开发从乙烯/乙烷混合物中提纯乙烯的成本/能源效率高的分离技术非常重要,但在工业过程中非常具有挑战性。
该文中,研究人员采用自下而上的[8+2]构建方法,合理设计并合成了具有8个连接bcu网络的三维共价有机框架(COFs),该框架可以高效地从乙烯/乙烷混合物中选择性去除乙烷。这些COF材料由cthemomer设计的八位醛单体与线性二氨基连接物缩合反应制成,具有高结晶度、良好的结构稳定性和高孔隙率。由于这些COFs具有组织良好的微孔和非极性/惰性孔环境,因此它们对乙烷的吸附能力高,对乙烯的选择性好,是乙烯净化的最佳乙烷选择性吸附剂之一。通过单次吸附法生产的高纯度乙烯(>99.99%)的动态突破实验,验证了其优异的乙烯/乙烷分离性能。分离性能超过了所有报道的C2H6选择性COFs,甚至超过了一些基准金属-有机框架。
研究工作为高附加值气体净化用新型吸附剂的设计提供了重要指导。
附:英文原文
Title: Bottom-Up Synthesis of 8-Connected Three-Dimensional Covalent Organic Frameworks for Highly Efficient Ethylene/Ethane Separation
Author: Fazheng Jin, En Lin, Tonghai Wang, Shubo Geng, Ting Wang, Wansheng Liu, Fanhao Xiong, Zhifang Wang, Yao Chen, Peng Cheng, Zhenjie Zhang
Issue&Volume: March 21, 2022
Abstract: Developing cost-/energy-efficient separation techniques for purifying ethylene from an ethylene/ethane mixture is highly important but very challenging in the industrial process. Herein, using a bottom-up [8 + 2] construction approach, we rationally designed and synthesized three three-dimensional covalent organic frameworks (COFs) with 8-connected bcu networks, which can selectively remove ethane from an ethylene/ethane mixture with high efficiency. These COF materials, which are fabricated by the condensation reaction of a customer-designed octatopic aldehyde monomer with linear diamino linkers, possess high crystallinity, good structural robustness, and high porosity. Attributed to the well-organized micro-sized pores with a nonpolar/inert pore environment, these COFs display high ethane adsorption capacity and good selectivity over ethylene, making them among the best ethane-selective adsorbents for ethylene purification. Their excellent ethylene/ethane separation performance is validated by dynamic breakthrough experiments with high-purity ethylene (>99.99%) produced through a single adsorption process. The separation performance surpasses all reported C2H6-selective COFs and even some benchmark metal–organic frameworks. This work provides important guidance for the design of new adsorbents for value-added gas purification.
DOI: 10.1021/jacs.2c01058
Source: https://pubs.acs.org/doi/10.1021/jacs.2c01058
JACS:《美国化学会志》,创刊于1879年。隶属于美国化学会,最新IF:14.612
官方网址:https://pubs.acs.org/journal/jacsat
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