Mechanistic and Stability Study of the Integrated CO2 Capture-Electroreduction Process in Ethanolamine Solution over Ni/NC Atomic Catalysts

● The optimal electrocatalytic conditions in MEA-CO 2 electrolyte were determined based on Ni/NC catalysts, maximun 91% of FE CO achieved. ● The reaction mechanism of the integrated CO 2 Capture-Electroreduction Process (ICCE) in ethanolamine solution was elucidated ● The significance of temperature and CO 2 loading in the solution for the faradaic efficiency of CO in ICCE process was verified. ● The operational durability of the ICCE process were demonstrated, 80% of FEco can be maintained during 10h electrochemical reduction. In recent years, the integrated systems for the cost-effective conversion of CO 2 into high-value products have emerged as a major research focus in advancing sustainable green chemistry. The integrated process not only addresses the high energy consumption during desorption but also simplifies the process and reduces costs. However, further improving CO 2 conversion efficiency and achieving system stability remain significant challenges. Here, we report an integrated CO 2 capture and electroreduction process (ICCE) using atomically dispersed Nickel catalysts (Ni/NC) for the direct electroreduction of CO 2 absorbed in 30 wt.% ethanolamine (MEA, MAE, EAE, DMEA) solutions to CO, achieving a high Faradaic efficiency of up to 91%. In addition, the authors compared the effects of different reaction temperatures and different partial pressures of CO 2 in the gas phase on the prolonged electroreduction reaction, and suggested that the integrated system maintaining a gas-liquid equilibrium, can be guaranteed to continuously electrolyze to produce CO at a high Faraday efficiency. Through multiple characterizations, like NMR spectroscopy and In-situ Raman spectroscopy, revealed that CO is primarily derived from interfacially regenerated free CO 2 , while carbamate species are not directly reduced but instead adsorb on the Ni/NC catalyst surface as inhibitory intermediates.