Abstract
Herein we report that mixed zirconium-cerium-MOFs with amino-functionalized linkers (2-amino-1,4-benzenedicarboxylate, BDC-NH2, and 4-aminonaphthalene-2,6-dicarboxylate, NDC-NH2) act as effective non-noble-metal-based heterogeneous catalysts, for both the aerobic photooxidation of benzylic alcohols and for the direct microwaves activation N-alkylation of amines with alcohols. The catalytic performance has been studied considering two different approaches: the effect of NH2 functionalized linkers and the effect of hosting CeIII species on Zr-MOFs. Zr- and ZrCe-MOFs resulted efficient visible-light-driven photocatalysts with high stability and considerable recyclability in the photocatalytic selective oxidation of alcohols to aldehydes using molecular oxygen as oxidant. These materials are also effective catalysts for the microwaves-assisted N-alkylation of amines with alcohols yielding selectively the imine (ZrCe-MOF) or the corresponding secondary amine (Ce-MOFs).
Highlights
Metal organic frameworks (MOFs), consisted of inorganic nodes and organic linkers with high surface areas, are the class of materials that have aroused more interest among researchers in recent years [1,2]
Zr- and mixed ZrCe-MOFs were prepared by direct synthesis under solvothermal conditions in a Teflon lined vessel at 120 ◦C for 24 h (Scheme 1) as described previously [31,47]
We have demonstrated that cerium (IV) can be employed as a FJU-6 MOF precursor in presence of H2O2(since ceric ammonium nitrate (CAN) is more oxidant than H2O2) when the same reaction was performed in presence of 2 equivalents of pure H2O2 a highly crystalline cerium(III) MOF with FJU-6 topology was obtained
Summary
Metal organic frameworks (MOFs), consisted of inorganic nodes and organic linkers with high surface areas, are the class of materials that have aroused more interest among researchers in recent years [1,2]. We report the synthesis of mixed ZrCe-MOFs with BDC-NH2 and a mix of naphthalene-2,6-dicarboxylate (NDC) and 4-aminonaphthalene-2,6-dicarboxylate (NDC-NH2) linkers to modulate the surface charge of MOF networks and concurrently change the active sites incorporating redox centers [51]. We evaluated their behavior as photocatalysts for the aerobic oxidation of benzylic alcohols to aldehydes and towards the microwaves-assisted N-alkylation of benzyl alcohols with amines
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