Phosphorus-Mediated Local Charge Distribution of N-Configuration Adsorption Sites with Enhanced Zincophilicity and Hydrophilicity for High-Energy-Density Zn-Ion Hybrid Supercapacitors

Tailor-made carbonaceous-based cathodes with zincophilicity and hydrophilicity are highly desirable for Zn-ion storage applications, but it remains a great challenge to achieve both advantages in the synthesis. In this work, a template electrospinning strategy is developed to synthesize nitrogen and...

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Bibliographic Details
Published in:Small (Weinheim an der Bergstrasse, Germany) Germany), 2023-11, Vol.19 (45), p.e2302629-e2302629
Main Authors: Lu, Wen, Xie, Bin-Bin, Yang, Chen, Tian, Cong, Yan, Lei, Ning, Jiqiang, Li, Sha, Zhong, Yijun, Hu, Yong
Format: Article
Language:English
Subjects:
Adsorption
Carbon fibers
Charge density
Charge distribution
Charge materials
Density functional theory
Electronegativity
Energy storage
Hydrophilicity
Ion migration
Ion storage
Molecular dynamics
Nanotechnology
Nitrogen
Reaction kinetics
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Summary:Tailor-made carbonaceous-based cathodes with zincophilicity and hydrophilicity are highly desirable for Zn-ion storage applications, but it remains a great challenge to achieve both advantages in the synthesis. In this work, a template electrospinning strategy is developed to synthesize nitrogen and phosphorous co-doped hollow porous carbon nanofibers (N, P-HPCNFs), which deliver a high capacity of 230.7 mAh g at 0.2 A g , superior rate capability of 131.0 mAh g at 20 A g , and a maximum energy density of 196.10 Wh kg at the power density of 155.53 W kg . Density functional theory calculations (DFT) reveal that the introduced P dopants regulate the distribution of local charge density of carbon materials and therefore facilitate the adsorption of Zn ions due to the increased electronegativity of pyridinic-N. Ab initio molecular dynamics (AIMD) simulations indicate that the doped P species induce a series of polar sites and create a hydrophilic microenvironment, which decreases the impedance between the electrode and the electrolyte and therefore accelerates the reaction kinetics. The marriage of ex situ/in situ experimental analyses and theoretical simulations uncovers the origin of the enhanced zincophilicity and hydrophilicity of N, P-HPCNFs for energy storage, which accounts for the faster ion migration and electrochemical processes.
ISSN:1613-6810
1613-6829
DOI:10.1002/smll.202302629