浙江大学黄飞鹤研究团队开发了用于潮湿环境下甲烷净化的超疏水自修复多孔有机大环晶体。相关研究成果发表在2025年1月23日出版的国际知名学术期刊《美国化学会杂志》。

使用吸附剂从天然气中净化甲烷不仅需要吸附剂具有优异的分离性能，还需要克服额外的艰巨挑战，如湿度干扰和可持续使用的耐久性要求。

该文制备了一种具有超疏水和自愈特性的新型大环（CaC9）多孔有机晶体，并将其用于在97%相对湿度下从三元甲烷/乙烷/丙烷混合物中纯化甲烷（纯度>99.99%）。对甲烷和耐水性的高选择性归因于CaC9独特的化学结构，具有固有的4.2孔以及用饱和烷基链修饰的孔环境。

此外，CaC9晶体具有自愈能力，可在15分钟内实现孔隙的原位重建。用正己烷蒸汽处理后，CaC9结晶可以很容易地从无孔状态转变为多孔状态，从而为增强多孔材料的可持续分离过程提供了一种新的解决方案。

该项工作介绍了一种用于天然气分离的新型分子级多孔吸附剂，为设计具有意想不到功能的新型吸附剂提供了宝贵的动力。

附：英文原文

Title: Superhydrophobic and Self-Healing Porous Organic Macrocycle Crystals for Methane Purification under Humid Conditions

Author: Zeju Wang, Li Zhao, Zhenguo Zhang, Xinru Sheng, Hanlin Yue, Rui Liu, Zhongwen Liu, Yating Li, Li Shao, YunLei Peng, Bin Hua, Feihe Huang

Issue&Volume: January 23, 2025

Abstract: Purifying methane from natural gas using adsorbents not only requires the adsorbents to possess excellent separation performance but also to overcome additional daunting challenges such as humidity interference and durability requirements for sustainable use. Herein, porous organic crystals of a new macrocycle (CaC9) with superhydrophobic and self-healing features are prepared and employed for the purification of methane (>99.99% purity) from ternary methane/ethane/propane mixtures under 97% relative humidity. The high selectivity for methane and water-resistance are attributed to the unique chemical structure of CaC9, possessing an intrinsic 4.2 pore along with a pore environment modified with saturated alkyl chains. Besides, CaC9 crystals exhibit a self-healing capacity to realize in situ reconstruction of porosity within 15 min. The transformation of CaC9 crystals from a nonporous state to a porous state can be easily achieved upon treatment with n-hexane vapor, thereby presenting a novel solution to enhance the sustainable separation processes of porous materials. This work introduces a novel molecular-level porous adsorbent for natural gas separation, providing a valuable impetus for designing novel adsorbents with unexpected functions.

DOI: 10.1021/jacs.4c14130

Source: https://pubs.acs.org/doi/abs/10.1021/jacs.4c14130