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Preparation and Catalytic Performances of a Molecularly Imprinted Ru‐Complex Catalyst with an NH 2 Binding Site on a SiO 2 Surface
Author(s) -
Yang Yong,
Weng Zhihuan,
Muratsugu Satoshi,
Ishiguro Nozomu,
Ohkoshi Shinichi,
Tada Mizuki
Publication year - 2012
Publication title -
chemistry – a european journal
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 1.687
H-Index - 242
eISSN - 1521-3765
pISSN - 0947-6539
DOI - 10.1002/chem.201100529
Subject(s) - catalysis , selectivity , adsorption , molecular imprinting , magic angle spinning , chemistry , hydrogen bond , materials science , photochemistry , stereochemistry , nuclear magnetic resonance spectroscopy , molecule , organic chemistry
A catalyst surface with an active metal site, a shape‐selective reaction space, and an NH 2 binding site for o ‐fluorobenzophenone was designed and prepared by the molecular imprinting of a supported metal complex on a SiO 2 surface. A ligand of a SiO 2 ‐supported Ru complex that has a similar shape to the product of o ‐fluorobenzophenone hydrogenation was used as a template. An NH 2 binding site for o ‐fluorobenzophenone was spatially arranged on the wall of a molecularly imprinted cavity with a similar shape to the template. The structures of the SiO 2 ‐supported and molecularly imprinted Ru catalysts were characterized in a step‐by‐step manner by means of solid‐state magic angle spinning (MAS) NMR, XPS, UV/Vis, N 2 adsorption, XRF, and Ru K‐edge EXAFS. The molecularly imprinted Ru catalyst exhibited excellent shape selectivity for the transfer hydrogenation of benzophenone derivatives. It was found that the NH 2 binding site on the wall of the molecularly imprinted cavity enhanced the adsorption of o ‐fluorobenzophenone, of which the reduction product was imprinted, whereas there was no positive effect in the case of o ‐methylbenzophenone, which cannot interact with the NH 2 binding site through hydrogen bonding.