Superharmonic proton motion in high-energy-density organic electrodes for aqueous zinc batteries

Boyu Li, Jiabin Ma, Ke Yang, Yuhang Li, Maggie Ng, Yuetao Ma, Xufei An, Xing Cheng, Jinshuo Mi, Man-Chung Tang (), Yan-Bing He () and Feiyu Kang ()
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Boyu Li: Tsinghua Shenzhen International Graduate School, Shenzhen All-Solid-State Lithium Battery Electrolyte Engineering Research Center, Institute of Materials Research (IMR)
Jiabin Ma: Tsinghua Shenzhen International Graduate School, Shenzhen All-Solid-State Lithium Battery Electrolyte Engineering Research Center, Institute of Materials Research (IMR)
Ke Yang: Tsinghua Shenzhen International Graduate School, Shenzhen All-Solid-State Lithium Battery Electrolyte Engineering Research Center, Institute of Materials Research (IMR)
Yuhang Li: Tsinghua Shenzhen International Graduate School, Shenzhen All-Solid-State Lithium Battery Electrolyte Engineering Research Center, Institute of Materials Research (IMR)
Maggie Ng: Tsinghua Shenzhen International Graduate School, Shenzhen All-Solid-State Lithium Battery Electrolyte Engineering Research Center, Institute of Materials Research (IMR)
Yuetao Ma: Tsinghua Shenzhen International Graduate School, Shenzhen All-Solid-State Lithium Battery Electrolyte Engineering Research Center, Institute of Materials Research (IMR)
Xufei An: Tsinghua Shenzhen International Graduate School, Shenzhen All-Solid-State Lithium Battery Electrolyte Engineering Research Center, Institute of Materials Research (IMR)
Xing Cheng: Tsinghua Shenzhen International Graduate School, Shenzhen All-Solid-State Lithium Battery Electrolyte Engineering Research Center, Institute of Materials Research (IMR)
Jinshuo Mi: Tsinghua Shenzhen International Graduate School, Shenzhen All-Solid-State Lithium Battery Electrolyte Engineering Research Center, Institute of Materials Research (IMR)
Man-Chung Tang: Tsinghua Shenzhen International Graduate School, Shenzhen All-Solid-State Lithium Battery Electrolyte Engineering Research Center, Institute of Materials Research (IMR)
Yan-Bing He: Tsinghua Shenzhen International Graduate School, Shenzhen All-Solid-State Lithium Battery Electrolyte Engineering Research Center, Institute of Materials Research (IMR)
Feiyu Kang: Tsinghua Shenzhen International Graduate School, Shenzhen All-Solid-State Lithium Battery Electrolyte Engineering Research Center, Institute of Materials Research (IMR)

Nature Communications, 2025, vol. 16, issue 1, 1-11

Abstract: Abstract The limited proton transfer kinetics within organic positive electrodes restricts the proton storage capacity and hinders achieving high energy density in aqueous zinc-organic batteries. Herein, we obtain superharmonic motion of proton by crosslinking short hydrogen-bonds network within the positive electrode matrix to achieve fast proton transfer. Specifically, the pyrazino[2, 3-g]quinoxaline-5, 10-dione owing strong electrostatic and hydrogen-bond interactions with hydrogen ions is synthesized, which could attract concentrated hydronium and trigger local proton enrichment. Spatially confined water-hydronium domains are therefore formed to generate short hydrogen bonds around pyrazino[2, 3-g]quinoxaline-5, 10-dione molecules. Moreover, the 4,4’-diaminodiphenylamine and polytetrafluoroethylene binder exhibits a mutual affinity with pyrazino[2, 3-g]quinoxaline-5, 10-dione due to the strong hydrogen-bond interactions of them, which reduce the intermolecular distance within positive electrode and construct a highly interconnected state of water-hydronium domains, thereby establishing the short hydrogen bonds network throughout the electrode matrix. The rapid proton transport through short hydrogen bonds consequently reduces the polarization of aqueous zinc-organic batteries (1.47 × 10−3 S cm−1). As a result, the composite positive electrode delivers specific energy of 400 Wh kg−1 at 0.1 A g−1.

Date: 2025
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DOI: 10.1038/s41467-025-65136-w

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