{"title":"宽温度范围下高性能碳纳米管超级电容器:电解离子扩散的几何效应。","authors":"Yunkuo Sun, , , Baohong Ding*, , , Yonghua Jiao, , and , Wei Sun*, ","doi":"10.1021/acs.langmuir.5c02191","DOIUrl":null,"url":null,"abstract":"<p >Supercapacitors (SCs) characterized by excellent charge and discharge rates, high power density, and stable cycling performance, exhibit crucial applications in various fields, while it faces significant performance degradation at low temperature. Herein, we systematically investigate the electrochemical performances of carbon nanotube (CNT)-based SCs over a temperature range of −18 to 60 °C and establish quantitative relationships between CNT geometry and temperature-dependent electrochemical kinetics in symmetric SCs. The results and analysis supported by electrochemical impedance spectroscopy (EIS) with Warburg diffusion analysis, Arrhenius modeling of ion diffusion kinetics, and multiterm self-discharge modeling reveal exceptional low-temperature resilience where CNT-based SCs retain >85% peak specific capacitance (75.76 F/g at 0.5 A/g) with 87% rate retention at 20 A/g (−18 °C), attributable to minimized diffusion barriers in CNTs with shorter length and wider channel that reduce Arrhenius activation energy by 33% (CNT-8-L: <i>Q</i> = 15.40 kJ/mol vs CNT-3-L: 23.07 kJ/mol). In addition, a symmetric CNT-based SC is successfully employed to power a digital thermometer. The self-discharge compensation effect enables optimized energy deliver of the CNT-based SC for over 40 min to the digital thermometer at −18 °C (approximately 4 times longer than at 60 °C) through suppression of current leakage as well as ion diffusion, although the specific capacitance is lower. The experimental findings and analyses contribute to the design and optimization of CNT geometries for low-temperature applications and deepen our understanding of the underlying energy storage mechanisms.</p>","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"41 38","pages":"25903–25918"},"PeriodicalIF":3.9000,"publicationDate":"2025-09-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"High-Performance Carbon-Nanotube-Based Supercapacitors at a Wide Temperature Range: Geometrical Effect on Diffusion of Electrolytic Ions\",\"authors\":\"Yunkuo Sun, , , Baohong Ding*, , , Yonghua Jiao, , and , Wei Sun*, \",\"doi\":\"10.1021/acs.langmuir.5c02191\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >Supercapacitors (SCs) characterized by excellent charge and discharge rates, high power density, and stable cycling performance, exhibit crucial applications in various fields, while it faces significant performance degradation at low temperature. Herein, we systematically investigate the electrochemical performances of carbon nanotube (CNT)-based SCs over a temperature range of −18 to 60 °C and establish quantitative relationships between CNT geometry and temperature-dependent electrochemical kinetics in symmetric SCs. The results and analysis supported by electrochemical impedance spectroscopy (EIS) with Warburg diffusion analysis, Arrhenius modeling of ion diffusion kinetics, and multiterm self-discharge modeling reveal exceptional low-temperature resilience where CNT-based SCs retain >85% peak specific capacitance (75.76 F/g at 0.5 A/g) with 87% rate retention at 20 A/g (−18 °C), attributable to minimized diffusion barriers in CNTs with shorter length and wider channel that reduce Arrhenius activation energy by 33% (CNT-8-L: <i>Q</i> = 15.40 kJ/mol vs CNT-3-L: 23.07 kJ/mol). In addition, a symmetric CNT-based SC is successfully employed to power a digital thermometer. The self-discharge compensation effect enables optimized energy deliver of the CNT-based SC for over 40 min to the digital thermometer at −18 °C (approximately 4 times longer than at 60 °C) through suppression of current leakage as well as ion diffusion, although the specific capacitance is lower. The experimental findings and analyses contribute to the design and optimization of CNT geometries for low-temperature applications and deepen our understanding of the underlying energy storage mechanisms.</p>\",\"PeriodicalId\":50,\"journal\":{\"name\":\"Langmuir\",\"volume\":\"41 38\",\"pages\":\"25903–25918\"},\"PeriodicalIF\":3.9000,\"publicationDate\":\"2025-09-18\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Langmuir\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://pubs.acs.org/doi/10.1021/acs.langmuir.5c02191\",\"RegionNum\":2,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Langmuir","FirstCategoryId":"92","ListUrlMain":"https://pubs.acs.org/doi/10.1021/acs.langmuir.5c02191","RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
High-Performance Carbon-Nanotube-Based Supercapacitors at a Wide Temperature Range: Geometrical Effect on Diffusion of Electrolytic Ions
Supercapacitors (SCs) characterized by excellent charge and discharge rates, high power density, and stable cycling performance, exhibit crucial applications in various fields, while it faces significant performance degradation at low temperature. Herein, we systematically investigate the electrochemical performances of carbon nanotube (CNT)-based SCs over a temperature range of −18 to 60 °C and establish quantitative relationships between CNT geometry and temperature-dependent electrochemical kinetics in symmetric SCs. The results and analysis supported by electrochemical impedance spectroscopy (EIS) with Warburg diffusion analysis, Arrhenius modeling of ion diffusion kinetics, and multiterm self-discharge modeling reveal exceptional low-temperature resilience where CNT-based SCs retain >85% peak specific capacitance (75.76 F/g at 0.5 A/g) with 87% rate retention at 20 A/g (−18 °C), attributable to minimized diffusion barriers in CNTs with shorter length and wider channel that reduce Arrhenius activation energy by 33% (CNT-8-L: Q = 15.40 kJ/mol vs CNT-3-L: 23.07 kJ/mol). In addition, a symmetric CNT-based SC is successfully employed to power a digital thermometer. The self-discharge compensation effect enables optimized energy deliver of the CNT-based SC for over 40 min to the digital thermometer at −18 °C (approximately 4 times longer than at 60 °C) through suppression of current leakage as well as ion diffusion, although the specific capacitance is lower. The experimental findings and analyses contribute to the design and optimization of CNT geometries for low-temperature applications and deepen our understanding of the underlying energy storage mechanisms.
期刊介绍:
Langmuir is an interdisciplinary journal publishing articles in the following subject categories:
Colloids: surfactants and self-assembly, dispersions, emulsions, foams
Interfaces: adsorption, reactions, films, forces
Biological Interfaces: biocolloids, biomolecular and biomimetic materials
Materials: nano- and mesostructured materials, polymers, gels, liquid crystals
Electrochemistry: interfacial charge transfer, charge transport, electrocatalysis, electrokinetic phenomena, bioelectrochemistry
Devices and Applications: sensors, fluidics, patterning, catalysis, photonic crystals
However, when high-impact, original work is submitted that does not fit within the above categories, decisions to accept or decline such papers will be based on one criteria: What Would Irving Do?
Langmuir ranks #2 in citations out of 136 journals in the category of Physical Chemistry with 113,157 total citations. The journal received an Impact Factor of 4.384*.
This journal is also indexed in the categories of Materials Science (ranked #1) and Multidisciplinary Chemistry (ranked #5).