergistic Modulation at Atomically Dispersed Fe/Au Interface for Selective CO₂ Electroreduction

Nano Lett. 2021 Jan 13;21(1):686-692. doi: 10.1021/acs.nanolett.0c04291. Epub 2020 Dec 11.

Authors

Xinyi Shen¹, Xiaokang Liu¹, Sicong Wang¹, Tao Chen^{1

2}, Wei Zhang¹, Linlin Cao¹, Tao Ding¹, Yue Lin³, Dong Liu¹, Lan Wang^{1

2}, Wei Zhang⁴, Tao Yao¹

Affiliations

¹ National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei 230029, P. R. China.
² School of National Defense Science and Technology, Southwest University of Science and Technology, Mianyang 621010, P. R. China.
³ Hefei National Laboratory for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei 230029, P. R. China.
⁴ Chinese Academy of Sciences, Chongqing Institute of Green and Intelligent Technology, Chongqing 400714, P. R. China.

PMID: 33305576
DOI: 10.1021/acs.nanolett.0c04291

Abstract

The electrocatalytic carbon dioxide reduction reaction (CO₂RR) offers an attractive route to fuels and feedstocks from renewable energy. Gold is active for the electrochemical CO₂RR 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 Fe₁/Au interface. During the reaction, the interaction between Fe and Au atoms becomes stronger, and the Fe₁/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^-1. These results highlight the significant importance of synergistic modulation for advancing the single-atom decorated nanoparticle catalysis.

Keywords: CO2 electroreduction; Dynamic structures; Interfacial sites; Operando XAFS; Synergistic strategy.