School of Engineering, University of British Columbia, Kelowna, BC, V1V 1V7, Canada.
Department of Chemical and Petroleum Engineering, Sharif University of Technology, Tehran, Iran.
J Environ Manage. 2020 Nov 15;274:111155. doi: 10.1016/j.jenvman.2020.111155. Epub 2020 Aug 14.
This work reports on the potential application of UiO-66 in gas sweetening and its structural stability against water, air, dimethylformamide (DMF), and chloroform. The UiO-66 nanoparticles were solvothermally synthesized at different scales and activated via solvent exchange technique using chloroform, methanol, and ethanol. Thus prepared and aged MOFs were characterized using Fourier transform infrared (FTIR) spectroscopy, X-ray diffraction (XRD), Field emission scanning electron microscopy (FESEM), and nitrogen adsorption-desorption analysis. The chloroform-activated MOF showed the largest surface area among all activation solvents, and presented high uptakes of 8.8 and 4.3 mmol/g for CO and CH, respectively, at 298 K and 30 bar. This might be due to removing all unreacted organic ligands and DMF molecules from the pores of the framework. The UiO-66 nanoparticles are stable at the experimental conditions with no significant loss in crystalline structure and gas adsorption ability even after aging under different conditions for one year. The UiO-66 could be easily regenerated at 373 K with no observed significant reduction in gas uptakes even after five consecutive adsorption-desorption cycles. The present findings suggest the excellent potential of the UiO-66-derived MOFs as the promising materials for CO/CH separation at low pressures and results can be applied in practical natural gas sweetening.
本工作报道了 UiO-66 在气体脱硫中的潜在应用及其对水、空气、二甲基甲酰胺(DMF)和氯仿的结构稳定性。UiO-66 纳米粒子在不同规模下通过溶剂热合成得到,并通过溶剂交换技术用氯仿、甲醇和乙醇进行活化。采用傅里叶变换红外(FTIR)光谱、X 射线衍射(XRD)、场发射扫描电子显微镜(FESEM)和氮气吸附-脱附分析对制备和老化的 MOF 进行了表征。在所有活化溶剂中,氯仿活化的 MOF 具有最大的表面积,在 298 K 和 30 巴下,对 CO 和 CH 的吸附量分别高达 8.8 和 4.3 mmol/g。这可能是由于从骨架的孔中去除了所有未反应的有机配体和 DMF 分子。UiO-66 纳米粒子在实验条件下稳定,即使在不同条件下老化一年后,其晶体结构和气体吸附能力也没有明显损失。UiO-66 可以在 373 K 下很容易地再生,即使在连续进行了五次吸附-脱附循环后,气体吸附量也没有明显减少。这些发现表明,UiO-66 衍生的 MOF 具有作为在低压力下 CO/CH 分离的有前途的材料的优异潜力,研究结果可应用于实际的天然气脱硫。