Selective oxidation of methane to organic oxygenates over metal–organic frameworks (MOFs) catalysts at low temperature is a challenging topic in the field of C1 chemistry because of the inferior stability of MOFs. Modifying the surface of Cu-BTC via hydrophobic polydimethylsiloxane (PDMS) at 235 °C under vacuum not only can dramatically improve its catalytic cycle stability in a liquid phase but also generate coordinatively unsaturated Cu(I) sites, which significantly enhances the catalytic activity of Cu-BTC catalyst. The results of spectroscopy characterizations and theoretical calculation proved that the coordinatively unsaturated Cu(I) sites made H
2
O
2
dissociative into •OH, which formed Cu(II)-O active species by combining with coordinatively unsaturated Cu(I) sites for activating the C−H bond of methane. The high productivity of C1 oxygenates (CH
3
OH and CH
3
OOH) of 10.67 mmol g
cat.
−1
h
−1
with super high selectivity of 99.6% to C1 oxygenates was achieved over Cu-BTC-P-235 catalyst, and the catalyst possessed excellent reusability.
A MOF named [(CH 3 )NH 2 ] [H 2 N(CH 3 ) 2 ][ZnTNC4A] ⋅ 4H 2 O (ZnTNC4A) was synthesized by a resorcinol[4]arene functionalized tetracarboxylic acid ligand (TNC4A = 2,8,14,12,18,10,16,arene). The three-dimensional framework with one-dimensional channels of ZnTNC4A was characterized by elemental analysis, powder X-ray diffraction, thermogravim-etry, UV-vis diffuse reflection spectrum, infrared spectrum and N 2 adsorption analyse. In addition, ZnTNC4A shows the ability of selective adsorption of methylene blue with a pseudosecond order kinetic model. The selective adsorption kinetics of a series of dyes showed that the ion exchanged separation process was related to the size and charge of organic dyes.
We report three lanthanide-coordination polymers assembled with a resorcin[4]arene ligand, where 1 and 2 could be applied as fluorescent sensors for N,N′-dimethylformamide and Fe3+ ion.
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