Chen Xiuling, Zhang Zhiguang, Xu Shan, Zhang Bin, Qin Yong, Ma Canghai, He Gaohong, Li Nanwen
State Key Laboratory of Coal Conversion, Institute of Coal Chemistry Chinese Academy of Sciences, Taiyuan, China.
Hubei Key Laboratory of Radiation Chemistry and Functional Materials, Hubei University of Science and Technology, Xianning, China.
Nat Commun. 2025 Jan 2;16(1):133. doi: 10.1038/s41467-024-54275-1.
To confront the energy consumption, high performance membrane materials are urgently needed. Carbon molecular sieve (CMS) membranes exhibit superior capability in separating gas mixtures efficiently. However, it remains a grand challenge to precisely tune the pore size and distribution of CMS membranes to further improve their molecular sieving properties. Herein, we report an approach of finely modulating CMS pore structure by using the reactive Al(CH) to in situ defluorinate the polymer precursor to form Al-F(CH) in the polymer matrix, which is further converted to atomic-level AlO and Al-F in the polymer matrix. These nanoparticles play the key role in regulating the pore size of CMS membranes by suppressing the formation of unfavorable large pores during pyrolysis, thus enhancing the gas selectivity considerably. The resultant CMS membranes demonstrate a H/CH and CO/CH selectivity of 192.6, and 58.4, respectively, 128% and 93% higher than the untreated samples, residing far above the latest upper bounds.
为应对能源消耗问题，迫切需要高性能的膜材料。碳分子筛（CMS）膜在高效分离气体混合物方面表现出卓越的能力。然而，精确调控CMS膜的孔径和孔径分布以进一步改善其分子筛分性能仍然是一个巨大的挑战。在此，我们报道了一种通过使用反应性Al(CH)对聚合物前驱体进行原位脱氟，在聚合物基体中形成Al-F(CH)，进而在聚合物基体中转化为原子级的AlO和Al-F，来精细调节CMS孔结构的方法。这些纳米颗粒在调节CMS膜孔径方面起着关键作用，通过抑制热解过程中不利的大孔形成，从而显著提高气体选择性。所得的CMS膜的H₂/CH₄和CO₂/CH₄选择性分别为192.6和58.4，比未处理的样品分别高出128%和93%，远远高于最新的上限。
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