Key Laboratory of Synthetic and Natural Functional Molecule Chemistry of the Ministry of Education, Shaanxi Key Laboratory of Physico-Inorganic Chemistry, College of Chemistry & Materials Science , Northwest University , Xi'an 710069 , P. R. China.
School of Chemical Engineering , The University of Queensland , Brisbane 4072 , Australia.
ACS Appl Mater Interfaces. 2018 Apr 4;10(13):10965-10973. doi: 10.1021/acsami.8b01291. Epub 2018 Mar 22.
Carrying out the strategy of incorporating rod secondary building units and polar functional groups in metal-organic frameworks (MOFs) to accomplish the separation of CO and C hydrocarbons over CH as well as CO fixation, an oxalamide-functionalized ligand N, N'-bis(isophthalic acid)-oxalamide (HBDPO) has been designed. The solvothermal reaction of HBDPO with the oxophilic alkaline-earth Ba ion afforded a honeycomb Ba-MOF, {[Ba(BDPO)(HO)]·DMA} (1). Due to the existence of Lewis basic oxalamide groups and unsaturated Lewis acid metal sites in the tubular channels, the activated framework presents not only high CH, CH, and CO uptakes and selective capture from CH, but also efficient CO chemical fixation as a recyclable heterogeneous catalyst. Grand canonical Monte Carlo simulations were combined to explore the adsorption selectivities for CH-CH and CH-CH mixtures as well as the interaction mechanisms between the framework and epoxides.
为了在 CH 上实现 CO 和 C 烃类的分离以及 CO 固定，从而完成将棒状二级构筑单元和极性官能团纳入金属-有机骨架（MOFs）的策略，设计了一种草酰胺功能化配体 N，N'-双（异酞酸）草酰胺（HBDPO）。HBDPO 与亲核性碱性土 Ba 离子的溶剂热反应得到了蜂窝状 Ba-MOF，{[Ba（BDPO）（HO）]·DMA}（1）。由于管状通道中存在路易斯碱性草酰胺基团和不饱和路易斯酸金属位点，活化骨架不仅具有高的 CH、CH 和 CO 吸附量，并且可以从 CH 混合物中选择性捕获，而且还可以作为可回收的非均相催化剂高效地进行 CO 化学固定。使用巨正则蒙特卡罗模拟来研究 CH-CH 和 CH-CH 混合物的吸附选择性以及骨架与环氧化物之间的相互作用机制。
