Defects vibrations engineering for enhancing interfacial thermal transport in polymer composites

Yijie Zhou; Robert Ciarla; Artittaya Boonkird; Saqlain Raza; Thanh Nguyen; Jiawei Zhou; Naresh C Osti; Eugene Mamontov; Zhang Jiang; Xiaobing Zuo; Jeewan Ranasinghe; Weiguo Hu; Brendan Scott; Jihua Chen; Dale K Hensley; Shengxi Huang; Jun Liu; Mingda Li; Yanfei Xu

doi:10.1126/sciadv.adp6516

Defects vibrations engineering for enhancing interfacial thermal transport in polymer composites

Sci Adv. 2025 Jan 24;11(4):eadp6516. doi: 10.1126/sciadv.adp6516. Epub 2025 Jan 22.

Authors

Yijie Zhou¹, Robert Ciarla², Artittaya Boonkird³, Saqlain Raza⁴, Thanh Nguyen³, Jiawei Zhou⁵, Naresh C Osti⁶, Eugene Mamontov⁶, Zhang Jiang⁷, Xiaobing Zuo⁷, Jeewan Ranasinghe⁸, Weiguo Hu⁹, Brendan Scott¹, Jihua Chen¹⁰, Dale K Hensley¹⁰, Shengxi Huang^{8

11}, Jun Liu⁴, Mingda Li³, Yanfei Xu^{1

2}

Affiliations

¹ Department of Mechanical and Industrial Engineering, University of Massachusetts Amherst, Amherst, MA 01003, USA.
² Department of Chemical Engineering, University of Massachusetts Amherst, Amherst, MA 01003, USA.
³ Department of Nuclear Science and Engineering, Massachusetts Institute of Technology, Cambridge, MA 02139, USA.
⁴ Department of Mechanical and Aerospace Engineering, North Carolina State University, Raleigh, NC 27695, USA.
⁵ Department of Materials Science and Engineering, Stanford University, Stanford, CA 94305, USA.
⁶ Neutron Scattering Division, Oak Ridge National Laboratory, Oak Ridge, TN 37831, USA.
⁷ Advanced Photon Source, Argonne National Laboratory, Argonne, IL 60439, USA.
⁸ Department of Electrical and Computer Engineering, Rice University, Houston, TX 77005, USA.
⁹ Department of Polymer Science and Engineering, University of Massachusetts Amherst, Amherst, MA 01003, USA.
¹⁰ Center for Nanophase Materials Sciences, Oak Ridge National Laboratory, Oak Ridge, TN 37831, USA.
¹¹ Rice Advanced Materials Institute, Rice University, Houston, TX 77005, USA.

PMID: 39841839
DOI: 10.1126/sciadv.adp6516

Abstract

To push upper boundaries of thermal conductivity in polymer composites, understanding of thermal transport mechanisms is crucial. Despite extensive simulations, systematic experimental investigation on thermal transport in polymer composites is limited. To better understand thermal transport processes, we design polymer composites with perfect fillers (graphite) and defective fillers (graphite oxide), using polyvinyl alcohol (PVA) as a matrix model. Measured thermal conductivities of ~1.38 ± 0.22 W m^-1 K^-1 in PVA/defective filler composites is higher than those of ~0.86 ± 0.21 W m^-1 K^-1 in PVA/perfect filler composites, while measured thermal conductivities in defective fillers are lower than those of perfect fillers. We identify how thermal transport occurs across heterogeneous interfaces. Thermal transport measurements, neutron scattering, quantum mechanical modeling, and molecular dynamics simulations reveal that vibrational coupling between PVA and defective fillers at PVA/filler interfaces enhances thermal conductivity, suggesting that defects in polymer composites improve thermal transport by promoting this vibrational coupling.