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.
| Original language | English |
|---|---|
| Article number | eadp4750 |
| Journal | Science Advances |
| Volume | 11 |
| Issue number | 4 |
| DOIs | |
| State | Published - Jan 24 2025 |
Funding
We thank D. Venkataraman from the University of Massachusetts Amherst for allowing us to access attenuated total reflectance Fourier transform infrared spectroscopy. Funding: This work was funded by the Faculty Startup Fund support from the University of Massachusetts Amherst awarded to Y.X., the National Science Foundation (award number 2312559) awarded to Y.X., the National Science Foundation (award numbers ECC S-1934977 and ECC S-2246564) awarded to S.H., the Air Force Office of Scientific Research (grant FA9550-22-1-0408) awarded to S.H., the National Science Foundation (award number CBET -1943813) awarded to J.L., the National Science Foundation (award number DMR-2118448) awarded to M. L., and the National Science Foundation (convergence accelerator award number 2235945) awarded to M.L. Work at Oak Ridge National Laboratory Spallation Neutron Source was sponsored by the Scientific User Facilities Division, Office of Basic Energy Sciences of the US Department of Energy. Oak Ridge National Laboratory is managed by UT-Battelle LLC for US DOE under contract no. DEAC05-00OR22725. The beam time was allocated to BASIS on proposal number IPTS-31174. This research used resources of the Advanced Photon Source, a US Department of Energy (DOE) Office of Science user facility at Argonne National Laboratory and is based on research supported by the US DOE Office of Science-Basic Energy Sciences, under contract no. DE-AC02-06CH11357. Electron microscopy was performed at the Center for Nanophase Materials Sciences (CNMS), which is a US Department of Energy, Office of Science User Facility at Oak Ridge National Laboratory. Author contributions: Project administration: S.H., J.L., M.L., and Y.X. Conceptualization: E.M., M.L., and Y.X. Methodology: Y.Z., A.B., S.R., N.C.O., E.M., J.R., W.H., S.H., J.L., M.L., and Y.X. Investigation: Y.Z., R.C., S.R., T.N., Z.J., N.C.O., E.M., X.Z., J.R., W.H., B.S., J.C., D.K.H., S.H., and Y.X. Visualization: Y.Z., S.R., J.Z., E.M., X.Z., J.R., W.H., B.S., J.C., S.H., M.L., and Y.X. Resources: T.N., S.H., and Y.X. Validation: Y.Z., R.C., T.N., E.M., Z.J., J.R., W.H., B.S., and Y.X. Data curation: Y.Z., R.C., S.R., J.R., W.H., B.S., S.H., and Y.X. Formal analysis: Y.Z., R.C., S.R., T.N., J.Z., N.C.O., Z.J., J.R., W.H., B.S., J.C., M.L., and Y.X. Software: A.B., S.R., and Y.X. Supervision: J.L. and Y.X. Writing-original draft: Y. Z., R.C., S.R., J.Z., J.R., W.H., and Y.X. Writing-review and editing: Y.Z., T. N., J. Z., J.R., W.H., B.S., S.H., J.L., M.L., and Y.X. Funding acquisition: S.H., M.L., J.L., and Y.X. Competing interests: The authors declare that they have no competing interests. Data and materials availability: All data needed to evaluate the conclusions in the paper are present in the paper and/or the Supplementary Materials.