Citation: Yuchun Wang, Huayan Zheng, Zhong Li. Effect of NH₄⁺ exchange on CuY catalyst for oxidative carbonylation of methanol[J]. Chinese Journal of Catalysis, ;2016, 37(8): 1403-1412. doi: 10.1016/S1872-2067(16)62490-7 shu

Effect of NH₄⁺ exchange on CuY catalyst for oxidative carbonylation of methanol

a. Key Laboratory of Coal Science and Technology of Ministry of Education and Shanxi Province, Taiyuan University of Technology, Taiyuan 030024, Shanxi, China;
b. Department of Applied Chemistry, Yuncheng University, Yuncheng 044000, Shanxi, China

Received Date: 4 May 2016
Revised Date: 15 June 2016

Fund Project: This work was supported by the National Natural Science Foundation of China (21276169).

NaY and ion exchanged NaNH₄Y zeolite with NH₄NO₃ were used as the support to prepare CuY catalysts by a high temperature anhydrous interaction between the support and copper (II) acetylacetonate Cu(acac)₂. The catalysts were used for the oxidative carbonylation of methanol to dimethyl carbonate (DMC) at atmospheric pressure. The textural and acidic properties of NaNH₄Y zeolite and the CuY catalysts were investigated by X-ray diffraction, scanning electron microscopy, N₂ adsorption-desorption, temperature programmed reduction of H₂, X-ray photoelectron spectroscopy and temperature programmed desorption of NH₃. With increasing NH₄NO₃ concentration, the NH₄⁺ exchange degree increased while the crystallinity of the zeolite remained intact. Crystalline CuO was formed when the NH₄⁺ exchange degree of NaNH₄Y was low, and the corresponding CuY catalyst showed low catalytic activity. With increasing of the NH₄⁺ exchange degree of NaNH₄Y, the content of surface bound Cu⁺ active centers increased and the catalytic activity of the corresponding CuY catalyst also increased. The surface bound Cu⁺ content reached its maximum when the NH₄⁺ exchange degree of NaNH₄Y reached towards saturation. The CuY exhibited optimal catalytic activity with 267.3 mg/(g·h) space time yield of DMC, 6.9% conversion of methanol, 68.5% selectivity of DMC.
- High temperature anhydrous interaction,
- NH₄⁺ exchange degree,
- CuY catalyst,
- Oxidative carbonylation,
- Dimethyl carbonate
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沈阳化工大学材料科学与工程学院沈阳 110142

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Effect of NH₄⁺ exchange on CuY catalyst for oxidative carbonylation of methanol