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

Abstract

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 °C) than those required in previous reports (> 700 °C). Rh sub-nano clusters with 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 H2/CO ratio of 2.0 at 600 °C even at a very high space velocity (1,200,000 mL h−1 g−1). No deactivation was observed in the durability test for 50 h, and turnover number of bulk Rh for the formation of CO reached 2,600,000. Kinetic and spectroscopic studies revealed that a combustion-reforming mechanism occurs on the metallic Rh sub-nano clusters. Acidity of the zeolite played no role in the reaction, but the ion-exchange properties of zeolites were crucial to prepare active Rh catalysts.

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Publication details

The article was accepted on 10 Nov 2017 and first published on 13 Nov 2017


Article type: Paper
DOI: 10.1039/C7CY02183F
Citation: Catal. Sci. Technol., 2017, Accepted Manuscript
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    Zeolite-supported rhodium sub-nano cluster catalyst for low-temperature selective oxidation of methane to syngas

    Y. Hou, S. Ogasawara, A. Fukuoka and H. Kobayashi, Catal. Sci. Technol., 2017, Accepted Manuscript , DOI: 10.1039/C7CY02183F

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