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  Liang, L.; Firschke, F.; Wang, J.; Yang, L.; Wang, X.; Ju, W.; Mayer, M.T.; Strasser, P.: Anion effects govern efficiency of electrochemical amine-mediated CO₂ capture/release. Nature Communications 17 (2026), p. 489/1-10

10.1038/s41467-025-67177-7
Open Access Version

Abstract:
Ambient electrochemical CO2 capture powered by renewable energy offers a promising carbon removal route, exemplified by the emerging electrochemically mediated amine regeneration (EMAR) process demonstrated in lab-scale single cells and stacks. However, molecular-level insight into EMAR interfacial kinetics is still missing, particularly at the anode, where CO2 release involves a mechanistically non-trivial re-complexation process at the electrode–electrolyte interface, coupling heterogeneous metal-ion release with bulk complexation. Here, we report the time-resolved characterization of the interfacial molecular processes of the EMAR CO2 release process. Using in situ Fourier-transform infrared (FTIR) spectroscopy and ultraviolet-visible (UV-vis) spectroscopy, cyclic voltammetry, and real-time differential electrochemical mass spectrometry (DEMS), we examine how the nature of the electrolyte anion affects the CO2 release onset potentials. The time-resolved analyses reveal that Cl⁻ ions are more effective in releasing Cu ions and hence CO2 than nitrate or perchlorate. Molecular dynamics simulations show that strong surface Cu–Cl interactions likely facilitate favorable CO2 and carbamate adsorption kinetics. We expect that this study paves the way for broader use of interfacial in-situ analytics in electrified CO2 capture and release.