Colossal C130 Fullertubes: Soluble [5,5] C130-D5h(1) Pristine Molecules with 70 Nanotube Carbons and Two 30-Atom Hemifullerene End-caps

Emmanuel Bourret; Xiaoyang Liu; Cora A. Noble; Kevin Cover; Tanisha P. Davidson; Rong Huang; Ryan M. Koenig; K. Shawn Reeves; Ivan V. Vlassiouk; Michel Côté; Jefferey S. Baxter; Andrew R. Lupini; David B. Geohegan; Harry C. Dorn; Steven Stevenson

doi:10.1021/jacs.3c09082

Colossal C₁₃₀ Fullertubes: Soluble [5,5] C₁₃₀-D_5h(1) Pristine Molecules with 70 Nanotube Carbons and Two 30-Atom Hemifullerene End-caps

Emmanuel Bourret, Xiaoyang Liu, Cora A. Noble, Kevin Cover, Tanisha P. Davidson, Rong Huang, Ryan M. Koenig, K. Shawn Reeves, Ivan V. Vlassiouk, Michel Côté, Jefferey S. Baxter, Andrew R. Lupini, David B. Geohegan, Harry C. Dorn, Steven Stevenson

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Abstract

We report the seminal experimental isolation and DFT characterization of pristine [5,5] C₁₃₀-D_5h(1) fullertubes. This achievement represents the largest soluble carbon molecule obtained in its pristine form. The [5,5] C₁₃₀ species is the highest aspect ratio fullertube purified to date and now surpasses the recent gigantic [5,5] C₁₂₀-D_5d(1). In contrast to C₉₀, C₁₀₀, and C₁₂₀ fullertubes, the longer C₁₃₀-D_5h has more nanotubular carbons (70) than end-cap fullerenyl atoms (60). Starting from 39,393 possible C₁₃₀ isolated pentagon rule (IPR) structures and after analyzing polarizability, retention time, and UV-vis spectra, these three layers of data remarkably predict a single candidate isomer and fullertube, [5,5] C₁₃₀-D_5h(1). This structural assignment is augmented by atomic resolution STEM data showing distinctive and tubular “pill-like” structures with diameters and aspect ratios consistent with [5,5] C₁₃₀-D_5h(1) fullertubes. The high selectivity of the aminopropanol reaction with spheroidal fullerenes permits facile separation and removal of fullertubes from soot extracts. Experimental analyses (HPLC retention time, UV-vis, and STEM) were synergistically used (with polarizability and DFT property calculations) to down select and confirm the C₁₃₀ fullertube structure. Achieving the isolation of a new [5,5] C₁₃₀-D_5h fullertube opens the door to application development and fundamental studies of electron confinement, fluorescence, and metallic character for a fullertube series of molecules with systematic tubular elongation. This [5,5] fullertube family also invites comparative studies with single-walled carbon nanotubes (SWCNTs), nanohorns (SWCNHs), and fullerenes.

Original language	English
Pages (from-to)	25942-25947
Number of pages	6
Journal	Journal of the American Chemical Society
Volume	145
Issue number	48
DOIs	https://doi.org/10.1021/jacs.3c09082
State	Published - Dec 6 2023

Funding

S.S. thanks the Chemistry Division of the National Science Foundation for grants RUI CHE-1856461 and CHE-2247272. H.C.D. thanks Heather Claire Dorn for assistance with Supporting Information figures. Advanced Research Computing at Virginia Tech is gratefully acknowledged for the computational work. Electron microscopy and graphene synthesis and processing conducted as part of a user project at the Center for Nanophase Materials Sciences (CNMS), which is a US Department of Energy, Office of Science User Facility at Oak Ridge National Laboratory and partially supported by the U.S. Department of Energy (DOE), Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division. This research was financially supported by the Natural Sciences and Engineering Research Council of Canada (NSERC), under the Discovery Grants program Grant No. RGPIN-2016-06666. This research was enabled in part by support provided by Calcul Québec and the Digital Research Alliance of Canada. The operation of the supercomputers used for this research is funded by the Canada Foundation for Innovation (CFI), the Ministère de la Science, de l’Économie et de l’Innovation du Québec (MESI), and the Fonds de recherche du Québec – Nature et technologies (FRQ-NT). E.B. and M.C. are members of the Regroupement québécois sur les matériaux de pointe (RQMP).

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Bourret, E., Liu, X., Noble, C. A., Cover, K., Davidson, T. P., Huang, R., Koenig, R. M., Reeves, K. S., Vlassiouk, I. V., Côté, M., Baxter, J. S., Lupini, A. R., Geohegan, D. B., Dorn, H. C., & Stevenson, S. (2023). Colossal C₁₃₀ Fullertubes: Soluble [5,5] C₁₃₀-D_5h(1) Pristine Molecules with 70 Nanotube Carbons and Two 30-Atom Hemifullerene End-caps. Journal of the American Chemical Society, 145(48), 25942-25947. https://doi.org/10.1021/jacs.3c09082

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title = "Colossal C130 Fullertubes: Soluble [5,5] C130-D5h(1) Pristine Molecules with 70 Nanotube Carbons and Two 30-Atom Hemifullerene End-caps",

abstract = "We report the seminal experimental isolation and DFT characterization of pristine [5,5] C130-D5h(1) fullertubes. This achievement represents the largest soluble carbon molecule obtained in its pristine form. The [5,5] C130 species is the highest aspect ratio fullertube purified to date and now surpasses the recent gigantic [5,5] C120-D5d(1). In contrast to C90, C100, and C120 fullertubes, the longer C130-D5h has more nanotubular carbons (70) than end-cap fullerenyl atoms (60). Starting from 39,393 possible C130 isolated pentagon rule (IPR) structures and after analyzing polarizability, retention time, and UV-vis spectra, these three layers of data remarkably predict a single candidate isomer and fullertube, [5,5] C130-D5h(1). This structural assignment is augmented by atomic resolution STEM data showing distinctive and tubular “pill-like” structures with diameters and aspect ratios consistent with [5,5] C130-D5h(1) fullertubes. The high selectivity of the aminopropanol reaction with spheroidal fullerenes permits facile separation and removal of fullertubes from soot extracts. Experimental analyses (HPLC retention time, UV-vis, and STEM) were synergistically used (with polarizability and DFT property calculations) to down select and confirm the C130 fullertube structure. Achieving the isolation of a new [5,5] C130-D5h fullertube opens the door to application development and fundamental studies of electron confinement, fluorescence, and metallic character for a fullertube series of molecules with systematic tubular elongation. This [5,5] fullertube family also invites comparative studies with single-walled carbon nanotubes (SWCNTs), nanohorns (SWCNHs), and fullerenes.",

author = "Emmanuel Bourret and Xiaoyang Liu and Noble, {Cora A.} and Kevin Cover and Davidson, {Tanisha P.} and Rong Huang and Koenig, {Ryan M.} and Reeves, {K. Shawn} and Vlassiouk, {Ivan V.} and Michel C{\^o}t{\'e} and Baxter, {Jefferey S.} and Lupini, {Andrew R.} and Geohegan, {David B.} and Dorn, {Harry C.} and Steven Stevenson",

note = "Publisher Copyright: {\textcopyright} 2023 American Chemical Society.",

year = "2023",

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doi = "10.1021/jacs.3c09082",

language = "English",

volume = "145",

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journal = "Journal of the American Chemical Society",

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Bourret, E, Liu, X, Noble, CA, Cover, K, Davidson, TP, Huang, R, Koenig, RM, Reeves, KS, Vlassiouk, IV, Côté, M, Baxter, JS , Lupini, AR, Geohegan, DB, Dorn, HC & Stevenson, S 2023, 'Colossal C₁₃₀ Fullertubes: Soluble [5,5] C₁₃₀-D_5h(1) Pristine Molecules with 70 Nanotube Carbons and Two 30-Atom Hemifullerene End-caps', Journal of the American Chemical Society, vol. 145, no. 48, pp. 25942-25947. https://doi.org/10.1021/jacs.3c09082

TY - JOUR

T1 - Colossal C130 Fullertubes

T2 - Soluble [5,5] C130-D5h(1) Pristine Molecules with 70 Nanotube Carbons and Two 30-Atom Hemifullerene End-caps

AU - Bourret, Emmanuel

AU - Liu, Xiaoyang

AU - Noble, Cora A.

AU - Cover, Kevin

AU - Davidson, Tanisha P.

AU - Huang, Rong

AU - Koenig, Ryan M.

AU - Reeves, K. Shawn

AU - Vlassiouk, Ivan V.

AU - Côté, Michel

AU - Baxter, Jefferey S.

AU - Lupini, Andrew R.

AU - Geohegan, David B.

AU - Dorn, Harry C.

AU - Stevenson, Steven

PY - 2023/12/6

Y1 - 2023/12/6

N2 - We report the seminal experimental isolation and DFT characterization of pristine [5,5] C130-D5h(1) fullertubes. This achievement represents the largest soluble carbon molecule obtained in its pristine form. The [5,5] C130 species is the highest aspect ratio fullertube purified to date and now surpasses the recent gigantic [5,5] C120-D5d(1). In contrast to C90, C100, and C120 fullertubes, the longer C130-D5h has more nanotubular carbons (70) than end-cap fullerenyl atoms (60). Starting from 39,393 possible C130 isolated pentagon rule (IPR) structures and after analyzing polarizability, retention time, and UV-vis spectra, these three layers of data remarkably predict a single candidate isomer and fullertube, [5,5] C130-D5h(1). This structural assignment is augmented by atomic resolution STEM data showing distinctive and tubular “pill-like” structures with diameters and aspect ratios consistent with [5,5] C130-D5h(1) fullertubes. The high selectivity of the aminopropanol reaction with spheroidal fullerenes permits facile separation and removal of fullertubes from soot extracts. Experimental analyses (HPLC retention time, UV-vis, and STEM) were synergistically used (with polarizability and DFT property calculations) to down select and confirm the C130 fullertube structure. Achieving the isolation of a new [5,5] C130-D5h fullertube opens the door to application development and fundamental studies of electron confinement, fluorescence, and metallic character for a fullertube series of molecules with systematic tubular elongation. This [5,5] fullertube family also invites comparative studies with single-walled carbon nanotubes (SWCNTs), nanohorns (SWCNHs), and fullerenes.

AB - We report the seminal experimental isolation and DFT characterization of pristine [5,5] C130-D5h(1) fullertubes. This achievement represents the largest soluble carbon molecule obtained in its pristine form. The [5,5] C130 species is the highest aspect ratio fullertube purified to date and now surpasses the recent gigantic [5,5] C120-D5d(1). In contrast to C90, C100, and C120 fullertubes, the longer C130-D5h has more nanotubular carbons (70) than end-cap fullerenyl atoms (60). Starting from 39,393 possible C130 isolated pentagon rule (IPR) structures and after analyzing polarizability, retention time, and UV-vis spectra, these three layers of data remarkably predict a single candidate isomer and fullertube, [5,5] C130-D5h(1). This structural assignment is augmented by atomic resolution STEM data showing distinctive and tubular “pill-like” structures with diameters and aspect ratios consistent with [5,5] C130-D5h(1) fullertubes. The high selectivity of the aminopropanol reaction with spheroidal fullerenes permits facile separation and removal of fullertubes from soot extracts. Experimental analyses (HPLC retention time, UV-vis, and STEM) were synergistically used (with polarizability and DFT property calculations) to down select and confirm the C130 fullertube structure. Achieving the isolation of a new [5,5] C130-D5h fullertube opens the door to application development and fundamental studies of electron confinement, fluorescence, and metallic character for a fullertube series of molecules with systematic tubular elongation. This [5,5] fullertube family also invites comparative studies with single-walled carbon nanotubes (SWCNTs), nanohorns (SWCNHs), and fullerenes.

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U2 - 10.1021/jacs.3c09082

DO - 10.1021/jacs.3c09082

M3 - Article

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AN - SCOPUS:85178316436

SN - 0002-7863

VL - 145

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EP - 25947

JO - Journal of the American Chemical Society

JF - Journal of the American Chemical Society

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Colossal C₁₃₀ Fullertubes: Soluble [5,5] C₁₃₀-D_5h(1) Pristine Molecules with 70 Nanotube Carbons and Two 30-Atom Hemifullerene End-caps

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