期刊
CHEMICAL ENGINEERING JOURNAL
卷 411, 期 -, 页码 -出版社
ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2021.128536
关键词
Mixed ligand; Copper; MOF; Desulfurization; Regeneration
资金
- Korea Institute of Civil Engineering and Building Technology (KICT), Republic of Korea [20200451-001]
A mixed ligand Cu-based MOF was synthesized and found to exhibit high adsorption capacity for H2S gas, with significantly improved performance after regeneration. The adsorption mechanism involved breaking Cu-carboxylate bonds and formation of CuS nanoparticles and sulfates, leading to enhanced adsorption capacity of the regenerated sample.
A mixed ligand Cu-based MOF, Cu(BDC)0.5(BDC-NH2)0.5 was synthesized by a rapid ultrasonication method for the adsorptive removal of hydrogen sulfide (H2S) gas at room temperature. The MOF has a sheet-like morphology with 100 nm thickness crystallized in the monoclinic symmetry (a = 11.27 angstrom, b = 14.82 angstrom, c = 7.95 angstrom, beta = 110.8 degrees) with C2/m space group. The surface area and pore volume was 19.4 m2 g-1 and 0.024 cm3 g-1, respectively. The XPS analysis confirmed a near equal proportion of Cu(I) and Cu(II)-sites in the MOF. The MOF showed the H2S adsorption capacity of 128.4 mg g(-1) for 500 ppm of H2S flowing at a rate of 100 mL min(-1), which is among the highest values reported for Cu-based MOFs. The spent MOF was regenerated by a methanol and UV-irradiation method, which significantly improved the adsorption capacity. The H2S adsorbed onto the MOF by breaking Cu-carboxylate bonds with the formation of covellite CuS nanoparticles and sulfates. The spectroscopic analysis predicted a Cu(OH)-type sites after UV-irradiation along with increased surface area, which were responsible for an enhanced adsorption capacity of the regenerated sample.
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