Citation: Wen-Yuan XU, Xi KUANG, Fei YAN, Yan WANG, Su-Ying LI, Lin HU. Active Center Changed: Disproportionation Mechanism for Preparing Dimethyldichlorosilane Catalyzed by Core(4T)-shell Catalyst[J]. Chinese Journal of Structural Chemistry, ;2020, 39(6): 1146-1156. doi: 10.14102/j.cnki.0254-5861.2011-2538 shu

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

School of Materials Science and Engineering, East China Jiaotong University, Nanchang 330013, China

Corresponding author: Wen-Yuan XU, xwyktz@163.com
Received Date: 19 July 2019
Accepted Date: 8 January 2020

Fund Project: the National Natural Science Foundation of China 21563011the National Natural Science Foundation of China 21872049

Figures(6)

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