Molecular‐Level Interface Engineering and Additive‐Induced Crystallinity Tuning for High‐Performance Thermally Conductive Polymer Composites

M Minwoo Rim (Department of Polymer‐Nano Science and Technology Department of Nano Convergence Engineering Jeonbuk National University Jeonju 54896 Republic of Korea) H Huan Huu Pham (Department of Polymer‐Nano Science and Technology Department of Nano Convergence Engineering Jeonbuk National University Jeonju 54896 Republic of Korea) H Hyerim Lee J Jaeseok Hyeong (Department of Polymer‐Nano Science and Technology Department of Nano Convergence Engineering Jeonbuk National University Jeonju 54896 Republic of Korea) Y Youngjae Wi (Department of Polymer‐Nano Science and Technology Department of Nano Convergence Engineering Jeonbuk National University Jeonju 54896 Republic of Korea) J Jahyeon Koo (Department of Polymer‐Nano Science and Technology Department of Nano Convergence Engineering Jeonbuk National University Jeonju 54896 Republic of Korea) D Duy Thanh Tran (Department of Polymer‐Nano Science and Technology Department of Nano Convergence Engineering Jeonbuk National University Jeonju 54896 Republic of Korea) S Seok‐In Na (Department of Flexible and Printable Electronics and LANL‐JBNU Engineering Institute‐Korea Jeonbuk National University Jeonju 54896 Republic of Korea) D Dong‐Gue Kang (Department of Polymer‐Nano Science and Technology Department of Nano Convergence Engineering Jeonbuk National University Jeonju 54896 Republic of Korea) K Kwang‐Un Jeong (Department of Polymer‐Nano Science and Technology Department of Nano Convergence Engineering Jeonbuk National University Jeonju 54896 Republic of Korea)

Abstract

Abstract To boost up the properties of thermally conductive polymer composites, it is essential to conduct comprehensive research focused on interface engineering between the polymer matrix and fillers. Hexagonal boron nitride (BN) or expanded graphite (EG) are commonly utilized as nanofillers to improve the thermal conductivity of polymer composites. However, the interfacial interactions between the polymer matrix and nanofillers are generally weak, making effective thermal conductivity challenging. To address this issue, we have designed and synthesized an electron‐rich and aromatic tetrathiafulvalene‐based reactive mesogen (TRM), which not only possesses high thermal conductivity but also exhibits excellent interfacial affinity with BN and EG at the molecular level. Systematic experiments, including photophysical, thermodynamic, structural, and computational analyses, reveal that the thermal conductivity of TRM‐based polymer composites is substantially enhanced due to effective interfacial interactions between TRM and fillers. The TRM composites experimentally show excellent thermal conductivity based on enhanced interfacial phonon transfer, and these results are supported by theoretical interpretations. These findings underscore the critical importance of interface engineering between the polymer matrix and fillers at the molecular level in maximizing the material properties of polymer composites.

Article Details

Volume / Issue Vol. 64, Issue 30
Published July 21, 2025
ISSN 1433-7851
Publisher Wiley

Journal Info

Angewandte Chemie International Edition

Wiley

ISSN: 1433-7851 Physical Sciences

Authors (10)

M

Minwoo Rim

Department of Polymer‐Nano Science and Technology Department of Nano Convergence Engineering Jeonbuk National University Jeonju 54896 Republic of Korea

H

Huan Huu Pham

Department of Polymer‐Nano Science and Technology Department of Nano Convergence Engineering Jeonbuk National University Jeonju 54896 Republic of Korea

H

Hyerim Lee

J

Jaeseok Hyeong

Department of Polymer‐Nano Science and Technology Department of Nano Convergence Engineering Jeonbuk National University Jeonju 54896 Republic of Korea

Y

Youngjae Wi

Department of Polymer‐Nano Science and Technology Department of Nano Convergence Engineering Jeonbuk National University Jeonju 54896 Republic of Korea

J

Jahyeon Koo

Department of Polymer‐Nano Science and Technology Department of Nano Convergence Engineering Jeonbuk National University Jeonju 54896 Republic of Korea

D

Duy Thanh Tran

Department of Polymer‐Nano Science and Technology Department of Nano Convergence Engineering Jeonbuk National University Jeonju 54896 Republic of Korea

S

Seok‐In Na

Department of Flexible and Printable Electronics and LANL‐JBNU Engineering Institute‐Korea Jeonbuk National University Jeonju 54896 Republic of Korea

D

Dong‐Gue Kang

Department of Polymer‐Nano Science and Technology Department of Nano Convergence Engineering Jeonbuk National University Jeonju 54896 Republic of Korea

K

Kwang‐Un Jeong

Department of Polymer‐Nano Science and Technology Department of Nano Convergence Engineering Jeonbuk National University Jeonju 54896 Republic of Korea