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

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

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 ^1, , 张一波 ^2, , 曾尚景 ^3, , 朱龙凤 ^4, , 孙琦 ^5, , 张海燕 ^6, , 杨承广 ^7, , 孟祥举 ^8, , 杨向光 ^9, , 肖丰收 ^10,

1.吉林大学无机合成与制备国家重点实验室,吉林长春130012

2.中国科学院长春应用化学研究所,吉林长春130022

3.吉林大学无机合成与制备国家重点实验室,吉林长春130012

4.吉林大学无机合成与制备国家重点实验室,吉林长春130012

5.浙江大学催化研究所,浙江杭州310028

6.吉林大学无机合成与制备国家重点实验室,吉林长春130012

7.吉林大学无机合成与制备国家重点实验室,吉林长春130012

8.浙江大学催化研究所,浙江杭州310028

9.中国科学院长春应用化学研究所,吉林长春130022

10.浙江大学催化研究所,浙江杭州310028

基金项目: 国家自然科学基金(20973079;21003107) 国家重点基础研究发展计划(973计划)(2009CB623507)

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

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

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.

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