Structural Regulation of Poly(benzoxazole imide)s and Their Composites with Fluorinated Graphene to Construct High-Performance Low Dielectric Films

Structural Regulation of Poly(benzoxazole imide)s and Their Composites with Fluorinated Graphene to Construct High-Performance Low Dielectric Films
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聚苯并恶唑酰亚胺及其与氟化石墨烯的复合材料的结构调控构建高性能低介电薄膜

DOI:
10.1021/acsapm.2c01729
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发表时间:
2022-12
影响因子:
5
通讯作者:
Bo Zhang
Bo Zhang
中科院分区:
化学2区
文献类型:
--
作者:
Zihua Yu;Shaohua Wu;Chuncheng Li;Yaonan Xiao;Jiajian Liu;Bo Zhang

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较差的加工性能长期以来限制了聚苯并恶唑在微电子领域的广泛应用。在此,通过5-氨基-2-(4-氨基苯)苯并恶唑与3,3',4,4'-联苯四甲酸二酐和4,4'-(六氟亚异丙叉)二邻苯二甲酸的聚合,设计并制备了一系列聚苯并恶唑酰亚胺(PBOI)共聚物。 酸酐。这些 PBOI 共聚物通过将预先形成的苯并恶唑结构整合到聚酰亚胺主链中,表现出优异的成膜性能。此外,PBOIs的分子和聚集结构,例如链刚性和堆积行为,可以通过控制共聚单体比例来轻松调节,从而显着影响其宏观性能。通过原位聚合将 PBOIs 与氟化石墨烯 (FG) 复合,可以进一步实现薄膜性能的突破。该系列FG/PBOI复合薄膜具有较高的机械强度(119.8–371.2 MPa)、模量(2.5–6.7 GPa)、耐热性(5%失重,551.3–620.6 °C)和疏水性(72 h内吸水率,0.8–2.5%)以及低介电常数(2.09–3.4),可以很好地 满足微电子封装的发展需要。这项工作也有望为高性能电介质的结构设计和性能研究提供理论指导。
The poor processability has long limited the broad application of polybenzoxazoles in microelectronics. Herein, a series of poly(benzoxazole imide) (PBOI) copolymers were designed and prepared through the polymerization of 5-amino-2-(4-aminobenzene) benzoxazole with 3,3′,4,4′-biphenyl tetracarboxylic dianhydride and 4,4′-(hexafluoro-isopropylidene)diphthalic anhydride. These PBOI copolymers show excellent film-forming properties by integrating preformed benzoxazole structures into the polyimide backbone. Moreover, the molecular and aggregate structures of PBOIs, such as chain rigidity and stacking behavior, can be facilely regulated by controlling the comonomer ratio, thereby significantly affecting their macroscopic properties. A breakthrough in film performance could be further achieved by compounding PBOIs with fluorinated graphene (FG) via in situ polymerization. This series of FG/PBOI composite films exhibit high mechanical strength (119.8–371.2 MPa), modulus (2.5–6.7 GPa), heat resistance (5% weight loss, 551.3–620.6 °C), and hydrophobicity (water absorption within 72 h, 0.8–2.5%) as well as a low dielectric constant (2.09–3.4), which can well meet the development needs of microelectronic packaging. This work is also believed to provide theoretical guidance for the structural design and performance research of high-performance dielectrics.
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