Issue 24, 2017

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

Abstract

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 °C) than those required in previous reports (>700 °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 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 the 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. 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.

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

Supplementary files

Article information

Article type
Paper
Submitted
25 Oct 2017
Accepted
10 Nov 2017
First published
13 Nov 2017

Catal. Sci. Technol., 2017,7, 6132-6139

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, 7, 6132 DOI: 10.1039/C7CY02183F

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