Citation: ZHENG Hua-Yan, GUO Tian-Yu, LI Zhong, MENG Fan-Hui, QIN Yao. Effect of Impregnation Strategy on Structure and Catalytic Performance of CuCe/AC Catalyst[J]. Chinese Journal of Inorganic Chemistry, ;2013, 29(12): 2575-2581. doi: 10.3969/j.issn.1001-4861.2013.00.388 shu

Effect of Impregnation Strategy on Structure and Catalytic Performance of CuCe/AC Catalyst

1.
Key Laboratory of Coal Science and Technology, Ministry of Education and Shanxi Province, Taiyuan University of Technology, Taiyuan 030024, China

Received Date: 18 March 2013
Available Online: 24 June 2013
Fund Project: 国家自然科学基金(No.20976113，21276169) (No.20976113，21276169)山西省科技攻关项目(20120321003-03) (20120321003-03)山西省归国留学基金(No.20100038)资助项目。 (No.20100038)

The effect of impregnation sequence on the surface structure and catalytic performance of CuCe/AC (Activated carbon) (by adding rare earth Ce promoter to Cu/AC) catalyst was studied for gas-phase oxidative carbonylation of methanol to dimethyl carbonate. The active component content, surface dispersion and valence state of as-prepared catalysts were characterized by X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), H₂-temperature programmed reduction(H₂-TPR), High resolution transmission electron microscope (HR-TEM). The results show that Ce promoter plays a key role for active component Cu to disperse on the surface of activated carbon in CuCe/AC catalyst prepared by co-impregnation. The Cu components are difficult to be reduced and difficult to contact with reactant molecules for CuCe/AC catalyst prepared by first impregnation with Cu and then with Ce because part of Cu components are covered by Ce impregnation leading to the decrease of catalytic activity. For CuCe/AC catalyst prepared by first impregnation with Ce and then with Cu, the Ce and Cu components interact with each other, resulting in an optimal catalytic performance because of a more uniform dispersion of Cu (0) and Cu(Ⅰ) species on the surface of the catalyst. The space time yield and selectivity of dimethyl carbonate are 142 mg·g^-1·h^-1 and 85%, respectively.
- Ce promoter;impregnation sequence;Cu/AC catalyst;oxidative carbonylation
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沈阳化工大学材料科学与工程学院沈阳 110142