期刊名称：Proceedings of the National Academy of Sciences
印刷版ISSN：0027-8424
电子版ISSN：1091-6490
出版年度：2022
卷号：119
期号：1
DOI：10.1073/pnas.2114964119
语种：English
出版社：The National Academy of Sciences of the United States of America
摘要：Significance
The development of highly efficient carbon capture technology is the most crucial step for achieving the carbon neutrality target, which is estimated to have a global market value up to $6.13 billion by 2027. Advanced membranes, as efficient CO
2 separation strategies, significantly promote the development of clean energy and low-carbon technologies. Studies on next-generation mixed matrix membranes (MMMs) are highly expected to combine excellent workability and high gas separation performance capable of sustainable energy-efficient carbon capture.
Mixed matrix membranes (MMMs) are one of the most promising solutions for energy-efficient gas separation. However, conventional MMM synthesis methods inevitably lead to poor filler–polymer interfacial compatibility, filler agglomeration, and limited loading. Herein, inspired by symbiotic relationships in nature, we designed a universal bottom-up method for in situ nanosized metal organic framework (MOF) assembly within polymer matrices. Consequently, our method eliminating the traditional postsynthetic step significantly enhanced MOF dispersion, interfacial compatibility, and loading to an unprecedented 67.2 wt % in synthesized MMMs. Utilizing experimental techniques and complementary density functional theory (DFT) simulation, we validated that these enhancements synergistically ameliorated CO
2 solubility, which was significantly different from other works where MOF typically promoted gas diffusion. Our approach simultaneously improves CO
2 permeability and selectivity, and superior carbon capture performance is maintained even during long-term tests; the mechanical strength is retained even with ultrahigh MOF loadings. This symbiosis-inspired de novo strategy can potentially pave the way for next-generation MMMs that can fully exploit the unique characteristics of both MOFs and matrices.
