魏艳飞,管斌,吴星泽,等.水热老化温度和时长对Cu-SSZ-13分子筛催化剂性能和理化特性影响的研究[J].内燃机工程,2022,43(4):100-108.
水热老化温度和时长对Cu-SSZ-13分子筛催化剂性能和理化特性影响的研究
Study on the Effects of Hydrothermal Aging Temperatures and Hours on the Performance and Physicochemical Properties of Cu-SSZ-13 Zeolite Catalyst
DOI:10.13949/j.cnki.nrjgc.2022.04.012
关键词:分子筛  水热老化  氧化还原性能  选择性催化还原
Key Words:zeolite  hydrothermal aging  redox performance  selective catalytic reduction(SCR)
基金项目:国家自然科学基金项目(52076134,51676127,51436005,51176118)
作者单位E-mail
魏艳飞* 上海交通大学 动力机械与工程教育部重点实验室上海 200240 weiyanfei@sjtu.edu.cn 
管斌* 上海交通大学 动力机械与工程教育部重点实验室上海 200240 guanbin@sjtu.edu.cn 
吴星泽 上海交通大学 动力机械与工程教育部重点实验室上海 200240  
刘子乾 上海交通大学 动力机械与工程教育部重点实验室上海 200240  
林赫 上海交通大学 动力机械与工程教育部重点实验室上海 200240  
黄震 上海交通大学 动力机械与工程教育部重点实验室上海 200240  
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摘要:通过离子交换法合成具有优异催化活性的Cu-SSZ-13分子筛催化剂,分别在不同的温度和时长条件下对其进行水热老化处理。比较了数个不同老化条件下的催化剂的NOx催化性能、NH3吸附性能,同时通过Brunauer–Emmett–Teller(BET)方法、X射线衍射(X-ray diffraction, XRD)和H2程序升温还原(temperature programmed reduction, TPR)方法对这些催化剂的孔特性、晶体结构和铜位点的数量分布等进行探究。测试结果发现水热老化会引起催化剂催化活性、催化温度窗口范围的全面下降,并导致气体吸附性能的下降和氧化还原性能的大幅改变。进一步研究发现水热老化引起晶体结构和孔结构的破坏,并导致大量活性位点的转变和流失。制备的Cu-SSZ-13分子筛催化剂总体上具有良好的耐久性,对老化温度的敏感性比老化时间更高。
Abstract:Cu-SSZ-13 zeolite catalysts with excellent catalytic activity were synthesized by ion-exchange method and subjected to hydrothermal aging at different temperatures and durations, respectively. The NOx catalytic performance and NH3 adsorption performance of the catalysts under different aging conditions were compared, and the pore properties of these catalysts were also investigated by the Brunauer–Emmett–Teller(BET) method, X-ray diffraction(XRD) and H2 temperature programmed reduction(TPR) to investigate the pore properties, crystal structure and the number distribution of copper sites of these catalysts. Test results show that hydrothermal aging causes an overall decrease in catalytic activity and catalytic temperature window range, as well as a decrease in gas adsorption performance and a significant change in redox performance. Further studies reveal that hydrothermal aging causes the destruction of crystal structure and pore structure, and leads to the transformation and loss of a large number of active sites. The Cu-SSZ-13 zeolite catalysts have good durability in general and are more sensitive to aging temperature than aging time.
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