Isolating the Roles of Hydrogen Exposure and Trace Carbon Contamination on the Formation of Active Catalyst Populations for Carbon Nanotube Growth

Carpena-Núñez, Jennifer; Boscoboinik, Jorge Anibal; Saber, Sammy; Rao, Rahul; Zhong, Jian-Qiang; Maschmann, Matthew R.; Kidambi, Piran R.; Dee, Nicholas T.; Zakharov, Dmitri N.; Hart, A. John; Stach, Eric A.; Maruyama, Benji

doi:10.1021/acsnano.9b01382

Isolating the Roles of Hydrogen Exposure and Trace Carbon Contamination on the Formation of Active Catalyst Populations for Carbon Nanotube Growth

Journal Article · Mon Jul 22 00:00:00 EDT 2019 · ACS Nano

DOI:https://doi.org/10.1021/acsnano.9b01382· OSTI ID:1571415

^[1]; ^[2]; Saber, Sammy ^[3]; ^[4]; ^[2]; ^[5]; ^[6]; ^[7]; Zakharov, Dmitri N. ^[2]; ^[7]; ^[8]; Maruyama, Benji ^[3]

Air Force Research Laboratory, Wright-Patterson Air Force Base, Dayton, OH (United States); Brookhaven National Lab. (BNL), Upton, NY (United States)
Brookhaven National Lab. (BNL), Upton, NY (United States)
Air Force Research Laboratory, Wright-Patterson Air Force Base, Dayton, OH (United States)
Air Force Research Laboratory, Wright-Patterson Air Force Base, Dayton, OH (United States); UES, Inc., Dayton, OH (United States)
Columbia Univ., New York, NY (United States)
Vanderbilt Univ., Nashville, TN (United States)
Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
Brookhaven National Lab. (BNL), Upton, NY (United States); Univ. of Pennsylvania, Philadelphia, PA (United States)

Limited understanding of the factors influencing the yield of carbon nanotubes (CNTs) relative to the number of catalyst particles remains an important barrier to their large-scale production with high quality, and to tailoring CNT properties for applications. This lack of understanding is evident in the frequent use of Edisonian approaches to give high-yield CNT growth, and in the sometimes-confusing influence of trace residues on the reactor walls. In order to create conditions wherein CNT yield is reproducible and to enable large-scale and reliable CNT synthesis, it is imperative to understand—fundamentally—how these common practices impact catalytic activity and thus CNT number density. In this paper, we use ambient pressure-X-ray photoelectron spectroscopy (AP-XPS) to reveal the influence of carbon and hydrogen on the coupling between catalyst reduction and CNT nucleation, from an iron catalyst film. We observe a positive correlation between the degree of catalyst reduction and the density of vertically aligned CNTs (forests), verifying that effective catalyst reduction is critical to CNT nucleation and to the resulting CNT growth yield. We demonstrate that the extent of catalyst reduction is the reason for low CNT number density and for lack of self-organization, lift-off, and growth of CNT forests. We also show that hydrocarbon byproducts from consecutive growths can facilitate catalyst reduction and increase CNT number density significantly. These findings suggest that common practices used in the field—such as reactor preconditioning—aid in the reduction of the catalyst population, thus improving CNT number density and enabling the growth of dense forests. Finally, our results also motivate future work using AP-XPS and complementary metrology tools to optimize CNT growth conditions according to the catalyst chemical state.

View Accepted Manuscript (DOE)

Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: SC0010795; SC0012704

OSTI ID:: 1571415

Alternate ID(s):: OSTI ID: 1689055

Report Number(s):: BNL--212227-2019-JAAM

Journal Information:: ACS Nano, Journal Name: ACS Nano Journal Issue: 8 Vol. 13; ISSN 1936-0851

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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