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Vol. 18 (2026)

Synergistic Ultramicropore and Hierarchical Pore Engineering in Heteroatom-Doped Carbon for High-Performance Zinc-Ion Capacitors

https://doi.org/10.1007/s40820-026-02181-0
Jiale Zhang
Department of Chemistry, College of Science, Hebei Agricultural University, Baoding 071001, People’s Republic of China
Ruifang Zhang
College of Land and Resources, Hebei Agricultural University, Baoding 071001, People’s Republic of China
Yangbo Du
Key Laboratory of Civil Aviation Thermal Disaster Control and Emergency, Civil Aviation University of China, Tianjin 300300, People’s Republic of China
Shuaihua Zhang
Department of Chemistry, College of Science, Hebei Agricultural University, Baoding 071001, People’s Republic of China
Runze Gao
Department of Chemistry, College of Science, Hebei Agricultural University, Baoding 071001, People’s Republic of China
Xuanqi Huang
Department of Chemistry, College of Science, Hebei Agricultural University, Baoding 071001, People’s Republic of China
Qi Yang
Key Laboratory of Civil Aviation Thermal Disaster Control and Emergency, Civil Aviation University of China, Tianjin 300300, People’s Republic of China
Debin Kong
Wuzhen Laboratory, Jiaxing 314500, People’s Republic of China
Zhichang Xiao
Department of Chemistry, College of Science, Hebei Agricultural University, Baoding 071001, People’s Republic of China

Corresponding Author: Zhichang Xiao

xiaozc@hebau.edu.cn

Nano-Micro Letters, Vol. 18 (2026), Article Number: 336

Abstract

Carbonaceous zinc-ion capacitors (ZICs) offer inherent advantages for energy storage, yet the role of pore structures in enabling high zinc-ion capacitance remains underexplored. Herein, a dual-molten-salt regulation strategy is employed to derive N/O/S-doped porous carbon nanomaterials, achieving a high specific surface area (SSA) of 2523 m2 g−1 with ultramicropores (< 0.86 nm) contributing 30.6% of the total SSA. Structural analyses reveal that increasing molten FeCl3 content yields materials with comparable heteroatom contents and defect structures, but a progressive shift from ultramicropores to mesopores. Crucially, the individual contributions of the pore structure are decoupled by both in situ characterizations and theoretical simulations: The ultramicropores facilitate the desolvation of [Zn(H2O)6]2+ (ultramicropore effect), while the hierarchical pores ensure rapid ion transport (hierarchical pore effect). The optimized HHPC-2 delivers a high specific capacitance of 222.6 F g−1 at 1 A g−1 and an energy density of 120.0 Wh kg−1 in ZICs. Intriguingly, its outstanding oxygen reduction reaction catalytic activity enables self-charging upon air exposure after a full discharge, achieving a self-charging rate of 15 mAh g−1 h−1 and recovering 80% of the externally charged capacity in subsequent discharge cycles. This positions the device as highly promising for practical deployment in regions with intermittent grid power supplies.


Highlights:
1 A series of N/O/S-doped porous carbons are synthesized through a dual-molten-salt regulation strategy with controllable ultramicropore and mesopore structures.
2 The distinct functions of ultramicropores and hierarchical pores are delineated experimentally and theoretically, demonstrating that ultramicropores are crucial for facilitating the desolvation of [Zn(H2O)6]2+, while the hierarchical network ensures rapid ion transport.
3 The optimized cathode delivers a high specific capacitance (336.9 F g−1), outstanding energy density (120.0 Wh kg−1) and excellent air self-charging capability.

Keywords

Ultramicropore Hierarchical pore Carbonaceous zinc-ion capacitor Desolvation effect Air self-charging
Zhang, Jiale, Ruifang Zhang, Yangbo Du, Shuaihua Zhang, Runze Gao, Xuanqi Huang, Qi Yang, Debin Kong, and Zhichang Xiao. 2026. “Synergistic Ultramicropore and Hierarchical Pore Engineering in Heteroatom-Doped Carbon for High-Performance Zinc-Ion Capacitors”. Nano-Micro Letters 18 (April):336. https://doi.org/10.1007/s40820-026-02181-0.
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