Liquid-state 29Si NMR Investigation on Ammonia-catalyzed Hydrolysis Kinetics of a Mixture of Tetraethoxysilane and Dimethyldiethoxysilane

Acta Chimica Sinica ›› 2005, Vol. 63 ›› Issue (23): 2103-2111. Next Articles

液态²⁹SiNMR研究TEOS/DDS混合体系的氨催化水解动力学

孙先勇^1,2, 徐耀¹, 徐武军^1,2, 吴东¹, 孙予罕¹, 杨永霞^2,3, 袁汉珍³, 邓风³

1. 中国科学院山西煤炭化学研究所, 煤转化国家重点实验室, 太原, 030001;
2. 中国科学院研究生院, 北京, 100039;
3. 中国科学院武汉物理与数学研究所, 波谱与原子分子物理国家重点实验室, 武汉, 430079

投稿日期:2005-05-30 修回日期:2005-08-11 发布日期:2014-02-14
通讯作者: 孙予罕,E-mail:yhsun@sxicc.ac.cn E-mail:yhsun@sxicc.ac.cn
作者简介:孙予罕,E-mail:yhsun@sxicc.ac.cn
基金资助:
国家自然科学重点基金(No.20133040)资助项目.

Liquid-state ²⁹Si NMR Investigation on Ammonia-catalyzed Hydrolysis Kinetics of a Mixture of Tetraethoxysilane and Dimethyldiethoxysilane

SUN Xian-Yong^1,2, XU Yao¹, XU Wu-Jun^1,2, WU Dong¹, SUN Yu-Han¹, YANG Yong-Xia^2,3, YUAN Han-Zhen³, DENG Feng³

1. State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan 030001;
2. Graduate School of the Chinese Academy of Sciences, Beijing 100039;
3. State Key Laboratory of Magnetic Resonance with Atomic and Molecular Physics, Institute of Physics and Mathematics, Chinese Academy of Sciences, Wuhan 430071

Received:2005-05-30 Revised:2005-08-11 Published:2014-02-14

Abstract

In situ liquid-state ²⁹Si NMR was used to follow the ammonia-catalyzed hydrolysis and conden-sation of tetraethoxysilane (TEOS) and dimethyldiethoxysilane (DDS) mixed systems with methanol used as solvent. By varying the molar ratio of TEOS, DDS, water and ammonia in initial solutions, the individual hydrolysis rate constants for TEOS and DDS in mixture were calculated as well as the corresponding reac-tive orders through fitting the concentration curves as functions of time for each intermediate species, which is similar to their individual systems, and under ammonia catalysis, the hydrolysis reaction orders of TEOS and DDS in mixed systems all retained the first-order. The hydrolysis rate constant of TEOS in mixed sys-tems was larger compared with TEOS in single precursor systems. Meanwhile, the hydrolysis rate constant of DDS in mixed system was smaller than the rate constant of DDS in the single DDS system. Another im-portant result was that the reactive orders of both ammonia and water were increased to different extent for TEOS and DDS in mixed systems. Hydrolysis and condensation kinetics show more compatible hydroly-sis-condensation relative rates between TEOS and DDS. Assisted by the solid ²⁹Si MAS NMR, XPS and SAXS, the obtained hybrid gel shows weak cross-condensation.

Key words: kinetics, sol-gel, hybrid, ²⁹Si NMR, hydrolysis, condensation

Cite this article

SUN Xian-Yong, XU Yao, XU Wu-Jun, WU Dong, SUN Yu-Han, YANG Yong-Xia, YUAN Han-Zhen, DENG Feng. Liquid-state ²⁹Si NMR Investigation on Ammonia-catalyzed Hydrolysis Kinetics of a Mixture of Tetraethoxysilane and Dimethyldiethoxysilane[J]. Acta Chimica Sinica, 2005, 63(23): 2103-2111.

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液态²⁹SiNMR研究TEOS/DDS混合体系的氨催化水解动力学

Liquid-state ²⁹Si NMR Investigation on Ammonia-catalyzed Hydrolysis Kinetics of a Mixture of Tetraethoxysilane and Dimethyldiethoxysilane

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液态29SiNMR研究TEOS/DDS混合体系的氨催化水解动力学