Self‐reporting and Biodegradable Thermosetting Solid Polymer Electrolyte

• Published in: Angewandte Chemie International Edition 2024-02, Vol.63 (7), p.e202319003-n/a
• Main Authors: Zhou, Ya‐Nan, Yong, Haiyang, Guo, Rui, Wang, Kaixuan, Li, Zhili, Hua, Weibo, Zhou, Dezhong
• Format: Article
• Language: English
• Subjects: Aliphatic amines; Amines; Amino acids; Biodegradability; Biodegradable; Biodegradation; Catalysis; Chemical damage; Conductivity; Electrolytes; Hyperbranched Polymer; Ion currents; Mechanical properties; Molten salt electrolytes; Poly(β-Amino Ester); Polymers; Polyols; Self-Fluorescence; Sodium; Solid electrolytes; Thermal stability; Topological Polymer
• ISSN: 1433-7851; 1521-3773
• DOI: 10.1002/anie.202319003

To date, significant efforts have been dedicated to improve their ionic conductivity, thermal stability, and mechanical strength of solid polymer electrolytes (SPEs). However, direct monitoring of physical and chemical changes in SPEs is still lacking. Moreover, existing thermosetting SPEs are hardly degradable. Herein, by overcoming the limitation predicted by Flory theory, self‐reporting and biodegradable thermosetting hyperbranched poly(β‐amino ester)‐based SPEs (HPAE‐SPEs) are reported. HPAE is successfully synthesized through a well‐controlled “A2+B4” Michael addition strategy and then crosslinked it in situ to produce HPAE‐SPEs. The multiple tertiary aliphatic amines at the branching sites confer multicolour luminescence to HPAE‐SPEs, enabling direct observation of its physical and chemical damage. After use, HPAE‐SPEs can be rapidly hydrolysed into non‐hazardous β‐amino acids and polyols via self‐catalysis. Optimized HPAE‐SPE exhibits an ionic conductivity of 1.3×10−4 S/cm at 60 °C, a Na+ transference number ( tNa+ ${{t}_{Na}^{+}}$ ) of 0.67, a highly stable sodium plating‐stripping behaviour and a low overpotential of ≈190 mV. This study establishes a new paradigm for developing SPEs by engineering multifunctional polymers. The self‐reporting and biodegradable properties would greatly expand the scope of applications for SPEs. Despite the significant effort to improve the performance of solid polymer electrolytes (SPEs), direct monitoring of physical and chemical changes as well as the sustainability in SPEs is still lacking. Here, we report a self‐reporting and biodegradable thermosetting SPE via well‐designed structure to analyze the performance mechanism behind SPEs and promote their environmental friendliness.