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Porous Structure‐Electrochemical Performance Relationship of Carbonaceous Electrode‐Based Zinc Ion Capacitors

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Advanced Functional Materials
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Kang Xiao at Nanchang University
Kang Xiao
Xudong Jiang
Xudong Jiang
Xudong Jiang
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Siping Zeng
Siping Zeng
Siping Zeng
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Jierui Chen
Jierui Chen
Jierui Chen
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Abstract and Figures

The porous structure is critical for carbonaceous electrode‐based zinc‐ion capacitors (ZICs) to achieve excellent electrochemical performance, but the corresponding porous structure‐electrochemical performance relationship is yet to be fully understand. Herein, three types of N‐doped carbons with different porous structures are developed to investigate the relationship between the pore size distribution and the electrochemical performance of the devices. The optimized porous carbon (LVCR) exhibits large electrochemical surface area, plentiful oxygen functional groups, and hierarchical porous structure that facilitates electron transfer and ion diffusion. Consequently, the LVCR‐based ZIC exhibits a remarkable peak power density of 31.4 kW kg⁻¹ and an impressive specific energy density of 126.6 Wh kg⁻¹. Moreover, it demonstrates exceptional longevity, retaining the capacitance of 97.7% even after undergoing 50 000 cycles. Systematic characterization demonstrates that the macroporous and mesoporous structures determine the different stages of Zn²⁺ storage kinetics. The excellent Zn²⁺ storage and electrochemical performance of LVCR are attributed to the fast ion transport channels provided by the hierarchical porous structure and facilitated reversible chemisorption and desorption. This work not only deepens the understanding of charge storage mechanism, but also provides guidelines for rationally designing carbonaceous materials toward high‐performance ZICs in the view of porous structure‐electrochemical performance relationship.
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RESEARCH ARTICLE
www.afm-journal.de
Porous Structure-Electrochemical Performance Relationship
of Carbonaceous Electrode-Based Zinc Ion Capacitors
Kang Xiao, Xudong Jiang, Siping Zeng, Jierui Chen, Ting Hu, Kai Yuan,*
and Yiwang Chen*
The porous structure is critical for carbonaceous electrode-based zinc-ion
capacitors (ZICs) to achieve excellent electrochemical performance, but the
corresponding porous structure-electrochemical performance relationship is
yet to be fully understand. Herein, three types of N-doped carbons with
different porous structures are developed to investigate the relationship
between the pore size distribution and the electrochemical performance of the
devices. The optimized porous carbon (LVCR) exhibits large electrochemical
surface area, plentiful oxygen functional groups, and hierarchical porous
structure that facilitates electron transfer and ion diffusion. Consequently, the
LVCR-based ZIC exhibits a remarkable peak power density of 31.4 kW kg−1
and an impressive specific energy density of 126.6 Wh kg−1.Moreover,it
demonstrates exceptional longevity, retaining the capacitance of 97.7% even
after undergoing 50 000 cycles. Systematic characterization demonstrates that
the macroporous and mesoporous structures determine the different stages
of Zn2+storage kinetics. The excellent Zn2+storage and electrochemical
performance of LVCR are attributed to the fast ion transport channels
provided by the hierarchical porous structure and facilitated reversible
chemisorption and desorption. This work not only deepens the understanding
of charge storage mechanism, but also provides guidelines for rationally
designing carbonaceous materials toward high-performance ZICs in the view
of porous structure-electrochemical performance relationship.
K. Xiao, X. Jiang, S. Zeng, J. Chen, K. Yuan, Y. Chen
College of Chemistry and Chemical Engineering/Film Energy Chemistry
for Jiangxi Provincial Key Laboratory (FEC)
Nanchang University
999 Xuefu Avenue, Nanchang 330031, China
E-mail: kai.yuan@ncu.edu.cn;ywchen@ncu.edu.cn
K. Xiao, T. Hu
School of Physics and Materials Science
Nanchang University
999 Xuefu Avenue, Nanchang 330031, China
Y. C h e n
College of Chemistry and Chemical Engineering/Key Laboratory of Fluorine
and Silicon for Energy Materials and Chemistry of Ministry of Education
Jiangxi Normal University
99 Ziyang Avenue, Nanchang 330022, China
The ORCID identification number(s) for the author(s) of this article
can be found under https://doi.org/10.1002/adfm.202405830
DOI: 10.1002/adfm.202405830
1. Introduction
Currently, the explosive growth of electric
vehicles, consumer electronics, and smart
grid energy storage has dramatically ac-
celerated the development of ecient and
economical electrochemical energy storage
(EES) systems.[–]Among numerous en-
ergy storage systems, aqueous EES sys-
tems have been extensively investigated for
their high safety and low cost.[–]However,
among the currently commercialized aque-
ous EES devices, such as lead-based and
nickel-based rechargeable batteries, they all
face problems including poor cycle life and
low energy density, which hinder their po-
tential for further applications.[,]Aque-
ous zinc-based energy storage devices are
receiving sustained interest due to in-
expensive aqueous electrolytes and high-
capacity zinc metal anodes.[–]Zinc metal
serves as a desirable anode with excel-
lent theoretical capacity (volumetric, 
mAh cm−; gravimetric,  mAh g−),
high hydrogen overpotential and low re-
dox potential (−. V vs standard hydro-
gen electrode (SHE)).[–]Nevertheless,
the commonly utilized transition metal ox-
ide cathodes in zinc ion batteries are prone
to dissolution during cycling, leading to structural disruption,
which greatly reduces the capacity and lifetime of the device.[,]
Zinc ion capacitors (ZICs) are usually composed of a capacitor-
type cathode (porous carbon) and a battery-type anode (zinc
metal), eectively combining the merits of the high power
density of supercapacitors and the superior energy density of
batteries.[–]Among them, the porous carbon cathode theo-
retically has infinite cycle life due to the reversible Zn+adsorp-
tion/desorption process.[–]However, porous carbon materials
currently face the problems of pore size mismatch with the size
of hydrated Zn+ions and the diculty of precise regulation of
the pore structure, which hinder the further improvement of the
energy density of ZICs.[]In ZICs, [Zn(HO)]+serves as the
main charge carrier during charging and discharging with the
ion size of . nm. Due to the uneven pore size distribution
of carbon materials, [Zn(HO)]+is hard to rapidly enter the
depths of porous carbon materials, and the slow ion diusion and
electron conduction lead to a serious decrease in electrochemi-
cal active sites utilization and poor Zn+storage capacity. In our
Adv. Funct. Mater. 2024, 2405830 © 2024 Wiley-VCH GmbH
2405830 (1 of 10)
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