{"title":"Effects of gadolinium modification on leakage conduction and energy storage performance of sol-gel derived (Ba0.85Ca0.15)(Zr0.2Ti0.8)O3 thin films","authors":"Ke Zhang, Chen Zhang, Haoliang Li, Jingwang Lu, Zhipeng Ma, Xing Zhang","doi":"10.1016/j.ceramint.2024.12.360","DOIUrl":null,"url":null,"abstract":"<div><div>The microstructures, leakage conduction and energy storage performances of Gadolinium (Gd<sup>3+</sup>) modified barium calcium zirconate titanate based thin films [Ba<sub>(0.85-x)</sub>Ca<sub>0.15</sub>Gd<sub>x</sub>][Zr<sub>0.2</sub>Ti<sub>0.8</sub>]O<sub>(3+0.5x)</sub> (<em>x</em> = 0, 0.005, 0.0075 and 0.01) prepared on the Pt/Ti/SiO<sub>2</sub>/Si substrates using sol-gel method were characterized and analyzed. The dense and uniform microstructure with fine nanocrystalline grains is obtained in low Gd<sup>3+</sup> concentration (<em>x</em> ≤ 0.0075) doped BCGZT thin films with single phase perovskite structure. With the increase of Gd<sup>3+</sup> content, the leakage current density of BCGZT films initially decreases to the minimum at <em>x</em> = 0.0075 due to the existing of defect dipoles V<sub>Ca</sub>″-V<sub>O</sub><sup>••</sup> caused by the Gd<sup>3+</sup> substitution for A site ions and then increases significantly due to the appearance of impurity phases. With the increase of electric field, the leakage mechanism for each BCGZT film transforms from ohmic conduction and/or SCL conduction to F-N tunneling. The remanent polarization keeps decreasing because of the weakened ferroelectricity of Gd<sup>3+</sup> modified BCZT perovskites and the decreasing average grain size as the Gd<sup>3+</sup> content increases. The BCGZT thin film with <em>x</em> = 0.0075 possesses an enhanced energy storage density of 55.1 J/cm<sup>3</sup> and an acceptable energy storage efficiency of 67.1 % at the ultra-high breakdown field of 4300 kV/cm, which is promising for capacitor applications.</div></div>","PeriodicalId":267,"journal":{"name":"Ceramics International","volume":"51 7","pages":"Pages 9248-9256"},"PeriodicalIF":5.1000,"publicationDate":"2025-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Ceramics International","FirstCategoryId":"88","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0272884224060310","RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"MATERIALS SCIENCE, CERAMICS","Score":null,"Total":0}
引用次数: 0
Abstract
The microstructures, leakage conduction and energy storage performances of Gadolinium (Gd3+) modified barium calcium zirconate titanate based thin films [Ba(0.85-x)Ca0.15Gdx][Zr0.2Ti0.8]O(3+0.5x) (x = 0, 0.005, 0.0075 and 0.01) prepared on the Pt/Ti/SiO2/Si substrates using sol-gel method were characterized and analyzed. The dense and uniform microstructure with fine nanocrystalline grains is obtained in low Gd3+ concentration (x ≤ 0.0075) doped BCGZT thin films with single phase perovskite structure. With the increase of Gd3+ content, the leakage current density of BCGZT films initially decreases to the minimum at x = 0.0075 due to the existing of defect dipoles VCa″-VO•• caused by the Gd3+ substitution for A site ions and then increases significantly due to the appearance of impurity phases. With the increase of electric field, the leakage mechanism for each BCGZT film transforms from ohmic conduction and/or SCL conduction to F-N tunneling. The remanent polarization keeps decreasing because of the weakened ferroelectricity of Gd3+ modified BCZT perovskites and the decreasing average grain size as the Gd3+ content increases. The BCGZT thin film with x = 0.0075 possesses an enhanced energy storage density of 55.1 J/cm3 and an acceptable energy storage efficiency of 67.1 % at the ultra-high breakdown field of 4300 kV/cm, which is promising for capacitor applications.
期刊介绍:
Ceramics International covers the science of advanced ceramic materials. The journal encourages contributions that demonstrate how an understanding of the basic chemical and physical phenomena may direct materials design and stimulate ideas for new or improved processing techniques, in order to obtain materials with desired structural features and properties.
Ceramics International covers oxide and non-oxide ceramics, functional glasses, glass ceramics, amorphous inorganic non-metallic materials (and their combinations with metal and organic materials), in the form of particulates, dense or porous bodies, thin/thick films and laminated, graded and composite structures. Process related topics such as ceramic-ceramic joints or joining ceramics with dissimilar materials, as well as surface finishing and conditioning are also covered. Besides traditional processing techniques, manufacturing routes of interest include innovative procedures benefiting from externally applied stresses, electromagnetic fields and energetic beams, as well as top-down and self-assembly nanotechnology approaches. In addition, the journal welcomes submissions on bio-inspired and bio-enabled materials designs, experimentally validated multi scale modelling and simulation for materials design, and the use of the most advanced chemical and physical characterization techniques of structure, properties and behaviour.
Technologically relevant low-dimensional systems are a particular focus of Ceramics International. These include 0, 1 and 2-D nanomaterials (also covering CNTs, graphene and related materials, and diamond-like carbons), their nanocomposites, as well as nano-hybrids and hierarchical multifunctional nanostructures that might integrate molecular, biological and electronic components.