Article(id=1320095757999395377, tenantId=1146029695717560320, journalId=1263187385517883426, issueId=1320095743872971684, articleNumber=null, orderNo=null, doi=10.14062/j.issn.0454-5648.20250535, pmid=null, cstr=null, oa=null, hot=null, price=null, onlineType=0, articleFormat=0, articleType=null, articleTypeStr=null, receivedDate=1751904000000, receivedDateStr=2025-07-08, revisedDate=1759507200000, revisedDateStr=2025-10-04, acceptedDate=null, acceptedDateStr=null, onlineDate=1792664954900, onlineDateStr=2026-10-22, pubDate=1778515200000, pubDateStr=2026-05-12, doiRegisterDate=null, doiRegisterDateStr=null, onlineIssueDate=1792664954900, onlineIssueDateStr=2026-10-22, onlineJustAcceptDate=null, onlineJustAcceptDateStr=null, onlineFirstDate=null, onlineFirstDateStr=null, sourceXml=null, magXml=null, createTime=1792664954900, creator=13701087609, updateTime=1792664954900, updator=13701087609, issue=Issue{id=1320095743872971684, tenantId=1146029695717560320, journalId=1263187385517883426, year='2026', volume='54', issue='6', pageStart='1881', pageEnd='2170', issueExtLink='null', onlineDate='null', pubDate='1781884800000', pubDateStr='2026-06-20', beforeIssueId=null, nextIssueId=null, price=null, status=1, issueComplete=1, articleOrder=1, issueType=-1, specialIssue=null, createTime=1792664951531, creator='13701087609', updateTime=1792738533970, updator='13701087609', preIssue=null, nextIssue=null, articleTotal=null, ext={EN=IssueExt(id=1320404371276411812, tenantId=1146029695717560320, journalId=1263187385517883426, issueId=1320095743872971684, language=EN, specialIssueTitle=, coverIllustrator=null, specialIssueEditor=, specialIssueAbout=), CN=IssueExt(id=1320404371276411813, tenantId=1146029695717560320, journalId=1263187385517883426, issueId=1320095743872971684, language=CN, specialIssueTitle=, coverIllustrator=null, specialIssueEditor=, specialIssueAbout=)}, issueFiles=null, downloadFileDto=null}, startPage=2080, endPage=2090, ext={EN=ArticleExt(id=1320095758192333362, articleId=1320095757999395377, tenantId=1146029695717560320, journalId=1263187385517883426, language=EN, title=Structural Stability of SiO
2@Al
2O
3 Hollow Particles at High Temperature, columnId=1263922769897599102, journalTitle=Journal of the Chinese Ceramic Society, columnName=Research Articles, runingTitle=null, highlight=null, articleAbstract=
Introduction Cutting-edge technologies such as hypersonic vehicles and reusable launch systems impose stringent requirements on thermal protection system, demanding for ultra-lightweight materials with extremely low thermal conductivity and high-temperature stability. Conventional SiO2 aerogels suffer from rapid sintering and densification at elevated temperatures, leading to pore collapse and decline in thermal insulation performance. Although introducing high-melting-point oxides or increasing particle size can delay the sintering process, it often results in a trade-off between thermal stability and insulation performance. To overcome this bottleneck, a hollow-core-shell synergistic design strategy is proposed. This approach is expected to simultaneously maintain low density and low thermal conductivity, while significantly enhancing the material's thermal stability via coupling the effects of micro-nano pore regulation and interfacial phonon scattering. In this work, the influence of Al2O3 coating thickness on the density, thermal conductivity, and thermal stability of large hollow particles of SiO2 coated with Al2O3 (SiO2@Al2O3) was investigated. The evolution behavior of this composite structure at high temperatures was elucidated, and the mechanism by which the Al2O3 shell could suppress a liquid-like atomic diffusion was revealed, providing some insights and theoretical guidance for the development of next-generation high-performance thermal insulation materials.
Methods A hard-template-assisted precipitation method was employed to synthesize SiO2@Al2O3 hollow particles. Polystyrene microspheres were used as templates, on which SiO2 was deposited to form large hollow structures. After calcination to remove the PS cores, SiO2 hollow particles were obtained. The SiO2 particles were dispersed in an aqueous phase, and Al(OH)3 was in-situ precipitated on their surfaces via the dropwise addition of AlCl3 and NaOH solutions with cetyltrimethyl ammonium bromide (CTAB) as a dispersant. Subsequent high-temperature calcination converted the hydroxide layer into an Al2O3 coating, yielding SiO2@Al2O3 core-shell hollow particles. A series of samples with different Al/Si mass ratios (i.e., 1%, 5%, and 10%) were prepared via adjusting the amount of AlCl3. The morphological evolution of the materials at 25-1200 ℃ was monitored in real time by in-situ transmission electron microscopy. The effective thermal conductivity of the samples at 25-1100 ℃ was measured by a Hot Disk thermal constants analyzer and the laser flash method. Furthermore, the molecular dynamics simulations were performed by Large-scale Atomic/Molecular Massively Parallel Simulator (LAMMPS), and a "liquid-like atom" cluster identification algorithm was applied to reveal the mechanism by which the Al2O3 shell could suppress surface diffusion and particle sintering in an atomic scale.
Results and discussion The results of in-situ TEM sintering experiments reveal that uncoated SiO2 hollow particles exhibit significant shrinkage and rupture at 1200 ℃ for only 2 min. In contrast, the sample coated with 3.9% Al2O3 (the sample with Al/Si of 5%) maintains its hollow structure after 30 min under the same conditions, with a linear shrinkage ratio of below 9%. However, the excessive coating (e.g., 10%) leads to the formation of a continuous Al2O3 layer between particles, increasing the effective contact area and promoting high-temperature mass transport and densification. The thermal property measurements further demonstrate that the 3.9% Al2O3-coated sample exhibits an ultralow effective thermal conductivity of 0.036 W·m-1·K-1 at 25 ℃, and a moderate increase to 0.074 W·m-1·K-1 at 1100 ℃, indicating the excellent high-temperature thermal insulation performance. The initial density of this sample is 0.268 6 g·cm-3, which is 14% lower than that of SiO2 solid nanoparticles with the size of 10 nm and shows a minimal variation (i.e., 0.268 6-0.298 8 g·cm-3) at 25-1200 ℃. Its effective thermal conductivity remains below that of various fiber-reinforced aerogel systems in the literature. The molecular dynamics simulations based on LAMMPS reveal the atomic-scale mechanism underlying the high-temperature stability of the Al2O3 shell. During heating, the number of "liquid-like atom" clusters increases continuously, while effectively suppressing their size growthes. This behavior significantly delays the kinetics of cluster coalescence, elevating the surface fusion completion temperature from approximately 1000 K in the uncoated system to 1500 K. The Al2O3 shell effectively delays the transition from surface diffusion-dominated sintering to volume diffusion-dominated sintering, providing the related mechanism and theoretical foundation for overcoming the intrinsic trade-off between low thermal conductivity and high-temperature stability.
Conclusions This study proposed a "large hollow structure with Al2O3 shell" synergistic design, enabling the controllable fabrication of SiO2@Al2O3 particles that could combine a structural stability at 1200 ℃ with ultralow thermal conductivity and low density. At 3.9% Al2O3 coating, the particles maintained a shrinkage ratio of below 9% after 30-min high-temperature exposure. The effective thermal conductivity increased modestly from 0.036 W·m-1·K-1 at 25 ℃ to 0.074 W·m-1·K-1 at 1100 ℃, while the density was 14% lower than that of conventional SiO2 solid nanoparticles with the size of 10 nm. The in-situ TEM spectra and molecular dynamics simulations confirmed that the Al2O3 shell significantly delayed sintering via suppressing cluster coalescence and the surface diffusion of liquid-like atoms, thus elucidating the high-temperature stabilization mechanism across multiple scales. This strategy could provide both experimental and theoretical foundations for controllable preparation of lightweight and high-temperature thermal insulating materials, offering a substantial engineering value for thermal protection in extreme environments and for additive manufacturing of complex lightweight thermal structures.
, authors=Qiaoling SI, Mingyang YANG, Rui YANG, Guihua TANG, authorsList=Qiaoling SI, Mingyang YANG, Rui YANG, Guihua TANG, authorCompany=null, correspAuthors=Guihua TANG, authorNote=
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2O
3包覆SiO
2大空心颗粒的制备及其高温结构稳定性, columnId=1263922770220560512, journalTitle=硅酸盐学报, columnName=研究论文, runingTitle=null, highlight=null, articleAbstract=
抑制纳米多孔隔热材料高温烧结、提升其结构稳定性是拓展使役温度的首要环节。采用硬模板辅助沉淀法制备了Al2O3包覆的SiO2大空心颗粒（大空心颗粒SiO2@Al2O3，直径约130 nm，壁厚约15 nm），协同利用Al2O3的抗烧结性与SiO2空心结构的低热导率、低密度优势，解决传统隔热材料热导率与结构热稳定性难以兼顾的难题。原位TEM结果表明，当Al2O3包覆量为3.9%（质量分数）时，颗粒经1200 ℃热处理30 min后仍保持空心结构完整，收缩率<9%；而未包覆SiO2大空心颗粒仅2 min即显著收缩并破裂。该样品室温有效热导率为0.036 W·m-1·K-1，1100 ℃条件下仅升至0.074 W·m-1·K-1，密度低至0.268 6 g·cm-3，较10 nm实心SiO2颗粒（密度0.312 8 g·cm-3）降低14%。基于分子动力学模拟，系统揭示了升温过程中该复合颗粒的高温演化行为，阐明了Al2O3壳层抑制类液态原子扩散的作用机制，该制备策略为轻质、高流动性高温隔热粉体的可控制备提供了实验与理论依据。
, authors=司巧玲, 杨铭扬, 杨睿, 唐桂华, authorsList=司巧玲, 杨铭扬, 杨睿, 唐桂华, authorCompany=null, correspAuthors=唐桂华, authorNote=
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唐桂华（1974—），男，教授。
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SI Qiaoling (1996-), female, Doctoral candidate. E-mail: 2696800067@qq.com
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司巧玲（1996—），女，博士研究生。
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