苯胺类烷基化铜基催化剂稳定性研究
发布时间：2018-07-18 08:09
【摘要】：环保法规的日益严格使清洁汽油成为必然,高辛烷值是清洁汽油的质量要求,添加抗爆剂是提高汽油辛烷值最简单、有效的方法,苯胺类烷基化衍生物是高效、低污染型汽油抗爆剂,铜基催化剂稳定性差是制约该产品工业化生产的主要因素。本论文通过XRD、BET、H2-TPR、TG-DTG等技术手段对新鲜、失活催化剂进行了表征,分析了催化剂的失活原因;探讨了组成、沉淀温度、沉淀pH、焙烧温度、助剂、使用条件等对催化剂稳定性的影响。结果表明,铜基催化剂连续运行400h后,转化率由67.98%降至57.55%,下降了15.34%,铜聚集、烧结、积炭和中毒导致催化剂失活,中毒为主要失活原因。调节制备条件、添加助剂、优化使用条件可改善铜基催化剂的稳定性,铝含量为10%(w)、铜锌比为1:1(mol)、沉淀温度为75℃、沉淀pH为8、焙烧温度为400℃时,制得的催化剂活性组分铜分散良好、稳定性提高,运行400h后转化率由69.16%降至60.22%,下降了12.93%;Ce助剂的添加不仅提高了铜的分散性,也增强了催化剂的抗硫氯中毒性能,催化剂的稳定性得到进一步提高,在Ce含量为6%(w),催化剂稳定性提高最为明显,400h后转化率由72.63%降至65.58%,降低了9.74%;在温度200℃、醇胺比2:1(mol)、空速(WHSV)0.6h-1的条件下反应,催化剂在运行400h时后转化率由73.74%降低到67.36%,下降了8.65%。铜基催化剂的活性、稳定性均得到提高。
[Abstract]:The increasingly strict environmental laws and regulations make clean gasoline inevitable, high octane number is the quality requirement of clean gasoline, adding antiknock agent is the simplest and most effective method to improve gasoline octane number, aniline alkylation derivative is efficient, Low-pollution gasoline antiknock agent and poor stability of copper-based catalyst are the main factors restricting the industrial production of this product. In this paper, the fresh and deactivated catalysts were characterized by XRDX BETH2-TPR-TG-DTG, the reasons of deactivation of the catalysts were analyzed, and the effects of composition, precipitation temperature, pH, calcination temperature, auxiliaries and application conditions on the stability of the catalysts were discussed. The results showed that the conversion rate of Cu-based catalyst decreased from 67.98% to 57.55% after 400 h continuous operation, and decreased 15.34%. Copper aggregation, sintering, carbon deposition and poisoning resulted in deactivation of catalyst, and poisoning was the main cause of deactivation. The stability of copper-based catalysts can be improved by adjusting the preparation conditions, adding additives and optimizing the application conditions. When the Al content is 10% (w), the copper-zinc ratio is 1:1, the (mol), precipitation temperature is 75 鈩，
本文编号：2131278
[Abstract]:The increasingly strict environmental laws and regulations make clean gasoline inevitable, high octane number is the quality requirement of clean gasoline, adding antiknock agent is the simplest and most effective method to improve gasoline octane number, aniline alkylation derivative is efficient, Low-pollution gasoline antiknock agent and poor stability of copper-based catalyst are the main factors restricting the industrial production of this product. In this paper, the fresh and deactivated catalysts were characterized by XRDX BETH2-TPR-TG-DTG, the reasons of deactivation of the catalysts were analyzed, and the effects of composition, precipitation temperature, pH, calcination temperature, auxiliaries and application conditions on the stability of the catalysts were discussed. The results showed that the conversion rate of Cu-based catalyst decreased from 67.98% to 57.55% after 400 h continuous operation, and decreased 15.34%. Copper aggregation, sintering, carbon deposition and poisoning resulted in deactivation of catalyst, and poisoning was the main cause of deactivation. The stability of copper-based catalysts can be improved by adjusting the preparation conditions, adding additives and optimizing the application conditions. When the Al content is 10% (w), the copper-zinc ratio is 1:1, the (mol), precipitation temperature is 75 鈩，
本文编号：2131278
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