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Chem. J. Chinese Universities ›› 2009, Vol. 30 ›› Issue (10): 2024.

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Chloride-free Cu2O/AC Catalyst Prepared by Pyrolysis of Copper Acetate and Catalytic Oxycarbonylation

LI Zhong*, WEN Chun-Mei, WANG Rui-Yu, ZHENG Hua-Yan, XIE Ke-Chang   

  1. Key Laboratory of Coal Science and Technology of Ministry of Education, Key Laboratory of Shanxi Province, Taiyuan University of Technology, Taiyuan 030024, China
  • Received:2009-01-17 Online:2009-10-10 Published:2009-10-10
  • Contact: LI Zhong. E-mail: lizhong@tyut.edu.cn
  • Supported by:

    国家自然科学基金(批准号: 20576085)和国家“九七三”计划(批准号: 2005CB221204)资助.

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Abstract:

The chloride-free Cu2O/AC catalyst was prepared via pyrolysis of copper acetate supported on active carbon Cu(CH3COO)2/AC and used to catalyze vapor-phase oxycarbonylation of methanol to dimethyl carbonate(DMC). The Cu(CH3COO)2/AC precursor was prepared by the incipient wetness impregnation. When Cu(CH3COO)2·H2O was heated from 30 ℃ to 450 ℃ under inert nitrogen atmosphere, it decomposed successively to Cu(CH3COO)2, Cu2O and Cu, corresponding to three chemical processes. Cu2O was obtained at 150—300 ℃ heating temperature, and Cu was formed at 300—450 ℃. When Cu(CH3COO)2·H2O/AC was heated at 200—350 ℃ for 4 h, Cu2O was gradually formed on the surface of AC. The Cu2O/AC catalyst with predominant Cu2O and only a little Cu was obtained when Cu(CH3COO)2·H2O/AC heated at 350 ℃ for 4 h. It was observed that the Cu2O/AC catalyst heat-treated at 300—350 ℃ for 4 h exhibited very high catalytic activity for methanol oxycarbonylation. On the conditions of n(CO)∶n(MeOH)∶n(O2)=4∶10∶1 and SV=5600 h-1, and in the presence of Cu2O/AC catalyst prepared at 300 ℃ for 4 h, the methanol conversion, the space time yield and the selectivity of DMC was reached 6.21%, 128.16 mg·g-1·h-1 and 64.26%, respectively.

Key words: Copper acetate; Pyrolysis; Cu2O/AC catalyst; Oxycarbonylation; Dimethyl carbonate

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