介孔硅铝酸盐的合成及其在傅克反应中的催化性能

引用本文: 李莎, 周慧, 范杰, 肖丽萍. 介孔硅铝酸盐的合成及其在傅克反应中的催化性能[J]. 无机化学学报, 2013, 29(5): 896-902. doi: 10.3969/j.issn.1001-4861.2013.00.160 shu

Citation: LI Sha, ZHOU Hui, FAN Jie, XIAO Li-Ping. Synthesis of Mesoporous Aluminum Silicates and Their Catalytic Activity in Friedel-Crafts Alkylation Reaction[J]. Chinese Journal of Inorganic Chemistry, 2013, 29(5): 896-902. doi: 10.3969/j.issn.1001-4861.2013.00.160 shu

介孔硅铝酸盐的合成及其在傅克反应中的催化性能

通讯作者: 肖丽萍,E-mail:lpxiao@zju.edu.cn

基金项目:
国家自然科学基金(No.21271153) (No.21271153)

浙江省创新团队项目(No.2012R10014-06) (No.2012R10014-06)

吉林大学无机合成与制备化学国家重点实验室开放基金 (2012-03)资助项目。 (2012-03)

摘要: 采用溶胶凝胶法合成了一系列有序性好且酸性较强的介孔硅铝酸盐材料。利用X射线粉末衍射(XRD)、透射电镜(TEM)、²⁷Al核磁共振(²⁷Al NMR)、氨气程序升温脱附(HN₃-TPD)及吡啶吸附红外光谱(Py-FT-IR)对制备的介孔硅铝酸盐材料的结构和性能进行表征,并考察了材料在苯甲醚和苯甲醇的傅克烷基化反应中的催化活性。实验结果表明:合成过程中,表面活性剂的用量、硅铝物质的量之比会影响材料结构的有序性,醋酸用量对材料结构有序性影响很小;进一步研究结果表明,n_Si/n_Al比会影响材料的酸催化活性,当n_Si/n_Al=10时材料的酸催化活性最高。氨气程序升温脱附和吡啶吸附红外光谱表明n_Si/n_Al=10的材料含有最多的B酸酸量。

关键词:

介孔材料;硅铝酸盐;酸催化;傅克反应

English

Synthesis of Mesoporous Aluminum Silicates and Their Catalytic Activity in Friedel-Crafts Alkylation Reaction

1.
Department of Chemistry, Zhejiang University, Hangzhou 310027, China

Corresponding author: 肖丽萍,E-mail:lpxiao@zju.edu.cn

Received Date: 16 December 2012
Fund Project:
国家自然科学基金(No.21271153)

浙江省创新团队项目(No.2012R10014-06)

吉林大学无机合成与制备化学国家重点实验室开放基金 (2012-03)资助项目。

Abstract: Ordered mesoporous aluminum silicates with strong acid sites were synthesized by sol-gel method. The resulted materials' structures were characterized by XRD, TEM, ²⁷Al NMR, NH₃-TPD and Py-FT-IR. The amount of surfactant and the Si/Al mole ratio would both affect the materials' meso-structure; while, the amount of HAc has little effect on the structure. TEM analysis confirmed that these aluminum silicates with different Si/Al mole ratios have an ordered 2D hexagonal regularity. Friedel-Crafts alkylation reaction of anisole and benzyl alcohol was used as the probe reaction to detect the acidic properties of these aluminum silicates. The Si/Al mole ratio played an important role in catalytic activity and the aluminum silicates with n_Si/n_Al=10 showed the best acid catalytic activity. NH₃-TPD and Py-FT-IR suggested that the aluminum silicates with n_Si/n_Al=10 had much more Brönsted acidic sites than that of other Si/Al ratios.

Key words:

mesoporous materials;aluminum silicate;acid catalysis;Friedel-Crafts alkylation reaction

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通讯作者: 陈斌, bchen63@163.com

1.
沈阳化工大学材料科学与工程学院沈阳 110142

介孔硅铝酸盐的合成及其在傅克反应中的催化性能

通讯作者: 肖丽萍,E-mail:lpxiao@zju.edu.cn

English

Synthesis of Mesoporous Aluminum Silicates and Their Catalytic Activity in Friedel-Crafts Alkylation Reaction

Corresponding author: 肖丽萍,E-mail:lpxiao@zju.edu.cn

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

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CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

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通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

介孔硅铝酸盐的合成及其在傅克反应中的催化性能

通讯作者: 肖丽萍,E-mail:lpxiao@zju.edu.cn

English

Synthesis of Mesoporous Aluminum Silicates and Their Catalytic Activity in Friedel-Crafts Alkylation Reaction

Corresponding author: 肖丽萍,E-mail:lpxiao@zju.edu.cn

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南： 你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

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通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

CCS Chemistry：颜徐州、鲍哲南：你的皮肤可能是一片SPMs