Volume 62, Issue 38 e202309446
Research Article

NH4+ Charge Carrier Coordinated H-Bonded Organic Small Molecule for Fast and Superstable Rechargeable Zinc Batteries

Dr. Ziyang Song

Dr. Ziyang Song

Shanghai Key Lab of Chemical Assessment and Sustainability, School of Chemical Science and Engineering, Tongji University, Shanghai, 200092 P. R. China

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Dr. Ling Miao

Dr. Ling Miao

Shanghai Key Lab of Chemical Assessment and Sustainability, School of Chemical Science and Engineering, Tongji University, Shanghai, 200092 P. R. China

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Dr. Yaokang Lv

Dr. Yaokang Lv

College of Chemical Engineering, Zhejiang University of Technology, Hangzhou, 310014 P. R. China

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Prof. Lihua Gan

Prof. Lihua Gan

Shanghai Key Lab of Chemical Assessment and Sustainability, School of Chemical Science and Engineering, Tongji University, Shanghai, 200092 P. R. China

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Prof. Mingxian Liu

Corresponding Author

Prof. Mingxian Liu

Shanghai Key Lab of Chemical Assessment and Sustainability, School of Chemical Science and Engineering, Tongji University, Shanghai, 200092 P. R. China

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First published: 28 July 2023
Citations: 34

Graphical Abstract

Ultrastable lock-and-key H-bonding networks between octuple-active 2, 7-dinitropyrene-4, 5, 9, 10-tetraone and tetrahedral NH4+ charge carrier are designed, which conquers its stability barrier in aqueous electrolyte and achieves fast diffusion kinetics of non-metallic charge carrier. A unique two-step four-electron NH4+ coordination mechanism brings the Zn-organic battery high capacity, superior rate capability and superstable cyclability.

Abstract

Organic small molecules as high-capacity cathodes for Zn-organic batteries have inspired numerous interests, but are trapped by their easy-dissolution in electrolytes. Here we knit ultrastable lock-and-key hydrogen-bonding networks between 2, 7-dinitropyrene-4, 5, 9, 10-tetraone (DNPT) and NH4+ charge carrier. DNPT with octuple-active carbonyl/nitro centers (H-bond acceptor) are redox-exclusively accessible for flexible tetrahedral NH4+ ions (H-bond donator) but exclude larger and rigid Zn2+, due to a lower activation energy (0.14 vs. 0.31 eV). NH4+ coordinated H-bonding chemistry conquers the stability barrier of DNPT in electrolyte, and gives fast diffusion kinetics of non-metallic charge carrier. A stable two-step 4e NH4+ coordination with DNPT cathode harvests a high capacity (320 mAh g−1), a high-rate capability (50 A g−1) and an ultralong life (60,000 cycles). This finding points to a new paradigm for H-bond stabilized organic small molecules to design advanced zinc batteries.

Conflict of interest

The authors declare no conflict of interest.

Data Availability Statement

The data that support the findings of this study are available from the corresponding author upon reasonable request.

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