Single-atom catalysts with bimetallic centers for high-performance electrochemical CO2 reduction

• DOI: 10.1016/j.mattod.2021.01.011
• Publication Date: 2021-02-27T10:05:58Z
• Authors: Xiao Yang; Trinny Tat; Alberto Libanori; Jun Cheng; Xiaoxu Xuan; Niu Liu; Xian Yang; Junhu Zhou; Ardo Nashalian; Jun Chen
• Keywords: Bimetallic strip; Molar ratio

Abstract The electrochemical CO2 reduction reaction (CO2RR) is a promising approach to alleviating global warming while concomitantly producing synthesis gas. Simultaneously achieving high current densities and tunable CO/H2 (syngas) ratios remains a highly desired yet difficult challenge. Herein, we developed a 3D carbon-based material exhibiting bimetallic centers (NiNC and FeNC) with synergistic effects for the CO2RR. The molar CO/H2 ratio (∼1:3 to ∼4:1) was altered by varying the configuration structures of the metal-N sites and tuning the applied potential for industrial applications of syngas. Density functional theory calculations verified these experimental results. Additionally, varying the configuration structures of bimetallic centers changed the rate-limiting steps of FePc@NiNC(+0.95 eV), NiNC/FeNC (+1.25 eV) and NiPc@FeNC (+1.37 eV) for CO2RR, while maintaining high catalytic activity with tunable syngas production. The reported materials system in this work represents a significant advancement of the CO2RR towards practical applications.