Designing Physicochemically‐Ordered Interphases for High‐Performance Composites

Gupta, Sumit; Sohail, Tanvir; Checa, Marti; Toomey, Michael D.; Kearney, Logan T.; Chahal, Rajni; Rohewal, Sargun S.; Kanbargi, Nihal; Ghosh, Swarnava; Collins, Liam; McConnell, David; Ivanov, Ilia N.; Naskar, Amit K.; Bowland, Christopher C.

doi:10.1002/adfm.202502972

Designing Physicochemically‐Ordered Interphases for High‐Performance Composites

Journal Article · Tue Feb 25 23:00:00 EST 2025 · Advanced Functional Materials

DOI:https://doi.org/10.1002/adfm.202502972· OSTI ID:2573463

^[1]; Sohail, Tanvir ^[1]; ^[2]; Toomey, Michael D. ^[1]; ^[1]; ^[1]; Rohewal, Sargun S. ^[1]; ^[1]; ^[1]; ^[1]; McConnell, David ^[1]; ^[1]; ^[1]; ^[1]

Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)

To enhance the mechanical properties of carbon fiber‐reinforced polymer composites, a physicochemical scaffold is designed incorporating microscopically architected chemically reactive nanofibers that act as a multiscale bridge between the carbon fibers and the matrix. Thermally activated nanofibers leverage their morphologically driven mechanochemical properties to form covalent bonds with adjacent polymer molecules, creating a co‐continuous network that dramatically enhances fiber‐matrix load transfer. By meticulously controlling the nanofiber architecture through variable surface area, functional group availability, and polymer chain alignment effects, the extent of covalent bonding between nanofibers and the matrix is manipulated ultimately resulting in improved carbon fiber‐matrix adhesion. Further, the concept was validated using polyacrylonitrile nanofibers within an acrylonitrile butadiene styrene matrix in a discontinuous carbon fiber‐reinforced composite system. Nanomechanical studies using atomic force microscopy and low‐field nuclear magnetic resonance spectroscopy confirmed immobilized, chemically transferred, and ordered nanostructures at the interphase. The resulting composites demonstrated ≈56% and ≈175% improvements in tensile strength and toughness, respectively, compared to composites without nanofiber. Comprehensive thermal, rheological, and X‐ray scattering analyses, along side all‐atomic molecular dynamics simulations, revealed the fundamental mechanisms behind these improvements in mechanical behavior. The versatility and efficacy of the approach have the potential to address longstanding interphase challenges in the composite industry.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Oak Ridge Leadership Computing Facility (OLCF)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Renewable Power Office. Wind Energy Technologies Office; USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 2573463

Alternate ID(s):: OSTI ID: 2526299

Journal Information:: Advanced Functional Materials, Journal Name: Advanced Functional Materials Journal Issue: 19 Vol. 35; ISSN 1616-301X; ISSN 1616-3028

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

References (46)

Synergistic Strengthening and Toughening the Interphase of Composites by Constructing Alternating “Rigid‐and‐Soft” Structure on Carbon Fiber Surface Wu, Qing; Wan, Qinqin; Liu, Qianli Advanced Materials Interfaces, Vol. 6, Issue 21 https://doi.org/10.1002/admi.201900970	journal	August 2019
An Engineered Multifunctional Composite for Passive Sensing, Power Harvesting, and In Situ Damage Identification with Enhanced Mechanical Performance Gupta, Sumit; Naskar, Amit K.; Bowland, Christopher C. Advanced Materials Technologies, Vol. 7, Issue 9 https://doi.org/10.1002/admt.202101549	journal	February 2022
Enhancing Composite Toughness Through Hierarchical Interphase Formation Gupta, Sumit; Sohail, Tanvir; Checa, Marti Advanced Science https://doi.org/10.1002/advs.202305642	journal	December 2023
Improving the interfacial and flexural properties of carbon fiber–epoxy composites via the grafting of a hyperbranched aromatic polyamide onto a carbon fiber surface on the basis of solution polymerization Wang, Gang; Ma, Lichun; Yang, Xiaobing Journal of Applied Polymer Science, Vol. 136, Issue 12 https://doi.org/10.1002/app.47232	journal	November 2018
Development of low field NMR technique for analyzing segmental mobility of crosslinked polymers Patel, Jigneshkumar P.; Hsu, Shaw Ling Journal of Polymer Science Part B: Polymer Physics, Vol. 56, Issue 8 https://doi.org/10.1002/polb.24583	journal	February 2018
The influence of electrospinning parameters on the morphology and diameter of poly(vinyledene fluoride) nanofibers- effect of sodium chloride Matabola, K. P.; Moutloali, R. M. Journal of Materials Science, Vol. 48, Issue 16 https://doi.org/10.1007/s10853-013-7341-6	journal	April 2013
Pyrolysis of polyacrylonitrile and related polymers—I. Thermal analysis of polyacrylonitrile Grassie, N.; McGuchan, R. European Polymer Journal, Vol. 6, Issue 9 https://doi.org/10.1016/0014-3057(70)90046-7	journal	September 1970
The effect of processing variables on the morphology of electrospun nanofibers and textiles Deitzel, J. M.; Kleinmeyer, J.; Harris, D. Polymer, Vol. 42, Issue 1 https://doi.org/10.1016/S0032-3861(00)00250-0	journal	January 2001
Plasma-grafting polymerization on carbon fibers and its effect on their composite properties Zhang, Huanxia; Li, Wei Applied Surface Science, Vol. 356 https://doi.org/10.1016/j.apsusc.2015.08.016	journal	November 2015
A facile one-pot fabrication of polyphosphazene microsphere/carbon fiber hybrid reinforcement and its effect on the interfacial adhesion of epoxy composites Chen, Xiang; Xu, Haibing; Liu, Dong Applied Surface Science, Vol. 410 https://doi.org/10.1016/j.apsusc.2017.03.104	journal	July 2017
The effect of self-synthesized hydroxyl-terminated hyperbranched polymer interface layer on the properties of carbon fiber reinforced epoxy composites Shi, Longlong; Ma, Lichun; Li, Peiyao Applied Surface Science, Vol. 479 https://doi.org/10.1016/j.apsusc.2019.02.090	journal	June 2019
Molecular dynamics simulation of the interface properties of continuous carbon fiber/ polyimide composites Yan, Yishu; Xu, Junbo; Zhu, Huajian Applied Surface Science, Vol. 563 https://doi.org/10.1016/j.apsusc.2021.150370	journal	October 2021
Increasing the interfacial strength in carbon fiber/epoxy composites by controlling the orientation and length of carbon nanotubes grown on the fibers Lv, Peng; Feng, Yi-yu; Zhang, Peng Carbon, Vol. 49, Issue 14 https://doi.org/10.1016/j.carbon.2011.06.064	journal	November 2011
Carbon nanotubes grown on carbon fiber yarns by a low temperature CVD method: A significant enhancement of the interfacial adhesion between carbon fiber/epoxy matrix hierarchical composites Felisberto, Marcos; Tzounis, Lazaros; Sacco, Leandro Composites Communications, Vol. 3 https://doi.org/10.1016/j.coco.2017.01.003	journal	March 2017
MD simulation of carbon nanotube pullout behavior and its use in determining mode I delamination toughness Yang, Lin; Tong, Liyong; He, Xiaodong Computational Materials Science, Vol. 55 https://doi.org/10.1016/j.commatsci.2011.12.014	journal	April 2012
Influence of electrochemical oxidation of carbon fiber on the mechanical properties of carbon fiber/graphene oxide/epoxy composites Jiang, Jianjun; Yao, Xuming; Xu, Chumeng Composites Part A: Applied Science and Manufacturing, Vol. 95 https://doi.org/10.1016/j.compositesa.2017.02.004	journal	April 2017
Polydopamine as sizing on carbon fiber surfaces for enhancement of epoxy laminated composites Han, Wei; Zhang, Hong-Ping; Tavakoli, Javad Composites Part A: Applied Science and Manufacturing, Vol. 107 https://doi.org/10.1016/j.compositesa.2018.02.003	journal	April 2018
Improved wettability and interfacial adhesion in carbon fibre/epoxy composites via an aqueous epoxy sizing agent Liu, Fuyao; Shi, Zhuo; Dong, Yubing Composites Part A: Applied Science and Manufacturing, Vol. 112 https://doi.org/10.1016/j.compositesa.2018.06.026	journal	September 2018
A review on the tensile properties of natural fiber reinforced polymer composites Ku, H.; Wang, H.; Pattarachaiyakoop, N. Composites Part B: Engineering, Vol. 42, Issue 4 https://doi.org/10.1016/j.compositesb.2011.01.010	journal	June 2011
The oxidation of carbon fibers through K2S2O8/AgNO3 system that preserves fiber tensile strength Yu, Jiali; Meng, Linghui; Fan, Dapeng Composites Part B: Engineering, Vol. 60 https://doi.org/10.1016/j.compositesb.2013.12.037	journal	April 2014
Reinforcing carbon fiber epoxy composites with triazine derivatives functionalized graphene oxide modified sizing agent Ma, Lichun; Zhu, Yingying; Feng, Peifeng Composites Part B: Engineering, Vol. 176 https://doi.org/10.1016/j.compositesb.2019.107078	journal	November 2019
Electrospinning of polymer nanofibers: Effects on oriented morphology, structures and tensile properties Baji, Avinash; Mai, Yiu-Wing; Wong, Shing-Chung Composites Science and Technology, Vol. 70, Issue 5 https://doi.org/10.1016/j.compscitech.2010.01.010	journal	May 2010
Effect of polyurethane dispersion as surface treatment for carbon fabrics on mechanical properties of carbon/Nylon composites Ma, Yan; Yokozeki, Tomohiro; Ueda, Masahito Composites Science and Technology, Vol. 151 https://doi.org/10.1016/j.compscitech.2017.08.031	journal	October 2017
Carbon fiber/epoxy matrix composite interphases modified with cellulose nanocrystals Reale Batista, Mariana Desireé; Drzal, Lawrence T. Composites Science and Technology, Vol. 164 https://doi.org/10.1016/j.compscitech.2018.05.010	journal	August 2018
Enhancing functionalities in carbon fiber composites by titanium dioxide nanoparticles Rankin, Susan M.; Moody, Mikayla K.; Naskar, Amit K. Composites Science and Technology, Vol. 201 https://doi.org/10.1016/j.compscitech.2020.108491	journal	January 2021
Electrospun nanofibers as reinforcement for composite laminates materials – A review Palazzetti, R.; Zucchelli, A. Composite Structures, Vol. 182 https://doi.org/10.1016/j.compstruct.2017.09.021	journal	December 2017
Hydrogels in a historical perspective: From simple networks to smart materials Buwalda, Sytze J.; Boere, Kristel W. M.; Dijkstra, Pieter J. Journal of Controlled Release, Vol. 190 https://doi.org/10.1016/j.jconrel.2014.03.052	journal	September 2014
Stretching-induced crystallinity and orientation to improve the mechanical properties of electrospun PAN nanocomposites Hou, Xiaoxiao; Yang, Xiaoping; Zhang, Liqun Materials & Design, Vol. 31, Issue 4 https://doi.org/10.1016/j.matdes.2009.01.051	journal	April 2010
Simultaneous improvement of interfacial strength and toughness between carbon fiber and epoxy by introducing amino functionalized ZrO2 on fiber surface Wu, Qing; Zhao, Ruyi; Liu, Qianli Materials & Design, Vol. 149 https://doi.org/10.1016/j.matdes.2018.03.054	journal	July 2018
A review of carbon fiber surface modification methods for tailor-made bond behavior with cementitious matrices Li, Huanyu; Liebscher, Marco; Zhao, Dong Progress in Materials Science, Vol. 132 https://doi.org/10.1016/j.pmatsci.2022.101040	journal	February 2023
Molecular orientation and mechanical property size effects in electrospun polyacrylonitrile nanofibers Naraghi, M.; Arshad, S. N.; Chasiotis, I. Polymer, Vol. 52, Issue 7 https://doi.org/10.1016/j.polymer.2011.02.013	journal	March 2011
Polymer crystallinity and crystallization kinetics via benchtop ¹H NMR relaxometry: Revisited method, data analysis, and experiments on common polymers Räntzsch, Volker; Haas, Manuel; Özen, Mürüvvet B. Polymer, Vol. 145, p. 162-173 https://doi.org/10.1016/j.polymer.2018.04.066	journal	June 2018
Tracking the origins of size dependency in the mechanical properties of polymeric nanofibers at the atomistic scale Peng, Kaiyuan; Nain, Amrinder; Mirzaeifar, Reza Polymer, Vol. 175 https://doi.org/10.1016/j.polymer.2019.05.014	journal	June 2019
The mechanism of thermal stabilization of polyacrylonitrile Szepcsik, Balázs; Pukánszky, Béla Thermochimica Acta, Vol. 671 https://doi.org/10.1016/j.tca.2018.12.004	journal	January 2019
Deep-Learning Interatomic Potential Connects Molecular Structural Ordering to the Macroscale Properties of Polyacrylonitrile Chahal, Rajni; Toomey, Michael D.; Kearney, Logan T. ACS Applied Materials & Interfaces, Vol. 16, Issue 28 https://doi.org/10.1021/acsami.4c04491	journal	July 2024
Interplay of Chain Orientation and Bond Length in Size Dependency of Mechanical Properties in Polystyrene Nanofibers Peng, Kaiyuan; Mirzaeifar, Reza ACS Applied Polymer Materials, Vol. 2, Issue 4 https://doi.org/10.1021/acsapm.0c00089	journal	March 2020
Codepositing Mussel-Inspired Nanohybrids onto One-Dimensional Fibers under “Green” Conditions for Significantly Enhanced Surface/Interfacial Properties Yang, Xiaobin; Du, Hongpeng; Li, Songwei ACS Sustainable Chemistry & Engineering, Vol. 6, Issue 3 https://doi.org/10.1021/acssuschemeng.8b00290	journal	February 2018
Predicting Polymer Nanofiber Interactions via Molecular Simulations Buell, Sezen; Rutledge, Gregory C.; Vliet, Krystyn J. Van ACS Applied Materials & Interfaces, Vol. 2, Issue 4 https://doi.org/10.1021/am1000135	journal	April 2010
Interfacial Microstructure and Properties of Carbon Fiber Composites Modified with Graphene Oxide Zhang, Xiaoqing; Fan, Xinyu; Yan, Chun ACS Applied Materials & Interfaces, Vol. 4, Issue 3 https://doi.org/10.1021/am201757v	journal	February 2012
Polydopamine As an Efficient and Robust Platform to Functionalize Carbon Fiber for High-Performance Polymer Composites Chen, Shusheng; Cao, Yewen; Feng, Jiachun ACS Applied Materials & Interfaces, Vol. 6, Issue 1 https://doi.org/10.1021/am404394g	journal	November 2013
Surface treatments for improving the mechanical properties of carbon nanofiber/thermoplastic composites Finegan, I. C.; Tibbetts, G. G.; Glasgow, D. G. Journal of Materials Science, Vol. 38, Issue 16, p. 3485-3490 https://doi.org/10.1023/A:1025109103511	journal	August 2003
Relationship between orientation factor of lead zirconate titanate nanowires and dielectric permittivity of nanocomposites Tang, Haixiong; Malakooti, Mohammad H.; Sodano, Henry A. Applied Physics Letters, Vol. 103, Issue 22 https://doi.org/10.1063/1.4833416	journal	November 2013
Interfacial shear strength of glass fiber reinforced polyketone measured by the single fiber pullout test Pearson, Adam; Liao, Weijian; Kazemi, Yasamin AIP Conference Proceedings https://doi.org/10.1063/5.0136855	conference	January 2023
Carbon Nanotubes with Temperature-Invariant Viscoelasticity from -196 to 1000 C Xu, M.; Futaba, D. N.; Yamada, T. Science, Vol. 330, Issue 6009 https://doi.org/10.1126/science.1194865	journal	December 2010
Effect of Experimental Parameters on Morphological, Mechanical and Hydrophobic Properties of Electrospun Polystyrene Fibers Huan, Siqi; Liu, Guoxiang; Han, Guangping Materials, Vol. 8, Issue 5 https://doi.org/10.3390/ma8052718	journal	May 2015
Testing the Physical and Mechanical Properties of Polyacrylonitrile Nanofibers Reinforced with Succinite and Silicon Dioxide Nanoparticles Lasenko, Inga; Grauda, Dace; Butkauskas, Dalius Textiles, Vol. 2, Issue 1 https://doi.org/10.3390/textiles2010009	journal	March 2022

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