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Synthesis and Testing of Supported Pt-Cu Solid Solution Nanoparticle Catalysts for Propane Dehydrogenation
Published on: July 18, 2017
Enhanced methane combustion performance and stability of the supported Pd nanoparticles by constructing the ordered
Mengwei Hua1, Yuxi Liu2, Xuehong Zi3
1Beijing Key Laboratory for Green Catalysis and Separation, State Key Laboratory of Materials Low-Carbon Recycling, Laboratory of Catalysis Chemistry and Nanoscience, Department of Chemical Engineering and Technology, College of Materials Science and Engineering, Beijing University of Technology, Beijing 100124, China.
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The development of CH4 low-temperature combustion catalysts with high efficiency and good stability faces a major challenge. In this work, the supported noble metal catalysts with ordered mesoporous Co3O4-CeO2 interfaces and highly dispersed Pd2+ active sites were prepared by the KIT-6-templating and NaBH4 reduction methods. It was found that compared to 1.39 wt.% Pd/meso‑Co3O4 (1.39Pd/meso‑Co3O4) and 1.26 wt.% Pd/meso‑CeO2 (1.26Pd/meso‑CeO2), 1.43 wt.% Pd/meso‑Co2Ce1 (1.43Pd/meso‑Co2Ce1; n(Co3O4)/n(CeO2) molar ratio = 2 : 1) exhibited better catalytic activity for methane combustion (T50% = 328 °C and T90% = 378 °C at space velocity = 20,000 mL/(g·h); specific reaction rate at 280 °C = 0.42 μmol/(gcat·s) or 29.4 μmol/(gPd·s); and turnover frequency (TOFPd) at 280 °C = 6.33 × 10-3 s-1). Furthermore, the 1.43Pd/meso‑Co2Ce1 sample showed good catalytic stability. The presence of the Co3O4-CeO2 ordered mesoporous interfaces in 1.43Pd/meso‑Co2Ce1 promoted the generation of active oxygen species and effectively stabilized PdO active site, thereby enhancing catalytic activity of 1.43Pd/meso‑Co2Ce1 for CH4 combustion. In addition, methane combustion pathways over 1.43Pd/meso‑Co2Ce1 might be as follows: gas-phase methane → adsorbed methane → formate or carbonate → carbon dioxide and water. This work provides novel insights into the role of redox binary metal oxide interfaces in methane combustion.
