Active Center Changed: Disproportionation Mechanism for Preparing Dimethyldichlorosilane Catalyzed by Core(4T)-shell Catalyst

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Dimethyldichlorosilane is a basic raw material for preparing a variety of organosilicon materials. The disproportionation method to synthesize it can solve the problem brought by direct synthesis. The B3LYP/6-31G and MP2/6-311++ G(3df, 2pd) methods were used to calculate the mechanism of the reaction catalyzed by localized core(4T)-shell catalyst. The energy barriers of the rate-determining steps of the main reaction at different active sites 1(5)～4 in the HZSM-5(4T)@γ-Al2O3 catalyst were 165.88, 129.99, 118.66 and 145.55 kJmol-1, respectively, and those in the side reaction are 131.98, 146.28, 146.53 and 164.17 kJmol-1, separately. The active site No. 3 was the easiest one to participate in the catalytic reaction. The energy barriers of the rate-determining steps of the main reaction catalyzed by the AlCl3/HZSM-5(4T)@γ-Al2O3 catalyst, involving configurations a and b, are 105.12 and 110.39 kJmol-1, respectively, and those of the side reaction are 144.26 and 159.55 kJmol-1, respectively. Both configurations produced dimethyldichlorosilane mainly, and configuration a is easier to catalyze the reaction process. And according to the bond order and locality analysis, the catalytic activity order was: configuration a > configuration b. This conclusion matched with the reaction energy barrier analysis. The AlCl3/HZSM-5(4T)@γ-Al2O3 catalyst had a better catalytic activity than HZSM-5(4T)@γ-Al2O3. The active center of the reaction system of HZSM-5(4T)@γ-Al2O3 was proton, Bronsted acidic center, and that of AlCl3/HZSM-5@γ-Al2O3 could be Lewis acidic center. The source of the Lewis acidic center was the multi-center bond formed by the delocalization of peripheral electrons of the atoms. The frontier orbital theory confirmed the mechanism and good selectivity of the reaction.

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	徐文媛
	况熙
	颜菲
	汪焱
	李素颖
	胡林

关键词 ： core-shell catalyst, Bronsted/Lewis acidic center, AlCl3/HZSM-5(4T)@γ-Al2O3, density functional theory (DFT)

Abstract：

Key words： core-shell catalyst Bronsted/Lewis acidic center AlCl3/HZSM-5(4T)@γ-Al2O3 density functional theory (DFT)

收稿日期: 2019-07-19 出版日期: 2020-06-10

基金资助:This work was financially supported by the National Natural Science Foundation of China (Nos. 21563011 and 21872049)

通讯作者: xwyktz@163.com E-mail: xwyktz@163.com

引用本文:

徐文媛;况熙;颜菲;汪焱;李素颖;胡林. Active Center Changed: Disproportionation Mechanism for Preparing Dimethyldichlorosilane Catalyzed by Core(4T)-shell Catalyst[J]. 结构化学, 2020, 39(6): 1146-1156.
XU Wen-Yuan; KUANG Xi;YAN Fei;WANG Yan;LI Su-Ying;HU Lin. Active Center Changed: Disproportionation Mechanism for Preparing Dimethyldichlorosilane Catalyzed by Core(4T)-shell Catalyst. CHINESE JOURNAL OF STRUCTURAL CHEMISTRY, 2020, 39(6): 1146-1156.

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http://manu30.magtech.com.cn/jghx/CN/ 或 http://manu30.magtech.com.cn/jghx/CN/Y2020/V39/I6/1146

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