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聚乙烯亚胺修饰的UiO-66-NH(Zr)金属有机框架:制备及其对CO选择性吸附的增强

Polyethyleneimine-Modified UiO-66-NH(Zr) Metal-Organic Frameworks: Preparation and Enhanced CO Selective Adsorption.

作者信息

Zhu Junjie, Wu Linbo, Bu Zhiyang, Jie Suyun, Li Bo-Geng

机构信息

State Key Laboratory of Chemical Engineering at ZJU, College of Chemical and Biological Engineering, Zhejiang University, Hangzhou 310027, China.

出版信息

ACS Omega. 2019 Feb 13;4(2):3188-3197. doi: 10.1021/acsomega.8b02319. eCollection 2019 Feb 28.

Abstract

UiO-66-NH, a zirconium-based functional metal-organic framework (MOF), was postsynthetically modified via Schiff base reaction between aldehyde groups in glutaraldehyde and amino groups in UiO-66-NH and CO-preabsorbed polyethyleneimine (PEI). The resulting PEI-modified MOFs, abbreviated as PEI@UiO, were characterized with H NMR, Fourier transform infrared, powder X-ray diffraction, Brunauer-Emmett-Teller, scanning electron microscopy, and thermogravimetric analysis and evaluated as CO adsorbents. In comparison with pristine UiO-66-NH, the PEI@UiO adsorbents have reduced specific surface area (7-150 m/g) but maintained the same crystal structure. Particularly, the PEI96@UiO adsorbent exhibited significantly improved CO/N adsorption selectivity (48 vs 25) and higher CO adsorption capacity (3.2 vs 2.7 mmol/g). The adsorbent also displayed moderate desorption energy (68 kJ/mol CO), superior moisture endurance, and recyclability, which are very desirable for practical applications.

摘要

UiO-66-NH是一种锆基金属有机骨架材料(MOF),通过戊二醛中的醛基与UiO-66-NH中的氨基以及预吸附的聚乙烯亚胺(PEI)之间的席夫碱反应进行后合成修饰。所得的PEI修饰的MOF,简称为PEI@UiO,通过核磁共振氢谱、傅里叶变换红外光谱、粉末X射线衍射、布鲁诺尔-埃米特-泰勒比表面积测定法、扫描电子显微镜和热重分析进行表征,并作为CO吸附剂进行评估。与原始的UiO-66-NH相比,PEI@UiO吸附剂的比表面积降低(7 - 150平方米/克),但保持相同的晶体结构。特别是,PEI96@UiO吸附剂表现出显著提高的CO/N吸附选择性(48对25)和更高的CO吸附容量(3.2对2.7毫摩尔/克)。该吸附剂还显示出适度的脱附能量(68千焦/摩尔CO)、优异的耐湿性和可回收性,这些对于实际应用非常理想。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c974/6648867/77d1352edce4/ao-2018-02319p_0011.jpg

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