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Title: Maximization of carbon nanotube yield by solid carbon-assisted dewetting of iron catalyst films

Abstract

Further understanding of how nanoparticle catalyst composition influences the yield of carbon nanotubes (CNTs) is key to their scalable, cost-effective manufacture. In particular, the role of trace carbon deposits on promoting CNT nucleation from the catalyst has been studied recently by our team. Here, we show that deposition of solid carbon onto an iron catalyst film prior to dewetting effectively amplifies the CNT yield. In this work, we investigated the effect of the amount of C and Fe on particle formation and reduction, and growth kinetics using a combination of in situ techniques – Raman spectroscopy, X-ray photoelectron spectroscopy and environmental transmission electron microscopy. We found that CNT growth rate and yield are maximized for specific relative thicknesses of C and Fe (~0.2 and 0.8 nm, respectively). The presence of carbon causes accelerated dewetting of the catalyst, and more rapidly forms a population of metallic Fe particles that grow CNTs at a higher yield. Additionally, these factors also cumulatively result in a lower incubation time and improved yield. Therefore, loading of catalyst particles with solid carbon is a straightforward and practical route towards boosting CNT yield and improving the efficiency of CNT growth by chemical vapor deposition.

Authors:
 [1];  [2];  [3];  [4];  [4];  [5];  [3];  [6]
  1. Air Force Research Lab. (AFRL), Wright-Patterson AFB, OH (United States); UES Inc., Dayton, OH (United States)
  2. Air Force Research Lab. (AFRL), Wright-Patterson AFB, OH (United States); UES Inc., Dayton, OH (United States); Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
  3. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
  4. Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
  5. Univ. of Pennsylvania, Philadelphia, PA (United States)
  6. Air Force Research Lab. (AFRL), Wright-Patterson AFB, OH (United States)
Publication Date:
Research Org.:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Aeronautics and Space Administration (NASA); U.S. Air Force Office of Scientific Research
OSTI Identifier:
1649992
Alternate Identifier(s):
OSTI ID: 1617109
Report Number(s):
BNL-216275-2020-JAAM
Journal ID: ISSN 0008-6223
Grant/Contract Number:  
SC0012704; NNX17AJ32G; 16RXCOR322; SC0010795
Resource Type:
Accepted Manuscript
Journal Name:
Carbon
Additional Journal Information:
Journal Volume: 165; Journal Issue: C; Journal ID: ISSN 0008-6223
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
77 NANOSCIENCE AND NANOTECHNOLOGY; Carbon nanotubes; Synthesis; CVD; Raman spectroscopy; In situ

Citation Formats

Rao, Rahul, Carpena-Núñez, Jennifer, Dee, Nicholas T., Zakharov, Dmitri N., Boscoboinik, J. Anibal, Stach, Eric A., Hart, A. John, and Maruyama, Benji. Maximization of carbon nanotube yield by solid carbon-assisted dewetting of iron catalyst films. United States: N. p., 2020. Web. doi:10.1016/j.carbon.2020.04.064.
Rao, Rahul, Carpena-Núñez, Jennifer, Dee, Nicholas T., Zakharov, Dmitri N., Boscoboinik, J. Anibal, Stach, Eric A., Hart, A. John, & Maruyama, Benji. Maximization of carbon nanotube yield by solid carbon-assisted dewetting of iron catalyst films. United States. https://doi.org/10.1016/j.carbon.2020.04.064
Rao, Rahul, Carpena-Núñez, Jennifer, Dee, Nicholas T., Zakharov, Dmitri N., Boscoboinik, J. Anibal, Stach, Eric A., Hart, A. John, and Maruyama, Benji. Tue . "Maximization of carbon nanotube yield by solid carbon-assisted dewetting of iron catalyst films". United States. https://doi.org/10.1016/j.carbon.2020.04.064. https://www.osti.gov/servlets/purl/1649992.
@article{osti_1649992,
title = {Maximization of carbon nanotube yield by solid carbon-assisted dewetting of iron catalyst films},
author = {Rao, Rahul and Carpena-Núñez, Jennifer and Dee, Nicholas T. and Zakharov, Dmitri N. and Boscoboinik, J. Anibal and Stach, Eric A. and Hart, A. John and Maruyama, Benji},
abstractNote = {Further understanding of how nanoparticle catalyst composition influences the yield of carbon nanotubes (CNTs) is key to their scalable, cost-effective manufacture. In particular, the role of trace carbon deposits on promoting CNT nucleation from the catalyst has been studied recently by our team. Here, we show that deposition of solid carbon onto an iron catalyst film prior to dewetting effectively amplifies the CNT yield. In this work, we investigated the effect of the amount of C and Fe on particle formation and reduction, and growth kinetics using a combination of in situ techniques – Raman spectroscopy, X-ray photoelectron spectroscopy and environmental transmission electron microscopy. We found that CNT growth rate and yield are maximized for specific relative thicknesses of C and Fe (~0.2 and 0.8 nm, respectively). The presence of carbon causes accelerated dewetting of the catalyst, and more rapidly forms a population of metallic Fe particles that grow CNTs at a higher yield. Additionally, these factors also cumulatively result in a lower incubation time and improved yield. Therefore, loading of catalyst particles with solid carbon is a straightforward and practical route towards boosting CNT yield and improving the efficiency of CNT growth by chemical vapor deposition.},
doi = {10.1016/j.carbon.2020.04.064},
journal = {Carbon},
number = C,
volume = 165,
place = {United States},
year = {Tue Sep 01 00:00:00 EDT 2020},
month = {Tue Sep 01 00:00:00 EDT 2020}
}

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