Regulation of Electron Delocalization Region in 2D Heteroligand-Based Copper-Organic Framework to Enhance [Formula: see text] Charge Storage

Hongyu Lu; Jisong Hu; Kaiqi Zhang; Yu Zhang; Botao Jiang; Miao Zhang; Shenzhen Deng; Jingxin Zhao; Huan Pang; Bingang Xu

doi:10.1002/adma.202408396

Regulation of Electron Delocalization Region in 2D Heteroligand-Based Copper-Organic Framework to Enhance ${NH}_{4}^{+}$ Charge Storage

Adv Mater. 2024 Sep;36(39):e2408396. doi: 10.1002/adma.202408396. Epub 2024 Aug 5.

Authors

Hongyu Lu^{1

2}, Jisong Hu³, Kaiqi Zhang⁴, Yu Zhang⁴, Botao Jiang², Miao Zhang⁵, Shenzhen Deng¹, Jingxin Zhao¹, Huan Pang⁶, Bingang Xu¹

Affiliations

¹ Nanotechnology Center, School of Fashion and Textiles, The Hong Kong Polytechnic University, Hung Hom, Kowloon, Hong Kong, 999077, P. R. China.
² State Key Laboratory of Advanced Welding and Joining, School of Materials Science and Engineering, Harbin Institute of Technology, Harbin, 150001, P. R. China.
³ School of Optical and Electronic Information, Huazhong University of Science and Technology, Wuhan, 430074, P. R. China.
⁴ School of Marine Science and Technology, Harbin Institute of Technology at Weihai, Weihai, 264209, P. R. China.
⁵ Department of Chemistry, School of Science, Tianjin University, Tianjin, 300072, P. R. China.
⁶ School of Chemistry and Chemical Engineering, Yangzhou University, Yangzhou, 225002, P. R. China.

PMID: 39101297
DOI: 10.1002/adma.202408396

Abstract

The rechargeable aqueous ammonium ion battery shows great potential in low-cost energy storage system because of its long life and environmental friendliness. However, most inorganic host materials used in ammonium ion batteries are still limited by slow diffusion kinetics. Herein, it is identified that a 2D heteroligand-based copper-organic framework featuring numerous ammonium ion adsorption site in the π-conjugated periodic skeleton supplies multiple accessible redox-active sites for high-performance ammonium storage. Benefitting from the effective regulation of electron delocalization by heteroligand and the inherent hydrogen bond cage mechanism between ammonium ions, the resultant full battery delivers a large specific energy density of 211.84 Wh kg^-1, and it can be stably operated for 12000 cycles at 5 A g^-1 for over 80 days. This explanatory understanding provides a new idea for the rational design of high-performance MOF-based ammonium ion battery cathode materials for efficient energy storage and conversion in the future.

Keywords: NH 4 + $ \rm {NH_{4}}{^+}$ charge storage; 2D metal‐organic framework; Cu‐HHTP‐THBQ; ammonium‐ion batteries; heteroligand.

Abstract

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