Catalytic activities and mechanism of formaldehyde oxidation over gold supported on MnO₂ microsphere catalysts at room temperature

Abstract

MnO₂ microspheres with various surface structures were prepared using the hydrothermal method, and Au/MnO₂ catalysts were synthesized using the sol-gel method. We obtained three MnO₂ microspheres and Au/MnO₂ samples: coherent solid spheres covered with wire-like nanostructures, solid spheres with nanosheets, and hierarchical hollow microspheres with nanoplatelets and nanorods. We investigated the properties and catalytic activities of formaldehyde oxidation at room temperature. Crystalline structures of MnO₂ are the main factor affecting the catalytic activities of these samples, and γ-MnO₂ shows high catalytic performance. The excellent redox properties are responsible for the catalytic ability of γ-MnO₂. The gold-supported interaction can change the redox properties of catalysts and accelerate surface oxygen species transition, which can account for the catalytic activity enhancement of Au/MnO₂. We also studied intermediate species. The dioxymethylene (DOM) and formate species formed on the catalyst surface were considered intermediates, and were ultimately transformed into hydrocarbonate and carbonate and then decomposed into CO₂. A proposed mechanism of formaldehyde oxidation over Au/MnO₂ catalysts was also obtained.

Keywords

MnO₂ microspheres / Au/MnO₂ / formaldehyde oxidation / γ-MnO₂

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Acknowledgements

This work is financially supported by the National Natural Science Foundation of China (Grant Nos. 21107124 and 21337003), Dean’s Award Startup Funds of the Chinese Academy of Sciences, the National High Technology Research and Development Program of China (No. 2012AA063101), and Science Promotion Program of Research Center for Eco-Environmental Sciences, CAS (YSW2013B05).

Supplementary material is available in the online version of this article at http://dx.doi.org/10.1007/s11783-015-0808-8 and is accessible for authorized users.

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