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2025 Vol.45, Issue 5 Preview Page

Research Article

Rapid Synthesis of Si3N4​ via a Two-Step Direct Nitridation Reaction Using Silicon Recycled from End-of-Life Photovoltaic (EoL PV) Modules

태양광 폐모듈로부터 회수한 실리콘의 2단계 직접 질화 반응을 통한 Si3N4 급속 합성

Seong-Pyo Lee12
,
Woo-Gyun Shin3
,
Suk-whan Ko4
,
Hye-mi Hwang4
,
Young-chul Ju3
,
Jeong-Gu Yeo5
,
So-Yeon Heo6
,
Gi-hwan Kang7
,
Hyo-Sik Chang8*
,
Jin-Seok Lee4*
이 성표12
,
신 우균3
,
고 석환4
,
황 혜미4
,
주 영철3
,
여 정구5
,
허 소연6
,
강 기환7
,
장 효식8*
,
이 진석4*
1Research Student, Renewable Energy System Laboratory, Korea Institute of Energy Research
2Master Course Student, Graduate School of Energy Science and Technology, Chungnam National University
3Senior Researcher, Renewable Energy System Laboratory, Korea Institute of Energy Research
4Principal Researcher, Renewable Energy System Laboratory, Korea Institute of Energy Research
5Principal Researcher, Energy Storage Research Department, Korea Institute of Energy Research
6Researcher, Energy Storage Research Department, Korea Institute of Energy Research
7Principal Researcher, Photovoltaics Research Department, Korea Institute of Energy Research
8Professor, Graduate School of Energy Science and Technology, Chungnam National University
1한국에너지기술연구원 신재생시스템연구실, 학생연구원
2충남대학교 에너지과학기술대학원, 석사과정
3한국에너지기술연구원 신재생시스템연구실, 선임연구원
4한국에너지기술연구원 신재생시스템연구실, 책임연구원
5한국에너지기술연구원 에너지저장연구단, 책임연구원
6한국에너지기술연구원 에너지저장연구단, 연구원
7한국에너지기술연구원 태양광연구단, 책임연구원
8충남대학교 에너지과학기술대학원, 교수
*Corresponding Author
30 October 2025. pp. 75-89
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Abstract

In this study, recycled Si (r-Si) recovered from end-of-life photovoltaic (EoL PV) modules was used to synthesize Si3N4. The recovered r-Si powder was treated via ball milling to obtain an average particle size of approximately 1 µm, after which it was subjected to two-step direct nitridation under a N2–H2 atmosphere. Specifically, first-step nitridation (conducted at 1350℃), which promoted surface nitridation, was followed by second-step nitridation (performed at 1450℃), which enabled complete conversion within 10 min. The resulting Si3N4 predominantly comprised the α-phase (87-91%), and the minor β-phase fraction (9-13%) was attributed to local heat-concentration-induced melting. Additionally, volatile SiO species, generated via the reduction of SiO2 or partial oxidation of Si, reacted with N2 in the gas phase, further contributing to β-Si3N4 formation. Analysis of particle sizes, along with scanning electron microscopy, confirmed grain coarsening at a prolonged holding time. The sample maintained at 1350℃ for 60 min, followed by 10 min at 1450℃ (#60-10), exhibited a smaller particle size with a short processing time, thus representing the optimal synthetic condition. In addition, the mechanism of phase formation was analyzed in terms of the overall two-step nitridation process and the reactions at each temperature. The findings experimentally validate the viability of utilizing r-Si derived from PV modules as a raw material for producing advanced ceramics, contributing to resource circulation and domestic material self-sufficiency.

Keywords
End-of-life photovoltaic (EoL PV) modules
Recycling
Silicon
Silicon nitride
Direct nitridation
키워드
태양광 폐모듈
재활용
실리콘
질화규소
직접질화
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Information
  • Publisher :Korean Solar Energy Society
  • Publisher(Ko) :한국태양에너지학회
  • Journal Title :Journal of the Korean Solar Energy Society
  • Journal Title(Ko) :한국태양에너지학회 논문집
  • Volume : 45
  • No :5
  • Pages :75-89
  • Received Date : 2025-09-11
  • Revised Date : 2025-10-02
  • Accepted Date : 2025-10-13
  • DOI :https://doi.org/10.7836/kses.2025.45.5.075
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