New Insights into the Structure of Nanoporous Carbons from NMR, Raman, and Pair Distribution Function Analysis

Forse, Alexander C.; Merlet, Céline; Allan, Phoebe K.; Humphreys, Elizabeth K.; Griffin, John M.; Aslan, Mesut; Zeiger, Marco; Presser, Volker; Gogotsi, Yury; Grey, Clare P.

doi:10.1021/acs.chemmater.5b03216

Title: New Insights into the Structure of Nanoporous Carbons from NMR, Raman, and Pair Distribution Function Analysis

Journal Article · Fri Sep 25 00:00:00 EDT 2015 · Chemistry of Materials

DOI:https://doi.org/10.1021/acs.chemmater.5b03216· OSTI ID:1241048

Forse, Alexander C. ^[1]; Merlet, Céline ^[1]; Allan, Phoebe K. ^[2]; Humphreys, Elizabeth K. ^[1]; Griffin, John M. ^[1]; Aslan, Mesut ^[3]; Zeiger, Marco ^[4]; Presser, Volker ^[4]; Gogotsi, Yury ^[5]; Grey, Clare P. ^[6]

Univ. of Cambridge (United Kingdom)
Univ. of Cambridge (United Kingdom); Gonville and Caius College, Cambridge (United Kingdom)
INM-Leibniz-Inst. for New Materials, Saarbrücken (Germany)
INM-Leibniz-Inst. for New Materials, Saarbrücken (Germany); Saarland Univ., Saarbrücken (Germany)
Drexel Univ., Philadelphia, PA (United States)
Univ. of Cambridge (United Kingdom); Stony Brook Univ., NY (United States)

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. In this paper, 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 for 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.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); Engineering and Physical Sciences Research Council (EPSRC); European Research Council (ERC); NanoDTC Cambridge; Federal Ministry of Education and Research (BMBF)

Grant/Contract Number:: 03EK3013; AC02-06CH11357

OSTI ID:: 1241048

Journal Information:: Chemistry of Materials, Vol. 27, Issue 19; ISSN 0897-4756

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: ENGLISH

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Cited by: 75 works

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Title: New Insights into the Structure of Nanoporous Carbons from NMR, Raman, and Pair Distribution Function Analysis

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