CJCU

Chem. J. Chinese Universities ›› 2010, Vol. 31 ›› Issue (1): 145.

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Effects of the Active Carbon Surface Properties on the Structure and Catalytic Activity of Cu2O/AC Catalyst

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

  1. Key Laboratory of Coal Science and Technology of Ministry of Education and Shanxi Province, Taiyuan University of Technology, Taiyuan 030024, China
  • Received:2009-04-03 Online:2010-01-10 Published:2010-01-10
  • Contact: LI Zhong. E-mail: lizhong@tyut.edu.cn
  • Supported by:

    国家自然科学基金(批准号: 20976113)和国家“九七三”计划项目(批准号: 2005CB221204)资助.

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Abstract:

The chloride-free Cu2O/AC catalyst was prepared by pyrolysis of copper acetate supported on active carbon(AC), which was used to catalyze the direct vapor-phase oxycarbonylation of methanol to dimethyl carbonate(DMC).When the AC support was treated with nitric acid or ammonia, the chemical property of AC surface was modified, resulting in the change of surface structure and high catalytic activity of Cu2O/AC catalyst. The experiments revealed that the new nitro-groups were formed and the oxy-groups(C—O—C, C—O and CO—O) increased, but the CO species decreased significantly or disappeared on the surface of active carbon treated with nitric acid or ammonia. The reduction of CuⅡ to CuⅠwas promoted by the nitro-groups electron donation and rich CO—O groups, which was propitious to obtain unique and well dispersed Cu2O supported catalysts and enhance the catalytic activity. The treatment of AC with ammonia was favor for the dispersion of Cu2O and improved catalytic activity furthermore. On the conditions of n(CO)∶n(MeOH)∶n(O2)=4∶10∶1 and SV=5600 h-1, the methanol conversion, the space time yield and the selectivity of DMC reached 7.0%, 145.1 mg/(g\5h) and 68.7%, respectively.

Key words: Active carbon(AC); Copper acetate; Cu2O/AC; Oxycarbonylation; Catalysis

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