To accelerate the discovery of promising adsorbents for CO₂ capture from flue gas, many efforts have been made toward the high-throughput computational prediction of new high-efficiency porous materials, such as aluminosilicate zeolites. To reduce the computational cost, most of the previous efforts evaluate the CO₂ capture capability according to the CO₂ adsorption selectivity estimated by empirical single-component simulations. In this study, we perform high-throughput grand canonical Monte Carlo (GCMC) simulations to predict the CO₂ capture capability of 2625 aluminosilicate zeolite structures, which are selected from 262,500 hypothetical ABC-6 models with Si/Al ratios ranging from 1.0 to 10. Different from previous efforts, our GCMC simulations are conducted on CO₂/N₂ binary mixtures, which are much closer to the realistic compositions of flue gas than conventional single-component simulations. Moreover, in addition to conventional CO₂ adsorption selectivity, we introduce working capacity, adsorbent performance score, and regenerability to get a comprehensive overview of the performance of these candidate structures under temperature swing adsorption (TSA), vacuum swing adsorption (VSA), and pressure swing adsorption (PSA) processes, respectively. We identify hundreds of hypothetical aluminosilicate zeolite structures that exhibit promising CO₂ capture capability in TSA and VSA processes even superior to zeolite Na-X, the most efficient zeolite for CO₂ capture known so far. Our results will provide important guidance toward experimental discovery of high-performance zeolites for practical CO₂ capture

为了加速发现从烟道气中捕集CO ₂的有前途的吸附剂，已对新型高效多孔材料（例如铝硅酸盐沸石）的高通量计算预测做出了许多努力。为了减少计算成本，以前的大多数工作都是根据经验性单组分模拟估算的CO ₂吸附选择性来评估CO ₂捕获能力的。在这项研究中，我们执行高通量大规范蒙特卡洛（GCMC）模拟以预测CO ₂捕获能力为2625个硅铝酸盐沸石结构，这些结构选自262,500个假设的ABC-6模型，Si / Al比为1.0到10。与以前的努力不同，我们对GC ₂ / N ₂二元混合物进行的GCMC模拟是比传统的单组分模拟更接近现实的烟气成分。而且，除了传统的CO ₂吸附选择性，我们介绍了工作容量，吸附剂性能评分和可再生性，以全面概述这些候​​选结构在变温吸附（TSA），真空变压吸附（VSA）和变压吸附（PSA）工艺下的性能，分别。我们确定了数百种假设的铝硅酸盐沸石结构，它们在TSA和VSA工艺中展现出有希望的CO ₂捕获能力，甚至优于Na-X沸石，Na-X是迄今为止已知的最有效的CO ₂捕获沸石。我们的结果将为实验发现用于实际CO ₂捕集的高性能沸石提供重要指导。