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链接剂辅助的卓越容积乙炔存储能力和金属有机骨架中 C H /C H 和 C H /CO 的基准分离。

De-Linker-Enabled Exceptional Volumetric Acetylene Storage Capacity and Benchmark C H /C H and C H /CO Separations in Metal-Organic Frameworks.

机构信息

Key Laboratory of Macromolecular Science of Shaanxi Province, Key Laboratory of Applied Surface and Colloid Chemistry, Ministry of Education, School of Chemistry & Chemical Engineering, Shaanxi Normal University, Xi'an, Shaanxi, 710062, China.

Department of Chemistry and Biochemistry, California State University, Long Beach, CA-90840, USA.

出版信息

Angew Chem Int Ed Engl. 2023 Mar 1;62(10):e202217839. doi: 10.1002/anie.202217839. Epub 2023 Jan 31.

Abstract

An ideal adsorbent for separation requires optimizing both storage capacity and selectivity, but maximizing both or achieving a desired balance remain challenging. Herein, a de-linker strategy is proposed to address this issue for metal-organic frameworks (MOFs). Broadly speaking, the de-linker idea targets a class of materials that may be viewed as being intermediate between zeolites and MOFs. Its feasibility is shown here by a series of ultra-microporous MOFs (SNNU-98-M, M=Mn, Co, Ni, Zn). SNNU-98 exhibit high volumetric C H uptake capacity under low and ambient pressures (175.3 cm  cm @ 0.1 bar, 222.9 cm  cm @ 1 bar, 298 K), as well as extraordinary selectivity (2405.7 for C H /C H , 22.7 for C H /CO ). Remarkably, SNNU-98-Mn can efficiently separate C H from C H /CO and C H /C H mixtures with a benchmark C H /C H (1/99) breakthrough time of 2325 min g , and produce 99.9999 % C H with a productivity up to 64.6 mmol g , surpassing values of reported MOF adsorbents.

摘要

一种理想的分离用吸附剂需要优化存储容量和选择性,但最大化这两者或实现期望的平衡仍然具有挑战性。在此,提出了一种解键合策略来解决金属有机骨架(MOF)中的这一问题。广义上讲,解键合的想法针对的是一类可能介于沸石和 MOF 之间的材料。通过一系列超微孔 MOF(SNNU-98-M,M=Mn、Co、Ni、Zn)证明了其可行性。SNNU-98 在低压和环境压力下(0.1 巴时为 175.3 cm 3 cm -3 ,1 巴时为 222.9 cm 3 cm -3 ,298 K)具有高体积 CH 4 吸附容量,以及非凡的选择性(CH 4 /CH 4 为 2405.7,CH 4 /CO 为 22.7)。值得注意的是,SNNU-98-Mn 可以有效地从 CH 4 /CO 和 CH 4 /C 2 H 4 混合物中分离出 CH 4 ,其 CH 4 /C 2 H 4 (1/99)突破时间为 2325 min·g -1 ,并以高达 64.6 mmol·g -1 的产率生产出 99.9999%的 CH 4 ,超过了报道的 MOF 吸附剂的值。

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