Oxygen-promoted catalyst sintering influences number density, alignment, and wall number of vertically aligned carbon nanotubes
Abstract
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 mechanismsmore »
- Authors:
-
- 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)
- Publication Date:
- Research Org.:
- Yale Univ., New Haven, CT (United States); Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)
- OSTI Identifier:
- 1376047
- Report Number(s):
- LLNL-JRNL-711500
Journal ID: ISSN 2040-3364
- Grant/Contract Number:
- AC52-07NA27344; AC02-05CH11231; 1120187; 1552993
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nanoscale
- Additional Journal Information:
- Journal Volume: 9; Journal Issue: 16; Journal ID: ISSN 2040-3364
- Publisher:
- Royal Society of Chemistry
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 77 NANOSCIENCE AND NANOTECHNOLOGY
Citation Formats
Shi, Wenbo, Li, Jinjing, Polsen, Erik S., Oliver, C. Ryan, Zhao, Yikun, Meshot, Eric R., Barclay, Michael, Fairbrother, D. Howard, Hart, A. John, and Plata, Desiree L. Oxygen-promoted catalyst sintering influences number density, alignment, and wall number of vertically aligned carbon nanotubes. United States: N. p., 2017.
Web. doi:10.1039/C6NR09802A.
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. Oxygen-promoted catalyst sintering influences number density, alignment, and wall number of vertically aligned carbon nanotubes. United States. https://doi.org/10.1039/C6NR09802A
Shi, Wenbo, Li, Jinjing, Polsen, Erik S., Oliver, C. Ryan, Zhao, Yikun, Meshot, Eric R., Barclay, Michael, Fairbrother, D. Howard, Hart, A. John, and Plata, Desiree L. Tue .
"Oxygen-promoted catalyst sintering influences number density, alignment, and wall number of vertically aligned carbon nanotubes". United States. https://doi.org/10.1039/C6NR09802A. https://www.osti.gov/servlets/purl/1376047.
@article{osti_1376047,
title = {Oxygen-promoted catalyst sintering influences number density, alignment, and wall number of vertically aligned carbon nanotubes},
author = {Shi, Wenbo and Li, Jinjing and Polsen, Erik S. and Oliver, C. Ryan and Zhao, Yikun and Meshot, Eric R. and Barclay, Michael and Fairbrother, D. Howard and Hart, A. John and Plata, Desiree L.},
abstractNote = {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.},
doi = {10.1039/C6NR09802A},
journal = {Nanoscale},
number = 16,
volume = 9,
place = {United States},
year = {Tue Apr 11 00:00:00 EDT 2017},
month = {Tue Apr 11 00:00:00 EDT 2017}
}
Web of Science
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