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HZSM-5分子筛催化剂脱硫脱硝研究

Studies on HZSM-5 Zeolite Catalysts for Desulfurization and Denitrification

【作者】 刁振恒

【导师】 王承学;

【作者基本信息】 长春工业大学 , 化学工艺, 2011, 硕士

【摘要】 本文对比研究了脱硫脱硝催化剂最佳载体的选取,研究脱硫催化剂V2O5/HZSM-5的最佳钒负载量和助剂改性以及评价,探索脱硝催化剂Ni-Cu-Ce-La-HZSM-5的最佳制备工艺,并且对其进行耐氧性研究以及评价。实验结果表明,脱硫和脱硝的最佳催化剂载体均是Si/Al=25的HZSM-5分子筛;脱硫催化剂V205的最佳负载量为8%;钴和硫酸钾改性的CoO-K2S04-V205/HZSM-5脱硫催化剂具有很好的催化脱硫活性和热稳定性,XRD及TEM分析结果显示,改性前后晶粒没有明显变化,制备分散度都很好。CoO-K2S04-V205/HZSM-5催化剂的部分孔径稍有变大。脱硝催化剂Ni-Cu-Ce-La-HZSM-5的最佳制备工艺为先将载体用硫酸酸化酸化,进行镍的离子交换,经过烘干焙烧后,在进行铜、铈、镧的离子交换时调节pH=7.8,最后烘干焙烧;催化脱硝率随氧气含量的增大而减小,镍、铈、镧的含量越大脱硝催化剂的耐氧性越好。调节pH=7.8不利于Ni2+的负载,但有利于Cu2+, Ce3+, La3+负载到催化剂上。联合反应脱硫脱硝效果好于单独脱硫和脱硝,联合实验NO和SO2最佳脱除率分别达到98.153%和99.416%。

【Abstract】 This article focused on the best carrier of desulfurization and denirification catalysts. The loading and modification of desulfurization catalyst V2O5/HZSM-5 were studied, and the best preparation procedure of denitrification catalyst Ni-Cu-Ce-La-HZSM-5 was investigated.Results showed that the best loading of V2O5 was 8%. CoO-K2S04-V205/HZSM-5 modified by cobalt and potassium sulphate had good activity and thermal stability. XRD and TEM results show modification with CoO, K2SO4 and MoO3 has little impact on the crystalline grain of carrier and catalysts. While the pore volume and pore diameter of CoO-K2SO4-V2O5/HZSM-5 get bigger.And the best preparation procedure of Ni-Cu-Ce-La-HZSM-5 was that HZSM-5 was acidulated by sulfuric acid solution firstly; and nickel ion exchange was implemented secondly; then the pH of the solution was adjusted to 7.8 thirdly when copper, cerium and lanthanum ion exchange was being implemented; and lastly, the catalyst could be produced after being dried and roasted. And acidic condition is conducive for nickel ion exchange, while pH=7.8 is conducive for copper, cerium and lanthanum ion exchange.Compared with technologies for desulfurization and denitrification separately, combined removal reaction is better. When the airspeed is 38.96min-1, the best desulfurization efficiency and denitrication efficiency could be up to 98.153% and 99.416% separately when being experimented combinedly.

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