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Oxidative bromination of methane on silica-supported non-noble metal oxide catalysts

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Abstract
Oxidative bromination of methane, mediated by HBr/H2O (solution), provides an original route for the
production of oxygenates and gasoline directly from natural gas. However, the reported catalysts for this
reaction all involved noble metals. From the consideration of replacing noble metal catalysts with
cheaper oxides, various silica-supported oxide catalysts were surveyed. It was found that the redox
ability of different metals had a strong impact on the product distribution. On the catalysts with metals
that lack facile redox ability, such as BaO/SiO2, both CH3Br and CO were main products. Otherwise, deep
oxidation proceeded. Moreover, methanol was firstly reported in this system. In order to obtain a molar
ratio of (CH3OH + CH3Br): CO = 1, which can provide a perfect feedstock for the synthesis of acetic acid,
the process variables were optimized on BaO/SiO2. It was demonstrated that 44.0% methane conversion
and 95% total selectivity of CH3Br, CH3OH and CO could be achieved at 620 8C, and the molar ratio of
(CH3Br + CH3OH): CO was close to 1. Time-on-stream tests showed declined catalytic performance after
30 h. The results from N2-adsorption, XRF and XRD implied that aggregation of bariumparticles occurred,
making the metathesis between BaO and BaBr2 difficult. The functions of BaO were also proposed.
Additionally, the activity data were compared with those of noble metal catalysts.

Keywords:Methane oxidative bromination, Non-noble metal oxide, BaO/SiO2, (CH3OH + CH3Br): CO, Metathesis
Deactivation mechanism

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Informasi Detail

Judul Seri

Applied Catalysis A: General

No. Panggil

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Penerbit

London : Elsevier B.V.., 2009

Deskripsi Fisik

Applied Catalysis A: General 353 (2009) 87–92

Bahasa

English

ISBN/ISSN

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Klasifikasi

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Tipe Isi

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Tipe Media

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Tipe Pembawa

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Edisi

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Subjek

KIMIA

Info Detail Spesifik

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Pernyataan Tanggungjawab

agus

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