ACS Applied Polymer Materials最新文献

{"title":"Sustainable Carbon Dots from Olive Pomace: Boosting CO2 Separation in Mixed Matrix Iongel Membranes","authors":"Diogo A. Sousa,&nbsp;Ana R. Nabais,&nbsp;José V. Prata* and Liliana C. Tomé*,&nbsp;","doi":"10.1021/acsapm.5c0023910.1021/acsapm.5c00239","DOIUrl":"https://doi.org/10.1021/acsapm.5c00239https://doi.org/10.1021/acsapm.5c00239","url":null,"abstract":"<p >Carbon dioxide (CO₂) separation remains a critical challenge in mitigating industrial emissions, driving the development of innovative membrane technologies to improve separation performance. In this study, carbon dots (CDs) obtained from wet olive pomace were incorporated into mixed matrix iongel membranes (MMIMs) by UV-initiated free radical polymerization of poly(ethylene glycol) diacrylate (PEGDA) in the presence of the [C₂mim][TFSI] ionic liquid. Dense and defect-free MMIMs with suitable thermal stability were successfully prepared, achieving a homogeneous dispersion of CDs within the iongel matrix at loadings of up to 1 wt %. Gas permeation experiments revealed a significant enhancement in the CO₂ permeability and ideal selectivity upon the incorporation of CDs. The MMIM containing 0.5 wt % CDs exhibited the best performance, achieving a CO₂ permeability of 725 Barrer, along with CO₂/N₂ and CO₂/CH₄ selectivities of 40 and 22, respectively. This outstanding performance surpasses that of previously reported MMIMs and approaches the upper bounds of CO₂/N₂ and CO₂/CH₄. Furthermore, the use of biomass-derived CDs as fillers not only improves the CO₂ separation performance of MMIMs, but also promotes the sustainable valorization of agricultural waste, offering both environmental and functional advantages.</p>","PeriodicalId":7,"journal":{"name":"ACS Applied Polymer Materials","volume":"7 10","pages":"5944–5951 5944–5951"},"PeriodicalIF":4.4,"publicationDate":"2025-05-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144114888","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Oil-Soluble and Core-Cross-linked Fibrous Nanofillers with Excellent Comprehensive Performances Generated by In Situ Cross-linking Polymerization-Induced Self-Assembly","authors":"Wen-Jian Zhang,&nbsp;Meng-Xin Fan,&nbsp;Jia-Qing Li,&nbsp;Xiao-Yu Cao,&nbsp;Jian-Chun Jiang,&nbsp;Zi-Xuan Chang,&nbsp;Wei Bai*,&nbsp;Ren-Man Zhu* and Chun-Yan Hong*,&nbsp;","doi":"10.1021/acsapm.5c0079410.1021/acsapm.5c00794","DOIUrl":"https://doi.org/10.1021/acsapm.5c00794https://doi.org/10.1021/acsapm.5c00794","url":null,"abstract":"<p >Reinforcement of polymeric materials by incorporating rigid nanofillers (especially nanofibers) is a promising strategy, which mainly relies on the elaborate design of nanofillers. Herein, we report an oil-soluble and core-cross-linked fibrous nanofiller with superior comprehensive properties. In situ cross-linking polymerization-induced self-assembly (PISA) in mineral oil is demonstrated to be a powerful strategy for producing oil-soluble nanofibers with excellent reproducibility (100% in 10 repeated experiments). The oil-soluble stabilizer enables good compatibility of the nanofibers with various hydrophobic polymer matrices, and the core-cross-linked structure endows the nanofibers with robust stability to resist the severe processing environment (high temperature and high shearing) of fabricating polymer–nanofiller composites. The nanofibers show superior reinforcement effects on the polymer–nanofiller composites but without the expense of transparency, recyclability, and self-healing ability. With only 1 wt % dosage of the nanofibers, the tensile stress, elongation, and toughness of the polymer–nanofiller composites increased by approximately 2.6, 3.5, and 7.2 times, respectively. The oil-soluble and core-cross-linked nanofibers based on the in situ cross-linking PISA strategy are attractive candidates of nanofillers to reinforce plastics, gels, or elastomers in various industrial applications, which not only have excellent comprehensive performances but also meet the requirements of sustainable development.</p>","PeriodicalId":7,"journal":{"name":"ACS Applied Polymer Materials","volume":"7 10","pages":"6326–6336 6326–6336"},"PeriodicalIF":4.4,"publicationDate":"2025-05-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144114532","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Investigating the Multistep Polymerization Reactions of DCPD with Grubbs’ First-Generation Catalyst","authors":"Başak Özeroğlu*,&nbsp; and ,&nbsp;Necati Özkan*,&nbsp;","doi":"10.1021/acsapm.5c0074010.1021/acsapm.5c00740","DOIUrl":"https://doi.org/10.1021/acsapm.5c00740https://doi.org/10.1021/acsapm.5c00740","url":null,"abstract":"<p >Self-healing polymer composites using Grubbs’ first-generation (G1) catalyst and dicyclopentadiene (DCPD) as the healing monomer are widely used in self-healing applications. In such systems, DCPD released from ruptured microcapsules reacts with dispersed G1, enabling healing without external intervention. This study simulates the local DCPD–G1 interaction at the crack site using Differential Scanning Calorimetry (DSC) analysis, imitating self-healing conditions. The polymerization reactions of the DCPD–G1 system were systematically investigated using DSC, Dynamic Mechanical Analysis (DMA), kinetic modeling, Fourier Transform Infrared (FT-IR), and nuclear magnetic resonance (¹H NMR) spectroscopy. One of the main outcomes of this work is the identification of three separate exothermic transitions in the DSC analysis. These results indicate that the polymerization follows a multistep pathway, starting with ROMP to form linear polydicyclopentadiene (L-PDCPD) and proceeding with cross-linking via olefin addition and metathesis reactions. DMA analysis, performed within temperature intervals identified in deconvoluted DSC peaks, further clarifies that the first process involves linear polymerization, while the second and third processes are associated with cross-linking reactions. A slight increase in glass transition temperature (<i>T</i>_g) and shear storage modulus (G′) in the first-process interval indicates linear PDCPD growth via increased molecular weight (<i>M</i>_w) and chain entanglements. In contrast, a sharp increase in <i>T</i>_g and G′ in the sample that passed through the second-process interval and a distinct stiffness increase at the onset of the third process (∼82 °C) indicate two distinct curing mechanisms. These findings are further supported by FT-IR analysis through the monitoring of the peaks at 972, 726, and 754 cm^–1. Kinetic modeling (Šesták–Berggren) closely matches experimental data, validating this multistep polymerization reaction. The findings can clearly show the multistep polymerization process for G1 – catalyzed DCPD.</p>","PeriodicalId":7,"journal":{"name":"ACS Applied Polymer Materials","volume":"7 10","pages":"6250–6261 6250–6261"},"PeriodicalIF":4.4,"publicationDate":"2025-05-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsapm.5c00740","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144114515","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Liquid Crystal Photoalignment Layer Using Coumarin-Containing Block Copolymers","authors":"Xinshi Chen,&nbsp; and ,&nbsp;Yue Zhao*,&nbsp;","doi":"10.1021/acsapm.5c0058210.1021/acsapm.5c00582","DOIUrl":"https://doi.org/10.1021/acsapm.5c00582https://doi.org/10.1021/acsapm.5c00582","url":null,"abstract":"<p >The intrinsic combination of anisotropy and fluidity of liquid crystals enables a wide range of their applications such as displays and optical and photonic devices, for which an initial orientation of liquid crystal molecules at the macroscopic scale is essential. The use of an optically treated surface, termed the photoalignment layer, to induce this initial liquid crystal orientation is an attractive alternative to the use of a mechanically rubbed surface because, among other advantages, using light makes it possible to spatially pattern the photoalignment layer to organize the liquid crystal orientation. Herein, we introduce coumarin-containing block copolymers as a material system for the surface photoalignment layer. A diblock copolymer comprising a non-photosensitive polyurethane and a photoactive polymethacrylate bearing coumarin side groups was synthesized in different compositions and was investigated for the use of a photoalignment layer for a nematic liquid crystal. The microphase separation in the block copolymer results in distinct self-assembled surface morphologies during the casting and processing of the alignment layers, which influence the induced liquid crystal orientation. Interestingly, even with the coumarin polymer forming nanodomains dispersed in the non-photosensitive polymer matrix, the photoalignment layer can effectively align liquid crystal molecules, demonstrating a dominant cooperative effect in propagating liquid crystal orientation in all directions. Given the numerous possibilities for designing photosensitive block copolymers, the concept of exploring photoalignment layers featuring not only surface anisotropy but also microphase separation of the blocks on the surface offers perspectives for controlling liquid crystal orientation crucial for applications.</p>","PeriodicalId":7,"journal":{"name":"ACS Applied Polymer Materials","volume":"7 10","pages":"6164–6174 6164–6174"},"PeriodicalIF":4.4,"publicationDate":"2025-05-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144114530","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Decoding Structure–Optical Property Relationships in TiO2 Nanocomposites through Hybrid Features Integration","authors":"Renquan Lv,&nbsp;Weiwei Han,&nbsp;Zixu Zeng,&nbsp;Yi He,&nbsp;Lecheng Lei,&nbsp;Ping Li and Xingwang Zhang*,&nbsp;","doi":"10.1021/acsapm.5c0086910.1021/acsapm.5c00869","DOIUrl":"https://doi.org/10.1021/acsapm.5c00869https://doi.org/10.1021/acsapm.5c00869","url":null,"abstract":"<p >Optical titanium dioxide nanocomposites have a wide range of applications, but ill-defined structure–property relationships pose a challenge to the systematic discovery of functional materials. We designed a TGEML multimodal nanocomposite processing framework to address this challenge. The framework consists of a polymer multimodal featurizer named TGEML-polymer and a nanoparticle-specialized featurizer named TGEML-nano. TGEML-polymer integrates a Transformer-based graph neural network specialized in representing polymer information to capture the chemical semantic sequence and graph information of polymers. TGEML-nano includes processing strategies for nanoparticle dispersion scattering and particle size distribution to provide a comprehensive picture of the nanosystem. We correlated polymer feature vectors with nanosystem parameters to generate hybrid features. This enabled the successful construction of a quantitative “structure–refractive index” mapping. Moreover, the structure–optical property relationships were decoded through a multilevel feature interpretability analysis. In conclusion, TGEML can provide powerful and useful hybrid features for artificial intelligence to accelerate the development and design process of nanocomposites.</p>","PeriodicalId":7,"journal":{"name":"ACS Applied Polymer Materials","volume":"7 10","pages":"6415–6426 6415–6426"},"PeriodicalIF":4.4,"publicationDate":"2025-05-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144114889","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Binary Solvent-Induced Ultra-Adhesive Gel for Underwater Motion and Water Flow Detection","authors":"Xiaolong Kan,&nbsp;Enpei Shi,&nbsp;Chenqi Zhu,&nbsp;Qian Wang*,&nbsp;Lulu Qu* and Xiaochen Dong*,&nbsp;","doi":"10.1021/acsapm.5c0100410.1021/acsapm.5c01004","DOIUrl":"https://doi.org/10.1021/acsapm.5c01004https://doi.org/10.1021/acsapm.5c01004","url":null,"abstract":"<p >Hydrogel-based sensors face significant limitations due to swelling in aqueous environments, which compromises their mechanical integrity and distorts sensing signals, thereby hindering their widespread application. Here, a water-submersible hydrogel sensor capable of long-term underwater monitoring was prepared through highly cross-linked copolymerization of hydrophilic and hydrophobic monomers in a binary solvent system. Originating from the difference in affinity to the solvent, the hydrophobic polymers were prone to polymerize and wrap around to promote microphase separation, and the localized reinforced entanglement and cross-linking enabled the hydrogel excellent hydrophobic property, extremely strong antiswelling property (0.13% after 5 days), and impressive mechanical reinforcement. The underwater adhesive properties of the hydrogel were further enhanced by the synergistic effects of multiple physical and chemical interactions and a water-induced surface rearrangement, achieving a maximum adhesion strength of 54.4 kPa underwater. With abundant charged functional groups and dissociable salts, the hydrogel sensor demonstrated high sensitivity, rapid response time, and superior electromechanical stability in both air and underwater, enabling prolonged monitoring of underwater human activities and hydrological conditions.</p>","PeriodicalId":7,"journal":{"name":"ACS Applied Polymer Materials","volume":"7 10","pages":"6523–6532 6523–6532"},"PeriodicalIF":4.4,"publicationDate":"2025-05-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144114891","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Impact of Interface Flexibility on Separation Force in Liquid Crystal Display Vat Photopolymerization: A Comprehensive Analysis","authors":"Sandeep Kumar Paral,&nbsp;Jeng-Ywan Jeng,&nbsp;Yih-Lin Cheng and Ding-Zheng Lin*,&nbsp;","doi":"10.1021/acsapm.5c0016710.1021/acsapm.5c00167","DOIUrl":"https://doi.org/10.1021/acsapm.5c00167https://doi.org/10.1021/acsapm.5c00167","url":null,"abstract":"<p >Liquid crystal display (LCD) vat photopolymerization (VPP) is becoming popular in additive manufacturing for its precision and affordability. However, the bottom-up approach generates a significant separation force when detaching the cured part from the interface. In the LCD VPP, the interface is edge-fixed and placed directly on the LCD panel, mentioned as a flexible interface. While most research focuses on separation force analysis based on rigid interfaces (interface fixed on a substrate) using the digital light processing VPP, the understanding of flexible interface behavior remains limited. This study comprehensively analyzes the interface flexibility’s impact on separation force using polydimethylsiloxane (PDMS) in both flexible and rigid configurations. Interface thickness emerges as a critical parameter, showing contrasting effects between flexible and rigid interfaces. Although the separation force increases with print object size, it has a lesser effect on flexible interfaces compared to that on rigid ones. Notably, the rigid PDMS interface exhibits up to a 100-fold higher separation force than the flexible interface under identical printing conditions. Additionally, commercially used Teflon as a flexible interface demonstrates a 10-fold higher separation force than flexible PDMS due to its higher elastic modulus. The proposed analytical model based on Kendall adhesion theory predicts maximum separation forces with error margins of 15% for flexible PDMS and 10% for Teflon. The study also highlights the importance of interface flexibility for achieving complex structures and high-resolution printing in an LCD VPP.</p>","PeriodicalId":7,"journal":{"name":"ACS Applied Polymer Materials","volume":"7 10","pages":"5898–5909 5898–5909"},"PeriodicalIF":4.4,"publicationDate":"2025-05-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsapm.5c00167","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144114886","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Understanding the Conductivity and Transference Trade-Off in Polymer Electrolytes Using a Robeson-Inspired Upper Bound","authors":"Zirong He,&nbsp; and ,&nbsp;Nitash P. Balsara*,&nbsp;","doi":"10.1021/acsapm.5c0028810.1021/acsapm.5c00288","DOIUrl":"https://doi.org/10.1021/acsapm.5c00288https://doi.org/10.1021/acsapm.5c00288","url":null,"abstract":"<p >The development of high-performance electrolytes is crucial for advancing next-generation lithium and sodium battery technologies. Since the cation is the working ion in both technologies, electrolytes exhibiting the rapid cation transport are essential for making progress. Pathways to optimize electrolytes are unclear due to the inherent trade-off between conductivity and cation transference. While this trade-off is sometimes recognized, there are no well-accepted methodologies for quantifying it. Inspired by the Robeson upper bound for the permeability–selectivity trade-off in gas separation membranes, we propose an approach for quantifying the trade-off in electrolytes using Newman’s concentrated solution theory. We suggest calling this the Newman upper bound. By analyzing published data from 30 polymer electrolytes containing univalent lithium and sodium salts, the Newman upper bound is expressed as κ = 2.0(1/ρ₊ – 1) where κ (mS/cm) is conductivity and ρ₊ is the current fraction measured in a symmetric cell as first described by Bruce et al. [<i>J. Electroanal. Chem. Interfacial Electrochem.</i> 1987, 225 (1), 1–17]. This formulation of the upper bound introduces a critical guiding metric for designing next-generation polymer electrolytes; it highlights factors underlying the trade-off, including the salt diffusion coefficient (<i>D</i>), cation transference number relative to solvent velocity (<i></i><math><msubsup><mi>t</mi><mo>+</mo><mn>0</mn></msubsup></math>), and thermodynamic factor (1 + (d lnγ_+–)/(d ln<i>m</i>)), where γ_+– is the mean molar activity coefficient and <i>m</i> is the molality. These parameters have been measured for very few electrolytes. We posit that establishing the molecular properties that govern these parameters will lead to improved electrolytes that greatly exceed the current upper bound.</p>","PeriodicalId":7,"journal":{"name":"ACS Applied Polymer Materials","volume":"7 10","pages":"5960–5968 5960–5968"},"PeriodicalIF":4.4,"publicationDate":"2025-05-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144114764","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Enhanced Recyclability and Durability of Solid Propellant Binders via a Dynamic Bicontinuous Structure with Self-Healing","authors":"Shengda Zhang,&nbsp;Zhuo Wu,&nbsp;Yi He,&nbsp;Pu Huang,&nbsp;Wei Li,&nbsp;Jin Huang*,&nbsp;Shuiping Zhou* and Lin Gan*,&nbsp;","doi":"10.1021/acsapm.5c0012210.1021/acsapm.5c00122","DOIUrl":"https://doi.org/10.1021/acsapm.5c00122https://doi.org/10.1021/acsapm.5c00122","url":null,"abstract":"<p >Polyurethane with a dynamic cross-linking network provides promising next-generation solid propellant binders due to its self-healing and recyclability for improved safety and durability. However, dynamic cross-linking networks with self-healing usually lead to insufficient mechanical properties due to the contradiction between their constitutive relation and molecular chain mobility. Here, a strategy of dynamic bicontinuous structure was proposed to regulate molecular chain motion for integrated good moderate-temperature self-healing, mechanical strength, toughness, and recyclability. The acylsemicarbazide group was introduced into the polyurethane molecular chain for the formation of a stable cross-linking network and intermolecular sextuple hydrogen bonds. An asymmetric structure was designed to convert the typical island-phase morphology into a unique bicontinuous phase. The optimized chain mobility was regulated by a noncovalent reversible network of hydrogen bonds coupled with an asymmetric structure-induced bicontinuous microstructure. The obtained polyurethane exhibited an excellent mechanical strength of 51 MPa, 1410% elongation at break, a toughness of 260 MJ·m^–3, and a fracture energy of 120.24 kJ·m^–2. An impressive moderate-temperature self-healing of 90% was achieved within 12 h. Such a strategy provides insights for the development of high-performance binders or other high-fill energetic materials.</p>","PeriodicalId":7,"journal":{"name":"ACS Applied Polymer Materials","volume":"7 10","pages":"5932–5943 5932–5943"},"PeriodicalIF":4.4,"publicationDate":"2025-05-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144114765","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Soluble Semi-Alicyclic Fluorinated Copolyimide Dielectrics for High-Temperature Capacitive Energy Storage","authors":"Ling Zhou,&nbsp;Jinhui Song,&nbsp;Ganbo Liang,&nbsp;Shiyu Qin,&nbsp;Hongmei Qin,&nbsp;Siyu Yu,&nbsp;Chuanxi Xiong and Shan Wang*,&nbsp;","doi":"10.1021/acsapm.5c0092010.1021/acsapm.5c00920","DOIUrl":"https://doi.org/10.1021/acsapm.5c00920https://doi.org/10.1021/acsapm.5c00920","url":null,"abstract":"<p >Polyimides are renowned for their excellent thermal stability and insulating properties, making them ideal candidates for high-temperature dielectric energy storage. However, traditional polyimides often suffer from a narrow bandgap and limited solubility, which complicates processing and restricts their widespread application in high-performance energy storage. In this work, we propose a molecular design strategy by copolymerizing rigid, low-polarity cyclobutane-1,2,3,4-tetracarboxylic dianhydride (CBDA), 4,4′-(hexafluoroisopropylidene)diphthalic anhydride (6FDA) with a bulky fluorinated bridge group, and 2,2′-bis(trifluoromethyl)benzidine (TFMB) to form wide-bandgap CBDA/6FDA/TFMB copolyimides, achieving a balanced performance with excellent solubility and high-temperature dielectric properties. Their electronic structure, molecular aggregation behavior, thermal stability, solubility, dielectric behavior, electrical breakdown strength, and high-temperature energy storage performance were systematically investigated as a function of 6FDA content. The results demonstrate that the copolyimide with 30% 6FDA content maintains good solubility while exhibiting excellent high-temperature dielectric polarization, low electrical conduction loss, and high breakdown strength. This leads to outstanding performance in high-temperature energy storage performance, with an energy storage density of 2.11 J/cm³ and a charge–discharge efficiency of 90.3% at 150 °C and 350 MV/m. Overall, this work demonstrates the successful design and synthesis of semi-alicyclic fluorinated copolyimides with tailored solubility and dielectric properties, underscoring their promising potential for high-temperature dielectric energy storage applications.</p>","PeriodicalId":7,"journal":{"name":"ACS Applied Polymer Materials","volume":"7 10","pages":"6469–6479 6469–6479"},"PeriodicalIF":4.4,"publicationDate":"2025-05-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144114795","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}