Covalent organic frameworks with tunable Co–N–C for high-performance carbamate decomposition via sulfonic modification in amine-based CO2 capture

Abstract

Nanowire-like COF support with sulfo group (-SO3H) decoration was designed and synthetized, to offer favourable conditions for atomically dispersing Co atoms (S–Co/NC). The ingenious coordination of sulfo group synergistically improved COF structure and Co–N–C scheme, creating high surface area and excellent catalytic activity. Lab-scale experimental evaluations confirmed that the maximum CO2 desorption rate of spent MEA-solvent increased significantly by 733 % (3.74 CO2 mmol/min) after introducing S–Co/NC catalysts, ascribed to its contribution for proton transfer and C-N break. Bench-scale experiments demonstrated that a mere 0.0125 wt% of catalyst in MEA-solvent substantially decreased the CO2 loading of lean solvent by 17.7 % at low desorption temperatures (120→110 °C), resulting in a 28.8 % reduction in energy consumption. Furthermore, the negligible degradation of catalytic performance during 100-h testing wall-validated the stability and durability of the S–Co/NC catalysts. This work provided a prominent COF-based solid acid catalysts for energy-saving solvent regeneration during amined-based CO2 capture.