Article(id=1325131283453584287, tenantId=1146029695717560320, journalId=1255847867265597444, issueId=1325123175192855060, articleNumber=null, orderNo=null, doi=10.11858/gywlxb.20261071, pmid=null, cstr=null, oa=null, hot=null, price=null, onlineType=0, articleFormat=0, articleType=null, articleTypeStr=research-article, receivedDate=1775059200000, receivedDateStr=2026-04-02, revisedDate=1776960000000, revisedDateStr=2026-04-24, acceptedDate=null, acceptedDateStr=null, onlineDate=1793865517723, onlineDateStr=2026-11-05, pubDate=1788537600000, pubDateStr=2026-09-05, doiRegisterDate=null, doiRegisterDateStr=null, onlineIssueDate=1793865517723, onlineIssueDateStr=2026-11-05, onlineJustAcceptDate=null, onlineJustAcceptDateStr=null, onlineFirstDate=null, onlineFirstDateStr=null, sourceXml=null, magXml=null, createTime=1793865517723, creator=13701087609, updateTime=1793865517723, updator=13701087609, issue=Issue{id=1325123175192855060, tenantId=1146029695717560320, journalId=1255847867265597444, year='2026', volume='40', issue='9', pageStart='090101-1', pageEnd='090114-12', issueExtLink='null', onlineDate='null', pubDate='1788537600000', pubDateStr='2026-09-05', beforeIssueId=null, nextIssueId=null, price=null, status=1, issueComplete=1, articleOrder=1, issueType=1, specialIssue=0, createTime=1793863584564, creator='13701087609', updateTime=1793864402827, updator='13701087609', preIssue=null, nextIssue=null, articleTotal=null, ext={EN=IssueExt(id=1325126607446356730, tenantId=1146029695717560320, journalId=1255847867265597444, issueId=1325123175192855060, language=EN, specialIssueTitle=, coverIllustrator=null, specialIssueEditor=, specialIssueAbout=), CN=IssueExt(id=1325126607450551035, tenantId=1146029695717560320, journalId=1255847867265597444, issueId=1325123175192855060, language=CN, specialIssueTitle=, coverIllustrator=null, specialIssueEditor=, specialIssueAbout=)}, issueFiles=null, downloadFileDto=null}, startPage=090111-1, endPage=090111-11, ext={EN=ArticleExt(id=1325131283709436832, articleId=1325131283453584287, tenantId=1146029695717560320, journalId=1255847867265597444, language=EN, title=Thermal Conductivity of AlN/Diamond Composites Sintered under High-Pressure and High-Temperature, columnId=1325123176816050710, journalTitle=Chinese Journal of High Pressure Physics, columnName=Carbon under High Pressure, runingTitle=null, highlight=null, articleAbstract=

Aluminum nitride (AlN) ceramics are important heat-dissipation materials for high-power electronic devices. However, the high sintering temperature required by conventional processing routes limits practical application of AlN ceramics and increases fabrication costs. Therefore, it is necessary to develop preparation method that is capable of achieving densification at relatively low temperature. To address the difficulty of simultaneously obtaining high densification and high thermal conductivity in polycrystalline AlN ceramics under reduced-temperature sintering conditions, this work adopts a stepwise research strategy. First, the densification behavior and thermal conductivity of pure AlN under high-pressure assistance were investigated to identify the optimal sintering conditions. Under additive-free conditions, pure-phase AlN ceramics with clean grain boundaries and high densification were prepared at 5.0 GPa and 1400 ℃, achieving a thermal conductivity of 101.6 W/(m·K). Based on these optimized conditions, the AlN/diamond composite system was further studied, and the effects of diamond volume fraction on the structure and properties of the composites were systematically examined. The results show that the thermal conductivity of the composites first decreases and then increases with increasing diamond volume fraction, reaching 112.4 W/(m·K) at 33.3%. Mechanistic analysis indicates that interfacial thermal resistance dominates at low diamond contents, whereas at high diamond contents the enhancement of heat transport by thermally conductive diamond pathways becomes more significant. By taking full advantage of the processing benefits of high-temperature and high-pressure technology, this work achieves substantial improvement of AlN-based materials at temperatures lower than those required in conventional sintering, thereby providing a new route for the low-temperature fabrication of high-performance thermally conductive ceramics.

, authors=Fa GONG1, Wenjia LIANG2, Qiming WANG1, Qian LI1, Hongwen LIU1, Peihong HE1, Duanwei HE1, Fang PENG1, authorsList=Fa GONG, Wenjia LIANG, Qiming WANG, Qian LI, Hongwen LIU, Peihong HE, Duanwei HE, Fang PENG, authorCompany=null, correspAuthors=Duanwei HE, Fang PENG, authorNote=null, correspAuthorsNote=null, copyrightStatement=Copyright © 2026 Chinese Journal of High Pressure Physics. All rights reserved., copyrightOwner=null, extLink=null, articleAbsUrl=null, sourceXml=null, magXml=null, pdfUrl=null, pdf=null, pdfFileSize=null, pdfExtLink=null, richHtmlUrl=null, mobilePdfUrl=null, reviewReport=null, pdfFirstPage=null, abstractGraph=null, abstractGraphContent=null, abstractVideo=null, citation=null, cebUrl=null, magXmlContent=null, mapNumber=null, fund=null), CN=ArticleExt(id=1325131286829999027, articleId=1325131283453584287, tenantId=1146029695717560320, journalId=1255847867265597444, language=CN, title=高温高压烧结AlN/金刚石复合材料的导热性, columnId=1325123177629745688, journalTitle=高压物理学报, columnName=高压下的碳材料, runingTitle=null, highlight=null, articleAbstract=

氮化铝(AlN)陶瓷是高功率电子器件散热的重要材料,然而,传统烧结方法的温度高,制约了其进一步应用,并提高了制备成本。因此,有必要发展在较低温度条件下实现AlN陶瓷致密化的制备方法。针对多晶AlN陶瓷在较低烧结温度下难以兼顾高致密化与高热导率的问题,采用分步研究思路。首先,研究纯相AlN在高压辅助下的致密化行为和导热性能,确定优化烧结条件。在无助剂、压力为5.0 GPa、温度为1400 ℃的条件下制备出晶界洁净、高致密的纯相AlN陶瓷,热导率达101.6 W/(m·K)。然后,在所确定的优化烧结条件下研究AlN/金刚石复合体系,系统考察金刚石含量对复合材料结构与性能的影响。结果表明,复合材料的热导率随金刚石体积分数的增加呈先降后升趋势,在金刚石体积分数为33.3%时达到112.4 W/(m·K)。机理分析表明:低金刚石含量时,界面热阻占主导;高金刚石含量时,金刚石形成的导热通路对热传导的增强作用更显著。研究工作充分发挥了高温高压技术优势,在比传统烧结技术更低的温度下实现了AlN基材料的大幅优化,为较低温制备高性能导热陶瓷提供了新途径。

, authors=龚发1, 梁文嘉2, 王齐明1, 李倩1, 刘洪汶1, 何沛宏1, 贺端威1, 彭放1, authorsList=龚发, 梁文嘉, 王齐明, 李倩, 刘洪汶, 何沛宏, 贺端威, 彭放, authorCompany=null, correspAuthors=贺端威, 彭放, authorNote=

龚 发(2000-),女,硕士研究生,主要从事高压科学研究. E-mail:

, correspAuthorsNote=
贺端威(1969-),男,博士,教授,主要从事高压物理、凝聚态物理、超硬材料研究. E-mail:
彭 放(1960-),男,博士,教授,主要从事高压物理、凝聚态物理、超硬材料研究. E-mail:
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Ceramics International, 2022, 48(18): 26022–26027., articleTitle=null, refAbstract=null)], funds=null, companyList=[AuthorCompany(id=1325131287031325620, tenantId=1146029695717560320, journalId=1255847867265597444, articleId=1325131283453584287, xref=1, ext=[AuthorCompanyExt(id=1325131287039714229, tenantId=1146029695717560320, journalId=1255847867265597444, articleId=1325131283453584287, companyId=1325131287031325620, language=EN, country=null, province=null, city=null, postcode=null, companyName=null, departmentName=null, remark=1Institute of Atomic and Molecular Physics, Sichuan University, Chengdu 610065, Sichuan, China), AuthorCompanyExt(id=1325131287056491446, tenantId=1146029695717560320, journalId=1255847867265597444, articleId=1325131283453584287, companyId=1325131287031325620, language=CN, country=null, province=null, city=null, postcode=null, companyName=null, departmentName=null, remark=1四川大学原子与分子物理研究所, 四川 成都 610065)]), AuthorCompany(id=1325131287131988919, tenantId=1146029695717560320, journalId=1255847867265597444, articleId=1325131283453584287, xref=2, ext=[AuthorCompanyExt(id=1325131287140377528, tenantId=1146029695717560320, journalId=1255847867265597444, articleId=1325131283453584287, companyId=1325131287131988919, language=EN, country=null, province=null, city=null, postcode=null, companyName=null, departmentName=null, remark=2School of Intelligent Manufacturing, Sichuan University of Arts and Science, Dazhou 635002, Sichuan, China), AuthorCompanyExt(id=1325131287148766137, tenantId=1146029695717560320, journalId=1255847867265597444, articleId=1325131283453584287, companyId=1325131287131988919, language=CN, country=null, province=null, city=null, postcode=null, companyName=null, departmentName=null, remark=2四川文理学院智能制造学院, 四川 达州 635002)])], figs=[ArticleFig(id=1325131293150815217, tenantId=1146029695717560320, journalId=1255847867265597444, articleId=1325131283453584287, language=EN, label=Fig. 1, caption=(a) Secondary electron SEM (SE-SEM) image and (b) XRD pattern of the as-received AlN powder; (c) SE-SEM image and (d) XRD pattern of the as-received diamond powder, figureFileSmall=i6z9eaj/YEFiWLJEGWyn2w==, figureFileBig=ujWwCMyEdX4nOMwD7lEkRQ==, tableContent=null), ArticleFig(id=1325131293553468402, tenantId=1146029695717560320, journalId=1255847867265597444, articleId=1325131283453584287, language=CN, label=图1, caption=初始AlN粉末的(a)二次电子SEM图像和(b) XRD谱以及初始金刚石粉末的(c) 二次电子SEM图像和(d) XRD谱, figureFileSmall=i6z9eaj/YEFiWLJEGWyn2w==, figureFileBig=ujWwCMyEdX4nOMwD7lEkRQ==, tableContent=null), ArticleFig(id=1325131295252161523, tenantId=1146029695717560320, journalId=1255847867265597444, articleId=1325131283453584287, language=EN, label=Fig. 2, caption=(a) Sample assembly of the high-pressure cell; (b) sintering temperature and pressure profiles, figureFileSmall=/kj3wBszmIcsh4usLeaK1A==, figureFileBig=7KwkciebMIckLuF9/tVs2g==, tableContent=null), ArticleFig(id=1325131295579317236, tenantId=1146029695717560320, journalId=1255847867265597444, articleId=1325131283453584287, language=CN, label=图2, caption=(a) 高压腔样品组装,(b) 烧结温度和烧结压力曲线, figureFileSmall=/kj3wBszmIcsh4usLeaK1A==, figureFileBig=7KwkciebMIckLuF9/tVs2g==, tableContent=null), ArticleFig(id=1325131295659009013, tenantId=1146029695717560320, journalId=1255847867265597444, articleId=1325131283453584287, language=EN, label=Fig. 3, caption=Fracture-surface SEM images of pure AlN ceramics prepared at 5.0 GPa and different sintering temperatures, figureFileSmall=Q9MP0XfqW8s9onGnpeQ5kQ==, figureFileBig=5G4Fq+qLfYYE3tAlhk8Ixw==, tableContent=null), ArticleFig(id=1325131295734506486, tenantId=1146029695717560320, journalId=1255847867265597444, articleId=1325131283453584287, language=CN, label=图3, caption=在5.0 GPa、不同烧结温度下制备的纯相AlN陶瓷断面的SEM图像, figureFileSmall=Q9MP0XfqW8s9onGnpeQ5kQ==, figureFileBig=5G4Fq+qLfYYE3tAlhk8Ixw==, tableContent=null), ArticleFig(id=1325131295810003959, tenantId=1146029695717560320, journalId=1255847867265597444, articleId=1325131283453584287, language=EN, label=Fig. 4, caption=(a) XRD patterns obtained at 5.0 GPa and different sintering temperatures; (b) variations in FWHM of the representative AlN reflections, (100), (002), (101), and (102), as a function of sintering temperature, figureFileSmall=DfiK8FoEO02ZwpJYx/K9xQ==, figureFileBig=vo8NbL7CEtvkJwri+2FK2g==, tableContent=null), ArticleFig(id=1325131295864529912, tenantId=1146029695717560320, journalId=1255847867265597444, articleId=1325131283453584287, language=CN, label=图4, caption=(a) 在5.0 GPa、不同烧结温度下的XRD谱,(b) AlN烧结样品代表性晶面(100)、(002)、(101)、(102)的XRD峰FWHM随烧结温度的变化, figureFileSmall=DfiK8FoEO02ZwpJYx/K9xQ==, figureFileBig=vo8NbL7CEtvkJwri+2FK2g==, tableContent=null), ArticleFig(id=1325131295944221689, tenantId=1146029695717560320, journalId=1255847867265597444, articleId=1325131283453584287, language=EN, label=Fig. 5, caption=(a) Relative density and thermal conductivity of AlN sintered bodies as a function of sintering temperature; (b) comparison between the thermal conductivity measured in this work and the thermal conductivity of pure AlN ceramics reported in previous studies, figureFileSmall=iYMqm8IigEstEnBA9YruCQ==, figureFileBig=WvdnzD+cvUXgSZ6GeP/05A==, tableContent=null), ArticleFig(id=1325131296019719162, tenantId=1146029695717560320, journalId=1255847867265597444, articleId=1325131283453584287, language=CN, label=图5, caption=(a) AlN烧结体的相对密度及热导率与烧结温度的关系,(b) 本实验测得的热导率与先前研究的纯AlN陶瓷的热导率的对比, figureFileSmall=iYMqm8IigEstEnBA9YruCQ==, figureFileBig=WvdnzD+cvUXgSZ6GeP/05A==, tableContent=null), ArticleFig(id=1325131296091022331, tenantId=1146029695717560320, journalId=1255847867265597444, articleId=1325131283453584287, language=EN, label=Fig. 6, caption=Polished cross-sectional BSE images of composite ceramics prepared at 5.0 GPa and 1400 ℃ with diamond volume fractions of 16.7%, 20.0%, 25.0%, and 33.3%, figureFileSmall=EjP8yhSvX1nYhIsHBhzzOQ==, figureFileBig=fRkgfdXHIazKv4pRHZvRdA==, tableContent=null), ArticleFig(id=1325131296158131196, tenantId=1146029695717560320, journalId=1255847867265597444, articleId=1325131283453584287, language=CN, label=图6, caption=在5.0 GPa、1400 ℃下制备的金刚石体积分数分别为16.7%、20.0%、25.0%、33.3%的复合陶瓷抛面BSE图像, figureFileSmall=EjP8yhSvX1nYhIsHBhzzOQ==, figureFileBig=fRkgfdXHIazKv4pRHZvRdA==, tableContent=null), ArticleFig(id=1325131296216851453, tenantId=1146029695717560320, journalId=1255847867265597444, articleId=1325131283453584287, language=EN, label=Fig. 7, caption=Fracture-surface SE-SEM images of composite ceramics prepared at 5.0 GPa and 1400 ℃ with diamond volume fractions of 16.7%, 20.0%, 25.0%, and 33.3%, figureFileSmall=IA4Bqya3URoB79D5OmPgGQ==, figureFileBig=3r8ZTpPUUnWG+C+E5elcGQ==, tableContent=null), ArticleFig(id=1325131296288154622, tenantId=1146029695717560320, journalId=1255847867265597444, articleId=1325131283453584287, language=CN, label=图7, caption=在5.0 GPa、1400 ℃下制备的金刚石体积分数分别为16.7%、20.0%、25.0%、33.3%的复合陶瓷断面SE-SEM图像, figureFileSmall=IA4Bqya3URoB79D5OmPgGQ==, figureFileBig=3r8ZTpPUUnWG+C+E5elcGQ==, tableContent=null), ArticleFig(id=1325131296413983743, tenantId=1146029695717560320, journalId=1255847867265597444, articleId=1325131283453584287, language=EN, label=Fig. 8, caption=(a) XRD patterns of sintered samples prepared from AlN/diamond mixed powders; (b) variation in the FWHM of the representative AlN reflections, (100), (002), and (101), and the representative diamond reflection, (111), with diamond volume fraction, figureFileSmall=s3cNRca1+zVKb6ltHWAqDw==, figureFileBig=skMRAe0cTLuwEH661mBPkw==, tableContent=null), ArticleFig(id=1325131296497869824, tenantId=1146029695717560320, journalId=1255847867265597444, articleId=1325131283453584287, language=CN, label=图8, caption=(a) AlN与金刚石混合粉末烧结样品的XRD谱,(b) AlN烧结样品代表性晶面(100)、(002)、(101)以及金刚石代表性晶面(111)衍射峰的FWHM随金刚石体积分数的变化, figureFileSmall=s3cNRca1+zVKb6ltHWAqDw==, figureFileBig=skMRAe0cTLuwEH661mBPkw==, tableContent=null), ArticleFig(id=1325131296569171968, tenantId=1146029695717560320, journalId=1255847867265597444, articleId=1325131283453584287, language=EN, label=Fig. 9, caption=(a) Relative density and thermal conductivity of AlN/diamond composite sintered bodies with different diamond volume fractions; (b) comparison of the thermal conductivity of the best-performing sample in this work with those of low-temperature additive-assisted sintered AlN ceramics reported in the literature, figureFileSmall=8FfVcXyZQWfE5Fjepj2sfQ==, figureFileBig=JDxnxogaO668FDXuTkteDg==, tableContent=null), ArticleFig(id=1325131296661446657, tenantId=1146029695717560320, journalId=1255847867265597444, articleId=1325131283453584287, language=CN, label=图9, caption=(a) 不同金刚石体积分数下AlN/金刚石复合陶瓷的相对密度与热导率,(b) 本研究所得最佳样品与文献报道的低温助剂烧结AlN陶瓷热导率的比较, figureFileSmall=8FfVcXyZQWfE5Fjepj2sfQ==, figureFileBig=JDxnxogaO668FDXuTkteDg==, tableContent=null), ArticleFig(id=1325131296741138434, tenantId=1146029695717560320, journalId=1255847867265597444, articleId=1325131283453584287, language=EN, label=Table 1, caption=Compositions of AlN/diamond mixtures, figureFileSmall=null, figureFileBig=null, tableContent=
Group No.AlN/diamond ratio (by vol.)ϕ/%
15∶116.7
24∶120.0
33∶125.0
42∶133.3
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氮化铝与金刚石的配比

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Group No.AlN/diamond ratio (by vol.)ϕ/%
15∶116.7
24∶120.0
33∶125.0
42∶133.3
), ArticleFig(id=1325131296946659332, tenantId=1146029695717560320, journalId=1255847867265597444, articleId=1325131283453584287, language=EN, label=Table 2, caption=SEM-EDS quantitative atomic compositions of the bright particles at grain boundaries in samples sintered at 1500−1700 ℃, with the 1400 ℃ sample included as a reference, figureFileSmall=null, figureFileBig=null, tableContent=
Temperature/℃Atom fraction of N/%Atom fraction of O/%Atom fraction of Al/%
140044.07±5.745.16±1.7150.77±6.30
150033.63±3.9328.43±4.9637.93±2.85
160035.30±5.0529.19±2.0735.51±3.26
170029.83±2.3632.94±3.8537.23±4.84
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1500~1700 ℃样品中晶界亮点颗粒的SEM-EDS原子组成分析结果(以1400 ℃样品为参考)

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Temperature/℃Atom fraction of N/%Atom fraction of O/%Atom fraction of Al/%
140044.07±5.745.16±1.7150.77±6.30
150033.63±3.9328.43±4.9637.93±2.85
160035.30±5.0529.19±2.0735.51±3.26
170029.83±2.3632.94±3.8537.23±4.84
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高温高压烧结AlN/金刚石复合材料的导热性
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龚发 1 , 梁文嘉 2 , 王齐明 1 , 李倩 1 , 刘洪汶 1 , 何沛宏 1 , 贺端威 1 , 彭放 1
高压物理学报 | 高压下的碳材料 2026,40(9): 090111-1-090111-11
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高压物理学报 |高压下的碳材料 2026 , 40 (9) : 090111-1 -090111-11
高温高压烧结AlN/金刚石复合材料的导热性
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龚发1 , 梁文嘉2, 王齐明1, 李倩1, 刘洪汶1, 何沛宏1, 贺端威1 , 彭放1
作者信息
  • 1四川大学原子与分子物理研究所, 四川 成都 610065
  • 2四川文理学院智能制造学院, 四川 达州 635002
通讯作者:
贺端威(1969-),男,博士,教授,主要从事高压物理、凝聚态物理、超硬材料研究. E-mail:
彭 放(1960-),男,博士,教授,主要从事高压物理、凝聚态物理、超硬材料研究. E-mail:
作者简介:

龚 发(2000-),女,硕士研究生,主要从事高压科学研究. E-mail:

Thermal Conductivity of AlN/Diamond Composites Sintered under High-Pressure and High-Temperature
Fa GONG1 , Wenjia LIANG2, Qiming WANG1, Qian LI1, Hongwen LIU1, Peihong HE1, Duanwei HE1 , Fang PENG1
Affiliations
  • 1Institute of Atomic and Molecular Physics, Sichuan University, Chengdu 610065, Sichuan, China
  • 2School of Intelligent Manufacturing, Sichuan University of Arts and Science, Dazhou 635002, Sichuan, China
出版时间: 2026-09-05 doi: 10.11858/gywlxb.20261071
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氮化铝(AlN)陶瓷是高功率电子器件散热的重要材料,然而,传统烧结方法的温度高,制约了其进一步应用,并提高了制备成本。因此,有必要发展在较低温度条件下实现AlN陶瓷致密化的制备方法。针对多晶AlN陶瓷在较低烧结温度下难以兼顾高致密化与高热导率的问题,采用分步研究思路。首先,研究纯相AlN在高压辅助下的致密化行为和导热性能,确定优化烧结条件。在无助剂、压力为5.0 GPa、温度为1400 ℃的条件下制备出晶界洁净、高致密的纯相AlN陶瓷,热导率达101.6 W/(m·K)。然后,在所确定的优化烧结条件下研究AlN/金刚石复合体系,系统考察金刚石含量对复合材料结构与性能的影响。结果表明,复合材料的热导率随金刚石体积分数的增加呈先降后升趋势,在金刚石体积分数为33.3%时达到112.4 W/(m·K)。机理分析表明:低金刚石含量时,界面热阻占主导;高金刚石含量时,金刚石形成的导热通路对热传导的增强作用更显著。研究工作充分发挥了高温高压技术优势,在比传统烧结技术更低的温度下实现了AlN基材料的大幅优化,为较低温制备高性能导热陶瓷提供了新途径。

氮化铝陶瓷  /  金刚石  /  高温高压  /  高压烧结  /  热导率

Aluminum nitride (AlN) ceramics are important heat-dissipation materials for high-power electronic devices. However, the high sintering temperature required by conventional processing routes limits practical application of AlN ceramics and increases fabrication costs. Therefore, it is necessary to develop preparation method that is capable of achieving densification at relatively low temperature. To address the difficulty of simultaneously obtaining high densification and high thermal conductivity in polycrystalline AlN ceramics under reduced-temperature sintering conditions, this work adopts a stepwise research strategy. First, the densification behavior and thermal conductivity of pure AlN under high-pressure assistance were investigated to identify the optimal sintering conditions. Under additive-free conditions, pure-phase AlN ceramics with clean grain boundaries and high densification were prepared at 5.0 GPa and 1400 ℃, achieving a thermal conductivity of 101.6 W/(m·K). Based on these optimized conditions, the AlN/diamond composite system was further studied, and the effects of diamond volume fraction on the structure and properties of the composites were systematically examined. The results show that the thermal conductivity of the composites first decreases and then increases with increasing diamond volume fraction, reaching 112.4 W/(m·K) at 33.3%. Mechanistic analysis indicates that interfacial thermal resistance dominates at low diamond contents, whereas at high diamond contents the enhancement of heat transport by thermally conductive diamond pathways becomes more significant. By taking full advantage of the processing benefits of high-temperature and high-pressure technology, this work achieves substantial improvement of AlN-based materials at temperatures lower than those required in conventional sintering, thereby providing a new route for the low-temperature fabrication of high-performance thermally conductive ceramics.

aluminum nitride ceramics  /  diamond  /  high-temperature and high-pressure  /  high-pressure sintering  /  thermal conductivity
龚发, 梁文嘉, 王齐明, 李倩, 刘洪汶, 何沛宏, 贺端威, 彭放. 高温高压烧结AlN/金刚石复合材料的导热性. 高压物理学报, 2026 , 40 (9) : 090111-1 -090111-11 . DOI: 10.11858/gywlxb.20261071
Fa GONG, Wenjia LIANG, Qiming WANG, Qian LI, Hongwen LIU, Peihong HE, Duanwei HE, Fang PENG. Thermal Conductivity of AlN/Diamond Composites Sintered under High-Pressure and High-Temperature[J]. Chinese Journal of High Pressure Physics, 2026 , 40 (9) : 090111-1 -090111-11 . DOI: 10.11858/gywlxb.20261071
随着高功率电子器件与先进封装技术向小型化、高集成度发展,对材料高效热传导能力的要求日益迫切。氮化铝(AlN)陶瓷因具有高热导率、优异的绝缘性以及与硅相匹配的热膨胀系数,成为理想的高功率散热材料[1–3]。然而,多晶AlN陶瓷的实际热导率通常远低于单晶理论值320 W/(m·K),这主要归因于材料内部孔隙、晶界以及氧杂质等缺陷对声子的强烈散射[4–5]。要实现高热导率,需要获得高致密、低缺陷的AlN微观结构。遗憾的是,AlN的强共价键特性导致其自扩散系数低、烧结致密化困难。在以往的研究中,Wang等[6]在1850 ℃下常压烧结4 h,所得的AlN陶瓷的热导率为87.1 W/(m·K)。Tang等[7]采用放电等离子烧结(spark plasma sintering,SPS)方法,在40 MPa、1800 ℃条件下烧结5 min,得到的AlN陶瓷的热导率为91.9 W/(m·K)。传统常压烧结需依赖高温,并且即便采用SPS等技术缩短烧结时间,对于纯AlN体系而言,仍难以在较低温度下实现高致密化与高热导率。目前,常用的解决方案是引入烧结助剂,通过液相烧结促进致密化,并净化晶格氧。以Huang等[8]的研究为例,其采用流延成形法在常压、1850 ℃条件下保温10 h(添加质量分数为8%的Y2O3)制备了AlN基板,其室温热导率高达205 W/(m·K)。由此可见,要获得高热导AlN陶瓷,通常需要依赖1700~1900 ℃的高温烧结窗口。然而,若将烧结窗口降至1400~1500 ℃,则致密化与热导率均面临严重制约。例如,采用SPS等快速烧结技术在低温下获得的AlN陶瓷的热导率多处于30~80 W/(m·K)范围[9]。上述结果一致表明,在低温条件下,晶界与各类缺陷对声子传输仍具有明显的散射作用,严重限制了热导率的提升。
基于此,本研究提出一种分步研究思路,旨在实现相对较低烧结温度窗口下AlN陶瓷热导率的有效提升[10–11]。首先,在无助剂条件下通过高温高压技术制备高致密、晶界洁净的AlN陶瓷基体,从而在较低温度下实现纯相材料的充分致密化。在此基础上,为进一步提高导热性能,创新性地引入高导热填料,以构建新的热导通路。鉴于金刚石具有极高的热导率(约2000 W/(m·K))和良好的绝缘性[12–13],选择金刚石作为增强相。当填料含量提高到能够形成有效导热通路时,体系的导热能力有望进一步增强。本研究的关键在于将纯相AlN在高压条件下的相对低温致密化研究与AlN/金刚石复合体系的导热调控结合起来,在低于传统AlN烧结温度的条件下实现热导率提升,从而为低温制备高导热绝缘陶瓷材料提供新的思路。
分别以纯AlN粉末、AlN/金刚石混合粉末为原料进行2组实验研究。
在第1组实验中,初始材料为上海超威纳米科技有限公司生产的AlN粉末(纯度99.9%),粒径范围为6~8 μm。图1显示了初始材料的扫描电子显微镜(scanning electron microscope, SEM)图像和X射线衍射(X-ray diffraction, XRD)谱。为了消除粉末表面吸附的杂质气体,在WZB-20型真空炉中对样品进行真空热处理;在烧结之前,将起始粉末置于钼(Mo)杯中,并预压缩至20 MPa,以形成直径约11.8 mm、高度约5.0 mm的圆柱体。为了消除钼表面的氧化物,在进行高温高压(high-pressure and high-temperature, HPHT)烧结之前,将钼在稀盐酸中浸泡10 min。使用室温下钡、铊和铋的压力诱导相变来校准烧结腔体压力[14],采用D型热电偶(W97Re3-W75Re25)标定温度[15]。HPHT烧结实验所用的高压腔样品组装如图2(a) 所示。采用DS6×14 MN六面顶压机进行HPHT烧结实验,图2(b)为烧结压力和烧结温度变化曲线。首先,将样品在室温下压缩至5.0 GPa的目标压力;然后,以100 ℃/min的速率加热至目标温度,保持10 min;烧结结束后,先将温度降至室温,而后降压,降压过程中设置一定的退火时间及保压时间,以消除样品内部的残余应力。
在第2组实验中,系统研究了金刚石的体积分数(ϕ)对复合材料性能的影响。所用金刚石粉末的平均晶粒尺寸为20 μm(纯度99.9%)。具体实验组别设计如表1所示。在HPHT合成前,将各比例的前驱体材料与无水乙醇在混料机中充分混合12 h。将混合物粉末以与第1组实验相同的流程进行组装,并在精确的温度和压力条件下烧结。为了便于后续表征,将烧结后的样品加工成直径为10 mm、高度为1~2 mm的圆柱体。
通过XRD(DX-2700,Cu Kα,波长λ=1.54056 Å)分析烧结样品的相组成。使用SEM(JSM-IT 500 HR)观察原料AlN粉末的形态和陶瓷的断裂表面。采用阿基米德原理,利用FK-120 Y型多功能固体密度计测定烧结试样的密度。使用激光导热分析仪(LFA1000),在室温(25 ℃)下进行热导率测试。测试前,在样品双面喷涂石墨涂层(厚度小于10 μm),确保红外吸收率大于95%。室温热导率k为
$ k=\alpha \rho {c}_{p} $
式中:α为激光闪射法实测的热扩散率;ρ为阿基米德法测得的体密度;cp为比定压热容,由石墨标准样品参比的比较法获得。每个样品重复测试 10 次,取平均值。
为探究烧结温度对纯多晶AlN微观结构的影响,在5.0 GPa压力下对600~1700 ℃烧结样品的断面进行SEM表征,如图3所示。结果表明:当温度低于1000 ℃时(图3(a)~图3(c)),样品呈现典型的颗粒堆积形貌,晶粒形状不规则,晶界粗糙且起伏明显,断面以沿晶断裂为主,存在较多孔隙;温度升至1200 ℃后(图3(d)),颗粒边缘形貌趋于规则,断裂模式开始向穿晶断裂过渡;当烧结温度为1400 ℃(图3(e))时,样品断面孔隙显著减少,晶粒普遍发育为规则多边形,且尺寸分布集中, 晶界连续;当温度升至1500~1700 ℃时(图3(f)~图3(h)),基体中沿晶界析出亮点状颗粒,局部晶界起伏增大,并伴有少量孔隙复现,导致界面连续性下降,晶粒尺寸较1400 ℃时未见明显变化。对晶界亮点颗粒进行了点扫能谱仪(energy dispersive spectroscopy,EDS)分析,结果见表2。与1400 ℃样品相比,1500~1700 ℃样品中该区域的O原子分数明显增加,而N原子分数整体下降,说明高温下晶界处出现了明显的氧富集现象。
为探究5.0 GPa高压烧结条件下AlN陶瓷的结构演变,对600~1700 ℃ 烧结样品进行了XRD分析。图4(a)表明,在600~1400 ℃温度范围内,仅有六方AlN的衍射特征峰,说明所得样品均为纯相AlN,未分解或生成其他杂相。当温度升至1500 ℃及以上时,图谱中开始出现α-Al2O3衍射峰,表明高温阶段发生了氧化反应[16]。这一结果与表2中晶界亮点颗粒区域氧含量增加的特征一致。对AlN的代表性晶面衍射峰的半高全宽(full width at half maximum, FWHM)进行分析,如图4(b)所示。在600~1400 ℃区间,FWHM随温度升高而整体下降,于1400 ℃ 达到最小;在1500 ℃时,FWHM出现回升;随后在1500~1700 ℃ 区间再次呈下降趋势。根据Williamson-Hall关系可知,XRD峰展宽主要源于晶粒尺寸效应与微应变效应,图3(a)~图3(h)表明,不同烧结温度下样品组织演变主要体现为孔隙状态、颗粒结合程度及晶界结构的变化,未见明显晶粒尺寸变化。因此,XRD峰展宽主要与晶体缺陷及残余应力演化有关[17–19]。结合断口SEM图像(图3(a)~图3(e))可知,在600~1400 ℃温区内,材料孔隙逐渐减少,并于1400 ℃达到最致密状态。该致密化过程有利于晶体缺陷的减少与残余应力的释放,从而显著降低微应变。因此,该温区FWHM的持续下降主要归因于致密化导致的微应变减小。升温至1500 ℃后,断口出现孔隙复现与晶界析出,同时检测到 α-Al2O3副相;在此条件下,副相的形成容易导致晶界连续性下降和引入局部应力不均,从而增强微应变对峰展宽的贡献,并导致FWHM回升。而在1500~1700 ℃区间,FWHM再次下降,可能与高温下缺陷重排及残余应力进一步释放有关。
AlN陶瓷的室温热导率随烧结温度的变化如图5(a)所示。在600~1400 ℃区间,热导率从约33 W/(m·K)迅速升高,并于1400 ℃达到峰值,约101.6 W/(m·K);当继续升温至1500 ℃后,热导率骤降至约40 W/(m·K);随后在1600~1700 ℃区间小幅回升至49~51 W/(m·K),但仍远低于1400 ℃时的最优值。该变化主要受孔隙率、晶体缺陷、残余应力以及晶界状态的影响[10, 20–21]。在600~1000 ℃阶段,相对密度由96.9%增至98.3%,热导率大幅上升,说明孔隙减少降低了声子散射;在1000~1400 ℃阶段,样品保持AlN单相,XRD峰的FWHM随温度升高持续减小,至1400 ℃降至最低,反映晶体缺陷与残余应力显著降低[22]。SEM分析表明,1400 ℃样品转变为穿晶断裂,晶界连续且变得较为模糊,说明晶界结合增强,该变化显著降低了声子在晶界的散射。二者的协同作用使得样品在1400 ℃达到热导率峰值。当温度升至1500 ℃后,样品虽进一步致密,但热导率却大幅下降。XRD结果显示,此温度下生成了α-Al2O3第二相,且AlN衍射峰的FWHM回升。结合SEM图像中晶界处观察到的析出物与孔隙,说明高温下晶界发生氧化反应,破坏了界面连续性,并引起局部应力集中,从而显著增强声子散射,最终导致热导率骤降。在1600~1700 ℃更高温度区间,热导率略有回升,同时XRD峰的FWHM再次减小,说明内部应力和缺陷得到部分缓解。然而,由于晶界第二相未能完全消除,热导率始终无法恢复至1400 ℃时的峰值。综上所述,仅需1400 ℃(5.0 GPa)即可获得101.6 W/(m·K)的高热导率,性能达到文献[6, 23–27]中1800 ℃以上才能达到的水平(图5(b))。这证明了高温高压烧结技术优化结构从而获得高性能的有效性。
为探索AlN/金刚石体系烧结过程中金刚石体积分数对微观结构演变的影响,在5.0 GPa、1400 ℃的烧结条件下,对不同金刚石体积分数样品的断面进行了SEM表征。图6显示,样品中存在灰、黑2种不同衬度的区域。结合背散射电子(back-scattered electron, BSE)图像衬度特征分析,可判断灰色连续相为AlN基体,黑色区域对应金刚石相。随着金刚石体积分数从16.7%增加至33.3%,可观察到代表金刚石的黑色区域面积显著增加,颗粒间距减小,且颗粒之间出现更多局部聚集、接触甚至形成连通趋势,表明金刚石相逐渐从孤立分布向局部聚集并形成网络连通过渡。此外,从图7可观察到金刚石颗粒边缘及聚集区域存在细微缝隙,这主要是由AlN与金刚石之间的热膨胀系数及弹性模量差异所致。在样品冷却降压过程中,界面附近因收缩不均而产生应力集中,进而诱发局部开裂[28–29]。
为探究5.0 GPa、1400 ℃下AlN/金刚石复合陶瓷的物相组成,对加入不同金刚石体积分数的AlN/金刚石复合样品进行了XRD分析,结果如图8(a)所示。可以看出,所有样品的XRD谱中仅检测到六方AlN与金刚石两相,未发现杂相衍射峰,表明材料在烧结后未发生明显的界面反应。进一步对各样品中AlN的(100)、(002)、(101)晶面以及金刚石(111)晶面衍射峰的FWHM进行定量分析,结果如图8(b)所示。随着金刚石含量增加,各代表峰的FWHM均呈现逐渐展宽的趋势。结合SEM分析结果可知,两相界面因热膨胀系数差异产生残余应力。随着金刚石含量增加,单位体积内的界面面积增加,残余应力分布范围扩大,微应变相应提高,最终在XRD谱中表现为衍射峰的系统性宽化[30–31]。
如图9(a)所示,随着金刚石体积分数ϕ的增加,AlN/金刚石复合陶瓷的热导率呈现先下降后上升的非单调变化趋势。以纯AlN陶瓷的热导率k0=101.6 W/(m·K)为参照,当ϕ=16.7%时,热导率下降至83.6 W/(m·K);随后热导率逐渐回升,在ϕ=25.0%时已超过纯AlN陶瓷;当ϕ=33.3%时,热导率进一步提升至112.4 W/(m·K)。这一趋势反映了材料内部热传导的主导机制随组分发生了转变。当金刚石含量较低时,AlN为连续相,金刚石作为分散相分布其中,热流主要沿AlN相传导。在此过程中,热流需反复穿过AlN/金刚石界面,从而受到界面热阻(interfacial thermal resistance, ITR)的影响。定义界面热阻RK为跨界面温降ΔT与界面法向热流密度q之比[32],即
$ {R}_{\text{K}}={\Delta }T/q $
式(2)表明,当热流垂直通过单位面积界面时,会因界面热阻而产生温降。实际材料中,热流会穿过大量界面,因此,需从宏观尺度评估其总体贡献。若将金刚石颗粒简化为半径为a的球体模型,则单位体积内的界面面密度[33]可近似为
$ \frac{{A}_{\text{int}}}{V}\approx \frac{3\varphi }{a} $
式中:Aint为总界面面积,V为样品总体积。式(3)表明,当固定金刚石颗粒半径a时,界面密度Aint/V随ϕ线性增加。从量纲角度分析,RK的量纲为m2·K·W−1,Aint/V的量纲为m−1,二者乘积与热阻率1/k的量纲一致,因此,界面效应在宏观上表现为对整体热阻率的附加贡献,并可初步估算为
$ {\Delta }\frac{1}{k}\sim {R}_{\text{K}} \frac{{A}_{\text{int}}}{V}=\frac{3\varphi {R}_{\text{K}}}{a} $
式(4)说明,在低ϕ 阶段,当热流主要沿AlN相传输并反复穿过界面,且a和RK固定时,整体热阻率的附加贡献随ϕ线性上升[34]。此外,尽管图9(a)显示样品的致密度随ϕ变化不大,但XRD峰展宽表明,随着ϕ增加,两相内部的缺陷与应变等声子散射源增强。对于以声子导热的AlN与金刚石,其热导率[35]可表示为
$ k=\frac{1}{3}Cvl $
式中:C 为体热容,v为声子群速度,l 为声子的平均自由程。缺陷与应变会加剧声子散射,降低 l,从而使得两相的实际热导率低于理想值。为此,本研究引入基线有效热导率kbase(ϕ),将其定义为仅考虑缺陷与应变导致的热导率衰减、不计入界面热阻RK时的理论值[34]。因此,在低ϕ阶段,热传导同时受到两相自身导热性能下降与界面附加热阻增加的双重抑制。此时,金刚石尚未形成有效导热通路,体系的有效热导率可定性表示为
$ \frac{1}{{k}_{\text{eff}}}\approx \frac{1}{{k}_{\text{base}}\left(\varphi \right)}+\frac{3\varphi {R}_{\text{K}}}{a}\;\;\;\;\;\;\;\;\;\varphi \lt {\varphi }_{\text{c}} $
式中:keff为实测有效热导率,ϕc为金刚石形成导热通路的临界阈值。式(6)表明,在ϕ<ϕc区间,随着ϕ增加,keff呈下降趋势。需要指出的是,式(6)中线性项3ϕRK/a成立的前提是热流反复穿越大量孤立界面,一旦金刚石逐渐连通形成导热通路,该表达形式及其权重将发生改变[36]。
当ϕ=25.0%时,颗粒间距缩小,相互接触概率增大,逐渐形成连通的导热网络。此时,热传导路径从主要由AlN基体承担,转变为AlN基体与金刚石网络并行的混合模式。这种连通结构带来的增强效应可采用连通导热网络的临界标度关系[37–38]进行定性描述
$ {k}_{\text{net}}\left(\varphi \right)\propto {\left(\varphi -{\varphi }_{\text{c}}\right)}^{t} $
式中:t为临界指数,knet为金刚石网络带来的额外导热贡献。式(7)表明,当ϕ达到甚至超过ϕc后,贯通的高导热通路形成,其贡献随ϕ呈幂指数增长。需要注意的是,在此阶段,XRD分析显示两相内部缺陷与应变仍在增强,两相自身导热性能持续下降,同时RK仍然存在。因此,整体热导率的变化取决于knet带来的增益与上述因素造成的热阻增加之间的竞争。当 $ {k}_{\text{net}} $增益占主导时,体系热导率超过纯AlN,即当ϕ≥25.0%时,样品的热导率高于纯AlN的热导率 $ {k}_{0} $。总之,通过在高压条件下实现AlN基体的低温致密化,并引入金刚石构建补充导热通路,在5.0 GPa、1400 ℃条件下制备的AlN/金刚石复合陶瓷在ϕ=33.3%时获得了112.4 W/(m·K)的热导率。为进一步评估其在较低烧结温度窗口下的性能,图9(b)给出了本工作最佳样品与文献[9, 27, 39]报道的低温助剂烧结AlN陶瓷结果的比较。可以看出,本研究所得样品的热导率较Kobayashi等[9]在约1450 ℃烧结样品的热导率(30~80 W/(m·K))提升了40.5%~274.7%,较Kim等[39]在1500 ℃低温热压获得的约91.2 W/(m·K)提升约23.2%,相比He等[27]在1400 ℃下烧结得到的AlN陶瓷热导率9.3 W/(m·K),提升幅度更大。
采用高温高压烧结方法,系统研究了纯相AlN陶瓷在5.0 GPa和相对较低的烧结温度条件下的致密化行为及导热性能,并在此基础上通过引入金刚石构建AlN/金刚石复合材料,进一步探讨了金刚石体积分数对复合体系导热性能的影响,得到如下主要结论。
(1) 在5.0 GPa、1400 ℃条件下成功制备出高致密纯相AlN陶瓷,其热导率达到101.6 W/(m·K),大部分高于常规高温烧结条件下的水平,说明高温高压烧结技术有利于在相对较低的温度下促进AlN陶瓷致密化,并实现导热性能的提升。
(2) 在固定5.0 GPa条件下,烧结温度对AlN陶瓷的物相组成及热导率具有显著影响。当烧结温度升高至1500 ℃以上时,样品中开始出现α-Al2O3杂相,说明高温条件下氧化反应加剧,与此同时,热导率明显下降,表明氧化杂相的形成及相关结构缺陷会对热传导产生不利影响。
(3) 在5.0 GPa、1400 ℃这一优化烧结条件下,进一步研究了AlN/金刚石复合材料的导热行为。复合材料的热导率随金刚石体积分数增加呈现先下降后上升的变化规律。当金刚石的体积分数为33.3%时,复合材料的热导率达到112.4 W/(m·K)。这说明在较低金刚石含量下,界面热阻对热传导的抑制作用较为明显,而在较高金刚石含量下,金刚石逐渐形成有效导热通路,其增强作用逐步占据主导。

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2026年第40卷第9期
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doi: 10.11858/gywlxb.20261071
  • 接收时间:2026-04-02
  • 首发时间:2026-11-05
  • 出版时间:2026-09-05
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  • 收稿日期:2026-04-02
  • 修回日期:2026-04-24
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    1四川大学原子与分子物理研究所, 四川 成都 610065
    2四川文理学院智能制造学院, 四川 达州 635002

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贺端威(1969-),男,博士,教授,主要从事高压物理、凝聚态物理、超硬材料研究. E-mail:
彭 放(1960-),男,博士,教授,主要从事高压物理、凝聚态物理、超硬材料研究. E-mail:
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2种不同金属材料的力学参数
科
Family
属数
Number of
genus
种数
Number of
species
占总种数比例
Percentage of
total species (%)
属
Genus
种数
Number of
species
占总种数比例
Percentage of total
species (%)
鹅膏菌科Amanitaceae 2 11 5.26 鹅膏菌属 Amanita 10 4.78
小菇科 Mycenaceae 2 12 5.74 丝盖伞属 Inocybe 5 2.39
多孔菌科 Polyporaceae 8 14 6.70 蜡蘑属 Laccaria 5 2.39
红菇科 Russulaceae 3 23 11.00 小皮伞属 Marasmius 6 2.87
小菇属 Mycena 11 5.26
光柄菇属 Pluteus 5 2.39
红菇属 Russula 17 8.13
栓菌属 Trametes 5 2.39
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