Building ultra-stable and low-temperature aqueous zinc–organic batteries via noncovalent supramolecular self-assembly strategy

• Published in: Chemical engineering journal (Lausanne, Switzerland : 1996) Vol. 487; p. 150527
• Main Authors: Xu, Jie, Yang, Yuting, Zhu, Acheng, Wang, Yuyang, Peng, Bo, Ma, Lianbo, Cao, Yongjie, Wang, Yonggang
• Format: Journal Article
• Language: English
• Published: Elsevier B.V 01.05.2024
• Subjects: Aqueous electrolyte; Hydrogen-bond polymer; Low-temperature operation; Ultra-stable cycling; Zinc-organic batteries; Hydrogen-bond polymer; Zinc-organic batteries; Low-temperature operation; Aqueous electrolyte; Ultra-stable cycling
• ISSN: 1385-8947; 1873-3212
• DOI: 10.1016/j.cej.2024.150527

[Display omitted] •Ultra-stable Zinc-organic batteries was built by H-bonded organic polymer cathode.•Zn//HOP cell shows stable cycling for 20,000 cycles at 2.0 A g−1 with 80 % retention.•The HOP cell can stably operate at –5 °C for 300 cycles without any capacity loss.•Co-insertion mechanism of Zn2+/H3O+ through CO/CO conversion was studied. Zinc-organic batteries (ZOB) have garnered significant attention owing to their design flexibility and abundant raw materials. However, a notable drawback arises from the tendency of organic electrodes to dissolve in the electrolyte during cycling, resulting in diminished cycle stability and a shortened lifespan. Herein, we propose a noncovalent supramolecular self-assembly approach to address the challenge of organic electrode dissolution, namely the hydrogen-bonded organic polymer (HOP) is introduced as the cathode ensuring the electrolyte/electrode stability in ZOB. The HOP comprises perylene anhydride units characterized by robust strong π-π stacking and hydrogen bond connections. This configuration enables the reversible storage of Zn2+/H3O+ through CO/CO bond conversion, as validated by in-situ ATR-FTIR and ex-situ XPS analyses. Employing a 1 m Zn(OTF)2 electrolyte, the Zn//HOP cell exhibited stable cycling at room temperature for 20,000 cycles with nearly 80 % capacity retention and operated at –5 °C for 300 cycles with 100 % capacity retention. Our findings explore the noncovalent supramolecular self-assembly strategy in producing organic electrodes resistant to dissolution.