无模板剂法合成过渡金属修饰的ZSM-5及催化氧化苯甲醇
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- 英文论文题名：Preparation of metal-ZSM-5 without organic template and catalytic oxidation of benzyl alcohol
- 论文作者：刘献锋 ; 杨福 ; 林伟 ; 孔岩
- 英文论文作者：Xian-feng Liu ; Fu Yang ; Wei Lin ; Yan Kong ; State Key Laboratory of Materials-Oriented Chemical Engineering ; College of Chemistry and Chemical Engineering ; Nanjing Tech University ; Department of Environment and Technology ; Nanjing Institute of Technology
- 年：2016
- 作者机构：南京工业大学化学化工学院;南京工程学院环境工程学院;
- 论文关键词：过渡金属 ; ZSM-5 ; 催化氧化 ; 苯甲醇 ; 苯甲醛
- 会议召开时间：2016-07-01
- 会议录名称：中国化学会第30届学术年会摘要集-第三十二分会： 多孔功能材料
- 语种：中文
- 分类号：O621.251
- 学会代码：ZGHY
- 会议名称：中国化学会第30届学术年会-第三十二分会 ; 多孔功能材料
- 会议地点：中国辽宁大连
- 主办单位：中国化学会
- 学会名称：中国化学会
- 页数：1
- 文件大小：266k
- 原文格式：D
- 会议级别：全国
摘要
不使用有机模板剂,在pH为1的水溶液中,用硝酸锰、硝酸铜、硫酸氧钒、硫酸钛等过渡金属盐和正硅酸四乙酯(TEOS)进行酸性共水解、碱性陈化24 h和180 °C水热晶化72 h,制得一系列过渡金属修饰的高结晶度的ZSM-5沸石(M-ZSM-5)。紫外漫反射证实:酸性水解时,金属离子和TEOS共同水解生成四配位结构M-O-Si键,金属原子成功进入到沸石骨架。而常规方法需要较高的碱性环境,金属离子形成氢氧化物沉淀,不能进入沸石骨架。不经过550 °C的高温焙烧,避免了沸石表面金属原子的氧化,降低了M-ZSM-5的制备成本。硅和铝的比例、金属的掺杂量、晶化温度和晶化时间明显影响ZSM-5沸石的晶化过程。V-ZSM-5和30%的过氧化氢分别作为催化剂和氧化剂,不使用有机溶剂,催化氧化苯甲醇,在80 °C反应6 h,苯甲醇的转化率48%,选择性96%。
Without organic template,a series of Mn~(2+)、 Cu~(2+)、 VO~(2+)、 Ti~(4+) was incorporated into framework of ZSM-5 by using three procedure including the co-hydrolysis of TEOS and metal salts in aqueous acid solution(pH=1),aging at 20 ℃ and crystallizing in autoclave at 180 ℃ for 72 h.The formation of metal-O-Si bond in the acid co-hydrolysis was demonstrated by Uv-vis.Neither needing organic template nor calcination at high temperature,the surface metal atom of M-ZSM-5 avoided oxidation to its higher chemical valence.The molar ratio of Si/Al,the content of metal,crystalline temperature and time obviously effect on the morphology and the relative crystalline of M-ZSM-5.Applied in the catalytic oxidation of benzyl alcohol at 80 ℃ for 6 h,V-ZSM-5 showed the best catalytic performance with 48%benzyl alcohol conversion and 96%selectivity of benzaldehyde.
Without organic template,a series of Mn~(2+)、 Cu~(2+)、 VO~(2+)、 Ti~(4+) was incorporated into framework of ZSM-5 by using three procedure including the co-hydrolysis of TEOS and metal salts in aqueous acid solution(pH=1),aging at 20 ℃ and crystallizing in autoclave at 180 ℃ for 72 h.The formation of metal-O-Si bond in the acid co-hydrolysis was demonstrated by Uv-vis.Neither needing organic template nor calcination at high temperature,the surface metal atom of M-ZSM-5 avoided oxidation to its higher chemical valence.The molar ratio of Si/Al,the content of metal,crystalline temperature and time obviously effect on the morphology and the relative crystalline of M-ZSM-5.Applied in the catalytic oxidation of benzyl alcohol at 80 ℃ for 6 h,V-ZSM-5 showed the best catalytic performance with 48%benzyl alcohol conversion and 96%selectivity of benzaldehyde.
引文
[1]Gu,J.;Zhang M J.;Wu Y J.;Wang,J.J.Mater.Chem.A,2013,(1):2453-2460.