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Molecular Insight into 6FD Polyimide-Branched Poly(phenylene) Copolymers: Synthesis, Block Compatibility, and Gas Transport Study
ACS Applied Polymer Materials ( IF 4.4 ) Pub Date : 2023-01-04 , DOI: 10.1021/acsapm.2c01509
Fei Huang 1 , Timothy Largier 2 , Lingping Luo 1 , Wenjian Zheng 3 , Chris J. Cornelius 4
ACS Applied Polymer Materials ( IF 4.4 ) Pub Date : 2023-01-04 , DOI: 10.1021/acsapm.2c01509
Fei Huang 1 , Timothy Largier 2 , Lingping Luo 1 , Wenjian Zheng 3 , Chris J. Cornelius 4
Affiliation
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A series of 6FDA-DABA (6FD) polyimide and branched poly(phenylene) (PP) block copolymers and homopolymers were successfully synthesized using Diels–Alder and polycondensation reactions. PP and 6FD homopolymer blends in tetrahydrofuran were immiscible. The result coincides with their large chemical dissimilarity and theoretical solubility parameter differences of 25.47 and 33.17 (MJ/m3)1/2. However, 6FD-PP block copolymer solutions were clear, and thin films were robust and creasable. Densities and fractional free volumes (FFV) (0.162–0.346) largely obeyed the rule of mixing, suggesting a “blend-like” morphology. At moderate PP block lengths, two distinct glass transition temperatures (340 and 420 °C) were evident, while large PP block lengths suppressed first-order polyimide transitions entirely. A small-angle X-ray scattering and atomic force microscopy morphological analysis revealed two distinct domains, with separation lengths increasing with the PP block length. Their gas permeation, diffusion, sorption, and separation properties were thoroughly investigated and exhibited a strong correlation with polymer chemistry, block length, and FFV. A block copolymer had an O2 permeability roughly between 6FD and PP, resulting in a 30% increase in O2/N2 selectivity. The N2/CH4 selectivities ranged from 4.2 to 0.58, suggesting that this 6FD-PP system could be efficiently tuned from highly N2-selective to CH4-selective performance. Five structural models, rule-of-mixture, Maxwell, equivalent box model, laminate, and blend, were used to predict gas transport properties. Compared with experimental data, the miscible blend model provided the best results for the 6FD-PP block copolymer system. Block copolymerization by combining highly selective polyimide and highly permeable branched poly(phenylene) provides an opportunity for gas separation tunability and improvement in selected gas pairs.
中文翻译：
6FD 聚酰亚胺支化聚（亚苯基）共聚物的分子洞察：合成、嵌段相容性和气体传输研究
使用 Diels-Alder 和缩聚反应成功合成了一系列 6FDA-DABA (6FD) 聚酰亚胺和支化聚亚苯基 (PP) 嵌段共聚物和均聚物。PP 和 6FD 均聚物在四氢呋喃中的混合物不混溶。该结果与它们较大的化学差异和理论溶解度参数差异 25.47 和 33.17 (MJ/m 3 ) 1/2相吻合. 然而，6FD-PP 嵌段共聚物溶液是透明的，薄膜坚固且易折皱。密度和自由体积分数 (FFV) (0.162–0.346) 在很大程度上服从混合规则，表明“混合状”形态。在中等 PP 嵌段长度下，两个明显的玻璃化转变温度（340 和 420 °C）很明显，而大 PP 嵌段长度则完全抑制了一级聚酰亚胺转变。小角度 X 射线散射和原子力显微镜形态分析揭示了两个不同的域，分离长度随着 PP 嵌段长度的增加而增加。它们的气体渗透、扩散、吸附和分离特性经过彻底研究，并显示出与聚合物化学、嵌段长度和 FFV 的强相关性。嵌段共聚物具有 O 2渗透率大致介于 6FD 和 PP 之间，导致 O 2 /N 2选择性增加 30%。N 2 /CH 4的选择性范围为 4.2 至 0.58，表明该 6FD-PP 系统可以从高 N 2选择性有效地调整为 CH 4-选择性表现。五种结构模型，混合规则，麦克斯韦，等效盒模型，层压板和混合，用于预测气体传输特性。与实验数据相比，混溶共混模型为 6FD-PP 嵌段共聚物体系提供了最佳结果。通过组合高选择性聚酰亚胺和高渗透性支化聚（亚苯基）进行嵌段共聚，为气体分离可调性和改进所选气体对提供了机会。
更新日期：2023-01-04
中文翻译：
6FD 聚酰亚胺支化聚（亚苯基）共聚物的分子洞察：合成、嵌段相容性和气体传输研究
使用 Diels-Alder 和缩聚反应成功合成了一系列 6FDA-DABA (6FD) 聚酰亚胺和支化聚亚苯基 (PP) 嵌段共聚物和均聚物。PP 和 6FD 均聚物在四氢呋喃中的混合物不混溶。该结果与它们较大的化学差异和理论溶解度参数差异 25.47 和 33.17 (MJ/m 3 ) 1/2相吻合. 然而，6FD-PP 嵌段共聚物溶液是透明的，薄膜坚固且易折皱。密度和自由体积分数 (FFV) (0.162–0.346) 在很大程度上服从混合规则，表明“混合状”形态。在中等 PP 嵌段长度下，两个明显的玻璃化转变温度（340 和 420 °C）很明显，而大 PP 嵌段长度则完全抑制了一级聚酰亚胺转变。小角度 X 射线散射和原子力显微镜形态分析揭示了两个不同的域，分离长度随着 PP 嵌段长度的增加而增加。它们的气体渗透、扩散、吸附和分离特性经过彻底研究，并显示出与聚合物化学、嵌段长度和 FFV 的强相关性。嵌段共聚物具有 O 2渗透率大致介于 6FD 和 PP 之间，导致 O 2 /N 2选择性增加 30%。N 2 /CH 4的选择性范围为 4.2 至 0.58，表明该 6FD-PP 系统可以从高 N 2选择性有效地调整为 CH 4-选择性表现。五种结构模型，混合规则，麦克斯韦，等效盒模型，层压板和混合，用于预测气体传输特性。与实验数据相比，混溶共混模型为 6FD-PP 嵌段共聚物体系提供了最佳结果。通过组合高选择性聚酰亚胺和高渗透性支化聚（亚苯基）进行嵌段共聚，为气体分离可调性和改进所选气体对提供了机会。
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