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In situ NMR and electrochemical quartz crystal microbalance techniques reveal the structure of the electrical double layer in supercapacitors

Research output: Contribution to Journal/Magazine › Journal article › peer-review

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In situ NMR and electrochemical quartz crystal microbalance techniques reveal the structure of the electrical double layer in supercapacitors. / Griffin, John M.; Forse, Alexander C.; Tsai, Wan-Yu et al.
In: Nature Materials, Vol. 14, No. 8, 08.2015, p. 812-819.

Research output: Contribution to Journal/Magazine › Journal article › peer-review

Harvard

Griffin, JM, Forse, AC, Tsai, W-Y, Taberna, P-L, Simon, P & Grey, CP 2015, 'In situ NMR and electrochemical quartz crystal microbalance techniques reveal the structure of the electrical double layer in supercapacitors', Nature Materials, vol. 14, no. 8, pp. 812-819. https://doi.org/10.1038/NMAT4318

APA

Griffin, J. M., Forse, A. C., Tsai, W-Y., Taberna, P-L., Simon, P., & Grey, C. P. (2015). In situ NMR and electrochemical quartz crystal microbalance techniques reveal the structure of the electrical double layer in supercapacitors. Nature Materials, 14(8), 812-819. https://doi.org/10.1038/NMAT4318

Vancouver

Griffin JM, Forse AC, Tsai W-Y, Taberna P-L, Simon P, Grey CP. In situ NMR and electrochemical quartz crystal microbalance techniques reveal the structure of the electrical double layer in supercapacitors. Nature Materials. 2015 Aug;14(8):812-819. doi: 10.1038/NMAT4318

Author

Griffin, John M. ; Forse, Alexander C. ; Tsai, Wan-Yu et al. / In situ NMR and electrochemical quartz crystal microbalance techniques reveal the structure of the electrical double layer in supercapacitors. In: Nature Materials. 2015 ; Vol. 14, No. 8. pp. 812-819.

Bibtex

@article{3268ec9ec79a4405a161eb1774bced31,
title = "In situ NMR and electrochemical quartz crystal microbalance techniques reveal the structure of the electrical double layer in supercapacitors",
abstract = "Supercapacitors store charge through the electrosorption of ions on microporous electrodes. Despite major efforts to understand this phenomenon, a molecular-level picture of the electrical double layer in working devices is still lacking as few techniques can selectively observe the ionic species at the electrode/electrolyte interface. Here, we use in situ NMR to directly quantify the populations of anionic and cationic species within a working microporous carbon supercapacitor electrode. Our results show that charge storage mechanisms are different for positively and negatively polarized electrodes for the electrolyte tetraethylphosphonium tetrafluoroborate in acetonitrile; for positive polarization charging proceeds by exchange of the cations for anions, whereas for negative polarization, cation adsorption dominates. In situ electrochemical quartz crystal microbalance measurements support the NMR results and indicate that adsorbed ions are only partially solvated. These results provide new molecular-level insight, with the methodology offering exciting possibilities for the study of pore/ion size, desolvation and other effects on charge storage in supercapacitors.",
keywords = "SOLID-STATE NMR, CARBON ELECTRODES, MAGNETIC-RESONANCE, SUBNANOMETER PORES, ENERGY-STORAGE, IONIC LIQUIDS, CAPACITANCE, DYNAMICS, MOLECULES, SPECTROSCOPY",
author = "Griffin, {John M.} and Forse, {Alexander C.} and Wan-Yu Tsai and Pierre-Louis Taberna and Patrice Simon and Grey, {Clare P.}",
year = "2015",
month = aug,
doi = "10.1038/NMAT4318",
language = "English",
volume = "14",
pages = "812--819",
journal = "Nature Materials",
issn = "1476-1122",
publisher = "Nature Publishing Group",
number = "8",

}

RIS

TY - JOUR

T1 - In situ NMR and electrochemical quartz crystal microbalance techniques reveal the structure of the electrical double layer in supercapacitors

AU - Griffin, John M.

AU - Forse, Alexander C.

AU - Tsai, Wan-Yu

AU - Taberna, Pierre-Louis

AU - Simon, Patrice

AU - Grey, Clare P.

PY - 2015/8

Y1 - 2015/8

N2 - Supercapacitors store charge through the electrosorption of ions on microporous electrodes. Despite major efforts to understand this phenomenon, a molecular-level picture of the electrical double layer in working devices is still lacking as few techniques can selectively observe the ionic species at the electrode/electrolyte interface. Here, we use in situ NMR to directly quantify the populations of anionic and cationic species within a working microporous carbon supercapacitor electrode. Our results show that charge storage mechanisms are different for positively and negatively polarized electrodes for the electrolyte tetraethylphosphonium tetrafluoroborate in acetonitrile; for positive polarization charging proceeds by exchange of the cations for anions, whereas for negative polarization, cation adsorption dominates. In situ electrochemical quartz crystal microbalance measurements support the NMR results and indicate that adsorbed ions are only partially solvated. These results provide new molecular-level insight, with the methodology offering exciting possibilities for the study of pore/ion size, desolvation and other effects on charge storage in supercapacitors.

AB - Supercapacitors store charge through the electrosorption of ions on microporous electrodes. Despite major efforts to understand this phenomenon, a molecular-level picture of the electrical double layer in working devices is still lacking as few techniques can selectively observe the ionic species at the electrode/electrolyte interface. Here, we use in situ NMR to directly quantify the populations of anionic and cationic species within a working microporous carbon supercapacitor electrode. Our results show that charge storage mechanisms are different for positively and negatively polarized electrodes for the electrolyte tetraethylphosphonium tetrafluoroborate in acetonitrile; for positive polarization charging proceeds by exchange of the cations for anions, whereas for negative polarization, cation adsorption dominates. In situ electrochemical quartz crystal microbalance measurements support the NMR results and indicate that adsorbed ions are only partially solvated. These results provide new molecular-level insight, with the methodology offering exciting possibilities for the study of pore/ion size, desolvation and other effects on charge storage in supercapacitors.

KW - SOLID-STATE NMR

KW - CARBON ELECTRODES

KW - MAGNETIC-RESONANCE

KW - SUBNANOMETER PORES

KW - ENERGY-STORAGE

KW - IONIC LIQUIDS

KW - CAPACITANCE

KW - DYNAMICS

KW - MOLECULES

KW - SPECTROSCOPY

U2 - 10.1038/NMAT4318

DO - 10.1038/NMAT4318

M3 - Journal article

VL - 14

SP - 812

EP - 819

JO - Nature Materials

JF - Nature Materials

SN - 1476-1122

IS - 8

ER -