Nanoengineered design of inside-heating hot nanoreactor surrounded by coolenvironment for selective hydrogenations.

Abstract

Catalysts with designable intelligent nanostructure may potentially drive the changes of chemical reaction techniques. Herein, we designed a multi-function integrating nanocatalyst, Pt-containing magnetic yolk-shell carbonaceous structure, having catalysis function, microenvironment heating, thermalinsulation and elevated pressure into a whole, 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 3bar instead of harsh requirements of 120°C and 30bar. We creatively demonstrate that the locally increased temperature and endogenous pressure (estimated as ∼120°C, 9.7bar) in the nano-sized space greatly facilitates the reaction kinetics under an alternating magnetic field. The outward-diffused products to the "cool environment" retain thermodynamically stable, avoiding the over-hydrogenation 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 -C = O 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. This article is protected by copyright. All rights reserved.