High hydrothermal stability of Cu-SAPO-34 catalysts for the NH3-SCR of NOx

High hydrothermal stability of Cu-SAPO-34 catalysts for the NH3-SCR of NOx
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用于 NOx NH3-SCR 的 Cu-SAPO-34 催化剂的高水热稳定性

DOI:
10.1016/j.cej.2016.02.086
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发表时间:
2016-06-15
影响因子:
15.1
通讯作者:
He, Hong
He, Hong
中科院分区:
工程技术1区
文献类型:
--
作者:
Niu, Can;Shi, Xiaoyan;He, Hong

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研究了焙烧温度、铜源以及共模板剂含量对一锅水热合成法制备的Cu - SAPO - 34催化剂的活性和水热稳定性的影响。适宜的焙烧温度对Cu - SAPO - 34催化剂的脱硝活性很重要。所得凝胶中铜源和共模板剂的量会影响最终Cu - SAPO - 34的铜负载量和结晶度。较好的是,在750℃下对铜负载量约为3.44%的Cu - SAPO - 34催化剂进行16小时的水热处理,由于氧化铜迁移为孤立的Cu²⁺,同时保持了结晶度和酸性,使得氨选择性催化还原(NH₃ - SCR)活性略有提高。此外,在800℃下老化16小时的催化剂在225℃至400℃时保持了>90%的氮氧化物转化率,并且在如此苛刻的处理后,Cu - SAPO - 34中的结晶度、活性Cu²⁺物种和酸性并未完全被破坏。同时,对新鲜的和老化的Cu - SAPO - 34样品进行了动力学分析,结论与氨选择性催化还原测试、氢气程序升温还原(H₂ - TPR)和氨程序升温脱附(NH₃ - TPD)结果一致。(C)2016爱思唯尔有限公司。保留所有权利。
The effects of calcination temperature, Cu source and co-template contents on the activity and hydrothermal stability of Cu-SAPO-34 catalysts prepared by the one-pot hydrothermal synthesis method were investigated. Appropriate calcination temperature was important for the deNOx activity of Cu-SAPO-34 catalyst. The amount of Cu source and co-template in the resulting gel could impact the Cu loading and the crystallization of the final Cu-SAPO-34. Preferably, hydrothermal treatment of the Cu-SAPO-34 catalyst with Cu loading ca. 3.44% at 750 degrees C for 16 h increased the NH3-SCR activity slightly due to migration of CuO to isolated Cu2+ and the maintenance of the crystallinity as well as the acidity. Moreover, the catalyst aged at 800 degrees C for 16 h maintained >90% NOx conversion from 225 to 400 degrees C, and the crystallinity, active Cu2+ species and acidity in Cu-SAPO-34 were not destroyed completely after such harsh treatment. Meanwhile, kinetic analysis over fresh and aged Cu-SAPO-34 samples were conducted and the conclusion were in agreement with the NH3-SCR tests, H-2-TPR and NH3-TPD results. (C) 2016 Elsevier B.V. All rights reserved.