物理化学学报 >> 2024, Vol. 40 >> Issue (1): 2304015.doi: 10.3866/PKU.WHXB202304015

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BaTiO3基超薄层BME MLCC的可靠性机理

朱超琼1, 蔡子明1,*(), 冯培忠1, 张伟晨2, 惠可臻2, 曹秀华3, 付振晓3, 王晓慧2,*   

  1. 1 中国矿业大学材料与物理学院, 江苏 徐州 221116
    2 清华大学材料学院, 新型陶瓷与精细工艺国家重点实验室, 北京 100084
    3 风华高新科技股份有限公司, 新型电子元器件关键材料与工艺国家重点实验室, 广东 肇庆, 526000
  • 收稿日期:2023-04-06 录用日期:2023-05-24 发布日期:2023-08-21
  • 通讯作者: 蔡子明,王晓慧 E-mail:zmcai@cumt.edu.cn
  • 基金资助:
    国家自然科学基金(52202153);中央高校基本科研业务费专项资金(2023QN1034);新型陶瓷与精细工艺国家重点实验室开放课题(KFZD202002);新型陶瓷与精细工艺国家重点实验室开放课题(KF202204);广东风华高新科技股份有限公司支持的高端电容技术攻关项目资助

Reliability Mechanisms of the Ultrathin-Layered BaTiO3-Based BME MLCC

Chaoqiong Zhu1, Ziming Cai1,*(), Peizhong Feng1, Weichen Zhang2, Kezhen Hui2, Xiuhua Cao3, Zhenxiao Fu3, Xiaohui Wang2,*   

  1. 1 School of Materials Science and Physics, China University of Mining and Technology, Xuzhou 221116, Jiangsu Province, China
    2 State Key Laboratory of New Ceramics and Fine Processing, School of Materials Science and Engineering, Tsinghua University, Beijing 100084, China
    3 State Key Laboratory of Advanced Materials and Electronic Components, Guangdong Fenghua Advanced Technology Holding Co., Ltd., Zhaoqing 526000, Guangdong Province, China
  • Received:2023-04-06 Accepted:2023-05-24 Published:2023-08-21
  • Contact: Ziming Cai, Xiaohui Wang E-mail:zmcai@cumt.edu.cn
  • Supported by:
    the National Natural Science Foundation of China(52202153);the Fundamental Research Funds for the Central Universities(2023QN1034);the State Key Laboratory of New Ceramic and Fine Processing Tsinghua University(KFZD202002);the State Key Laboratory of New Ceramic and Fine Processing Tsinghua University(KF202204);the High-end MLCC Key Project Supported by Guangdong Fenghua Advanced Technology Holding Co., Ltd.

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摘要：

多层陶瓷电容器(Multilayer ceramic capacitors，MLCC)作为市场占有率最高的无源电子元器件，是基础电子元件产业中需要突破关键技术的重点产品之一，在汽车电子、5G通讯、电网调频、航空航天等领域有广泛的应用。在小型化、薄层化发展趋势下，MLCC的介质层厚度不断降低，单层介质在相同电压下的电场显著增大，尤其是中高压超薄层MLCC。因此，MLCC的可靠性愈发成为一项关键的产品质量指标。本文结合加速老化测试、高温阻抗谱、漏电流测试，系统研究超薄层MLCC的劣化机理，揭示抑制氧空位的迁移与富集是保证超薄层MLCC可靠性的重中之重。为此，应减小介质层内部的氧空位浓度，增大其迁移所需的激活能，提高界面肖特基势垒，从而提升超薄层MLCC的可靠性。本文的研究成果为超薄层MLCC介质材料的设计提供了有力指导。

关键词: 钛酸钡, 多层陶瓷电容器, 可靠性, 加速老化, 氧空位

Abstract:

Currently, the world is at the intersection of the energy and computer revolutions. The electronic information industry, driven by the fields of 5G communication, smartphones, and new energy vehicles, is booming and has become an important pillar of the economic market. Multilayer ceramic capacitors (MLCC), which are passive electronic components with the highest market share, are one of the key products that require breakthroughs in key technologies in the basic electronic component industry, with wide applications in automotive electronics, power grid frequency modulation, aerospace, and other fields. With the trend of miniaturization and thin lamination, the thickness of the dielectric layer in the MLCC is decreasing continuously, whereas the electric field on the single dielectric layer is increasing significantly when the MLCC is applied under the same voltage, particularly for the ultrathin-layered MLCC served under medium/high voltage. Consequently, the reliability of MLCC has become a key product quality indicator. In this study, the deterioration mechanism of ultrathin-layer MLCC is systematically studied via accelerated aging tests, high-temperature impedance spectroscopy, and leakage current tests. During the accelerated aging test, the ceramic dielectrics degrades under the applied strict electric field and temperature, and the oxygen vacancies gradually migrate in grains and transgranularly, finally accumulating near the cathode, as observed by transmission electron microscopy. Consequently, a semiconducting layer with poor insulation performance near the cathode is formed, and the barrier height at the interface is reduced. Based on the results of the high-temperature impedance spectroscopy and leakage current test, the activation energy at the grain boundary and dielectric-electrode interface decreases, and the leakage current density increases significantly for the aged MLCC. The formation of an oxygen-vacancy-enriched semiconducting layer is a great threat to the reliability of MLCC, particularly under the trend of developing increasingly thinner dielectric layers. Therefore, inhibiting the migration and enrichment of oxygen vacancies is a top priority for ensuring the reliability of MLCC. To improve the reliability of ultrathin-layered MLCC, the oxygen vacancy concentration in ceramic dielectrics should be reduced, the activation energy required for its migration should be increased, and the Schottky barrier at the interface should be improved. All these results provide a powerful guide for the design of ultrathin-layered MLCC dielectric materials, which is expected to promote the upgrade iteration of high-end MLCC.

Key words: Barium titanate, Multilayer ceramic capacitor, Reliability, Accelerated aging, Oxygen vacancy