High-temperature molecular screening of hybrid polyOAPS-imide networks based on octa(aminophenyl)silsesquioxane for increased thermomechanical resistance

Literature Information

Publication Date 2021-04-30
DOI 10.1039/D1CP01052B
Impact Factor 3.676
Authors

Sylvie Neyertz, Saman Salimi, Farzaneh Radmanesh, Nieck E. Benes, David Brown


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Abstract

A new family of hybrid hyper-cross-linked thin films based on inorganic polyhedral oligomeric silsesquioxane (POSS) cages covalently bound with short organic imides has recently been developed using interfacial polycondensation followed by high-temperature imidization. These polyPOSS-imide networks were aimed at gas separations under harsh conditions, but the aliphatic arms of the initial POSS precursor, octa(aminopropyl)silsesquioxane, were found to be a weak link. This work investigates the replacement of the aliphatic arm by a phenyl derivative, octa(aminophenyl)silsesquioxane (OAPS). Although this new precursor is expected to be more thermoresistant, it introduces extra degrees of complexity since the functional -NH2 group on the phenyl ring can either be attached at a meta, a para or an ortho position. In order to avoid a costly programme of synthesis and testing, molecular dynamics (MD) simulations have been used to efficiently screen a large number of candidate structures based on mixtures of the three OAPS isomers, the initial POSS and three organic precursors, the PMDA, 6FDA and ODPA dianhydrides. Following cross-linking at room temperature, twenty-two model networks were further relaxed at the imidization temperature and directly tested under harsh conditions at 300 °C. The screening stage included the characterization of their intercage single-links and double-links, which reinforce the structures, and intracage links, which have the opposite effect. Carrying out the cross-linking reactions to completion significantly improved the resistance to isotropic dilation. The initial POSS as well as the flexible 6FDA and ODPA linkers were found to be prone to large deformations, whereas the orthoOAPS, metaOAPS, paraOAPS and the PMDA linker prevented volume dilations. Upon uniaxial tension, the Young's moduli varied in the order paraOAPS < POSS ≈ metaOAPS < orthoOAPS for the inorganic precursors and in the order 6FDA < ODPA < PMDA for the organic precursors. In all cases, the networks based on either orthoOAPS and/or PMDA displayed superior resistance. Nine polyOAPS-imides were further heated up to 400 °C, i.e. closer to the expected degradation, and re-submitted to isotropic dilations and uniaxial tensions. They confirmed the trends found at 300 °C with no signs of structural collapse. Using OAPS as the inorganic precursor thus significantly reinforces the thermoresistance of these hybrid hyper-cross-linked networks.

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Physical Chemistry Chemical Physics

Physical Chemistry Chemical Physics
CiteScore: 5.5
Self-citation Rate: 10.3%
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Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.

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