4.6 Article

Zeolite-supported rhodium sub-nano cluster catalyst for low-temperature selective oxidation of methane to syngas

Journal

CATALYSIS SCIENCE & TECHNOLOGY
Volume 7, Issue 4, Pages 6132-6139

Publisher

ROYAL SOC CHEMISTRY
DOI: 10.1039/c7cy02183f

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Funding

  1. Japan Science and Technology Agency (JST) CREST [JPMJCR15P4]

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The conversion of methane to syngas under mild conditions is a key to efficiently utilise natural gas, including shale gas, in chemical industries. In this work, we demonstrate that Rh sub-nano clusters formed on zeolites catalyse the partial oxidation of methane to syngas at substantially lower temperatures (450-600 degrees C) than those required in previous reports (>700 degrees C). Rh sub-nano clusters of 0.6 nm diameter were prepared by a simple ion-exchange method. The catalyst gave 84% conversion of methane with 91% selectivity for CO and a H-2/CO ratio of 2.0 at 600 degrees C even at a very high space velocity (1200000 mL h(-1) g(-1)). No deactivation was observed in the durability test for 50 h, and the turnover number of bulk Rh for the formation of CO reached 2600000. Kinetic and spectroscopic studies revealed that a combustion-reforming mechanism occurs on the metallic Rh sub-nano clusters. The acidity of the zeolite played no role in the reaction, but the ion-exchange properties of zeolites were crucial to prepare the active Rh catalysts.

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