Study on the catalytic synthesis of diethyl carbonate from CO and ethyl nitrite over supported Pd catalysts

Study on the catalytic synthesis of diethyl carbonate from CO and ethyl nitrite over supported Pd catalysts
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DOI:
10.1016/j.catcom.2004.09.013
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发表时间:
2004-12
影响因子:
3.7
通讯作者:
Xinbin Ma;Mingming Fan;Pingbo Zhang
Xinbin Ma;Mingming Fan;Pingbo Zhang
中科院分区:
化学3区
文献类型:
--
作者:
Xinbin Ma;Mingming Fan;Pingbo Zhang

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在常压连续流微型固定床反应器中,以一氧化碳和亚硝酸乙酯为原料气相合成碳酸二乙酯。与其他二元催化剂体系相比,PdCl2-CuCl2 /AC(活性炭)催化剂表现出更好的催化活性。适宜的pd负载量为2.0 wt%左右,添加LaCl3、CeCl3、PrCl3有利于提高DEC的收率和选择性。考察了不同反应参数对DEC收率和选择性的影响。考虑到DEC的产生和CO的转化,最佳反应温度为378 ~ 388 K,适宜的气体时空速(GHSV)范围为2500 ~ 3000 h−1。催化活性的最佳CO/C2H5ONO摩尔比为1/1。考察了PdCl2-CuCl2 /AC催化剂和PdCl2-CuCl2 - cecl3 /AC催化剂的稳定性。通过XRD分析,探讨了催化剂失活的可能原因。
A vapor phase synthesis of diethyl carbonate (DEC) from carbon monoxide and ethyl nitrite (EN) was studied in a continuous flow micro fixed-bed reactor at atmospheric pressure. PdCl2–CuCl2/AC (activated carbon) catalyst exhibited better catalytic activity compared with other binary catalyst systems. The suitable Pd-loading is about 2.0 wt%, and some additives (LaCl3, CeCl3, PrCl3) are benefit for the DEC yield and selectivity. Influences of various reaction parameters on the DEC yield and selectivity were tested. The optimum reaction temperature lies in 378–388 K and the suitable gas hourly space velocity (GHSV) range is 2500–3000 h−1considering both factors of DEC production and CO conversion. An optimum CO/C2H5ONO mole ratio exists for catalytic activity, which is about 1/1. The stability of PdCl2–CuCl2/AC catalyst and PdCl2–CuCl2–CeCl3/AC catalyst was also investigated. The possible reason of the deactivation behavior of catalysts was discussed with the help of XRD.