Intensified gas-phase hydrogenation of acetone to isopropanol catalyzed at metal-oxide interfacial sites

Abstract

The gas-phase acetone hydrogenation to isopropanol is an environmentally benign process relevant to chemical, energy and medical fields, but the catalysts qualified at low temperature and pressure remain challenging. Herein, we show the intensified gas-phase hydrogenation of acetone to isopropanol at metal-oxide interface. The Pt/CeO2 catalyst with highly active and stable Pt-CeO2 interface delivers 92 % acetone conversion with 99 % isopropanol selectivity at 80 °C, weight hourly space velocity of 10 h−1, H2/acetone molar ratio of 2, and 0.1 MPa, and its catalytic performance is preserved during a single-running test of 200 h. A series of electron microscopic, thermal, and spectroscopic analyses testify that acetone could be efficiently adsorbed on oxygen vacancy at Pt-CeO2 interface. The H atoms dissociated by Pt spill over to the interface to hydrogenate the chemically-adsorbed acetone thereon to form isopropanol. Inspired by such observation, the Pt-CeO2 interface was extended to other metal-oxide interfaces (metal: Pt and Ni; oxide: CeO2, TiO2, ZrO2 and Fe3O4), all exhibiting excellent catalytic performance. For example, the Ni/CeO2 could offer 91 % acetone conversion and 99 % isopropanol selectivity, identical to that of Pt/CeO2 under the same conditions. This work particularly investigated the acetone adsorption at the metal-oxide interface, establishing the foundation for rational design of high cost performance catalysts for aldehydes/ketones hydrogenation and other reactions.