Abstract

ABSTRACT In the Siemens method, high-purity Si is produced by reducing SiHCl3 source gas with H2 ambient under atmospheric pressure. Since the pyrolysis of SiHCl3, which produces SiCl4 as a byproduct, occurs dominantly in the practical Siemens process, the Si yield is low (~30%). In the present study, we generated hydrogen radicals (H-radicals) at pressures greater than 1 atm using tungsten filaments and transported the H-radicals into a reactor. On the basis of the absorbance at 600 nm of WO3-glass exposed to H-radicals in the reactor, we observed that H-radicals with a density of ~1.1 × 1012 cm−3 were transported approximately 30 cm under 1 atm. When SiCl4 was supplied as a source into the reactor containing H-radicals and allowed to react at 850°C or 900°C, Si was produced more efficiently than in reactions conducted under H2 ambient. Because the H-radicals can effectively reduce SiCl4, which is a byproduct in the Siemens method, their use is expected to increase the Si yield for this method.

Highlights

  • Si is regarded as strategic and important material because it is a necessary component of computers, motor vehicles, and various household appliances

  • To improve the Si yield of the Siemens method, we have focused on hydrogen radicals (H-radicals) as a reducing agent [5,6]

  • The H-radicals should be generated at a pressure greater than 1 atm (~101 kPa) and trans­ ported into the 1 atm reaction chamber, because the conventional Siemens method is operated under ~1 atm to obtain enough Si production rate

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Summary

Introduction

Si is regarded as strategic and important material because it is a necessary component of computers, motor vehicles, and various household appliances. In the Siemens method, high-purity trichlorosilane (SiHCl3) and H2 gas are introduced into a bell jar; the SiHCl3 is reduced by H2 into Si on heated Si rods at approximately 1000–1200°C at 1 atm (eq 1): SiHCl3ðgÞþH2ðgÞ ! For H-radicals to be used in the Siemens method, they should be remotely supplied into the bell jar (reaction chamber) to prevent con­ taminants from the source gas or synthesized Si from affecting the H-radical generation process. The H-radicals should be generated at a pressure greater than 1 atm (~101 kPa) and trans­ ported into the 1 atm reaction chamber, because the conventional Siemens method is operated under ~1 atm to obtain enough Si production rate. We generated H-radicals at pressures greater than 1 atm with the filament method and transported them into a 1 atm chamber. In addi­ tion, the effect of H-radicals on the reduction of SiCl4 at 1 atm was investigated to enable the future applica­ tion of H-radicals in the Siemens method

Apparatus for H-radical generation and transportation
Apparatus for H-radical reduction of SiCl4
H-radical reduction of SiCl4
Characterization
Results and discussion
Reduction of SiCl4 by H-radicals at relatively low pressures
Reduction of SiCl4 by H-radicals at 1 atm
Conclusions

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