Citation: ZHU Li-hua, XU Feng, WANG Jue, ZHAO Xiao-peng. Selective oxidation of methane to methanol in acetic acid solvent over Pd-CuPc/Y catalyst[J]. Journal of Fuel Chemistry and Technology, ;2013, 41(8): 985-990. shu

Selective oxidation of methane to methanol in acetic acid solvent over Pd-CuPc/Y catalyst

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School of Safety Engineering and Technology, Heilongjiang University of Science and Technology, Harbin 150022, China

Corresponding author: ZHU Li-hua,
Received Date: 24 May 2013
Available Online: 9 June 2013
Fund Project: 国家自然科学基金(51004045) (51004045) 黑龙江省教育厅科学技术研究项目(12511481) (12511481) 哈尔滨市科技创新人才研究专项资金项目(2013RFQXJ085). (2013RFQXJ085)

The CuPc/Y which is copper phthalocyanine encapsulated inside the supercage of zeolite-Y was prepared with copper dichloride, ammonium molybdate, phthalic anhydride, urea and NaY molecular sieve by means of phthalic anhydride-urea solid state synthesis method. By using CuPc/Y as support, Pd-CuPc/Y composite catalyst was prepared by equivalent-volumetric impregnation method. The catalytic activity of the composite catalyst for selective aerobic oxidation of methane to methanol in acetic acid solvent was investigated. The results showed that the catalytic performance of the composite catalyst was related to reaction temperature, volume ratio of CH₃COOH to H₂O in acetic acid solvent, amount of p-benzoquinone and reaction time. The optimal yield of methanol was 1 840 μmol under the reaction conditions: 0.5 g of 0.5%Pd-0.5%CuPc/Y, 4 to 1 of volume ratio of CH₃COOH to H₂O in acetic acid solvent, 1 000 μmol of p-benzoquinone, 3 h of reaction time and 150 ℃ of reaction temperature. Pd-CuPc/Y catalyst could be reused repeatedly. However, the catalytic activity of reused catalyst decreased by catalyst loss and Pd particle aggregation. The selective oxidation of methane catalyzed by Pd-CuPc/Y catalyst in acetic acid solution possibly involved electrophilic substitute reaction and reactive oxygen species oxidation reaction.
- phthalocyanine,
- palladium,
- molecular sieve,
- methane,
- methanol,
- acetic acid
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沈阳化工大学材料科学与工程学院沈阳 110142