A family of two-dimensional salen-type lanthanide complexes was synthesized through a facile solution diffusion method. The two-dimensional lanthanide complexes were characterized by single-crystal X-ray diffraction (SCXRD) and X-ray photoelectron spectroscopy (XPS) analytical techniques. The SCXRD and XPS analyses reveal that the obtained two-dimensional structures are rich in uncoordinated imine (-CH═N-) groups located on the skeleton of the salen-type organic ligand, which retain strong coordination ability with metal ions. On the basis of this unique feature, a highly dispersed CeO-supported Ni catalyst (Ni/CeO-CAS) with highly strong metal-support interaction was first synthesized via a coordination-assisted synthesis (CAS) method, which exhibits a much better catalytic activity in the hydrogenation of nitrobenzene than the traditional Ni/CeO-IWI catalyst prepared by incipient wetness impregnation (IWI). The origin of the improved catalytic activity of Ni/CeO-CAS as well as the role of Ni@Ce-Hsalen was revealed by using diverse characterizations. On the basis of the comparative characterization results, the superior catalytic performance of Ni/CeO-CAS to Ni/CeO-IWI could have resulted from the smaller and highly dispersed Ni nanoparticulates, the intensified Ni-CeO interaction, the enhanced NiO reducibility, and the higher concentration of oxygen vacancies, favoring the H dissociation and adsorption of the nitrobenzene reactant. The Ni/CeO-CAS catalyst also exhibits high catalytic performance for reduction of diverse nitroarenes to their corresponding functionalized arylamines. We anticipated that this coordination-assisted strategy may provide a new way for preparing other highly oxide-supported catalysts with potential applications in various catalytic reactions.
In this work, the postcombustion CO 2 capture performance was explored in 100.000 g of a nonaqueous solution, 30 wt % monoethylethanolamine (EMEA) and 70 wt % diethylethanolamine (DEEA). Porous solids (multiwalled carbon nanotubes (MWCNTs), silica gel (SG), and MCM-41) with mass fractions (0.025, 0.050, 0.100 and 0.200%) were added into the pure nonaqueous solution forming the new absorbents to improve the CO 2 capture performance. The CO 2 absorption (313 K) and desorption (383 K) of the new absorbents were operated in the absorption−desorption apparatus under atmospheric pressure. The results show that the addition of the porous solids in the nonaqueous solution led to a 2% decrease in the absorption loading, while contributing to a 10 min decrease in the desorption time under the same desorption extent. The maximum desorption rates of the new absorbents peaked about 5 min earlier than that of the nonaqueous solution, with an enhancement order of MWCNTs > MCM-41 > SG. Meanwhile, the new absorbent, nonaqueous solution mixed with 0.050% MWCNTs, had the best enhancement in the desorption process and exhibited a good stability in the absorption−desorption experiment. Analytic methods (XRD, BET, FT-IR, and SEM) were used to characterize MWCNTs before and after the five absorption−desorption cycles, which showed a good stability of MWCNTs with no significant change in the structure and activity.
Lithium-ion-encapsulated fullerenes (Li+@C60) are 3D superatoms with rich oxidative states. Here we show a conductive and magnetically frustrated metal–fullerene-bonded framework {[Cu4(Li@C60)(L)(py)4](NTf2)(hexane)}n (1) (L = 1,2,4,5-tetrakis(methanesulfonamido)benzene, py = pyridine, NTf2− = bis(trifluoromethane)sulfonamide anion) prepared from redox-active dinuclear metal complex Cu2(L)(py)4 and lithium-ion-encapsulated fullerene salt (Li+@C60)(NTf2−). Electron donor Cu2(L)(py)2 bonds to acceptor Li+@C60 via eight Cu‒C bonds. Cu–C bond formation stems from spontaneous charge transfer (CT) between Cu2(L)(py)4 and (Li+@C60)(NTf2−) by removing the two-terminal py molecules, yielding triplet ground state [Cu2(L)(py)2]+(Li+@C60•−), evidenced by absorption and electron paramagnetic resonance (EPR) spectra, magnetic properties and quantum chemical calculations. Moreover, Li+@C60•− radicals (S = ½) and Cu2+ ions (S = ½) interact antiferromagnetically in triangular spin lattices in the absence of long-range magnetic ordering to 1.8 K. The low-temperature heat capacity indicated that compound 1 is a potential candidate for an S = ½ quantum spin liquid (QSL).
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