In conclusion, four anthraquinone-functionalized carbon electrodes were synthesized and studied in this work to investigate how the pore structure and pre-existing functional groups impact electrochemical CO2 capture. The impact of pore structure on quinone grafting was investigated using gas sorption measurements and solid-state NMR, which revealed that the anthraquinone grafted in different pore environments in the different materials. All four materials showed the electrochemical capture and release of carbon dioxide, albeit with varying performance and stability. It was found that the presence of carbon mesopores (as in CMK-3) increased the grafted amount of quinone on the surface, but another factor, possibly multilayer stacks, limited stability when charging under CO2. Predominantly microporous materials (i.e. YP-80F) had lower quinone loadings on the surface but showed increased stability during cycling with competitive CO2 adsorption capacities. The removal of pre-existing functional groups before quinone grafting improved the quinone loading but did not result in any improvement in material stability under electrochemical cycling. Overall, f-YP-80F was the most promising material developed in this study with a CO2 capture capacity of 0.3 mmol g -1 after 200 cycles showing a large improvement in stability compared to mesoporous carbon samples. Overall, this study provides guidance on what is the preferable carbon structure for functionalized carbon electrodes for electrochemical CO2 capture. Further studies are needed for a detailed mechanistic study of degradation, to study the selectivity of this system under gas mixtures, and to scale up the electrodes, all of which will help to reach the full potential of this technology.