Nanosilica polyamidoamine dendrimers for enhanced direct air CO2 capture

Abstract

Exploring efficient systems to recover CO2 from the atmosphere could be a way to address the global carbon emissions issue. Herein, we report the synthesis of nanosilica (NS) functionalized with polyamidoamine (PAMAM) dendrimers (NS-PAMAM) as efficient adsorbents for CO2 capture under simulated direct air capture (DAC) (400 ppm CO2 in helium at 30 °C) and indoor air (≥400 ppm, 50 ± 3% RH at 30 °C) conditions. The results inferred that the 1st (NS-G1.0), 2nd (NS-G2.0), 3rd (NS-G3.0), and 4th (NS-G4.0) generations of the NS-PAMAM dendrimers exhibited excellent performance for CO2 capture. Compared to the other generations, NS-G3.0 demonstrated superior CO2 adsorption capacities of 0.50 mmol g−1 under simulated dry CO2 conditions (400 ppm in He), 1.02 mmol g−1 under indoor air (dry) CO2 conditions (≥400 ppm, 26 ± 3% RH), and 1.54 mmol g−1 under indoor air (humid) CO2 conditions (≥400 ppm, 50 ± 3% RH). The study included the evaluation of CO2 adsorption-desorption performance of the NS-PAMAM dendrimers under varying structural and chemical parameters, kinetics, regeneration at low temperature (80 °C), as well as CO2 adsorption under humid conditions. Additionally, NS-G3.0 displayed a substantially superior performance with stable CO2 capture displayed during ten short temperature swing adsorption (TSA) cycles, making it a promising candidate for CO2 capture from ambient air. Finally, we demonstrated the recovery and reutilization of the captured CO2 for both the synthesis of formate via carbonate hydrogenation and for the production of calcium carbonate pellets. © 2024 The Royal Society of Chemistry.