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二价铬/钼/镍空配位MOFs的CH4/N2吸附分离研究
引用本文:贾晓霞,王丽,元宁,杨江峰,李晋平.二价铬/钼/镍空配位MOFs的CH4/N2吸附分离研究[J].化工学报,2018,69(9):3896-3904.
作者姓名:贾晓霞  王丽  元宁  杨江峰  李晋平
作者单位:1. 太原理工大学化学化工学院精细化工研究所, 山西 太原 030024; 2. 气体能源高效清洁利用山西省重点实验室, 山西 太原 030024
基金项目:国家自然科学基金项目(51672186,21676175)。
摘    要:基于金属有机骨架材料中金属空配位对气体的强吸附作用,利用具有较高活性的二价金属Cr2+/Mo2+/Ni2+与均苯三酸(H3BTC)配位合成了HKUST-1(Cu-BTC)同构系列材料M-BTC(M=Cr、Mo、Ni),并与Cu-BTC对比分析了该类型材料中不同金属空配位对甲烷和氮气的吸附性能。实验结果显示,此三种材料均具有较好的甲烷选择吸附性,其中含Ni2+金属空位的Ni-BTC以其尤为突出的甲烷吸附热值而呈现较好的CH4/N2分离潜力;Cr2+空配位虽具有较强活性,但是对于甲烷的选择性吸附性能却低于含Cu2+空位的Cu-BTC材料。结合吸附选择性IAST计算分析得到此三种含较高活性不饱和金属空配位的MOFs材料对于甲烷选择性吸附作用能顺序为:Ni-BTC > Mo-BTC > Cu-BTC > Cr-BTC。

关 键 词:甲烷  氮气  吸附  吸附剂  不饱和金属空配位  
收稿时间:2018-03-21
修稿时间:2018-06-05

CH4/N2 adsorption separation research of MOFs with divalent Cr/Mo/Ni unsaturated metal sites
JIA Xiaoxia,WANG Li,YUAN Ning,YANG Jiangfeng,LI Jinping.CH4/N2 adsorption separation research of MOFs with divalent Cr/Mo/Ni unsaturated metal sites[J].Journal of Chemical Industry and Engineering(China),2018,69(9):3896-3904.
Authors:JIA Xiaoxia  WANG Li  YUAN Ning  YANG Jiangfeng  LI Jinping
Affiliation:1. College of Chemistry and Chemical Engineering, Research Institute of Special Chemicals, Taiyuan University of Technology, Taiyuan 030024, Shanxi, China; 2. Shanxi Key Laboratory of Gas Energy Efficient and Clean Utilization, Taiyuan 030024, Shanxi, China
Abstract:Based on the strong interaction energy between the coordinatively unsaturated metal sites (UMSs) and the gas molecules, M-BTC(M=Cr, Mo, Ni), isostructural with HKUST-1 (Cu-BTC), were successfully synthesized via the coordination reaction of the high activity divalent metal (Cr2+/Mo2+/Ni2+) and organic ligand (H3BTC), and then to gain insight into the impact of gas-metal interactions on the selective adsorption of CH4 from N2 by comparing with classical materials (Cu-BTC). The results show the good CH4 selective adsorption properties of M-BTC (M=Cr, Mo, Ni) with UMSs. Among these materials, Ni-BTC with unsaturated Ni2+ sites presents the highest adsorption heat value for CH4, leading to the excellent CH4/N2 adsorption separation properties; but the Cr-BTC with high Cr2+ activity shows the lower ability for CH4/N2 separation than Cu-BTC. Combined the IAST calculation results, we verified the ability for the selective adsorption of CH4 molecules on M-BTC (M=Cr, Mo, Ni) and Cu-BTC followed as Ni-BTC > Mo-BTC > Cu-BTC > Cr-BTC.
Keywords:methane  nitrogen  adsorption  adsorbents  coordinatively unsaturated metal sites  
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