Oxygen-promoted catalyst sintering influences number density, alignment, and wall number of vertically aligned carbon nanotubes

Shi, Wenbo; Li, Jinjing; Polsen, Erik S.; Oliver, C. Ryan; Zhao, Yikun; Meshot, Eric R.; Barclay, Michael; Fairbrother, D. Howard; Hart, A. John; Plata, Desiree L.

doi:10.1039/C6NR09802A

Title: Oxygen-promoted catalyst sintering influences number density, alignment, and wall number of vertically aligned carbon nanotubes

Journal Article · Tue Apr 11 00:00:00 EDT 2017 · Nanoscale

DOI:https://doi.org/10.1039/C6NR09802A· OSTI ID:1376047

^[1]; Li, Jinjing ^[2]; Polsen, Erik S. ^[2]; Oliver, C. Ryan ^[3]; Zhao, Yikun ^[4]; Meshot, Eric R. ^[5]; Barclay, Michael ^[6];

^[6];

^[3];

^[1]

Yale Univ., New Haven, CT (United States)
Univ. of Michigan, Ann Arbor, MI (United States)
Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
Duke Univ., Durham, NC (United States)
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
Johns Hopkins Univ., Baltimore, MD (United States)

A lack of synthetic control and reproducibility during vertically aligned carbon nanotube (CNT) synthesis has stifled many promising applications of organic nanomaterials. Oxygen-containing species are particularly precarious in that they have both beneficial and deleterious effects and are notoriously difficult to control. In this paper, we demonstrated diatomic oxygen's ability, independent of water, to tune oxide-supported catalyst thin film dewetting and influence nanoscale (diameter and wall number) and macro-scale (alignment and density) properties for as-grown vertically aligned CNTs. In particular, single- or few-walled CNT forests were achieved at very low oxygen loading, with single-to-multi-walled CNT diameters ranging from 4.8 ± 1.3 nm to 6.4 ± 1.1 nm over 0–800 ppm O₂, and an expected variation in alignment, where both were related to the annealed catalyst morphology. Morphological differences were not the result of subsurface diffusion, but instead occurred via Ostwald ripening under several hundred ppm O₂, and this effect was mitigated by high H₂ concentrations and not due to water vapor (as confirmed in O₂-free water addition experiments), supporting the importance of O₂ specifically. Further characterization of the interface between the Fe catalyst and Al₂O₃ support revealed that either oxygen-deficit metal oxide or oxygen-adsorption on metals could be functional mechanisms for the observed catalyst nanoparticle evolution. Finally, taken as a whole, our results suggest that the impacts of O₂ and H₂ on the catalyst evolution have been underappreciated and underleveraged in CNT synthesis, and these could present a route toward facile manipulation of CNT forest morphology through control of the reactive gaseous atmosphere alone.

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Research Organization:: Yale Univ., New Haven, CT (United States); Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)

Grant/Contract Number:: AC52-07NA27344; AC02-05CH11231; 1120187; 1552993

OSTI ID:: 1376047

Report Number(s):: LLNL-JRNL-711500

Journal Information:: Nanoscale, Vol. 9, Issue 16; ISSN 2040-3364

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 29 works

Citation information provided by
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Carbon monoxide-induced adatom sintering in a Pd–Fe3O4 model catalyst Parkinson, Gareth S.; Novotny, Zbynek; Argentero, Giacomo Nature Materials, Vol. 12, Issue 8 https://doi.org/10.1038/nmat3667	journal	June 2013
Growth of Ultrahigh Density Single-Walled Carbon Nanotube Forests by Improved Catalyst Design Zhong, Guofang; Warner, Jamie H.; Fouquet, Martin ACS Nano, Vol. 6, Issue 4 https://doi.org/10.1021/nn203035x	journal	March 2012
Multiple Alkynes React with Ethylene To Enhance Carbon Nanotube Synthesis, Suggesting a Polymerization-like Formation Mechanism Plata, Desirée L.; Meshot, Eric R.; Reddy, Christopher M. ACS Nano, Vol. 4, Issue 12 https://doi.org/10.1021/nn101842g	journal	November 2010
Aligned Single-Walled Carbon Nanotube Arrays from Rhodium Catalysts with Unexpected Diameter Uniformity Independent of the Catalyst Size and Growth Temperature Li, Pan; Zhang, Xiao; Liu, Jie Chemistry of Materials, Vol. 28, Issue 3 https://doi.org/10.1021/acs.chemmater.5b04358	journal	January 2016
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Iron-Based Catalysts with Improved Oxygen Reduction Activity in Polymer Electrolyte Fuel Cells Lefèvre, Michel; Proietti, Eric; Jaouen, Frédéric Science, Vol. 324, Issue 5923, p. 71-74 https://doi.org/10.1126/science.1170051	journal	April 2009
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Graphene/pyrrolic-structured nitrogen-doped CNT nanocomposite supports for Pd-catalysed Heck coupling and chemoselective hydrogenation of nitroarenes Labulo, Ayomide H.; Omondi, Bernard; Nyamori, Vincent O. SN Applied Sciences, Vol. 1, Issue 2 https://doi.org/10.1007/s42452-018-0146-0	journal	January 2019
Process-morphology scaling relations quantify self-organization in capillary densified nanofiber arrays Kaiser, Ashley L.; Stein, Itai Y.; Cui, Kehang Physical Chemistry Chemical Physics, Vol. 20, Issue 6 https://doi.org/10.1039/c7cp06869g	journal	January 2018
Synthesis Procedure of Highly Densely Packed Carbon Nanotube Forests on TiN Campo, Teresa; Pinilla, Sergio; Gálvez, Santos Nanomaterials, Vol. 9, Issue 4 https://doi.org/10.3390/nano9040571	journal	April 2019

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