Simultaneous Capture of CO2 Boosting Its Electroreduction in the Micropores of a Metal–organic Framework

• Published in: Angewandte Chemie International Edition Vol. 62; no. 52; pp. e202311265 - n/a
• Main Authors: Liu, Yuan‐Yuan, Huang, Jia‐Run, Zhu, Hao‐Lin, Liao, Pei‐Qin, Chen, Xiao‐Ming
• Format: Journal Article
• Language: English
• Published: Weinheim Wiley Subscription Services, Inc 21.12.2023
• Edition: International ed. in English
• Subjects: Atmosphere; Carbon dioxide; Carbon sequestration; Catalysts; Chemical reduction; CO2 Enrichment/Capture; CO2 Relays; Electrochemical CO2 Reduction; Electrochemistry; Energy conversion; Energy conversion efficiency; Flue gas; Metal-organic frameworks; Metal–Organic Framework; Simulated Flue Gas; Simulation
• ISSN: 1433-7851; 1521-3773; 1521-3773
• DOI: 10.1002/anie.202311265

Integration of CO2 capture capability from simulated flue gas and electrochemical CO2 reduction reaction (eCO2RR) active sites into a catalyst is a promising cost‐effective strategy for carbon neutrality, but is of great difficulty. Herein, combining the mixed gas breakthrough experiments and eCO2RR tests, we showed that an Ag12 cluster‐based metal–organic framework (1‐NH2, aka Ag12bpy‐NH2), simultaneously possessing CO2 capture sites as “CO2 relays” and eCO2RR active sites, can not only utilize its micropores to efficiently capture CO2 from simulated flue gas (CO2 : N2=15 : 85, at 298 K), but also catalyze eCO2RR of the adsorbed CO2 into CO with an ultra‐high CO2 conversion of 60 %. More importantly, its eCO2RR performance (a Faradaic efficiency (CO) of 96 % with a commercial current density of 120 mA cm−2 at a very low cell voltage of −2.3 V for 300 hours and the full‐cell energy conversion efficiency of 56 %) under simulated flue gas atmosphere is close to that under 100 % CO2 atmosphere, and higher than those of all reported catalysts at higher potentials under 100 % CO2 atmosphere. This work bridges the gap between CO2 enrichment/capture and eCO2RR. Electrochemical CO2 reduction reaction occurs in the pores of a porous catalyst possessing CO2 capture sites, which boosts the catalytic performance virtually independent on the CO2 concentration.