Issue

Vol. 18 (2026)

Hydrogen-Bonded Interfacial Super-Assembly of Spherical Carbon Superstructures for High-Performance Zinc Hybrid Capacitors

https://doi.org/10.1007/s40820-025-01883-1
Yang Qin
Shanghai Key Lab of Chemical Assessment and Sustainability, School of Chemical Science and Engineering, Tongji University, 1239 Siping Rd., Shanghai 200092, People’s Republic of China
Chengmin Hu
Department of Chemistry, Shanghai Key Lab of Molecular Catalysis and Innovative Materials and Collaborative Innovation Center of Chemistry for Energy Materials, Fudan University, 2005 Songhu Rd., Shanghai 200438, People’s Republic of China
Qi Huang
Institute for Electric Light Sources, School of Information Science and Technology, Fudan University, 2005 Songhu Rd., Shanghai 200438, People’s Republic of China
Yaokang Lv
College of Chemical Engineering, Zhejiang University of Technology, 18 Chaowang Rd., Hangzhou 310014, People’s Republic of China
Ziyang Song
Shanghai Key Lab of Chemical Assessment and Sustainability, School of Chemical Science and Engineering, Tongji University, 1239 Siping Rd., Shanghai 200092, People’s Republic of China
Lihua Gan
Shanghai Key Lab of Chemical Assessment and Sustainability, School of Chemical Science and Engineering, Tongji University, 1239 Siping Rd., Shanghai 200092, People’s Republic of China
Mingxian Liu
Shanghai Key Lab of Chemical Assessment and Sustainability, School of Chemical Science and Engineering, Tongji University, 1239 Siping Rd., Shanghai 200092, People’s Republic of China

Corresponding Author: Mingxian Liu

liumx@tongji.edu.cn

Nano-Micro Letters, Vol. 18 (2026), Article Number: 38

Abstract

Carbon superstructures with multiscale hierarchies and functional attributes represent an appealing cathode candidate for zinc hybrid capacitors, but their tailor-made design to optimize the capacitive activity remains a confusing topic. Here we develop a hydrogen-bond-oriented interfacial super-assembly strategy to custom-tailor nanosheet-intertwined spherical carbon superstructures (SCSs) for Zn-ion storage with double-high capacitive activity and durability. Tetrachlorobenzoquinone (H-bond acceptor) and dimethylbenzidine (H-bond donator) can interact to form organic nanosheet modules, which are sequentially assembled, orientally compacted and densified into well-orchestrated superstructures through multiple H-bonds (N–H···O). Featured with rich surface-active heterodiatomic motifs, more exposed nanoporous channels, and successive charge migration paths, SCSs cathode promises high accessibility of built-in zincophilic sites and rapid ion diffusion with low energy barriers (3.3 Ω s−0.5). Consequently, the assembled Zn||SCSs capacitor harvests all-round improvement in Zn-ion storage metrics, including high energy density (166 Wh kg−1), high-rate performance (172 mAh g−1 at 20 A g−1), and long-lasting cycling lifespan (95.5% capacity retention after 500,000 cycles). An opposite charge-carrier storage mechanism is rationalized for SCSs cathode to maximize spatial capacitive charge storage, involving high-kinetics physical Zn2+/CF3SO3− adsorption and chemical Zn2+ redox with carbonyl/pyridine groups. This work gives insights into H-bond-guided interfacial super-assembly design of superstructural carbons toward advanced energy storage.


Highlights:
1 The spherical carbon superstructures (SCS-6) are synthesized by a hydrogen-bonded interfacial super-assembly, owning surface-opening pores, interconnected channels and rich heteroatom species.
2 Maximized accessibility of surface-active sites and opposite charge-carrier storage mechanism ensure high ion storage efficiency.
3 The assembled zinc-ion hybrid capacitor based on SCS-6 delivers ultrahigh energy density (166 Wh kg−1) and super-stable cycle lifespan (500,000 cycles).

Keywords

Hydrogen bonds Interfacial super-assembly Spherical carbon superstructures Zn hybrid capacitors Energy storage
Qin, Yang, Chengmin Hu, Qi Huang, Yaokang Lv, Ziyang Song, Lihua Gan, and Mingxian Liu. 2025. “Hydrogen-Bonded Interfacial Super-Assembly of Spherical Carbon Superstructures for High-Performance Zinc Hybrid Capacitors”. Nano-Micro Letters 18 (August):38. https://doi.org/10.1007/s40820-025-01883-1.
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