Digital and Experimental Design of CO₂-Responsive Polymers based on Acrylamide Monomers for Carbon Capture

Abstract

This study provides a comprehensive evaluation of the CO₂ capture performance of the CO₂-responsive homopolymer poly (N‐[3‐(dimethylamino)propyl]‐acrylamide) (PDMAPAm) and its diblock copolymer poly (N‐[3‐(dimethylamino)propyl]‐acrylamide)‐b‐poly(methyl methacrylate) (PDMAPAm‐b‐PMMA), with a particular emphasis on their integration into membrane adsorbers for direct air capture (DAC) applications. A key focus is the coupling of polymerization kinetics with adsorption kinetics to enable the rational design of polymer materials based on their CO₂ adsorption behavior. By systematically varying the molar mass of the amine-functional PDMAPAm block and the poly(methyl methacrylate) ( PMMA) content, the study identifies optimal polymer compositions that balance high CO₂ uptake with favorable processing characteristics. Adsorption experiments conducted under dry conditions revealed a physisorption-dominated mechanism, where CO₂ primarily interacts with tertiary amine and carbonyl functional groups. A unified kinetic model was developed to integrate both adsorption and polymerization processes, allowing predictive optimization of polymer structure and performance. Furthermore, the influence of temperature and pressure on CO₂ uptake was assessed, establishing optimal operating conditions for DAC.