Samsung Advanced Institute of Technology

Climate change has driven the need for carbon capture to mitigate anthropogenic greenhouse gas emissions, yet current thermochemical methods are hampered by high energy intensities. Electrochemically mediated carbon capture (EMCC) utilizing redox-active carbon dioxide (CO₂) carriers is an attractive alternative for carbon capture. Here, we introduce an economical vat dye compound, indigo, that can reversibly capture and release CO₂ upon electrochemical reduction and oxidation, respectively. Electrode and electrolyte engineering strategies were utilized to improve the reversibility and stability of indigo for EMCC. We also constructed a bench-scale prototypical fixed-bed carbon capture device to demonstrate indigo’s EMCC performance under various practically relevant conditions, such as simulated flue gas and extremely dilute sources pertinent to direct air capture. A hybrid sorbent electrode-gas diffusion layer approach was revealed to alleviate CO₂ mass transport limitations, achieving ~80% CO₂ capacity utilization under a 15% CO₂ feed stream. Furthermore, a reactive-diffusive mass transport model was developed to illustrate engineering approaches that can be universally applied to optimize fixed-bed EMCC systems. This work introduces the potential for a class of low-cost sorbents for EMCC while underscoring the importance of molecular, electrolyte, materials, and device engineering strategies to enable high-performance carbon capture.