Citation: LI Yan-Jiao, YAN Li-Fei, ZHENG Hua-Yan, LI Zhong. Effects of Acid Treatment on Pore Structure and Oxidation Carbonylation Performance of CuY Catalysts[J]. Chinese Journal of Inorganic Chemistry, ;2015, (12): 2315-2323. doi: 10.11862/CJIC.2015.313 shu

Effects of Acid Treatment on Pore Structure and Oxidation Carbonylation Performance of CuY Catalysts

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

Corresponding author: LI Zhong,
Received Date: 15 May 2015
Available Online: 19 October 2015
Fund Project: 国家自然科学基金(No.21276169)资助项目。 (No.21276169)

The NaY zeolite with n_Si/n_Al=2.65 was treated by oxalic acid aqueous solutions and used as supports to prepare CuY catalysts by liquid ion exchange for oxidative carbonylation of methanol to dimethyl carbonate (DMC) in atmospheres condition. The NaY zeolites and their corresponding CuY catalysts were characterized intensively by N₂ adsorption-desorption, TEM, XRD, ²⁹Si MAS NMR, NH₃-TPD, Py-FTIR and H₂-TPR. The results revealed that framework aluminum was leached out by acid, resulting in increase of the framework n_Si/n_Al ratio, decrease of the relative crystallinity, and formation of mesopores which are favor for diffusion of the products molecules and significantly affect the catalytic activity. Compared with the untreated sample, CuY catalysts treated by 4 h, 0.2 mol·L^-1 oxalic acid exhibited higher catalytic performance with the increased space-time yield to DMC and conversion of methanol of 184.9 mg·g^-1·h^-1 and 10.2% from 103.6 mg·g^-1 ·h^-1 and 6.3% respectively. It is found the formed mesopores in CuY catalyst enhance the accessibility of Cu active sites by reactants and the diffusion of reactants and products molecules.
- CuY catalysts;oxidative carbonylation;acid treatment;pore structure
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沈阳化工大学材料科学与工程学院沈阳 110142