自然科学版
陕西师范大学学报(自然科学版)
双碳背景下的稀土催化专刊
MnCu-SSZ-13@CeO2分子筛核壳结构催化剂的合成及其NH3-SCR性能
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王志恒1,2,何丹丹1,刘立成1*
(1 中国科学院 青岛生物能源与过程研究所,山东 青岛 266100;2 中国科学院大学,北京 100049)
刘立成,男,研究员,博士生导师,主要研究方向为多相催化。E-mail: liulc@qibebt.ac.cn
摘要:
通过离子交换和自组装过程制备了具有核壳结构的MnCu-SSZ-13@CeO2分子筛催化剂,并将其应用于NH3-SCR反应。X射线衍射(XRD)、扫描电镜(SEM)和透射电镜(TEM)分析结果表明:该催化剂不仅具有SSZ-13晶体的衍射特征峰,而且出现了明显的CeO2 特征峰。形貌和线扫分析结果进一步表明:CeO2 外壳均匀地包覆于分子筛外表面,构建了较为规整的核壳结构。通过NH3程序升温脱附(NH3-TPD)和H2程序升温还原(H2-TPR)技术对比了不同催化剂的氧化还原能力及表面酸性位点的含量和分布,阐明了包覆CeO2前后催化剂化学性质的变化。催化反应测试结果表明:MnCu-SSZ-13催化剂在200~450 ℃温度范围内的NOx转化率约为85%,而具备核壳结构的MnCu-SSZ-13@CeO2催化剂活性明显提高;当CeO2 质量分数为3.16%时,MnCu-SSZ-13@CeO2在250~500 oC范围内实现了接近100%的NOx转化率。耐硫测试结果表明:当CeO2 质量分数为3.16%、温度为300 ℃、反应原料中SO2体积分数为0.01%时,核壳结构催化剂具有良好的耐硫性能。
关键词:
MnCu-SSZ-13;CeO2包覆;脱硝活性;耐硫性
收稿日期:
2021-09-21
中图分类号:
TB565.1
文献标识码:
A
文章编号:
1672-4291(2022)02-0051-08
基金项目:
国家自然科学基金(21676288)
Doi:
10.15983/j.cnki.jsnu.2022007
Synthesis of MnCu-SSZ-13@CeO2 catalyst with core-shell structure using for NH3-SCR reaction
WANG Zhiheng1,2, HE Dandan1, LIU Licheng1*
(1 Qingdao Institute of Bioenergy and Bioprocess Technology, Chinese Academy of Sciences, Qingdao 266100, Shandong, China; 2 University of Chinese Academy of Sciences, Beijing 100049, China)
Abstract:
MnCu-SSZ-13@CeO2 zeolite catalyst with core-shell structure was prepared by ion exchange and self-assembly methods. The structure and morphology of the catalyst were studied by X-ray diffraction (XRD), scanning electron microscope (SEM) and transmission electron microscope (TEM). The results showed that the characteristic peaks of both SSZ-13 zeolite and CeO2 were observed in the XRD spectrum of MnCu-SSZ-13@CeO2 catalyst, and the CeO2 shell was uniformly coated on the outer surface of the zeolite catalyst. Furthermore, the redox capacity as well as the content and distribution of the surface acid sites were analyzed by H2 temperature programmed reduction (H2-TPR) and NH3 temperature programmed desorption (NH3-TPD) techniques. The evolution of chemical properties of the catalysts before and after CeO2 coating was clarified. The catalytic activity and sulfur resistance of the catalysts in NH3-SCR reaction were investigated. The results showed that the NOx conversion rate of uncoated MnCu-SSZ-13 catalyst in NH3-SCR reaction was about 85% between 200 ℃ and 450 ℃, while the catalytic activity was significantly enhanced after CeO2 coating. When the mass fraction of CeO2 was 3.16%, MnCu-SSZ-13@CeO2 catalyst achieved nearly 100% of NOx conversion rate between 200 ℃ and 500 ℃. The MnCu-SSZ-13@CeO2 catalyst also showed good sulfur resistance at 300 oC when the feeding reactant contained SO2 of 0.01%(volumn fraction).
KeyWords:
MnCu-SSZ-13; CeO2 coating; denitration activity; sulfur resistance