Dielectric ultracapacitors based on columnar nano-grained ferroelectric oxide films with gradient phases along the growth direction  

作　　者：Chuanqi Song Feifan Zheng Yuan Zhang Hongbo Cheng Long Teng Kun Wang Hanfei Zhu Chao Liu Li Wang Zhengyan Liang Jun Ouyang 

机构地区：[1]Institute of Advanced Energy Materials and Chemistry,School of Chemistry and Chemical Engineering,Qilu University of Technology(Shandong Academy of Sciences),Jinan 250353,China [2]Department of Materials Science and Engineering,Southern University of Science and Technology,Shenzhen 518055,China [3]Key Laboratory of Key Film Materials&Application for Equipment(Hunan Province),School of Materials Science and Engineering,Xiangtan University,Xiangtan 411105,China [4]China Tobacco Shandong Industrial Co.,Ltd.,Jinan 250104,China

出　　处：《Journal of Advanced Ceramics》2024年第7期1072-1079,共8页先进陶瓷（英文）

基　　金：the financial support from the Natural Science Foundation of Shandong Province(Nos.ZR2022ZD39,ZR2022ME031,ZR2023QB119,ZR2023QE138,ZR2020QE042,and ZR2022QB138);the National Natural Science Foundation of China(No.52002192);the Science,Education and Industry Integration Pilot Projects of Qilu University of Technology(Shandong Academy of Sciences)(Nos.2022GH018,2023PX062,and 2023PX041);the Training Plan Project of Qilu University of Technology(Nos.2023RCKY093 and 2023RCKY095);the support from the Jinan City Science and Technology Bureau(No.2021GXRC055);the Education Department of Hunan Province/Xiangtan University(No.KZ0807969)。

摘　　要：In this work,dielectric ultracapacitors were designed and fabricated using a combination of phase boundary and nanograin strategies.These ultracapacitors are based on submicron-thick Ba(Zr_(0.2)Ti_(0.8))O_(3) ferroelectric films sputterdeposited on Si at 500℃.With a composition near a polymorphic phase boundary(PPB),a compressive strain,and a high nucleation rate due to the lowered deposition temperature,these films exhibit a columnar nanograined microstructure with gradient phases along the growth direction.Such a microstructure presents three-dimensional polarization inhomogeneities on the nanoscale,thereby significantly delaying the saturation of the overall electric polarization.Consequently,a pseudolinear,ultraslim polarization(P)-electric field(E)hysteresis loop was obtained,featuring a high maximum applicable electric field(~5.7 MV/cm),low remnant polarization(~5.2μC/cm^(2))and high maximum polarization(~92.1μC/cm^(2)).This P-E loop corresponds to a high recyclable energy density(W_(rec)~208 J/cm^(3))and charge‒discharge efficiency(~88%).An indepth electron microscopy study revealed that the gradient ferroelectric phases consisted of tetragonal(T)and rhombohedral(R)polymorphs along the growth direction of the film.The T-rich phase is abundant near the bottom of the film and gradually transforms into the R-rich phase near the surface.These films also exhibited a high Curie temperature of~460℃and stable capacitive energy storage up to 200℃.These results suggest a feasible pathway for the design and fabrication of high-performance dielectric film capacitors.

关 键 词：FERROELECTRIC thin films energy storage phase coexistence NANOGRAIN silicon 

分 类 号：TB383.2[一般工业技术—材料科学与工程]