Improved Energy Storage Density and Efficiency of Nd and Mn Co-Doped Ba<sub>0.7</sub>Sr<sub>0.3</sub>TiO<sub>3</sub> Ceramic Capacitors Via Defect Dipole Engineering
Hyunsu Choi,
Srinivas Pattipaka,
Yong Hoon Son,
Young Min Bae,
Jung Hwan Park,
Chang Kyu Jeong,
Han Eol Lee,
Sung-Dae Kim,
Jungho Ryu,
Geon-Tae Hwang
Affiliations
Hyunsu Choi
Department of Materials Science and Engineering, Pukyong National University, 45, Yongso-Ro, Nam-Gu, Busan 48513, Republic of Korea
Srinivas Pattipaka
Department of Materials Science and Engineering, Pukyong National University, 45, Yongso-Ro, Nam-Gu, Busan 48513, Republic of Korea
Yong Hoon Son
Department of Materials Science and Engineering, Pukyong National University, 45, Yongso-Ro, Nam-Gu, Busan 48513, Republic of Korea
Young Min Bae
Department of Materials Science and Engineering, Pukyong National University, 45, Yongso-Ro, Nam-Gu, Busan 48513, Republic of Korea
Jung Hwan Park
Department of Mechanical Engineering, Department of Aeronautics, Mechanical and Electronic Convergence Engineering, Kumoh National Institute of Technology, 61 Daehak-Ro, Gumi 39177, Republic of Korea
Chang Kyu Jeong
Division of Advanced Materials Engineering, Jeonbuk National University, Jeonju 54896, Republic of Korea
Han Eol Lee
Division of Advanced Materials Engineering, Jeonbuk National University, Jeonju 54896, Republic of Korea
Sung-Dae Kim
Department of Materials Science and Engineering, Pukyong National University, 45, Yongso-Ro, Nam-Gu, Busan 48513, Republic of Korea
Jungho Ryu
School of Materials Science and Engineering, Yeungnam University, 280 Daehak-Ro, Gyeongsan-si 38541, Republic of Korea
Geon-Tae Hwang
Department of Materials Science and Engineering, Pukyong National University, 45, Yongso-Ro, Nam-Gu, Busan 48513, Republic of Korea
In this paper, we investigate the structural, microstructural, dielectric, and energy storage properties of Nd and Mn co-doped Ba0.7Sr0.3TiO3 [(Ba0.7Sr0.3)1−xNdxTi1−yMnyO3 (BSNTM) ceramics (x = 0, 0.005, and y = 0, 0.0025, 0.005, and 0.01)] via a defect dipole engineering method. The complex defect dipoles (MnTi”−VO∙∙)∙ and (MnTi”−VO∙∙) between acceptor ions and oxygen vacancies capture electrons, enhancing the breakdown electric field and energy storage performances. XRD, Raman, spectroscopy, XPS, and microscopic investigations of BSNTM ceramics revealed the formation of a tetragonal phase, oxygen vacancies, and a reduction in grain size with Mn dopant. The BSNTM ceramics with x = 0.005 and y = 0 exhibit a relative dielectric constant of 2058 and a loss tangent of 0.026 at 1 kHz. These values gradually decreased to 1876 and 0.019 for x = 0.005 and y = 0.01 due to the Mn2+ ions at the Ti4+- site, which facilitates the formation of oxygen vacancies, and prevents a decrease in Ti4+. In addition, the defect dipoles act as a driving force for depolarization to tailor the domain formation energy and domain wall energy, which provides a high difference between the maximum polarization of Pmax and remnant polarization of Pr (ΔP = 10.39 µC/cm2). Moreover, the complex defect dipoles with optimum oxygen vacancies in BSNTM ceramics can provide not only a high ΔP but also reduce grain size, which together improve the breakdown strength from 60.4 to 110.6 kV/cm, giving rise to a high energy storage density of 0.41 J/cm3 and high efficiency of 84.6% for x = 0.005 and y = 0.01. These findings demonstrate that defect dipole engineering is an effective method to enhance the energy storage performance of dielectrics for capacitor applications.
