硅酸盐学报

热管理用氮化硅陶瓷热导率影响因素及改善途径

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王峰 ¹ , 贺智勇 ¹ , 王晓波 ¹ , 王不赖 ² , 孟晴 ³ , 李江涛 ³

硅酸盐学报 | 综合评述 2024,52(12): 3868-3883

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硅酸盐学报 |综合评述 2024 , 52 (12) : 3868 -3883

热管理用氮化硅陶瓷热导率影响因素及改善途径

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王峰¹, 贺智勇¹, 王晓波¹, 王不赖², 孟晴³, 李江涛³

作者信息

^1．中国钢研科技集团有限公司，北京 100081

^2．中国地质大学材料科学与工程学院，北京 100083

^3．中国科学院理化技术研究所，低温工程重点实验室，北京 100190

通讯作者:

贺智勇（1970—），男，正高级工程师。

孟晴（1994—），女，工程师。

作者简介:

王峰（1983—），男，博士，高级工程师。

Influencing Factors and Improvement Approaches of Thermal Conductivity of Silicon Nitride Ceramics for Thermal Management

Feng WANG¹, Zhiyong HE¹, Xiaobo WANG¹, Bulai WANG², Qing MENG³, Jiangtao LI³

Affiliations

^1.China Iron & Steel Research Institute Group, Beijing 100081, China

^2.School of Materials Science and Technology, China University of Geosciences, Beijing 100083, China

^3.Key Laboratory of Cryogenics, Technical Institute of Physics and Chemistry, Chinese Academy of Science, Beijing 100190, China

Corresponding Author:

HE Zhiyong (1970-), male, Professorate Senior Engineer. E-mail: hezhiyong@cisri.com.cn;

MENG Qing (1994-), female, Engineer. mengqing@mail.ipc.ac.cn

WANG Feng (1983-), male, Ph.D., Senior Engineer. E-mail: hawk16181618@163.com

出版时间: 2024-12-20 doi: 10.14062/j.issn.0454-5648.20240331

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摘要

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随着电子功率器件向高电压、大电流、高功率密度发展，其在运行过程中会产生更多的热量，承受更大的热应力，这就对器件用陶瓷基板的散热性能及可靠性提出了更高的要求。传统陶瓷基板如氧化铝（热导率低）、氮化铝（力学性能差）已难以满足大功率器件要求。氮化硅陶瓷由于兼具较高的理论热导率与优异的力学性能而成为大功率器件用陶瓷基板的首选材料。但是氮化硅陶瓷的实际热导率与理论值尚存在较大差距，晶格氧含量是主要影响因素。另外，氮化硅陶瓷在制备过程中需要引入适宜的烧结助剂，由烧结助剂引入而引起氮化硅陶瓷显微结构（致密度、晶粒形貌、晶界相含量与分布及平均晶界薄膜厚度等）的变化也会影响其热导率。氮化硅陶瓷显微结构的演变又与其成型技术、烧结工艺密切相关。降低晶格氧含量，减少晶界相，获得具有由细小晶粒与大长柱状晶粒组成的双峰结构是获得高导热氮化硅陶瓷的关键。本文从氮化硅结构与热学性质入手，对晶格氧与显微结构对氮化硅陶瓷热导率的影响作用机制进行了讨论，从原料粉体、烧结助剂、烧结工艺、结构织构化4个方面对氮化硅陶瓷中晶格氧的调控作用、显微结构的演变过程及热导率的强化机理进行了阐述，对高导热氮化硅陶瓷发展现状及面临的挑战进行了探讨，最后对高导热氮化硅陶瓷未来发展前景进行了展望。

关键词

氮化硅陶瓷 / 氧杂质 / 显微结构 / 热导率 / 改善途径

Abstract

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With the development of electronic power devices towards high voltage, high current and high power density, they will generate more heat and bear greater thermal stress during the operation, which puts forward higher requirements for the heat dissipation ability and reliability of ceramic substrates used for devices. Conventional ceramic substrates such as alumina (i.e., low thermal conductivity, only 20-30 W·m⁻¹·K⁻¹) and aluminum nitride (i.e., poor mechanical property, such as bending strength of 300 MPa and fracture toughness of 3-4 MPa·m^1/2) are difficult to meet the requirements of high power devices. Silicon nitride (Si₃N₄) ceramic becomes an ideal ceramic substrate for high power devices due to the high theoretical thermal conductivity and excellent mechanical properties. However, there is still a significant gap between the actual and theoretical values of thermal conductivity for Si₃N₄ ceramics, and the lattice oxygen content is a main affecting factor. Moreover, suitable sintering additives need to be added during the preparation of Si₃N₄ ceramics, and the microstructure (i.e., density, grain morphology, grain boundary phase content and distribution, and average thickness of grain boundary film) changes due to the introduction of sintering additives, which affects the thermal conductivity of Si₃N₄ ceramics. The microstructure evolution of Si₃N₄ ceramics is also closely related to the forming technology and sintering system. Therefore, the optimization of preparation processes of Si₃N₄ ceramics has a positive effect on its thermal conductivity improvement.

In the review, the microstructures and thermal properties of Si₃N₄ ceramics were introduced. Some influencing factors of the thermal conductivity of Si₃N₄ ceramics were discussed and the related impact mechanism were illustrated. The α-Si₃N₄ phase is metastable and transforms to β-Si₃N₄ phase through the dissolution precipitation reaction at a high temperature. A lattice reconstruction also occurs at the same time. The β-Si₃N₄ phase exhibits a high ideal thermal conductivity. The actual thermal conductivity of Si₃N₄ ceramics deteriorates gradually with increasing the lattice oxygen and grain boundary phase contents. Similarly, the continuous-distributed grain boundary phase is also harmful to the thermal conductivity of Si₃N₄ ceramics. These existed defects and microstructures lead to increased phonon scattering during the transmission process, which does not favor the thermal conductivity improvement. The large elongated β-Si₃N₄ grains are beneficent to the thermal conductivity enhancement because of the decreased phonon scattering.

The ways to improve the thermal conductivity of Si₃N₄ ceramics are to regulate their lattice oxygen and microstructures. In the review, the lattice oxygen regulation role, the microstructure evolution process and the thermal conductivity enhancement mechanism of Si₃N₄ ceramics could be elaborated from four aspects, i.e., raw material powder, sintering additives, sintering process and structural texture. The introduction of oxygen impurity content could be reduced with high purity silicon nitride powder as a raw material and the ball milling process optimization. And the microstructure and lattice oxygen content can be regulated via selecting rare-earth oxides with small ion radius and non-oxides as sintering additives and optimizing the sintering process (i.e., sintering temperature, soaking time, sintering atmosphere and so on), which are beneficial to promoting the thermal conductivity. In addition, the high thermal conductivity along the direction of Si₃N₄ grains orientation can be also obtained through a structural texture technology.

The development status and challenges of high thermal conductive Si₃N₄ ceramics were discussed. The routes to realize the localization of high thermal conductive Si₃N₄ ceramics are to strengthen the source control of raw material production, thus improving the performance of production equipment and establishing the evaluation standard system of product performance.

Summary and prospects

The Si₃N₄ ceramic is an ideal substrate material for high power device, and its high thermal conductivity is essential. However, there is still a significant gap between the actual and theoretical values of the thermal conductivity of Si₃N₄ ceramics due to the influence of lattice oxygen impurity and microstructure composition. The approaches to obtain Si₃N₄ ceramics with a high thermal conductivity are to decrease the lattice oxygen content, reduce the grain boundary phase and obtain the double peak structure composed of fine grains and a high aspect ratio β-Si₃N₄ grains through improving the purity of raw materials, selecting appropriate sintering aids and forming methods and optimizing the sintering system.

To obtain high thermal conductive Si₃N₄ ceramics, a research on the raw material powder with a high purity and a low oxygen content should be strengthened. The high quality equipment for Si₃N₄ ceramics production should be developed through controlling the sintering and processing technology. The practical application research should be promoted continuously and the completed application closed loop should be formed among powder production companies, product manufacturing enterprises and users. The timely feedback and response about the problems discovered during this process should be provided quickly to improve the performance of high thermal conductive Si₃N₄ ceramic products.

Key words

silicon nitride ceramics / oxygen impurity / microstructure / thermal conductivity / improvement approach

引用本文

王峰, 贺智勇, 王晓波, 王不赖, 孟晴, 李江涛. 热管理用氮化硅陶瓷热导率影响因素及改善途径. 硅酸盐学报, 2024 , 52 (12) : 3868 -3883 . DOI: 10.14062/j.issn.0454-5648.20240331

Feng WANG, Zhiyong HE, Xiaobo WANG, Bulai WANG, Qing MENG, Jiangtao LI. Influencing Factors and Improvement Approaches of Thermal Conductivity of Silicon Nitride Ceramics for Thermal Management[J]. Journal of the Chinese Ceramic Society, 2024 , 52 (12) : 3868 -3883 . DOI: 10.14062/j.issn.0454-5648.20240331

基金

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国家自然科学基金(92263205)

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2024年第52卷第12期

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文章信息

doi: 10.14062/j.issn.0454-5648.20240331

接收时间：2024-05-11
首发时间：2026-10-22
出版时间：2024-12-20

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收稿日期：2024-05-11
修回日期：2024-06-18

基金

国家自然科学基金(92263205)

作者信息

^1．中国钢研科技集团有限公司，北京 100081

^2．中国地质大学材料科学与工程学院，北京 100083

^3．中国科学院理化技术研究所，低温工程重点实验室，北京 100190

通讯作者:

贺智勇（1970—），男，正高级工程师。

孟晴（1994—），女，工程师。

参考文献

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https://castjournals.cast.org.cn/joweb/gsyxb/CN/10.14062/j.issn.0454-5648.20240331

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2种不同金属材料的力学参数

科 Family	属数 Number of genus	种数 Number of species	占总种数比例 Percentage of total species (%)	属 Genus	种数 Number of species	占总种数比例 Percentage of total species (%)
鹅膏菌科Amanitaceae	2	11	5.26	鹅膏菌属 Amanita	10	4.78
小菇科 Mycenaceae	2	12	5.74	丝盖伞属 Inocybe	5	2.39
多孔菌科 Polyporaceae	8	14	6.70	蜡蘑属 Laccaria	5	2.39
红菇科 Russulaceae	3	23	11.00	小皮伞属 Marasmius	6	2.87
				小菇属 Mycena	11	5.26
				光柄菇属 Pluteus	5	2.39
				红菇属 Russula	17	8.13
				栓菌属 Trametes	5	2.39

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