锆锡钛酸镧铅反铁电体陶瓷的低温烧结和储能特性  

Low-Temperature Sintering and Energy Storage Properties of Lead Lanthanum Zirconate Stannate–Titanate Antiferroelectric Ceramics

作　　者：余宇梁 王世斌 李伟湫 何厚铸 赵小波 姚英邦 陶涛 梁波 鲁圣国 YU Yuliang;WANG Shibin;LI Weiqiu;HE Houzhu;ZHAO Xiaobo;YAO Yingbang;TAO Tao;LIANG Bo;LU Sheng Guo(School of Materials and Energy,Guangdong University of Technology,Guangdong Provincial Research Center on Smart Materials and Energy Conversion Devices,Guangzhou 510006,China;Dongguan South China Design and Innovation Institute,Dongguan 523830,Guangdong,China)

机构地区：[1]广东工业大学材料与能源学院,广东省智能材料和能量转化器件工程技术研究中心,广州510006 [2]东莞华南设计创新院,广东东莞523830

出　　处：《硅酸盐学报》2024年第4期1403-1412,共10页Journal of The Chinese Ceramic Society

基　　金：国家自然科学基金(51872053,52272105);国家自然科学基金委–广东省联合基金(U1501246);广东省自然科学基金(2015A030308004);东莞市核心技术攻关前沿项目(2019622101006);先进能源科学与技术广东省实验室佛山分中心佛山仙湖实验室开放基金(XHT2020-011);国家自然科学基金面上项目(51372042)。

摘　　要：随着风电、光电等绿色能源的利用和对大功率电力电子装备需求的增加,大功率储能器件受到了广泛的关注,而具有高储能密度和高储能效率的(Pb,La)(Zr,Sn,Ti)O_(3)(PLZST)反铁电体陶瓷用于超级介电储能电容器具有明显的优势。但是,受到陶瓷本身高烧结温度(1200~1300℃)的限制,难以适应贱金属内电极多层陶瓷电容器的应用。为了适应贱金属铜(Cu)内电极的烧结,将玻璃粉MgO–Al_(2)O_(3)–ZnO–B_(2)O_(3)–SiO_(2)(MAZBS)添加到(Pb_(0.97)La_(0.02))(Zr_(0.55)Sn_(0.41)Ti_(0.04))O_(3)(PLZST)反铁电体陶瓷中,使烧结温度低于铜内电极的熔点。研究结果表明:当添加了玻璃粉MAZBS的质量分数为0.75%时,PLZST陶瓷在较低的温度(930℃)下可以实现致密烧结,且陶瓷在室温和外加电场300 kV/cm下具有较高的放电储能密度(6.08 J/cm^(3)),和储能效率(77%)。Introduction There exist severe problems in the society,i.e.,environmental pollution,energy shortage,and climate change.These problems directly affect the living environment and have significant threats to globally sustainable development.In the past decades,some low-carbon new energy solutions are developed to address the continuously growing energy demand and mitigate the adverse impacts of climate change.Despite of the continuous emergence of new energy devices,it is still important to face the challenges,i.e.,relatively low power density,safety,large volume,etc..In this paper,the dielectric materials for multilayer energy storage capacitors(MLCC)were prepared by a solid-state reaction method at a lower sintering temperature with low-cost base metal electrodes(e.g.,Cu).In addition,the energy storage properties of the MLCC were also characterized.Methods(Pb_(0.97)La_(0.02))(Zr_(0.55)Sn_(0.41)Ti_(0.04))O_(3)(PLZST)–x%MgO–Al_(2)O_(3)–ZnO–B_(2)O_(3)–SiO_(2)(MAZBS,x=0.00,0.25,0.50,0.75,1.00,1.25)ceramics were synthesized by a conventional solid-state reaction method.The fabricated ceramics were characterized by Fourie transformation infrared spectroscopy(FTIR),thermal analysis,X-ray diffraction(XRD),and scanning electron microscopy(SEM).The dielectric,ferroelectric,and energy storage properties were examined by a LCR impedance analyzer and a polarization–electric field(P–E)hysteresis loop analyzer.PbO(purity:99.0%in mass fraction,the same below),La2O3(99.5%),ZrO2(99.5%),SnO_(2)(99.8%),and TiO_(2)(99.8%)were used as raw materials to synthesize PLZST.MAZBS glass powders were prepared by a water quench method.Afterwards,they were mixed with the oxides powders in a designed mass ratio,ground by high-energy ball milling for 24 h,dried at 80℃for 10 h,and then sintered to form PLZST–x%MAZBS(x=0.00,0.25,0.50,0.75,1.00,1.25)antiferroelectric ceramics.The calcined powders with 5%polyvinyl butyral(PVB)as a binder were pressed into discs with 12 mm in diameter and 1 mm in thickness at 20 MPa.Finally,the green

关 键 词：锆锡钛酸镧铅 反铁电陶瓷 低温烧结 储能密度 储能效率 

分 类 号：TQ174.75[化学工程—陶瓷工业] O487[化学工程—硅酸盐工业]