Kulkarni Vaishnavi, Parthiban Jayashree, Singh Sanjay Kumar
Department of Chemistry, Indian Institute of Technology Indore, Simrol, Indore 453552, Madhya Pradesh, India.
Nanoscale. 2024 Sep 12;16(35):16571-16581. doi: 10.1039/d4nr01744g.
Exploring efficient systems to recover CO 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 CO capture under simulated direct air capture (DAC) (400 ppm CO in helium at 30 °C) and indoor air (≥400 ppm, 50 ± 3% RH at 30 °C) conditions. The results inferred that the 1 (NS-G1.0), 2 (NS-G2.0), 3 (NS-G3.0), and 4 (NS-G4.0) generations of the NS-PAMAM dendrimers exhibited excellent performance for CO capture. Compared to the other generations, NS-G3.0 demonstrated superior CO adsorption capacities of 0.50 mmol g under simulated dry CO conditions (400 ppm in He), 1.02 mmol g under indoor air (dry) CO conditions (≥400 ppm, 26 ± 3% RH), and 1.54 mmol g under indoor air (humid) CO conditions (≥400 ppm, 50 ± 3% RH). The study included the evaluation of CO adsorption-desorption performance of the NS-PAMAM dendrimers under varying structural and chemical parameters, kinetics, regeneration at low temperature (80 °C), as well as CO adsorption under humid conditions. Additionally, NS-G3.0 displayed a substantially superior performance with stable CO capture displayed during ten short temperature swing adsorption (TSA) cycles, making it a promising candidate for CO capture from ambient air. Finally, we demonstrated the recovery and reutilization of the captured CO for both the synthesis of formate carbonate hydrogenation and for the production of calcium carbonate pellets.
探索从大气中回收一氧化碳的高效系统可能是解决全球碳排放问题的一种途径。在此，我们报告了用聚酰胺胺（PAMAM）树枝状大分子功能化的纳米二氧化硅（NS）（NS-PAMAM）的合成，其作为在模拟直接空气捕获（DAC）（30℃下氦气中400 ppm一氧化碳）和室内空气（≥400 ppm，30℃下50±3%相对湿度）条件下捕获一氧化碳的高效吸附剂。结果表明，NS-PAMAM树枝状大分子的第1代（NS-G1.0）、第2代（NS-G2.0）、第3代（NS-G3.0）和第4代（NS-G4.0）在捕获一氧化碳方面表现出优异性能。与其他代相比，NS-G3.0在模拟干燥一氧化碳条件（氦气中400 ppm）下表现出0.50 mmol/g的卓越一氧化碳吸附容量，在室内空气（干燥）一氧化碳条件（≥400 ppm，26±3%相对湿度）下为1.02 mmol/g，在室内空气（潮湿）一氧化碳条件（≥400 ppm，50±3%相对湿度）下为1.54 mmol/g。该研究包括评估NS-PAMAM树枝状大分子在不同结构和化学参数下的一氧化碳吸附-解吸性能、动力学、低温（80℃）再生以及潮湿条件下的一氧化碳吸附。此外，NS-G3.0在十个短周期变温吸附（TSA）循环中表现出稳定的一氧化碳捕获性能，性能显著优越，使其成为从环境空气中捕获一氧化碳的有前景的候选材料。最后，我们展示了捕获的一氧化碳用于合成甲酸盐 碳酸加氢以及生产碳酸钙颗粒的回收和再利用。
