TY - JOUR
T1 - Approach to generating the right active phase in the “Direct” synthesis of trimethoxysilanes using the CuCl-Cu2O catalyst
AU - Su, Kai
AU - Ji, Yongjun
AU - Zhou, Xiwen
AU - Jiang, Xingyu
AU - Li, Huifang
AU - Zhu, Yongxia
AU - Li, Jing
AU - Liu, Hezhi
AU - Xiao, Junping
AU - Zhong, Ziyi
AU - Su, Fabing
N1 - Publisher Copyright:
© 2021 Elsevier B.V.
Copyright:
Copyright 2021 Elsevier B.V., All rights reserved.
PY - 2021/4/1
Y1 - 2021/4/1
N2 - The “direct” synthesis of trimethoxysilane (M3) by the reaction of Si with methanol over the CuCl catalyst often generates a large amount of erosive HCl gas, causing severe environmental pollution. Thus, it calls for the development of greener and more efficient composite catalysts. In this work, to reduce the amount of CuCl, we employed three pretreatment methods to activate the contact mass of Si powder and the composite catalyst of CuCl and Cu2O. It was found that the contact mass activated by argon (Ar), hydrogen argon (H2/Ar) and methyl chloride (CH3Cl), respectively, exhibited different catalytic performances: the highest Si conversion (34.1%) and M3 yield (24.0%) were obtained on the sample activated by CH3Cl. Notably, the M3 yield was increased 8-fold than that of the un-activated sample. The X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS) studies revealed that different activation methods led to the generation of different kinds of CuxSi phases, such as Cu3Si and Cu4Si, both of which gradually transformed into Cu15Si4 during the reaction process. Pretreatment of the contact mass with CH3Cl promoted the formation of CuxSi, which contributed to the generation of more Cu15Si4 active phase, and finally to the superior catalytic performance.
AB - The “direct” synthesis of trimethoxysilane (M3) by the reaction of Si with methanol over the CuCl catalyst often generates a large amount of erosive HCl gas, causing severe environmental pollution. Thus, it calls for the development of greener and more efficient composite catalysts. In this work, to reduce the amount of CuCl, we employed three pretreatment methods to activate the contact mass of Si powder and the composite catalyst of CuCl and Cu2O. It was found that the contact mass activated by argon (Ar), hydrogen argon (H2/Ar) and methyl chloride (CH3Cl), respectively, exhibited different catalytic performances: the highest Si conversion (34.1%) and M3 yield (24.0%) were obtained on the sample activated by CH3Cl. Notably, the M3 yield was increased 8-fold than that of the un-activated sample. The X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS) studies revealed that different activation methods led to the generation of different kinds of CuxSi phases, such as Cu3Si and Cu4Si, both of which gradually transformed into Cu15Si4 during the reaction process. Pretreatment of the contact mass with CH3Cl promoted the formation of CuxSi, which contributed to the generation of more Cu15Si4 active phase, and finally to the superior catalytic performance.
KW - Active phase
KW - Catalytic performance
KW - Composite catalyst
KW - Pretreatment
KW - Trimethoxysilane
UR - http://www.scopus.com/inward/record.url?scp=85099228249&partnerID=8YFLogxK
U2 - 10.1016/j.apsusc.2020.148915
DO - 10.1016/j.apsusc.2020.148915
M3 - 文章
AN - SCOPUS:85099228249
SN - 0169-4332
VL - 544
JO - Applied Surface Science
JF - Applied Surface Science
M1 - 148915
ER -