Stable, active CO2 reduction to formate via redox-modulated stabilization of active sites

Author:

Li Le,Ozden Adnan,Guo Shuyi,Garcı́a de Arquer F. PelayoORCID,Wang Chuanhao,Zhang Mingzhe,Zhang Jin,Jiang Haoyang,Wang WeiORCID,Dong HaoORCID,Sinton DavidORCID,Sargent Edward H.ORCID,Zhong Miao

Abstract

AbstractElectrochemical reduction of CO2 (CO2R) to formic acid upgrades waste CO2; however, up to now, chemical and structural changes to the electrocatalyst have often led to the deterioration of performance over time. Here, we find that alloying p-block elements with differing electronegativities modulates the redox potential of active sites and stabilizes them throughout extended CO2R operation. Active Sn-Bi/SnO2 surfaces formed in situ on homogeneously alloyed Bi0.1Sn crystals stabilize the CO2R-to-formate pathway over 2400 h (100 days) of continuous operation at a current density of 100 mA cm−2. This performance is accompanied by a Faradaic efficiency of 95% and an overpotential of ~ −0.65 V. Operating experimental studies as well as computational investigations show that the stabilized active sites offer near-optimal binding energy to the key formate intermediate *OCHO. Using a cation-exchange membrane electrode assembly device, we demonstrate the stable production of concentrated HCOO solution (3.4 molar, 15 wt%) over 100 h.

Publisher

Springer Science and Business Media LLC

Subject

General Physics and Astronomy,General Biochemistry, Genetics and Molecular Biology,General Chemistry

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