Integrated Electrochemical Carbon Capture and Utilization by Redox‐Active Amine Grafted Gold Nanoparticles

Abstract Electrochemical carbon capture and utilization (eCCU) from flue gas CO 2 could avoid high energy consumption and capital input in conventional capture, storage, and utilization, which is a promising approach for achieving negative emissions and producing “e‐chemicals.” However, low CO 2 concentration and leftover O 2 in the flue gas presumably lowers the eCCU performance. Herein, redox‐active 2‐amino‐5‐mercapto‐1,3,4‐thiadiazole (AMT) functionalized gold nanoparticles are synthesized to achieve integrated electrochemical capture and reduction of CO 2 in simulated flue gas (SFG, 15% CO 2 , 4% O 2 , balanced with N 2 ), achieving maximum CO Faradaic efficiency of 80.2% at −0.45 V versus RHE in H‐type cell, and 66.0% at voltage of 2.7 V in a full cell, respectively. The AMT ligand can capture CO 2 by strong interaction with CO 2 in the reduced state and serve as a selective layer to suppress O 2 reduction, which provides the ability of electrochemical carbon capture from SFG and significantly decreases energy required for CO 2 electro‐reduction.