A postsynthetic covalent strategy involving dual-acyl chloride has been developed to introduce uncoordinated carboxyl groups into amine containing metal–organic frameworks (MOFs). The carboxyl group functionalized MOFs have been characterized by various techniques, including X-ray diffraction patterning, scanning electron microscopy, Fourier transform infrared spectroscopy, nuclear magnetic resonance, thermal gravimetric analysis, and gas adsorption. Results clearly indicated uncoordinated carboxyl groups were successfully grafted to the MIL-101(Cr)–NH2 framework. In addition, most of the amine groups (>80%) were grafted with carboxyl groups, which indicates this method is very effective. The thermal stability and adsorption selectivity of CO2/N2 were substantially enhanced, albeit the BET surface areas and total pore volumes were reduced. These observations could be explained by the effect of elimination of macropores in the framework due to the projecting of new functional groups in pore apertures. Here the successful fabrication of a MOF with uncoordinated carboxyl groups provides the possibility of efficiently modifying other MOFs.
1 July 2021 in Separation and Purification Technology
The solar-driven desalination is seen as a sustainable way to combat water scarcity. However, the solar steam generation efficiency has long been restricted by the high vaporization enthalpy of water and low energy density of natural sunlight. We introduced graphene oxide (GO) cross-linked with polyethyleneimine (PEI) as the photothermal material, with the enriched ammonic functional groups in modified GO membrane (GPM) activating water molecules to evaporate with much lower energy consumption. The vaporization enthalpy at the air-film interface is reduced up to 42% in GPM film by tuning the thermodynamic states of water. Consequently, GPM film enables a high evaporation rate of 2.48 kg m−2 h−1 with 95.7% energy conversion efficiency under 1 sun. With the aid of positive charges introduced by hydrolysis of PEI, the GPM exhibits excellent salt resistance and delivers an evaporation rate around 1.8 kg m−2 h−1 when treating 20 wt % NaCl solution.