Tuning the Phase Composition of Metal–Organic Framework Membranes for Helium Separation through Incorporation of Fullerenes,Journal of the American Chemical Society

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Tuning the Phase Composition of Metal–Organic Framework Membranes for Helium Separation through Incorporation of Fullerenes
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2023-06-23 , DOI: 10.1021/jacs.3c03362
Jiuli Han ₁ , Haoyu Wu ₁ , Hongwei Fan ₂ , Li Ding ₁ , Guangtong Hai ₁ , Jürgen Caro ₃ , Haihui Wang ₁

Affiliation

Metal–organic framework (MOF) membranes have attracted significant research interest in gas separation, but efficient helium (He) separation remains a challenge due to the weak polarizability of He and the intrinsic pore size flexibility of MOFs. Herein, incorporated fullerenes (C₆₀ and C₇₀) were used to tune the crystallographic phase composition of ZIF-8 membranes, thus creating small and fixed apertures for selective He permeation. The fullerene-modified ZIF-8 (C₆₀@ZIF-8 and C₇₀@ZIF-8) membranes contain about 20% of the rigid-lattice ZIF-8_I-43m phase and have been prepared as 200–350 nm thick supported layers through electrochemical synthesis. They show a significantly enhanced molecular sieving for He/N₂,CH₄ together with a satisfactory He permeance of >200 GPU. Specifically, the He/N₂ selectivity of the C₇₀@ZIF-8 membrane is up to 30.4, which is much higher than that of the fullerene-free ZIF-8 membrane (5.1) and nearly an order of magnitude higher than those of other reported He-selective MOF membranes. A continuous long-term gas permeation test over 780 h under dry and humid conditions proved the excellent stability of the fullerene-modified ZIF-8 membranes. The general validity and versatility of the proposed strategy for MOF membrane preparation are also demonstrated by the enhancement of the separation performance of a fullerene-modified ZIF-76 membrane.

中文翻译：

通过掺入富勒烯调整用于氦分离的金属有机框架膜的相组成

金属有机框架（MOF）膜在气体分离领域引起了广泛的研究兴趣，但由于He的极化性较弱以及MOF固有的孔径灵活性，有效的氦（He）分离仍然是一个挑战。在此，掺入的富勒烯（C ₆₀和 C ₇₀）用于调节 ZIF-8 膜的晶体相组成，从而产生用于选择性 He 渗透的小且固定的孔径。富勒烯修饰的 ZIF-8（C ₆₀ @ZIF-8 和 C ₇₀ @ZIF-8）膜含有约 20% 的刚性晶格 ZIF-8_I-43m 相，并已制备为 200–350 nm 厚的支撑层通过电化学合成。_{它们显示出显着增强的 He/N 2}分子筛分能力,CH ₄以及 >200 GPU 的令人满意的 He 性能。具体而言， C _{70 @ZIF-8膜的He/N}₂选择性高达30.4，远高于不含富勒烯的ZIF-8膜（5.1），并且比无富勒烯的ZIF-8膜高出近一个数量级。其他报道的 He 选择性 MOF 膜。在干燥和潮湿条件下连续超过780小时的长期气体渗透测试证明了富勒烯修饰的ZIF-8膜具有优异的稳定性。富勒烯修饰的 ZIF-76 膜分离性能的增强也证明了所提出的 MOF 膜制备策略的普遍有效性和多功能性。

更新日期：2023-06-23

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