Abstract:

Direct air capture of CO₂ is a necessary component for global warming suppression, and developing efficient technologies for low-concentration CO₂ separation has become a focus of scientific research in recent years. In this study, fluorine-containing 1F-PUiO-66, a polymer-MOF composite, was used as a filler material and blended with the corresponding cPIM-1 polymer matrix to construct mixed matrix membranes with loading of up to 50%(mass) and high affinity for CO₂, achieving efficient separation of low-concentration CO₂. Specifically, the prepared 50%(mass) 1F-PUiO-66/cPIM-1 membrane exhibited a CO₂ permeability as high as 6428.3 Barrer under 1%(vol) low CO₂ concentration inlet condition, and the CO₂/N₂ selectivity increased to 69.13, which improved the performance values by 1167.3% and 81.2%, respectively, compared to cPIM-1 pure membranes, and substantially exceeded the 2019 Robeson upper bound. This study demonstrates the significant CO₂/N₂ separation potential of polymer-MOF composite materials under low CO₂ concentration inlet conditions, which is important for actual industrial gas separation.

Key words: metal-organic framework, composite filler, mixed matrix membrane, gas separation, low concentration CO₂

摘要：

二氧化碳的直接空气捕获是抑制全球变暖的一个必要组成部分，开发高效、低浓度CO₂分离技术成为近年来研究的焦点。本研究采用聚合物-MOF复合的含氟1F-PUiO-66作为填料材料，并与对应的cPIM-1聚合物基质共混构建出负载量高达50%（质量）且对CO₂具有高亲和力的混合基质膜，实现低浓度CO₂的高效分离。所制备的50%（质量） 1F-PUiO-66/cPIM-1膜在1%（体积）低CO₂浓度进气条件下，CO₂渗透通量高达6428.3 Barrer，CO₂/N₂选择性提高至69.13，相较于cPIM-1纯膜分别提升1167.3%和81.2%，大幅度超越了2019年Robeson上限。本研究的聚合物-MOF复合填料材料在低CO₂浓度进气条件下显著的CO₂/N₂分离潜力，可为工业实际气体分离提供参考。

关键词: 金属-有机骨架, 复合填料, 混合基质膜, 气体分离, 低浓度CO ₂