A highly stable dimethyl-functionalized Ce(IV)-based UiO-66 metal-organic framework material for gas sorption and redox catalysis

作者：Dalapati Rana; Sakthivel Balasubramanian; Dhakshinamoorthy Amarajothi^*; Buragohain Amlan; Bhunia Asamanjoy; Janiak Christoph; Biswas Shyam^*

来源：CrystEngComm, 2016, 18(40): 7855-7864.

DOI：10.1039/c6ce01704e

The new, dimethyl-functionalized Ce(IV)-based UiO-66 (UiO = University of Oslo) metal-organic framework (MOF) material Ce-UiO-66-(CH3)(2) (1) was successfully synthesized under solvothermal conditions (100 degrees C, 15 min) by employing ammonium cerium(IV) nitrate and the 2,5-dimethyl-1,4-benzenedicarboxylate (H2BDC-(CH3)(2)) ligand in a DMF/H2O (DMF = N,N-dimethyl formamide) mixture. The phase purity of the as-synthesized and thermally activated form (1') of the compound was confirmed by a combination of X-ray powder diffraction (XRPD) analysis, Fourier transform infrared (FT-IR) spectroscopy and thermogravimetric (TG) analysis. As verified by the thermogravimetric analysis, the compound is thermally stable up to 300 degrees C in air atmosphere. Based on the XRPD measurements, the material retains its crystallinity after treatment with water, methanol, acetic acid and 1 M HCl. As confirmed by the gas sorption experiments, the compound shows significant microporosity towards N-2 (BET surface area = 845 m(2) g(-1)) and CO2 (adsorption capacity = 34 cm(3) g(-1) at 0 degrees C and 1 bar). The catalytic activity of 1' has been studied in the oxidation of styrene and cyclohexene using tert-butylhydroperoxide (TBHP) as the terminal oxidant. The catalyst is reusable for four cycles with no significant drop in its activity which is further confirmed by a hot filtration experiment.

• 出版日期2016