Designing Physicochemically-Ordered Interphases for High-Performance Composites

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Abstract

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. 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.

Original languageEnglish
Article number2502972
JournalAdvanced Functional Materials
Volume35
Issue number19
DOIs
StatePublished - May 9 2025

Funding

This manuscript had been authored by UT-Battelle, LLC under Contract No. DE-AC05-00OR22725 with the U.S. Department of Energy. The United States Government retains and the publisher, by accepting the article for publication, acknowledges that the United States Government retains a non-exclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript or allow others to do so, for United States Government purposes. The Department of Energy will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan (http://energy.gov/downloads/ doe-public-access-plan). This research at Oak Ridge National Laboratory, managed by UT Battelle, LLC, for the U.S. Department of Energy (DOE) under Contract No. DE-AC05-00OR22725, was sponsored by the Vehicle Technologies Office (VTO) (Award #: DE-LC-0000021) within the Office of Energy Efficiency and Renewable Energy (EERE).Partial support was also received through DOE's Wind Energy Technology Office's (WETO) FY24 Lab Incubator Request for Innovation. LTK and MT acknowledge support from the US Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences, and Engineering Division [FWP#ERKCK60] for X-ray and NMR characterization of nanofiber-matrix interface. AFM imaging was performed (MC, LC, II) at the Center for Nanophase Materials Sciences (CNMS), which is a US Department of Energy, Office of Science User Facility at ORNL. This research used resources of the Oak Ridge Leadership Computing Facility at the Oak Ridge National Laboratory, which is supported by the Office of Science of the U.S. Department of Energy under Contract No. DE-AC05-00OR22725.The authors would like to thank Ms. Atreyi Samaddar ([email protected]) for voluntarily designing the potential cover art. This manuscript had been authored by UT‐Battelle, LLC under Contract No. DE‐AC05‐00OR22725 with the U.S. Department of Energy. The United States Government retains and the publisher, by accepting the article for publication, acknowledges that the United States Government retains a non‐exclusive, paid‐up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript or allow others to do so, for United States Government purposes. The Department of Energy will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan ( http://energy.gov/downloads/ doe‐public‐access‐plan). This research at Oak Ridge National Laboratory, managed by UT Battelle, LLC, for the U.S. Department of Energy (DOE) under Contract No. DE‐AC05‐00OR22725, was sponsored by the Vehicle Technologies Office (VTO) (Award #: DE‐LC‐0000021) within the Office of Energy Efficiency and Renewable Energy (EERE).Partial support was also received through DOE's Wind Energy Technology Office's (WETO) FY24 Lab Incubator Request for Innovation. LTK and MT acknowledge support from the US Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences, and Engineering Division [FWP#ERKCK60] for X‐ray and NMR characterization of nanofiber‐matrix interface. AFM imaging was performed (MC, LC, II) at the Center for Nanophase Materials Sciences (CNMS), which is a US Department of Energy, Office of Science User Facility at ORNL. This research used resources of the Oak Ridge Leadership Computing Facility at the Oak Ridge National Laboratory, which is supported by the Office of Science of the U.S. Department of Energy under Contract No. DE‐AC05‐00OR22725.The authors would like to thank Ms. Atreyi Samaddar ([email protected]) for voluntarily designing the potential cover art.

Keywords

  • co-continuous
  • fiber-matrix interphases
  • fiber-reinforced polymer composites
  • multiscale
  • nanofibers
  • tough

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