Symbiosis-inspired de novo synthesis of ultrahigh MOF growth mixed matrix membranes for sustainable carbon capture.
Symbiosis-inspired de novo synthesis of ultrahigh MOF growth mixed matrix membranes for sustainable carbon capture.
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DOI：
10.1073/pnas.2114964119
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发表时间：
2022-01-04
影响因子：
11.1
通讯作者：
Shao L
中科院分区：
文献类型：
--
作者：
He S;Zhu B;Jiang X;Han G;Li S;Lau CH;Wu Y;Zhang Y;Shao L
开发高效的碳捕获技术是实现碳中和目标的最关键步骤，预计到2027年，碳中和目标的全球市场价值将达到61.3亿美元。先进膜作为一种高效的CO2分离策略，对清洁能源和低碳技术的发展具有重要的推动作用。下一代混合基质膜（MMMs）的研究备受期待，它将具有优异的可操作性和高气体分离性能，能够实现可持续的节能碳捕获。混合基质膜（MMMs）是最有前途的节能气体分离解决方案之一。然而，传统的MMM合成方法不可避免地导致填料-聚合物界面相容性差、填料团聚和负载有限。在此，受自然界共生关系的启发，我们设计了一种通用的自下而上的方法，用于在聚合物基质中原位组装纳米金属有机框架（MOF）。因此，我们的方法消除了传统的合成后步骤，显著提高了MOF的分散性、界面相容性和负载，在合成的mm中达到了前所未有的67.2%。利用实验技术和互补密度泛函理论（DFT）模拟，我们验证了这些增强可以协同改善二氧化碳的溶解度，这与其他研究中MOF通常促进气体扩散的情况有很大不同。我们的方法同时提高了二氧化碳的渗透性和选择性，即使在长期测试中也能保持优越的碳捕获性能；即使在超高MOF载荷下，机械强度也能保持不变。这种共生激发的从头开始的策略可能为下一代mm铺平道路，可以充分利用mof和矩阵的独特特性。
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 CO2 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 CO2 solubility, which was significantly different from other works where MOF typically promoted gas diffusion. Our approach simultaneously improves CO2 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.
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影响因子：
15.1
作者：
Liu, Min;Nothling, Mitchell D.;Qiao, Greg G.
通讯作者：
Qiao, Greg G.
影响因子：
56.9
作者：
Carta, Mariolino;Malpass-Evans, Richard;McKeown, Neil B.
通讯作者：
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影响因子：
5.5
作者：
Baker, Richard W.;Low, Bee Ting
通讯作者：
Low, Bee Ting
影响因子：
4.9
作者：
Budd, PM;Ghanem, BS;Tattershall, CE
通讯作者：
Tattershall, CE
影响因子：
9.5
作者：
Heuchel, Matthias;Fritsch, Detlev;Hofmann, Dieter
通讯作者：
Hofmann, Dieter