Study on the Li⁺ Desolvation Mechanism of Doped Carbon Nanotubes and Their Regulatory Effect on the Performance of Organic Supercapacitors.
- 1School of Metallurgy and Materials Engineering, Liaoning Institute of Science and Technology, Benxi 117004, China.
Abstract
Organic supercapacitors (OSCs) suffer from sluggish Li⁺ desolvation and ion diffusion kinetics, limiting their electrochemical performance and practical application. Heteroatom doping is a valid strategy to improve the capacitive properties of carbon electrode materials. Herein, density functional theory (DFT) first-principles calculations were adopted to systematically investigate and compare the effects of equal-concentration N and P doping on the Li⁺ desolvation behavior, capacitance performance, and ion diffusion kinetics of single-walled carbon nanotubes (SWCNTs) in acetonitrile-based electrolytes. The results show that N doping maintains the [Li(AN)]⁺ critical desolvation size (5.91 Å) of pristine SWCNTs, while P doping increases this size to 6.11 Å. Benefiting from the optimized desolvation behavior, P-doped SWCNTs achieve a maximum relative capacitance 1.9 times that of pristine SWCNTs, outperforming N-doped SWCNTs (1.3 times). Moreover, P doping significantly reduces the [Li(AN)]⁺ diffusion barrier to 0.99 eV, much lower than that of pristine and N-doped SWCNTs, thereby accelerating ion migration. Electronic structure analysis confirms that heteroatom doping weakens electron localization and C-heteroatom covalent bonding, and the weaker P-C bonding further accounts for the superior performance of P-doped SWCNTs. This study clarifies the intrinsic regulatory mechanism of N/P doping on Li⁺ desolvation and electrochemical performance of SWCNTs, providing a theoretical guideline for the design of high-performance carbon-based electrodes for OSCs.
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BibTeX
@article{si2026study,
title = {{Study on the Li⁺ Desolvation Mechanism of Doped Carbon Nanotubes and Their Regulatory Effect on the Performance of Organic Supercapacitors.}},
author = {Yuwei Si and Fudong Liu and Bo Yang and Shuai Yu and Yinping Chen and Beiqi Zhang},
journal = {Materials (Basel, Switzerland)},
year = {2026},
month = sep,
doi = {10.3390/ma19194090},
url = {https://europepmc.org/article/MED/42882589},
note = {CC BY},
}
RIS
TY - JOUR
TI - Study on the Li⁺ Desolvation Mechanism of Doped Carbon Nanotubes and Their Regulatory Effect on the Performance of Organic Supercapacitors.
AU - Yuwei Si
AU - Fudong Liu
AU - Bo Yang
AU - Shuai Yu
AU - Yinping Chen
AU - Beiqi Zhang
PY - 2026
DA - 2026/09/24
JO - Materials (Basel, Switzerland)
DO - 10.3390/ma19194090
UR - https://europepmc.org/article/MED/42882589
AB - Organic supercapacitors (OSCs) suffer from sluggish Li⁺ desolvation and ion diffusion kinetics, limiting their electrochemical performance and practical application. Heteroatom doping is a valid strategy to improve the capacitive properties of carbon electrode materials. Herein, density functional theory (DFT) first-principles calculations were adopted to systematically investigate and compare the effects of equal-concentration N and P doping on the Li⁺ desolvation behavior, capacitance performance, and ion diffusion kinetics of single-walled carbon nanotubes (SWCNTs) in acetonitrile-based electrolytes. The results show that N doping maintains the [Li(AN)]⁺ critical desolvation size (5.91 Å) of pristine SWCNTs, while P doping increases this size to 6.11 Å. Benefiting from the optimized desolvation behavior, P-doped SWCNTs achieve a maximum relative capacitance 1.9 times that of pristine SWCNTs, outperforming N-doped SWCNTs (1.3 times). Moreover, P doping significantly reduces the [Li(AN)]⁺ diffusion barrier to 0.99 eV, much lower than that of pristine and N-doped SWCNTs, thereby accelerating ion migration. Electronic structure analysis confirms that heteroatom doping weakens electron localization and C-heteroatom covalent bonding, and the weaker P-C bonding further accounts for the superior performance of P-doped SWCNTs. This study clarifies the intrinsic regulatory mechanism of N/P doping on Li⁺ desolvation and electrochemical performance of SWCNTs, providing a theoretical guideline for the design of high-performance carbon-based electrodes for OSCs.
SN - 1996-1944
ER -