Enhanced catalytic performance of oxidized Ru supported on N-doped mesoporous carbon for acetylene hydrochlorination

Abstract Herein, experiments and DFT calculations were co-researched on high-performance catalysts for acetylene hydrochlorination. Firstly, the mesoporous carbon materials with adjustable N-doping content (MC-xN, x = 0, 0.5, 1, 2) were successfully synthesized. And the oxidized Ru species were further loaded (Ru-MC-xN) through simple hydrothermal method. Under the experimental condition of T = 170 °C, GHSV(C2H2) = 360 h−1, V(HCl)/V(C2H2) = 1.15, Ru-MC-2N shows excellent catalytic activity, with the acetylene conversion of 98.0 %. Characterized by various techniques, N-doping is confirmed to relatively inhibit the coke deposition and increase the percentage of oxidized Ru species which is attributed to regulation of the adsorption energy. Catalytic pathways of Ru in different valences are also revealed by DFT method. Results show that oxidized Ru species own higher catalytic activities than Ru0 species and manifest the molecular mechanism for HCl activation of RuO2. These findings provide theoretical basis for designs and applications of Ru-based catalysts in acetylene hydrochlorination.