无机材料学报

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钐掺杂钪钽酸铅基弛豫铁电体的电卡性能调控

罗文灿1, 谢榜贤1, 翟晨希1, 彭彪林2, 陈雪3, 刘来君1   

  1. 1.桂林理工大学 材料科学与工程学院 广西光电功能材料与器件重点实验室,桂林 541004;
    2.西安电子科技大学 先进材料与纳米科技学院,西安 710072;
    3.桂林电子科技大学 机电工程学院,桂林 541004
  • 收稿日期:2026-09-22 修回日期:2026-10-14
  • 通讯作者: 刘来君, 教授. E-mail: ljliu2@163.com; 陈 雪, 教授. Email: chenxue@guet.edu.cn
  • 作者简介:罗文灿(2005-), 女, 硕士研究生. E-mail: wencan7162026@163.com
  • 基金资助:
    国家自然科学基金(12264012); 广西科技计划项目(AA23023027); 八桂学者项目(DT2400004027)

Regulation of Electrocaloric Performance in Sm-doped Lead Scandium Tantalate-based Relaxor Ferroelectric Ceramics

LUO Wencan1, XIE Bangxian1, ZHAI Chenxi1, PENG Biaolin2, CHEN Xue3, LIU Laijun1   

  1. 1. College of Materials Science and Engineering, Guangxi Key Laboratory of Optoelectronic Materials and Devices, Guilin University of Technology, Guilin 541004, China;
    2. School of Advanced Materials and Nanotechnology, Xidian University, Xi'an 710072, China;
    3. School of Mechanical and Electrical Engineering, Guilin University of Electronic Technology, Guilin 541004, China
  • Received:2026-09-22 Revised:2026-10-14
  • Contact: LIU Laijun, professor. E-mail: ljliu2@163.com; CHEN Xue, professor. Email: chenxue@guet.edu.cn
  • About author:LUO Wencan (2005-), female, Master candidate. E-mail: wencan7162026@163.com
  • Supported by:
    National Natural Science Foundation of China (12264012); Guangxi Science and Technology Program (AA23023027); Bagui Scholar Program (DT2400004027) 

摘要: 电卡制冷是固态制冷的重要途径,但陶瓷材料在中等电场下同时获得较大绝热温变与宽工作温区仍面临挑战。本文以0.9PST-0.1PT弛豫固溶体为基体,研究Sm掺杂对其结构、介电行为及电卡性能的影响,以优化温变幅值与工作温区的协同。采用传统固相反应法制备Pb1-xSmx(Sc0.45Ta0.45Ti0.1)O3(x=0.005、0.01、0.02、0.03)陶瓷,结合XRD、SEM、XPS及畴结构表征分析结构变化,通过间接法与直接量热法评价电卡响应。随Sm含量增加,晶粒细化,菱方相比例降低,介电弥散指数由1.56增至1.85,Tm由32 ℃下移至−11 ℃;x≥0.02时出现少量焦绿石相。在共同100 kV/cm电场下,基于统一温区、正电场下降分支由间接法得到的四组峰值温变依次为2.34、2.48、2.09和1.58 K,x=0.01的温变不低于峰值80%的温区覆盖至少98.43 K。该组分在120 kV/cm下的间接法峰值温变为2.92 K,在303 K下的直接量热温变为2.15 K。结构、介电及畴结构表征支持适量Sm掺杂调节局域极化环境并拓宽极化温度响应的解释;较高掺杂量下的次相出现伴随同场温变降低。x=0.01在本研究所测组分中兼具较大温变与宽温区响应,为PST-PT基电卡陶瓷的组成优化提供了依据。

关键词: 电卡效应, 钪钽酸铅, 施主掺杂, 弛豫铁电体

Abstract: Electrocaloric cooling offers a promising route to solid-state refrigeration, but combining a large adiabatic temperature change with a broad working temperature range under moderate electric fields remains challenging in ceramic materials. This study investigates the effects of Sm content on the structure, dielectric behavior and electrocaloric performance of 0.9PST-0.1PT ceramics, with the aim of improving the trade-off between temperature change and operating temperature span. Pb1-xSmx(Sc0.45Ta0.45Ti0.1)O3 ceramics with x = 0.005, 0.01, 0.02 and 0.03 were prepared by the conventional solid-state reaction method. X-ray diffraction, scanning electron microscopy, X-ray photoelectron spectroscopy and domain characterization were combined with dielectric and polarization measurements. The electrocaloric responses were evaluated using the Maxwell relation and direct calorimetry. With increasing Sm content, the grains became finer, the rhombohedral phase fraction decreased, the dielectric diffuseness exponent increased from 1.56 to 1.85, and the peak permittivity temperature shifted from 32 to −11 ℃. Minor pyrochlore-related reflections appeared at x ≥ 0.02. Calculations based on a unified temperature range and the descending branch of the positive-field P-E loops gave peak adiabatic temperature changes of 2.34, 2.48, 2.09 and 1.58 K for x = 0.005, 0.01, 0.02 and 0.03, respectively, at a common field of 100 kV/cm. For x = 0.01, the temperature interval over which ΔT remained at or above 80% of its peak value spanned at least 98.43 K within the measured range. This composition exhibited an indirectly determined peak temperature change of 2.92 K at 120 kV/cm and a directly measured value of 2.15 K at 303 K under the same field. Structural, dielectric and domain observations support the interpretation that moderate Sm substitution modifies the local polarization environment and broadens the temperature-dependent polarization response, whereas secondary-phase formation at higher Sm contents is accompanied by reduced temperature changes at the common field. The x = 0.01 composition combines a relatively large temperature change with broad temperature coverage, thus providing a basis for optimizing PST-PT electrocaloric ceramics.

Key words: electrocaloric effect, lead scandium tantalate, donor doping, relaxor ferroelectric

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