Interface Engineering of Silver-Based Heterostructures for CO2 Reduction Reaction

Xiaolei Yuan, Yueshen Wu, Bei Jiang, Zishan Wu, Zixu Tao, Xu Lu, Jie Liu, Tao Qian, Haiping Lin, Qiao Zhang

Research output: Contribution to journalArticlepeer-review

2 Scopus citations

Abstract

The production of CO from the CO2 reduction reaction (CO2RR) is of great interest in the renewable energy storage and conversion, the neutral carbon emission, and carbon recycle utilization. Silver (Ag) is one of the catalytic metals that are active for electrochemical CO2 reduction into CO, but the catalysis requires a large overpotential to achieve higher selectivity. Constructing a metal-oxide interface could be an effective strategy to boost both activity and selectivity of the catalysis. Herein, density functional theory (DFT) calculations were first conducted to reveal the chemical insights of the catalytic performance on the interface between metal oxide and Ag(111) (MOx/Ag(111)). The results show that the *COOH intermediates can be more stabilized on the surfaces of MOx/Ag(111) than pure Ag(111). The hydrogen evolution reaction on MOx/Ag(111) can be suppressed due to the significantly higher Gibbs free energy for hydrogen adsorption (ΔGH*), thereby enhancing the selectivity toward CO2RR. A series of MOx/Ag composites with the unique interface based on the DFT results were then introduced though a two-step approach. The as-obtained MOx/Ag catalysts boosted both the CO activity and selectivity at a relatively positive potential range, especially in the case of MnO2/Ag. The reduction current density on the MnO2/Ag catalyst can reach 4.3 mA cm-2 at -0.7 V (vs RHE), which is 21.5 times higher than that on pure Ag, and the overpotential of CO2 to CO (390 mV) possesses is much lower than that on pure Ag NPs (690 mV). This study proposes an effective design strategy to construct a metal-oxide interface for CO2RR based on the synergistic effect between metals and MOx.
Original languageEnglish (US)
Pages (from-to)56642-56649
Number of pages8
JournalACS Applied Materials and Interfaces
Volume12
Issue number50
DOIs
StatePublished - Dec 16 2020
Externally publishedYes

ASJC Scopus subject areas

  • Materials Science(all)

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