Use of the active-phase Cu₃Si alloy as superior catalyst to direct synthesis of trichlorosilane via silicon hydrochlorination

TY - JOUR

T1 - Use of the active-phase Cu3Si alloy as superior catalyst to direct synthesis of trichlorosilane via silicon hydrochlorination

AU - Su, Kai

AU - Luo, Jiachengjun

AU - Ji, Yongjun

AU - Jiang, Xingyu

AU - Li, Jing

AU - Zhang, Jianling

AU - Zhong, Ziyi

AU - Su, Fabing

N1 - Publisher Copyright: © 2021 Elsevier Inc.

PY - 2021/12

Y1 - 2021/12

N2 - Here we report the first synthesis of nearly pure-phase Cu3Si alloy that can be a highly efficient catalyst in the hydrochlorination of silicon reaction. This material was prepared by a high-temperature (1050 ​°C) calcination method in which copper and silicon powders were used as the reactants. The X-ray photoelectron spectroscopy (XPS) study revealed that the Cu and Si atoms in the Cu3Si alloy carried part of positive and negative charge, respectively. When employed as the catalyst in the silicon hydrochlorination to SiHCl3 (TCS) for the production of Si polycrystals for Solar cell, the sample Cu3Si exhibited excellent low-temperature catalytic performance: the Si conversion and TCS selectivity respectively achieved 41.1% and 96.1% at 250 ​°C. Notably, its TCS yield at 250 ​°C was 1.2 times higher than that of the industrial catalyst-free system at 350 ​°C. Detailed analysis of the reaction process showed that the positively charged Cu atoms and negatively charged Si atoms in Cu3Si alloy could cleave the H–Cl bond in the reactant HCl and make the combination of H and Cl atom with Si atoms easier. Meanwhile, the reaction between the remaining Cu atom and Si was accelerated, leading to the generation of more active Cu6.69Si and ultimately superior catalytic performance. This work deepens the fundamental understanding of the hydrochlorination of silicon reaction, and provides an avenue for the synthesis of Si-based alloy catalysts.

AB - Here we report the first synthesis of nearly pure-phase Cu3Si alloy that can be a highly efficient catalyst in the hydrochlorination of silicon reaction. This material was prepared by a high-temperature (1050 ​°C) calcination method in which copper and silicon powders were used as the reactants. The X-ray photoelectron spectroscopy (XPS) study revealed that the Cu and Si atoms in the Cu3Si alloy carried part of positive and negative charge, respectively. When employed as the catalyst in the silicon hydrochlorination to SiHCl3 (TCS) for the production of Si polycrystals for Solar cell, the sample Cu3Si exhibited excellent low-temperature catalytic performance: the Si conversion and TCS selectivity respectively achieved 41.1% and 96.1% at 250 ​°C. Notably, its TCS yield at 250 ​°C was 1.2 times higher than that of the industrial catalyst-free system at 350 ​°C. Detailed analysis of the reaction process showed that the positively charged Cu atoms and negatively charged Si atoms in Cu3Si alloy could cleave the H–Cl bond in the reactant HCl and make the combination of H and Cl atom with Si atoms easier. Meanwhile, the reaction between the remaining Cu atom and Si was accelerated, leading to the generation of more active Cu6.69Si and ultimately superior catalytic performance. This work deepens the fundamental understanding of the hydrochlorination of silicon reaction, and provides an avenue for the synthesis of Si-based alloy catalysts.

KW - Alloy

KW - Cu.Si

KW - CuSi

KW - Silicon hydrochlorination

KW - Superior catalyst

KW - Trichlorosilane

UR - http://www.scopus.com/inward/record.url?scp=85115132751&partnerID=8YFLogxK

U2 - 10.1016/j.jssc.2021.122591

DO - 10.1016/j.jssc.2021.122591

M3 - 文章

AN - SCOPUS:85115132751

SN - 0022-4596

VL - 304

JO - Journal of Solid State Chemistry

JF - Journal of Solid State Chemistry

M1 - 122591

ER -