极端服役温度对增材制造氮化硅微观组织和强度的影响

Effect of extreme service temperatures on microstructure and strength of additively manufactured silicon nitride

摘要

增材制造技术可为氮化硅陶瓷复杂结构制备提供新工艺。本工作研究增材制造氮化硅在1200～1500 ℃含氧气氛下连续热暴露24 h后的微观组织和抗弯强度演化规律。采用SEM、XRD、EBSD和EPMA表征形貌、相组成和元素分布。结果表明：随着热暴露温度升高，氮化硅发生α→β相转变，β-Si₃N₄相转变率由63.02%（体积分数，下同）增加至74.15%；晶粒尺寸同步增大，由1200 ℃时的1.33 μm增至1500 ℃的1.97 μm。抗弯强度随热暴露温度升高，呈先升后降趋势，在1200 ℃时达到峰值，为722.67 MPa，1500 ℃时最低，为242.67 MPa，较未热暴露时下降约66.00%。晶粒长大及热暴露过程中产生的孔隙、裂纹是造成氮化硅强度降低的主要原因。此外，高温氧化反应会生成强度较低的二氧化硅，同时引入尺寸误差，进一步削弱增材制造氮化硅的力学性能，导致抗弯强度在高温区间随热暴露温度升高明显降低。

Abstract

Additive manufacturing technology provides a novel approach for the production of complex-structured silicon nitride ceramics. In this study, the microstructural and strength evolution of additively manufactured silicon nitride after continuous thermal exposure for 24 hours in an oxygen-containing atmosphere at 1200-1500 ℃ are investigated. The morphology, phase compositions and element distribution are characterized by SEM, XRD, EBSD and EPMA. The results show that with increasing exposure temperature, α→β phase transformation occurs, and the volume fraction of β-Si₃N₄ increases from 63.02% to 74.15%. Meanwhile, the grain size of silicon nitride grows from 1.33 μm at 1200 ℃ to 1.97 μm at 1500 ℃. The flexural strength exhibits a rise-then-fall trend with increasing temperature, reaching a peak value of 722.67 MPa at 1200 ℃ and dropping to a minimum of 242.67 MPa at 1500 ℃, which represents a reduction of approximately 66.00% compared to the unexposed condition. Grain coarsening, as well as the formation of pores and microcracks during thermal exposure, are the primary causes of strength degradation. In addition, high-temperature oxidation reactions lead to the formation of mechanically weak SiO₂ phases and introduce dimensional inaccuracies, further compromising the mechanical performance of the additively manufactured silicon nitride. As a result, flexural strength continues to decrease with increasing exposure temperature. This study reveals the microstructural and mechanical evolution mechanisms of additively manufactured silicon nitride ceramics under extreme high-temperature service conditions, providing a theoretical foundation for improving their service reliability and process optimization.

关键词

增材制造 / 氮化硅 / 极端服役温度 / 微观组织 / 抗弯强度

Key words

additive manufacturing / silicon nitride / extreme service temperature / microstructure / flexural strength

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基金资助

国家重点研发计划(2024YFB3714504)

国家重点研发计划(2024YFB3714503)

辽宁省科学技术计划项目(2024JH2/101900011)

国家自然科学基金(52402094)

国家自然科学基金(U234120139)

国家自然科学基金(U22A20129)

国防基础科研计划(JCKY2022130C005)

中国博士后科学基金(2023M743571)

国家资助博士后研究人员计划(GZC20232743)

中国科学院金属研究所创新基金(2024-PY11)

高端装备铸造技术全国重点实验室开放基金(CAT2023-006)

安徽省研究生教育质量工程(2023cxcysj015)