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无机材料学报

• 研究论文 •    

氧气氛热压烧结提升高温硅油介质中偏铌酸铅绝缘性能的研究

王一1,2, 李玉臣1, 范晓荣1, 梁瑞虹1   

  1. 1.中国科学院 上海硅酸盐研究所,上海 200050;
    2.中国科学院大学,材料科学与光电工程中心,北京 100049
  • 收稿日期:2026-03-13 修回日期:2026-04-03
  • 通讯作者: 梁瑞虹, 研究员. E-mail: liangruihong@mail.sic.ac.cn
  • 作者简介:王 一(1999-), 男, 硕士研究生. E-mail: wangyi21@mails.ucas.ac.cn
  • 基金资助:
    油气重大专项(2025ZD1402003); 国家自然科学基金(U2241242); 国家重点研发计划(2022YFF0709702)

Enhanced Insulation Performance of Lead Metaniobate in High-temperature Silicone Oil via Oxygen-atmosphere Hot-pressing Sintering

WANG Yi1,2, LI Yuchen1, FAN Xiaorong1, LIANG Ruihong1   

  1. 1. Shanghai Institute of Ceramics, Chinese Academy of Sciences, Shanghai 200050, China;
    2. Center of Materials Science and Optoelectronics Engineering, University of Chinese Academy of Sciences, Beijing 100049, China
  • Received:2026-03-13 Revised:2026-04-03
  • Contact: LIANG Ruihong, professor. E-mail: liangruihong@mail.sic.ac.cn
  • About author:WANG Yi (1999-), male, Master candidate. E-mail: wangyi21@mails.ucas.ac.cn
  • Supported by:
    Oil & Gas Major Project (2025ZD1402003); National Natural Science Foundation of China (U2241242); National Key Reaearch and Development Program of China (2022YFF0709702)

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摘要： 偏铌酸铅(PbNb2O6, PN)压电陶瓷具有高居里温度(TC = 570 ℃℃)和极低的机械品质因数(Qm~10),是深井高温超声换能器的理想候选材料。然而,常规烧结PN陶瓷在高温(>200 ℃)硅油中电阻率大幅下降,严重制约了其在深层石油勘探中的应用。本研究通过氧气氛热压烧结工艺提高Pb0.86Ba0.14Nb2O6(PBN)压电陶瓷的致密度,从而改善其在高温硅油介质中的绝缘性能。采用传统烧结(Conventional sintering, CS)和热压烧结(Hot-pressing sintering, HPS)制备PBN陶瓷样品,系统研究了烧结温度(1230~1310 ℃)、烧结气氛(空气/氧气)和施加压力(10~20 MPa)对致密度的影响。利用扫描电子显微镜(SEM)、X射线衍射(XRD)和Rietveld精修表征微观结构和相结构,在25~235 ℃硅油中测试电阻率,并在235 ℃浸泡3 h后评价高温稳定性。热压烧结将PBN陶瓷致密度从传统烧结的89.13%提高至95.18%。Rietveld精修表明,正交铁电相含量从89.70%降至83.85%(质量百分数),三方非铁电相相应增加。HPS-PBN在235 ℃硅油中的电阻率达到3.1×107 Ω·m,较传统烧结提高1~2个数量级。压电电压常数g33分别为30.97×10-3 (V·m)/N(CS-PBN)和26.99×10-3 (V·m)/N(HPS-PBN)。高温浸泡测试后,HPS-PBN性能衰减幅度小于CS-PBN,表现出更优的热稳定性。虽然热压烧结使压电系数d33从85 pC/N降至65 pC/N,但270 ℃介电异常峰的消除以及高温绝缘性能的显著提升,使其在深井测井应用中更具优势。氧气氛热压烧结工艺为解决PN压电陶瓷在高温硅油中的绝缘失效问题提供了切实可行的方案,在230 ℃以上的深井测井环境中具有重要工程应用价值。

关键词: 热压烧结, 偏铌酸铅, 高温, 致密度, 电阻率

Abstract: Lead metaniobate (PbNb2O6, PN) piezoelectric ceramics are promising candidates for deep-well high-temperature ultrasonic transducers owing to their high Curie temperature (TC = 570 ℃) and exceptionally low mechanical quality factor (Qm~10). However, the significant decrease in electrical resistivity of conventionally sintered PN ceramics in high-temperature (> 200 ℃) silicone oil severely limits their application in deep petroleum exploration. This study aims to enhance the insulation performance of Pb0.86Ba0.14Nb2O6 (PBN) piezoelectric ceramics in high-temperature silicone oil by improving their relative density through oxygen-atmosphere hot-pressing sintering. PBN ceramic samples were fabricated via conventional sintering (CS) and hot-pressing sintering (HPS) with systematic investigation of sintering temperature (1230-1310 ℃), atmosphere (air/oxygen), and applied pressure (10-20 MPa). The microstructure and phase structure were characterized by scanning electron microscopy (SEM), X-ray diffraction (XRD), and Rietveld refinement. The electrical resistivity was measured in silicone oil from 25 ℃ to 235 ℃, and the high-temperature stability was evaluated after 3-h immersion at 235 ℃. Hot-pressing sintering increased the relative density of PBN ceramics from 89.13% (CS) to 95.18% (HPS). Rietveld refinement revealed that the orthorhombic ferroelectric phase content decreased from 89.70% to 83.85% (in mass), while the trigonal non-ferroelectric phase increased correspondingly. The resistivity of HPS-PBN in silicone oil at 235 ℃ reached 3.1×107 Ω·m, which is one to two orders of magnitude higher than that of CS-PBN. The piezoelectric voltage constant g33 was calculated to be 30.97×10-3 (V·m)/N (CS-PBN) and 26.99×10-3 (V·m)/N (HPS-PBN), respectively. After high-temperature immersion testing, HPS-PBN exhibited smaller performance degradation compared to CS-PBN, demonstrating superior thermal stability. Although hot-pressing sintering reduced the piezoelectric coefficient d33 from 85 pC/N to 65 pC/N due to decreased ferroelectric phase content, the elimination of the anomalous dielectric peak at 270 ℃ and the significant improvement in high-temperature insulation performance outweigh this drawback for deep-well logging applications. Oxygen-atmosphere hot-pressing sintering provides a practical and effective solution for the insulation failure of PBN piezoelectric ceramics in high-temperature silicone oil, demonstrating significant engineering application potential for deep-well logging environments above 230 ℃.

Key words: hot-pressing sintering, lead metaniobate, high temperature, relative density, electrical resistivity

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