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Catalysts with designable intelligent nanostructure may potentially drive the changes in chemical reaction techniques. Herein, a multi‐function integrating nanocatalyst, Pt‐containing magnetic yolk‐shell carbonaceous structure, having catalysis function, microenvironment heating, thermal insulation, and elevated pressure into a whole is designed, which induces selective hydrogenation within heating‐constrained nanoreactors surrounded by ambient environment. As a demonstration, carbonyl of α, β‐unsaturated aldehydes/ketones are selectively hydrogenated to unsaturated alcohols with a >98% selectivity at a nearly complete conversion under mild conditions of 40 °C and 3 bar instead of harsh requirements of 120 °C and 30 bar. It is creatively demonstrated that the locally increased temperature and endogenous pressure (estimated as ≈120 °C, 9.7 bar) in the nano‐sized space greatly facilitate the reaction kinetics under an alternating magnetic field. The outward‐diffused products to the “cool environment” remain thermodynamically stable, avoiding the over‐hydrogenation that often occurs under constantly heated conditions of 120 °C. Regulation of the electronic state of Pt by sulfur doping of carbon allows selective chemical adsorption of the CO group and consequently leads to selective hydrogenation. It is expected that such a multi‐function integrated catalyst provides an ideal platform for precisely operating a variety of organic liquid‐phase transformations under mild reaction conditions.
A multi‐function nanocatalyst, integrating locally inside‐heating, thermal insulation, and high‐dispersed Pt into a whole, induces selective hydrogenations within heat‐constrained nanoreactors (120 °C) surrounded by a cool environment (40 °C). A 20.1‐fold increase in reaction rate is achieved compared to the conventional outside‐in heating. The diffusion of target products into a cool environment ensures the high selectivity (>98%) under high conversion (≈100%).