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

Abstract Electrochemical carbon capture and utilization (eCCU) from flue gas CO₂ 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 CO₂ concentration and leftover O₂ 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 CO₂ in simulated flue gas (SFG, 15% CO₂, 4% O₂, balanced with N₂), 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 CO₂ by strong interaction with CO₂ in the reduced state and serve as a selective layer to suppress O₂ reduction, which provides the ability of electrochemical carbon capture from SFG and significantly decreases energy required for CO₂ electro‐reduction.