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CuY Zeolite Catalysts Prepared by Ultrasonication-assisted Ion-exchange for Oxidative Carbonylation of Methanol to Dimethyl Carbonate
Ultrasonics Sonochemistry ( IF 8.4 ) Pub Date : 2018-02-07 , DOI: 10.1016/j.ultsonch.2018.02.013
Je-Min Woo , Jung Yoon Seo , Hyunuk Kim , Dong-Ho Lee , Young Cheol Park , Chang-Keun Yi , Yeong Seong Park , Jong-Ho Moon

The influence of ultrasonication treatment on the catalytic performance of CuY zeolite catalysts was investigated for the liquid-phase oxidative carbonylation of methanol to dimethyl carbonate (DMC). The deammoniation method of NH4Y into HY zeolites was optimized and characterized by elemental analyzer, derivative thermogravimetry, Brunauer−Emmett−Teller (BET) analyzer, and powder X-ray diffractometry, revealing that the HY zeolite deammoniated at 400 °C presented the highest surface area, complete ammonium/proton ion exchange, and no structure collapse, rendering it the best support from all the prepared zeolites. CuY zeolites were prepared via aqueous phase ion exchange with the aid of ultrasonication. Upon ultrasonication, the Cu+ active centers were uniformly dispersed in the Y zeolites, penetrating the core of the zeolite particles in a very short time. In addition to enhancing the Cu dispersity, the ultrasonication treatment influenced the BET surface area, acid amount, Cu+/Cu2+ ratio, and also had a relatively small impact on the Cu loading. Consequently, adequate exposure to ultrasonication was able to increase the conversion rate of methanol into dimethyl carbonate up to 11.4% with a comparable DMC selectivity of 23.7%. This methanol conversion is 2.65 times higher than that obtained without the ultrasonication treatment.



中文翻译:

超声辅助离子交换制备CuY沸石催化剂催化甲醇氧化羰基化合成碳酸二甲酯

研究了超声处理对CuY沸石催化剂催化性能的影响,该反应用于甲醇液相氧化羰基化为碳酸二甲酯(DMC)。通过元素分析仪,导数热重分析仪,Brunauer-Emmett-Teller(BET)分析仪和粉末X射线衍射仪对NH 4 Y脱氨方法进行了优化和表征,揭示了在400°C脱氨的HY沸石具有以下特点:最大的表面积,完全的铵/质子离子交换,并且没有结构崩溃,使其成为所有制备的沸石的最佳载体。通过水相离子交换借助于超声来制备CuY沸石。超声处理后,Cu +活性中心均匀地分散在Y沸石中,在很短的时间内穿透沸石颗粒的核。超声处理除了提高Cu的分散性外,还影响BET表面积,酸含量,Cu + / Cu 2+比率,并且对Cu的负载量影响相对较小。因此,充分暴露于超声处理能够将甲醇转化为碳酸二甲酯的转化率提高至11.4%,而DMC的选择性为23.7%。该甲醇转化率是未经超声处理获得的甲醇转化率的2.65倍。

更新日期:2018-02-08
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