Correlation of Performance and Structure of Supported Rhenium Catalysts for Methanol Selective Oxidation

Abstract

Abstract: Supported Re catalysts were prepared by impregnation of ammonium perrhenate precursor on oxide supports, followed by calcination at 673 Kin He steam.Iron-oxides and V₂O₅ supported Re catalysts showed a higher activity and selectivity for the catalytic methanol oxidation to dimethoxymethane [3CH₃OH + (1/2)O₂ CH₂(OCH₃)₂ + 2H₂O].The selectivity was as high as 90—94% (molar fraction) at 513 K.The highest reaction rate of 450 mmol·h^-1·g^-1 Re on -Fe₂O₃ supported Re catalysts was achieved with the Re loading weight of 2%(mass fraction).The reaction rate gradually decreased with the increase of Re loading weight.Calcination of ammonium perrhenate alone at 673 Kin He gave mono-clinic ReO₂ as a main product.However, the application of the iron-oxide may prevent Re⁷⁺ from reducting to Re⁴⁺ during the calcination at 673 Kin He in the case of proper Re loading weight probably through the interaction of ammonium perrhenate with the supports, leading to the growth of Re⁶⁺ on the catalyst surface.Above the monolayer loading weight of ReO₃, there was coexistence of Re⁶⁺ and Re⁴⁺ on the catalyst surface.Aredox mechanism between Re⁶⁺ and Re⁴⁺ species on the catalyst surface was proposed to be responsible for the high performance in the methanol selective oxidation to dimethoxymethane.

Key words: Supported rhenium catalyst, Methanol, Selective oxidation, Dimethoxymethane

CLC Number:

O643.3

TrendMD:

YUAN You-Zhu, CAO Wei, TSAI Khi-Rui, IWASAWA Yasuhiro. Correlation of Performance and Structure of Supported Rhenium Catalysts for Methanol Selective Oxidation[J]. Chem. J. Chinese Universities, 2002, 23(5): 902.

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Correlation of Performance and Structure of Supported Rhenium Catalysts for Methanol Selective Oxidation

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