【摘要】 随着全球工业化进程的加速，能源消耗持续增加带来CO₂的过度排放，引发了严重的气候与环境问题。在众多应对措施中，以具有独特孔隙特征的MOF材料为代表的物理吸附技术成为该领域的研究热点。基于PtS型MOF材料，设计构建并优化了一系列硝基（—NO₂）和三嗪修饰的MOF结构，通过巨正则蒙特卡洛（GCMC）理论模拟研究了不同—NO₂数量对MOF材料的CO₂气体吸附分离性能的影响。结果表明：在298K和1.0bar条件下，引入—NO₂后，材料对CO₂的捕获量从PtS的1.92mmol/g提升到了PtS-2NO₂的2.52mmol/g,增加—NO₂数量后PtS-4NO₂的CO₂吸附量提升到了5.02mmol/g,而同时修饰三嗪结构后CO₂吸附量达到5.93mmol/g。计算不同结构的等温吸附热、van der Waals/Coulomb相互作用和选择性等揭示了MOF结构中引入—NO₂对其CO₂选择性吸附能力的促进作用和机制，对高性能MOF基CO₂吸附剂材料的开发具有重要的指导意义。更多还原

【Abstract】 With the acceleration of global industrialization, the continuous increase in energy consumption has led to excessive CO₂ emissions, causing severe climate and environmental issues.Among various countermeasures, physical adsorption technology represented by MOF materials with unique pore characteristics has become a research hotspot in this field.Based on PtS-type MOF materials, a series of MOF structures modified with nitro（—NO₂） and triazine were designed, constructed and optimized.The effect of different amounts of —NO₂ on the CO₂ gas adsorption and separation performance of MOF materials was simulated and investigated by grand canonical Monte Carlo（GCMC） theory.The results showed that at 298K and 1.0bar, the introduction of —NO₂ increased the CO₂ capture amount from 1.92mmol/g of PtS to 2.52mmgl/g of PtS-2NO₂,and further augmentation of —NO₂ groups raised the CO₂ adsorption capacity to 5.02mmol/g of PtS-4NO₂,while the CO₂ adsorption reached 5.93mmol/g after simultaneous modification with triazine structure.Calculation of isosteric heat of adsorption, van der Waals/Coulomb interactions, and selectivity also demonstrated the enhancement of CO₂ selective adsorption performance due to —NO₂ functionalization.In addition, the mechanisms by which —NO₂ facilitated this enhancement were elucidated through van der Waals/Coulomb interactions.This research provides significant guidance for the development of MOF-based CO₂ adsorbent materials.更多还原