Rights statement: This document is the Accepted Manuscript version of a Published Work that appeared in final form in Chemistry of Materials, copyright © 2015 American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see http://pubs.acs.org/doi/10.1021/acs.chemmater.5b03216
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Final published version
Research output: Contribution to Journal/Magazine › Journal article › peer-review
Research output: Contribution to Journal/Magazine › Journal article › peer-review
}
TY - JOUR
T1 - New insights into the structure of nanoporous carbons from NMR, Raman, and pair distribution function analysis
AU - Forse, Alexander C.
AU - Merlet, Celine
AU - Allan, Phoebe K.
AU - Humphreys, Elizabeth K.
AU - Griffin, John M.
AU - Aslan, Mesut
AU - Zeiger, Marco
AU - Presser, Volker
AU - Gogotsi, Yury
AU - Grey, Clare P.
N1 - This document is the Accepted Manuscript version of a Published Work that appeared in final form in Chemistry of Materials, copyright © 2015 American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see http://pubs.acs.org/doi/10.1021/acs.chemmater.5b03216
PY - 2015/10/13
Y1 - 2015/10/13
N2 - The structural characterization of nanoporous carbons is a challenging task as they generally lack long-range order and can exhibit diverse local structures. Such characterization represents an important step toward understanding and improving the properties and functionality of porous carbons, yet few experimental techniques have been developed for this purpose. Here we demonstrate the application of nuclear magnetic resonance (NMR) spectroscopy and pair distribution function (PDF) analysis as new tools to probe the local structures of porous carbons, alongside more conventional Raman spectroscopy. Together, the PDFs and the Raman spectra allow the local chemical bonding to be probed, with the bonding becoming more ordered for carbide-derived carbons (CDCs) synthesized at higher temperatures. The ring currents induced in the NMR experiment (and thus the observed NMR chemical shifts adsorbed species) are strongly dependent on the size of the aromatic carbon domains. We exploit this property and use computer simulations to show that the carbon domain size increases with the temperature used in the carbon synthesis. The techniques developed here are applicable to a wide range of porous carbons and offer new insights into the structures of CDCs (conventional and vacuum-annealed) and coconut shell-derived activated carbons.
AB - The structural characterization of nanoporous carbons is a challenging task as they generally lack long-range order and can exhibit diverse local structures. Such characterization represents an important step toward understanding and improving the properties and functionality of porous carbons, yet few experimental techniques have been developed for this purpose. Here we demonstrate the application of nuclear magnetic resonance (NMR) spectroscopy and pair distribution function (PDF) analysis as new tools to probe the local structures of porous carbons, alongside more conventional Raman spectroscopy. Together, the PDFs and the Raman spectra allow the local chemical bonding to be probed, with the bonding becoming more ordered for carbide-derived carbons (CDCs) synthesized at higher temperatures. The ring currents induced in the NMR experiment (and thus the observed NMR chemical shifts adsorbed species) are strongly dependent on the size of the aromatic carbon domains. We exploit this property and use computer simulations to show that the carbon domain size increases with the temperature used in the carbon synthesis. The techniques developed here are applicable to a wide range of porous carbons and offer new insights into the structures of CDCs (conventional and vacuum-annealed) and coconut shell-derived activated carbons.
KW - DOUBLE-LAYER CAPACITORS
KW - CARBIDE-DERIVED CARBONS
KW - ELECTRICAL DOUBLE-LAYER
KW - IN-SITU NMR
KW - INDEPENDENT CHEMICAL-SHIFT
KW - CHARGE STORAGE MECHANISM
KW - MICROPOROUS CARBONS
KW - MAGNETIC-RESONANCE
KW - SIZE DISTRIBUTION
KW - AMORPHOUS-CARBON
U2 - 10.1021/acs.chemmater.5b03216
DO - 10.1021/acs.chemmater.5b03216
M3 - Journal article
VL - 27
SP - 6848
EP - 6857
JO - Chemistry of Materials
JF - Chemistry of Materials
SN - 0897-4756
IS - 19
ER -