4.8 Article

A Novel Hydrogen-Bonded Organic Framework with Highly Permanent Porosity for Boosting Ethane/Ethylene Separation

期刊

ACS MATERIALS LETTERS
卷 3, 期 5, 页码 497-503

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AMER CHEMICAL SOC
DOI: 10.1021/acsmaterialslett.1c00013

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资金

  1. National Natural Science Foundation of China [52073251]
  2. Zhejiang University 100 Talent Program

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A novel diamondoid hydrogen-bonded organic framework (ZJU-HOF-10) was developed with significantly enhanced permanent porosity through the use of supercritical carbon dioxide (sc-CO2) drying method, leading to improved ethane/ethylene separation efficiency. The nonpolar pore surfaces in ZJU-HOF-10(sc) were found to play a key role in stronger multipoint interactions with C2H6, resulting in enhanced C2H6 uptake capacity and selectivity. Actual breakthrough experiments demonstrated the capability of ZJU-HOF-10(sc) to efficiently separate ethane from C2H6/C2H4 mixtures at ambient conditions, providing high polymer-grade C2H4 productivity.
The establishment of highly permanent porosity in hydrogen-bonded organic frameworks (HOFs) is a long-standing challenge due to the fragile nature of hydrogen bonds, which delimits their broad applications in gas separation. Herein, we report a novel diamondoid HOF (termed as ZJU-HOF-10) and utilize the supercritical carbon dioxide (sc-CO2) drying method to significantly improve its permanent porosity for highly boosting ethane/ ethylene (C2H6/C2H4) separation. Compared with the commonly used heat/ vacuum activation, the sc-CO2 activated ZJU-HOF-10(sc) exhibits a significantly improved BET surface area of 1169 m(2) g(-1) over 295 m(2) g(-1). Such enhanced porosity in ZJU-HOF-10(sc) thus leads to a notably increased C2H6 uptake capacity (1.65 mmol g(-1) at 296 K and 0.5 bar) and C2H6/C2H4 selectivity (1.9), both of which are comparable to those of the benchmark HOF-76a reported (1.69 mmol g(-1) and 2.0). Theoretical calculations reveal that the inherent feature of nonpolar pore surfaces in ZJU-HOF-10(sc) plays the key role to result in stronger multipoint interactions with C2H6 over C2H4. Actual breakthrough experiments affirm that ZJU-HOF-10(sc) is capable of efficiently separating ethane from 50/50 (v/v) or 10/90 C2H6/C2H4 mixtures at ambient conditions, affording a high polymer-grade C2H4 productivity of 6.9 or 13.1 L kg(-1), respectively.

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