Study on deuterium exchange in surface CHx species formed from methane over platinum, ruthenium and cobalt under non-oxidative conditions

Abstract

Dissociative chemisorption of methane over ruthenium, cobalt, platinum and their bimetallic counterparts supported by alumina and NaY was investigated under a wide range of temperatures. The extent of hydrogen loss from methane was monitored by deuterium uptake of the surface CHx species formed from methane during the course of methane chemisorption. The presence of a high average number of deuterium in the desorbing methane suggested a widespread dissociation of methane. The initial distribution of the deuterated products generally decreased in the sequence CD4 > CI-ID3 > CH2D2. The amount of chemisorbed methane during methane chemisorption increases with temperature and it follows the sequence of reducibility of the supported metals and particle size which, in turn, depends on the support and the alloy formed. CHx (x = 1) species prevailed on alumina supported catalysts, while on NaY supported metals, CH2 species are dominant when small metal particles are stabilized inside the supercage.

Non-oxidative methane transformations into higher hydrocarbons over bimetallic Pt–Co catalysts supported on Al2O3 and NaY

“…In our earlier works [15][16][17][18][19][20][21] the advantages of the bimetallic Co-based catalysts compared with the monometallic ones in the NOCM process were demonstrated: Pt-Co > Pd-Co > Ru-Co > Re-Co > Co. To optimize the NOCM it is necessary to obtain detailed knowledge on the mechanism of the gas phase and surface chemistry. Although NOCM occurs on numerous monometallic catalysts (like Co, Ru), our earlier works shows the advantages of the cobalt-based bimetallic catalysts as compared with the monometallic ones.…”