Sulfur-containing activated carbons with greatly reduced content of bottle neck pores for double-layer capacitors: a case study for pseudocapacitance detection

[EN] Synthesis of S-doped activated carbons (ACs) by carbonization and simultaneous activation of S-based polymers was found to be an efficient route to produce porous carbons for double layer capacitors (EDLCs) with high specific energy and power densities combined with low self-discharge. Here we investigate for the first time the processing-structure–property relationships related to the formation of polythiophene-derived ACs for EDLC applications. Sulfide bridges present in the polymer precursor were found to depress the shrinkage of the smallest micropores during the carbonization process and allow for the enhanced ion transport within the produced AC electrodes. The cyclic voltammetry (CV) measurements on S-doped ACs produced at 800 and 850 °C showed high specific capacitance (up to [similar]200 F g−1) and no significant self-discharge in neutral aqueous electrolytes. More importantly, these capacitance values remained virtually identical for a sweep rate increasing from 1 to 50 mV s−1. The observed capacitance retention is quite remarkable for thick electrodes of [similar]200 μm and a large AC particle size of 10–100 μm. It indicates great potential of the proposed synthesis technology for EDLCs operating at high frequencies and high currents. In the course of our systematic studies of AC performance in different electrolytes we found a strong correlation between the large pseudocapacitance and the significant self-discharge in ACs. We harness the difference between the characteristic times required to establish a double layer and that of the pseudocapacitive redox reactions and propose a simple method to estimate the fraction of pseudocapacitance. The proposed method is particularly valuable in cases when CV measurements do not show clear characteristic reduction–oxidation peaks.

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Main Authors: Gu, Wentian, Sevilla Solís, Marta, Magasinski, Alexandre, Fuertes Arias, Antonio Benito, Yushin, Gleb
Format: artículo biblioteca
Language:English
Published: Royal Society of Chemistry (UK) 2013-05-16
Subjects:Supercapacitor, Microporous, Mesoporous, Carbon, Graphene, Nanotubes, Doping, Leakage,
Online Access:http://hdl.handle.net/10261/91747
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spelling dig-incar-es-10261-917472018-11-15T11:03:27Z Sulfur-containing activated carbons with greatly reduced content of bottle neck pores for double-layer capacitors: a case study for pseudocapacitance detection Gu, Wentian Sevilla Solís, Marta Magasinski, Alexandre Fuertes Arias, Antonio Benito Yushin, Gleb Supercapacitor Microporous Mesoporous Carbon Graphene Nanotubes Doping Leakage [EN] Synthesis of S-doped activated carbons (ACs) by carbonization and simultaneous activation of S-based polymers was found to be an efficient route to produce porous carbons for double layer capacitors (EDLCs) with high specific energy and power densities combined with low self-discharge. Here we investigate for the first time the processing-structure–property relationships related to the formation of polythiophene-derived ACs for EDLC applications. Sulfide bridges present in the polymer precursor were found to depress the shrinkage of the smallest micropores during the carbonization process and allow for the enhanced ion transport within the produced AC electrodes. The cyclic voltammetry (CV) measurements on S-doped ACs produced at 800 and 850 °C showed high specific capacitance (up to [similar]200 F g−1) and no significant self-discharge in neutral aqueous electrolytes. More importantly, these capacitance values remained virtually identical for a sweep rate increasing from 1 to 50 mV s−1. The observed capacitance retention is quite remarkable for thick electrodes of [similar]200 μm and a large AC particle size of 10–100 μm. It indicates great potential of the proposed synthesis technology for EDLCs operating at high frequencies and high currents. In the course of our systematic studies of AC performance in different electrolytes we found a strong correlation between the large pseudocapacitance and the significant self-discharge in ACs. We harness the difference between the characteristic times required to establish a double layer and that of the pseudocapacitive redox reactions and propose a simple method to estimate the fraction of pseudocapacitance. The proposed method is particularly valuable in cases when CV measurements do not show clear characteristic reduction–oxidation peaks. The financial support for this research work provided by the US Army Research Office (grant W911NF-12-1-0259), by the Spanish MINECO (CQT2011-24776 and MAT2012-31651) and by the Energy Efficiency & Resources program of the Korea Institute of Energy Technology Evaluation and Planning (KETEP) funded by the Korea government Ministry of Knowledge Economy (grant 20118510010030) is gratefully acknowledged. M. S. thanks the Spanish MINECO for the award of a Ramón y Cajal contract. Peer reviewed 2014-02-13T12:46:26Z 2014-02-13T12:46:26Z 2013-05-16 artículo http://purl.org/coar/resource_type/c_6501 Energy and Environmental Science 6: 2465-2476 (2013) 1754-5692 http://hdl.handle.net/10261/91747 10.1039/C3EE41182F 1754-5706 en http://dx.doi.org/10.1039/C3EE41182F open Royal Society of Chemistry (UK)
institution INCAR ES
collection DSpace
country España
countrycode ES
component Bibliográfico
access En linea
databasecode dig-incar-es
tag biblioteca
region Europa del Sur
libraryname Biblioteca del INCAR España
language English
topic Supercapacitor
Microporous
Mesoporous
Carbon
Graphene
Nanotubes
Doping
Leakage
Supercapacitor
Microporous
Mesoporous
Carbon
Graphene
Nanotubes
Doping
Leakage
spellingShingle Supercapacitor
Microporous
Mesoporous
Carbon
Graphene
Nanotubes
Doping
Leakage
Supercapacitor
Microporous
Mesoporous
Carbon
Graphene
Nanotubes
Doping
Leakage
Gu, Wentian
Sevilla Solís, Marta
Magasinski, Alexandre
Fuertes Arias, Antonio Benito
Yushin, Gleb
Sulfur-containing activated carbons with greatly reduced content of bottle neck pores for double-layer capacitors: a case study for pseudocapacitance detection
description [EN] Synthesis of S-doped activated carbons (ACs) by carbonization and simultaneous activation of S-based polymers was found to be an efficient route to produce porous carbons for double layer capacitors (EDLCs) with high specific energy and power densities combined with low self-discharge. Here we investigate for the first time the processing-structure–property relationships related to the formation of polythiophene-derived ACs for EDLC applications. Sulfide bridges present in the polymer precursor were found to depress the shrinkage of the smallest micropores during the carbonization process and allow for the enhanced ion transport within the produced AC electrodes. The cyclic voltammetry (CV) measurements on S-doped ACs produced at 800 and 850 °C showed high specific capacitance (up to [similar]200 F g−1) and no significant self-discharge in neutral aqueous electrolytes. More importantly, these capacitance values remained virtually identical for a sweep rate increasing from 1 to 50 mV s−1. The observed capacitance retention is quite remarkable for thick electrodes of [similar]200 μm and a large AC particle size of 10–100 μm. It indicates great potential of the proposed synthesis technology for EDLCs operating at high frequencies and high currents. In the course of our systematic studies of AC performance in different electrolytes we found a strong correlation between the large pseudocapacitance and the significant self-discharge in ACs. We harness the difference between the characteristic times required to establish a double layer and that of the pseudocapacitive redox reactions and propose a simple method to estimate the fraction of pseudocapacitance. The proposed method is particularly valuable in cases when CV measurements do not show clear characteristic reduction–oxidation peaks.
format artículo
topic_facet Supercapacitor
Microporous
Mesoporous
Carbon
Graphene
Nanotubes
Doping
Leakage
author Gu, Wentian
Sevilla Solís, Marta
Magasinski, Alexandre
Fuertes Arias, Antonio Benito
Yushin, Gleb
author_facet Gu, Wentian
Sevilla Solís, Marta
Magasinski, Alexandre
Fuertes Arias, Antonio Benito
Yushin, Gleb
author_sort Gu, Wentian
title Sulfur-containing activated carbons with greatly reduced content of bottle neck pores for double-layer capacitors: a case study for pseudocapacitance detection
title_short Sulfur-containing activated carbons with greatly reduced content of bottle neck pores for double-layer capacitors: a case study for pseudocapacitance detection
title_full Sulfur-containing activated carbons with greatly reduced content of bottle neck pores for double-layer capacitors: a case study for pseudocapacitance detection
title_fullStr Sulfur-containing activated carbons with greatly reduced content of bottle neck pores for double-layer capacitors: a case study for pseudocapacitance detection
title_full_unstemmed Sulfur-containing activated carbons with greatly reduced content of bottle neck pores for double-layer capacitors: a case study for pseudocapacitance detection
title_sort sulfur-containing activated carbons with greatly reduced content of bottle neck pores for double-layer capacitors: a case study for pseudocapacitance detection
publisher Royal Society of Chemistry (UK)
publishDate 2013-05-16
url http://hdl.handle.net/10261/91747
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