催化学报

催化学报 ›› 2012, Vol. 33 ›› Issue (1): 92-105.DOI: 10.1016/S1872-2067(10)60280-X

• 研究论文 • 上一篇    下一篇

由新型铜胺络合物模板剂设计合成活性优异的 Cu-SSZ-13 分子筛

任利敏 2, 张一波 3, 曾尚景 2, 朱龙凤 2, 孙琦 1, 张海燕 2, 杨承广 2, 孟祥举 1, 杨向光 3, 肖丰收 1,*   

  1. 1 浙江大学催化研究所, 浙江杭州 310028; 2 吉林大学无机合成与制备国家重点实验室, 吉林长春 130012; 3 中国科学院长春应用化学研究所, 吉林长春 130022
  • 收稿日期:2011-08-04 修回日期:2011-09-12 出版日期:2012-01-16 发布日期:2015-05-26

Design and Synthesis of a Catalytically Active Cu-SSZ-13 Zeolite from a Copper-Amine Complex Template

REN Limin2, ZHANG Yibo3, ZENG Shangjing2, ZHU Longfeng2, SUN Qi1, ZHANG Haiyan2, YANG Chengguang2, MENG Xiangju1, YANG Xiangguang3, XIAO Feng-Shou1,*   

  1. 1Department of Chemistry, Zhejiang University, Hangzhou 310028, Zhejiang, China; 2State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, Jilin University, Changchun 130012, Jilin, China; 3Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun 130022, Jilin, China
  • Received:2011-08-04 Revised:2011-09-12 Online:2012-01-16 Published:2015-05-26

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61

摘要： 以低廉的铜胺络合物为新型模板剂, 成功地合成了含铜的 SSZ-13 沸石分子筛 (Cu-ZJM-1). 在合成过程中, 铜胺络合物既是模板分子, 又是催化活性组分铜物种的直接来源. 理论计算表明, 该模板分子的构型与尺寸恰好与构成 SSZ-13 分子筛结构的 CHA 笼相匹配, 因而可以成功地导向该沸石分子筛结构. 采用 X 射线衍射、扫描电镜、氮气吸附、红外、紫外-可见吸收光谱、差热-热重分析、氨气程序升温脱附及氢气程序升温还原等手段对样品的性质及模板分子的状态进行了系统表征. 结果表明, 所制 Cu-ZJM-1 样品为结晶度很高的 SSZ-13 沸石结构, 硅铝比和铜负载量可调且铜处于高分散状态, 在 NH3 选择催化还原氮氧化物反应中表现出优异的催化性能.

关键词: 新型模板剂, 铜胺络合物, 设计合成, Cu-SSZ-13, 理论计算, 氨还原消除氮氧化物反应

Abstract: The modern synthesis of zeolites typically uses organic structure-directing agents. Therefore, the developing of new templates is part of zeolite research. The design and synthesis of Cu-SSZ-13 using a novel template of a low-cost copper amine complex (Cu2+ coordinated with tetraethylenepentamine) were reported, where the copper amine complex is both a template for synthesizing the SSZ-13 structure and a source of copper species in the zeolite. The calculated size of the complex (0.728 nm ´ 0.922 nm) matches well with the CHA cages (0.73 nm ´ 1.2 nm), which are the building units of the SSZ-13 zeolite. Various techniques were used to investigate the chemical and physical properties of the synthesized zeolite. The results showed that the sample has the SSZ-13 zeolite structure, high crystallinity, adjustable Si/Al ratios, and controllable copper loading. Catalytic tests using the selective catalytic reduction of NOx with NH3 showed that the Cu-SSZ-13 was a superior catalyst, and it can be important for the abatement of environmentally harmful NOx.

Key words: novel template, copper amine complex, designed synthesis, Cu-SSZ-13, theoretical calculation, selective catalytic reduction of NOx with NH3