粉末热压法制备高性能n型PVDF/Ag2Se自支撑柔性复合热电薄膜OA
High-performance n-type PVDF/Ag2Se Free-standing Flexible Composite Thermoelectric Films Fabricated by Powder Hot-pressing
可穿戴设备、微电子器件和物联网等领域应用的快速发展,对自支撑柔性薄膜热电材料提出了迫切需求.当前,n 型自支撑有机/无机复合柔性薄膜热电材料的研究进展滞后,亟需通过优化制备工艺来提升薄膜性能.本研究采用简便高效的粉末热压工艺,开发出高性能 n 型聚偏氟乙烯/硒化银(PVDF/Ag2Se)自支撑柔性复合热电薄膜.热压过程的高温高压环境诱导 Ag2Se 晶粒再结晶和长大,有效减少了晶界数量,显著降低了载流子散射和界面电阻,从而使载流子迁移率、电导率和塞贝克系数同步提升.并且,热压过程中熔融态 PVDF 能填充 Ag2Se 导电网络的间隙,在提高材料致密度的同时显著增强了柔韧性.实验结果表明,Ag2Se 质量分数为 80%的热压复合薄膜展现出优异的室温热电性能:电导率达 277.0 S·cm-1,塞贝克系数为-135 μV·K-1,功率因子(PF)和热电优值(ZT)分别达到 509 μW·m-1·K-1 和 0.26.这些性能不仅显著优于已报道的同类型 PVDF/Ag2Se 自支撑薄膜,在 Ag2Se 基有机/无机复合自支撑柔性热电薄膜中也处于领先水平.力学性能测试显示,该薄膜在 5 mm 半径下经过 500 次弯曲循环后,电导率保持率仍超过 92%,最大拉伸应变是纯 Ag2Se 薄膜的 4 倍.本研究为有机/无机复合热电材料中热电性能与力学柔性的协同优化提供了新思路.
Rapid development of applications in wearable devices,microelectronics,and internet of things has created an urgent demand for free-standing flexible thermoelectric films.Currently,research on n-type free-standing flexible thermoelectric films significantly lags behind,and there is an urgent need to enhance film performance through the optimization of preparation processes.In this study,high-performance n-type poly(vinylidene fluoride)/silver selenide(PVDF/Ag2Se)free-standing flexible thermoelectric composite films were developed using a simple and efficient powder hot-pressing method.The high-temperature and high-pressure conditions during hot pressing induced recrystallization and grain growth of Ag2Se,effectively reducing grain boundary density,significantly decreasing carrier scattering and interfacial resistance,thereby simultaneously enhancing carrier mobility,electrical conductivity and Seebeck coefficient.Meanwhile,the melted PVDF filled interstices of the Ag2Se conductive network during hot pressing,substantially improving material flexibility while increasing density.Experimental results demonstrate that the hot-pressed sample with 80%(in mass)Ag2Se exhibits outstanding room-temperature thermoelectric performance with an electrical conductivity of 277.0 S·cm-1 and a Seebeck coefficient of-135 μV·K-1,and thermoelectric power factor(PF)and estimated figure of merit(ZT)reach 509 μW·m-1·K-2 and 0.26,respectively.This performance not only significantly surpasses that of previously reported PVDF/Ag2Se free-standing films but also ranks among the highest for all reported Ag2Se-based organic/inorganic free-standing flexible thermoelectric films.Furthermore,mechanical tests reveal that the film maintains over 92%of its original conductivity after 500 bending cycles at a 5 mm radius,while exhibiting a maximum tensile strain four times greater than pure Ag2Se films.This study provides a novel strategy for synergistic optimization of thermoelectric performance and mechanical flexibility in organic/inorganic composite thermoelectric materials.
徐子硕;胡悦娟;胡宇晨;陈立东;姚琴
中国科学院 上海硅酸盐研究所,关键陶瓷材料全国重点实验室,上海 200050||中国科学院大学 材料科学与光电工程中心,北京 100049中国科学院 上海硅酸盐研究所,关键陶瓷材料全国重点实验室,上海 200050||中国科学院大学 材料科学与光电工程中心,北京 100049中国科学院 上海硅酸盐研究所,关键陶瓷材料全国重点实验室,上海 200050||上海科技大学 物质科学与技术学院,上海 201210中国科学院 上海硅酸盐研究所,关键陶瓷材料全国重点实验室,上海 200050||中国科学院大学 材料科学与光电工程中心,北京 100049中国科学院 上海硅酸盐研究所,关键陶瓷材料全国重点实验室,上海 200050||中国科学院大学 材料科学与光电工程中心,北京 100049
通用工业技术
硒化银复合热电薄膜自支撑柔性热压
silver selenidecomposite thermoelectric filmfree-standingflexiblehot-pressing
《无机材料学报》 2026 (4)
462-468,中插5,8
国家自然科学基金(U23A20685)国家重点研发计划(2024YFF0505900) National Natural Science Foundation of China(U23A20685)National Key Research and Development Program of China(2024YFF0505900)
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