The synthesis of acetic acid from methane via oxidative bromination, carbonylation, and hydrolysis

K. X. Wang; H. F. Xu; W. S. Li; C. T. Au; X. P. Zhou

doi:10.1016/j.apcata.2006.02.035

The synthesis of acetic acid from methane via oxidative bromination, carbonylation, and hydrolysis

K. X. Wang, H. F. Xu, W. S. Li, C. T. Au, X. P. Zhou^*

^*Corresponding author for this work

Department of Chemistry

Research output: Contribution to journal › Journal article › peer-review

42 Citations (Scopus)

Abstract

Acetyl bromide and acetic acid (AA) were synthesized from methane by an energy-saving process. By reacting methane with oxygen in the presence of HBr and H₂O over a 2.5% Ba 2.5% La 0.5% Ni 0.1% Ru/SiO₂ catalyst, methane was converted to CH₃Br and CO (CH₃Br/CO molar ratio = 1/1) with a CH₄ single-pass conversion of 70% at 660 °C. Our results showed that CH₃Br was formed via the interaction of methane with bromine radicals whereas CO was generated in the oxidation of CH₃Br. Through the carbonylation of CH₃Br over RhCl₃-KI or RhCl₃-PPh₃ (triphenyl phosphine) catalyst in propanoic acid, acetyl bromide could be synthesized and readily hydrolysed to acetic acid at room temperature (with more than 99.7% yield based on CH₃Br). The promotional action of PPh₃ and KI is realized via the direct coordination of PPh₃ to Rh and the conversion of CH₃Br to CH₃I by means of Br-I exchange, respectively.

Original language	English
Pages (from-to)	168-177
Number of pages	10
Journal	Applied Catalysis A: General
Volume	304
Issue number	1-2
DOIs	https://doi.org/10.1016/j.apcata.2006.02.035
Publication status	Published - 10 May 2006

Scopus Subject Areas

Catalysis
Process Chemistry and Technology

User-Defined Keywords

Acetic acid synthesis
Carbonylation
Carbonylation catalyst
Methane oxidative bromination

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10.1016/j.apcata.2006.02.035

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title = "The synthesis of acetic acid from methane via oxidative bromination, carbonylation, and hydrolysis",

abstract = "Acetyl bromide and acetic acid (AA) were synthesized from methane by an energy-saving process. By reacting methane with oxygen in the presence of HBr and H2O over a 2.5% Ba 2.5% La 0.5% Ni 0.1% Ru/SiO2 catalyst, methane was converted to CH3Br and CO (CH3Br/CO molar ratio = 1/1) with a CH4 single-pass conversion of 70% at 660 °C. Our results showed that CH3Br was formed via the interaction of methane with bromine radicals whereas CO was generated in the oxidation of CH3Br. Through the carbonylation of CH3Br over RhCl3-KI or RhCl3-PPh3 (triphenyl phosphine) catalyst in propanoic acid, acetyl bromide could be synthesized and readily hydrolysed to acetic acid at room temperature (with more than 99.7% yield based on CH3Br). The promotional action of PPh3 and KI is realized via the direct coordination of PPh3 to Rh and the conversion of CH3Br to CH3I by means of Br-I exchange, respectively.",

keywords = "Acetic acid synthesis, Carbonylation, Carbonylation catalyst, Methane oxidative bromination",

author = "Wang, {K. X.} and Xu, {H. F.} and Li, {W. S.} and Au, {C. T.} and Zhou, {X. P.}",

note = "Funding Information: This work was supported by the Excellent Young Scientist Supporting Program of the Chinese Ministry of Education and the Analysis National Key laboratory at Hunan University. C.T.A. thanks the Hunan University for an adjunct professorship.",

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AU - Wang, K. X.

AU - Xu, H. F.

AU - Li, W. S.

AU - Au, C. T.

AU - Zhou, X. P.

N1 - Funding Information: This work was supported by the Excellent Young Scientist Supporting Program of the Chinese Ministry of Education and the Analysis National Key laboratory at Hunan University. C.T.A. thanks the Hunan University for an adjunct professorship.

PY - 2006/5/10

Y1 - 2006/5/10

N2 - Acetyl bromide and acetic acid (AA) were synthesized from methane by an energy-saving process. By reacting methane with oxygen in the presence of HBr and H2O over a 2.5% Ba 2.5% La 0.5% Ni 0.1% Ru/SiO2 catalyst, methane was converted to CH3Br and CO (CH3Br/CO molar ratio = 1/1) with a CH4 single-pass conversion of 70% at 660 °C. Our results showed that CH3Br was formed via the interaction of methane with bromine radicals whereas CO was generated in the oxidation of CH3Br. Through the carbonylation of CH3Br over RhCl3-KI or RhCl3-PPh3 (triphenyl phosphine) catalyst in propanoic acid, acetyl bromide could be synthesized and readily hydrolysed to acetic acid at room temperature (with more than 99.7% yield based on CH3Br). The promotional action of PPh3 and KI is realized via the direct coordination of PPh3 to Rh and the conversion of CH3Br to CH3I by means of Br-I exchange, respectively.

AB - Acetyl bromide and acetic acid (AA) were synthesized from methane by an energy-saving process. By reacting methane with oxygen in the presence of HBr and H2O over a 2.5% Ba 2.5% La 0.5% Ni 0.1% Ru/SiO2 catalyst, methane was converted to CH3Br and CO (CH3Br/CO molar ratio = 1/1) with a CH4 single-pass conversion of 70% at 660 °C. Our results showed that CH3Br was formed via the interaction of methane with bromine radicals whereas CO was generated in the oxidation of CH3Br. Through the carbonylation of CH3Br over RhCl3-KI or RhCl3-PPh3 (triphenyl phosphine) catalyst in propanoic acid, acetyl bromide could be synthesized and readily hydrolysed to acetic acid at room temperature (with more than 99.7% yield based on CH3Br). The promotional action of PPh3 and KI is realized via the direct coordination of PPh3 to Rh and the conversion of CH3Br to CH3I by means of Br-I exchange, respectively.

KW - Acetic acid synthesis

KW - Carbonylation

KW - Carbonylation catalyst

KW - Methane oxidative bromination

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The synthesis of acetic acid from methane via oxidative bromination, carbonylation, and hydrolysis

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