A Self-Healing Adhesive Exploiting Hydrogen-Bonding Interactions and Aromatic Disulfide Units in Energetic Composites
- 1Xi’an Modern Chemistry Research Institute, Xi’an 710065, China
- 2State Key Laboratory of Advanced Polymer Materials, Polymer Research Institute of Sichuan University, Sichuan University, Chengdu 610065, China
Abstract
Energetic composites with high solid content are prone to microcracking and interfacial debonding, which can compromise mechanical integrity and service reliability. To address these long-standing durability challenges, herein, a self-healing polyurethane with hydrogen bonds and disulfide bonds (PUHD) was designed by integrating hydrogen-bond reorganization with dynamic disulfide-bond exchange. PUHD was synthesized using polytetramethylene ether glycol (PTMEG) as the soft segment and isophorone diisocyanate (IPDI) and 4,4′-dihydroxydiphenyl disulfide (DHDPS) as hard-segment components. FT-IR, Raman, XRD, GPC, and DSC analyses confirmed the successful construction of a predominantly amorphous dual dynamic network with suitable chain mobility and thermal stability for energetic-composite applications. The neat PUHD exhibited a hardness of 0.94 MPa and a storage modulus of 3.15 MPa at 20 °C and 5 Hz; surface cracks disappeared within 24 h at ambient temperature, and the storage-modulus recovery reached approximately 97%. In sample filler-containing composites, increasing solid content enhanced hardness and modulus but restricted polymer-chain mobility, thereby slowing crack repair and reducing healing recovery. In nitrocellulose/nitroglycerin (NC/NG)-containing composites, the visible crack closure could be achieved within 24 h, while maintaining useful mechanical properties after self-healing. Notably, JQ-e showed the highest initial hardness of 2.69 MPa and retained 2.19 MPa after healing. These findings collectively demonstrate that the synergistic dynamic network not only enables efficient room-temperature crack repair but also preserves adequate mechanical reinforcement, thus offering a viable pathway toward more reliable energetic-composite formulations.
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BibTeX
@article{zhao2026selfhealing,
title = {{A Self-Healing Adhesive Exploiting Hydrogen-Bonding Interactions and Aromatic Disulfide Units in Energetic Composites}},
author = {Huan Zhao and Xiuduo Song and Weilu Yang and Yiwen Hu and Jiangfeng Pei and Bofan Shen and Zhiyu Chen and Jian Kang},
journal = {Polymers},
year = {2026},
month = oct,
doi = {10.3390/polym18212608},
url = {https://www.mdpi.com/2073-4360/18/21/2608},
note = {CC BY 4.0},
}
RIS
TY - JOUR
TI - A Self-Healing Adhesive Exploiting Hydrogen-Bonding Interactions and Aromatic Disulfide Units in Energetic Composites
AU - Huan Zhao
AU - Xiuduo Song
AU - Weilu Yang
AU - Yiwen Hu
AU - Jiangfeng Pei
AU - Bofan Shen
AU - Zhiyu Chen
AU - Jian Kang
PY - 2026
DA - 2026/10/22
JO - Polymers
DO - 10.3390/polym18212608
UR - https://www.mdpi.com/2073-4360/18/21/2608
AB - Energetic composites with high solid content are prone to microcracking and interfacial debonding, which can compromise mechanical integrity and service reliability. To address these long-standing durability challenges, herein, a self-healing polyurethane with hydrogen bonds and disulfide bonds (PUHD) was designed by integrating hydrogen-bond reorganization with dynamic disulfide-bond exchange. PUHD was synthesized using polytetramethylene ether glycol (PTMEG) as the soft segment and isophorone diisocyanate (IPDI) and 4,4′-dihydroxydiphenyl disulfide (DHDPS) as hard-segment components. FT-IR, Raman, XRD, GPC, and DSC analyses confirmed the successful construction of a predominantly amorphous dual dynamic network with suitable chain mobility and thermal stability for energetic-composite applications. The neat PUHD exhibited a hardness of 0.94 MPa and a storage modulus of 3.15 MPa at 20 °C and 5 Hz; surface cracks disappeared within 24 h at ambient temperature, and the storage-modulus recovery reached approximately 97%. In sample filler-containing composites, increasing solid content enhanced hardness and modulus but restricted polymer-chain mobility, thereby slowing crack repair and reducing healing recovery. In nitrocellulose/nitroglycerin (NC/NG)-containing composites, the visible crack closure could be achieved within 24 h, while maintaining useful mechanical properties after self-healing. Notably, JQ-e showed the highest initial hardness of 2.69 MPa and retained 2.19 MPa after healing. These findings collectively demonstrate that the synergistic dynamic network not only enables efficient room-temperature crack repair but also preserves adequate mechanical reinforcement, thus offering a viable pathway toward more reliable energetic-composite formulations.
SN - 2073-4360
ER -