Modulating Electronic Structure with Linearly Fused Pyrazine Units for High-Voltage and Stable Zinc-Organic Batteries Cathode

Authors

• Min-Jian Zhao, Shanghai Key Laboratory of Materials Protection and Advanced Materials in Electric Power, College of Environmental and Chemical Engineering, Shanghai University of Electric Power, Shanghai 200090, China
• Li-Bin Zhang, Shanghai Key Laboratory of Materials Protection and Advanced Materials in Electric Power, College of Environmental and Chemical Engineering, Shanghai University of Electric Power, Shanghai 200090, China
• Jin-Tao Wang, Shanghai Key Laboratory of Materials Protection and Advanced Materials in Electric Power, College of Environmental and Chemical Engineering, Shanghai University of Electric Power, Shanghai 200090, China
• Kun Ding, Shanghai Key Laboratory of Materials Protection and Advanced Materials in Electric Power, College of Environmental and Chemical Engineering, Shanghai University of Electric Power, Shanghai 200090, ChinaFollow
• Hai-Mei Liu, Shanghai Key Laboratory of Materials Protection and Advanced Materials in Electric Power, College of Environmental and Chemical Engineering, Shanghai University of Electric Power, Shanghai 200090, ChinaFollow
• Yong-Gang Wang, Department of Chemistry and Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Institute of New Energy, Fudan University, Shanghai 200433, ChinaFollow

Corresponding Author

Kun Ding (kunding@shiep.edu.cn);
Hai-Mei Liu (liuhm@shiep.edu.cn);
Yong-Gang Wang (ygwang@fudan.edu.cn)

Abstract

High-voltage n-type organic cathode materials are critical for constructing zinc-organic batteries (ZOBs) with high energy density and long cycle life. However, the intrinsically unfavorable electronic structures and relatively high LUMO energy levels of most n-type materials often lead to sluggish kinetics, high solubility, and suboptimal discharge voltages (< 0.8 V). Here, we design a small molecule, quinoxalino[2’,3’:5,6]pyrazino[2,3-f][1,10]phenanthroline (DPQP), as a ZOB cathode by introducing locally electron-deficient motifs into the conjugated backbone of aromatic compounds. The linearly fused pyrazine units extending the pyrazine–benzene framework effectively optimize the electronic structure, thereby significantly enhancing the discharge voltage. Meanwhile, the expanded π-conjugated plane suppresses dissolution and accelerates charge-transfer kinetics. Benefiting from these features, the DPQP electrode exhibits an exceptional increase in average operating voltage from 0.61 V to 1.07 V (vs. Zn²⁺/Zn) at 0.1 A·g^–¹, with an overpotential of only 140 mV. Notably, no discernible voltage decay occurs as the current density increases, indicating rapid and highly reversible redox kinetics. Furthermore, the DPQP cathode delivers outstanding cycling stability, maintaining over 2000 h of continuous operation at 0.1 A·g^–¹ and retaining 82.5% of its capacity after more than 10,000 cycles at 10 A·g^–¹. Remarkably, the DPQP electrode also demonstrates excellent tolerance to extreme temperatures, achieving stable electrochemical performance across a wide temperature range from –20 °C to 60 °C. In addition, a series of spectroscopic and microscopic characterizations confirm the highly reversible redox behavior and Zn²⁺ storage mechanism of the DPQP cathode.

Graphical Abstract

Keywords

Aqueous zinc batteries, Organic cathode, n-type material, Electronic structure design, High voltage

DOI Link

https://doi.org/10.61558/2993-074X.3609

Creative Commons License

This work is licensed under a Creative Commons Attribution 4.0 International License.

Publication Date

2026-05-28

Online Available Date

2026-03-31

Revised Date

2026-03-11

Received Date

2025-12-28

Recommended Citation

Min-Jian Zhao, Li-Bin Zhang, Jin-Tao Wang, Kun Ding, Hai-Mei Liu, Yong-Gang Wang. Modulating Electronic Structure with Linearly Fused Pyrazine Units for High-Voltage and Stable Zinc-Organic Batteries Cathode[J]. Journal of Electrochemistry, 2026, 32(5): 2512291.
DOI: 10.61558/2993-074X.3609
Available at: https://jelectrochem.xmu.edu.cn/journal/vol32/iss5/1