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通过取代-插入机制实现选择性化学吸附的定向一维金属有机框架

Oriented 1D Metal-Organic Frameworks for Selective Chemisorption by a Substitution-Insertion Mechanism.

作者信息

Sun Qian, Du Jingcheng, Song Ziye, Yao Ayan, Liu Linghao, Ma Ji, Cao Dong, He Wen, Hassan Shabi Ul, Guan Jian, Liu Jiangtao

机构信息

Department of Environmental Science and Engineering University of Science and Technology of China, Hefei, Anhui 230052, China.

出版信息

Nano Lett. 2024 Oct 2. doi: 10.1021/acs.nanolett.4c02921.

DOI:10.1021/acs.nanolett.4c02921
PMID:39356732
Abstract

Chemisorption on organometallic-based adsorbents is crucial for the controlled separation and purification of targeted systems. Herein, oriented 1D NH-CuBDC·HO metal-organic frameworks (MOFs) featuring accessible Cu sites are successfully fabricated by bottom-up interfacial polymerization. The prepared MOFs, as deliberately self-assembled secondary particles, exhibit a visually detectable coordination-responsive characteristic induced by the nucleophilic substitution and competitive coordination of guest molecules. As a versatile phase-change chemosorbent, the MOFs exhibit unprecedented NH capture (18.83 mmol g at 298 K) and bioethanol dehydration performance (enriching ethanol from 99% to 99.99% within 10 min by direct adsorption separation of liquid mixtures of ethanol and water). Furthermore, the raw materials for preparing the 1D MOFs are inexpensive and readily available, and the facile regeneration with water washing at room temperature effectively minimizes the energy consumption and cost of recycling, enabling it to be the most valuable adsorbent for the removal and separation of target substances.

摘要

基于有机金属的吸附剂上的化学吸附对于目标体系的可控分离和纯化至关重要。在此,通过自下而上的界面聚合成功制备了具有可及铜位点的定向一维NH-CuBDC·H₂O金属有机框架(MOF)。所制备的MOF作为精心自组装的二次颗粒,表现出由客体分子的亲核取代和竞争配位诱导的视觉上可检测的配位响应特性。作为一种通用的相变化学吸附剂,该MOF展现出前所未有的NH₃捕获能力(298 K时为18.83 mmol g⁻¹)和生物乙醇脱水性能(通过乙醇和水的液体混合物的直接吸附分离在10分钟内将乙醇从99%富集到99.99%)。此外,制备一维MOF的原材料价格低廉且易于获得,在室温下用水洗涤即可轻松再生,有效降低了能耗和回收成本,使其成为去除和分离目标物质最有价值的吸附剂。

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