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Tuning Counterion Chemistry to Reduce Carrier Localization in Doped Thermoelectric Carbon Nanotube Networks

33 Pages Posted: 29 Nov 2022 Publication Status: Published

See all articles by Tucker L. Murrey

Tucker L. Murrey

National Renewable Energy Laboratory - Materials, Chemical and Computational Science Directorate

Taylor J. Aubry

National Renewable Energy Laboratory - Materials, Chemical and Computational Science Directorate

Omar Leon Ruiz

University of California, Los Angeles (UCLA) - Department of Chemistry and Biochemistry

Kira A. Thurman

National Renewable Energy Laboratory - Materials, Chemical and Computational Science Directorate

Klaus H. Eckstein

University of Würzburg - Institute of Physical and Theoretical Chemistry

Evan A. Doud

University of California, Los Angeles (UCLA) - Department of Chemistry and Biochemistry

Julia M. Stauber

University of California, Los Angeles (UCLA) - Department of Chemistry and Biochemistry

Alexander M. Spokoyny

University of California, Los Angeles (UCLA) - Department of Chemistry and Biochemistry

Benjamin J. Schwartz

University of California, Los Angeles (UCLA) - Department of Chemistry and Biochemistry

Tobias Hertel

University of Würzburg - Institute of Physical and Theoretical Chemistry

Jeff Blackburn

National Renewable Energy Laboratory - Materials, Chemical and Computational Science Directorate; National Renewable Energy Laboratory - Biosciences Center

Andrew John Ferguson

National Renewable Energy Laboratory - Materials, Chemical and Computational Science Directorate

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Abstract

Semiconducting single-walled carbon nanotubes (s SWCNTs) have demonstrated promising performance for several electronic and energy harvesting devices such as low-temperature thermoelectric converters. A fundamental challenge for incorporating s-SWCNTs (and other pi-conjugated semiconductors) into such applications is exerting fine control over charge carrier densities via electronic doping while simultaneously ensuring these charge carriers are not localized due to the inherently low Coulomb screening. Here, we compare a series of molecular charge-transfer dopants based on functionalized icosahedral dodecaborane (DDB) clusters with small molecules to explore the impact of the dopant’s chemical and electronic structure on the doping efficacy and charge carrier transport in s-SWCNT networks. Analysis of the thermoelectric properties indicates that localization of electron density on the DDB core counterion reduces the coulombic interactions that contribute to hole localization in the s-SWCNTs, thereby increasing the charge carrier mobility. The enhanced delocalization ultimately allows for an increase in the thermopower and electrical conductivity at lower charge carrier densities, yielding enhanced thermoelectric transport and a thermoelectric power factor that surpasses the previous best-in-class for enriched s-SWCNT thin film networks.

Keywords: carbon nanotubes, charge transfer, carrier doping, carrier transport, thermoelectric, delocalization, dodecaborane

Suggested Citation

Murrey, Tucker L. and Aubry, Taylor J. and Ruiz, Omar Leon and Thurman, Kira A. and Eckstein, Klaus H. and Doud, Evan A. and Stauber, Julia M. and Spokoyny, Alexander M. and Schwartz, Benjamin J. and Hertel, Tobias and Blackburn, Jeff and Ferguson, Andrew John, Tuning Counterion Chemistry to Reduce Carrier Localization in Doped Thermoelectric Carbon Nanotube Networks. Available at SSRN: https://ssrn.com/abstract=4287840 or http://dx.doi.org/10.2139/ssrn.4287840
This version of the paper has not been formally peer reviewed.

Tucker L. Murrey

National Renewable Energy Laboratory - Materials, Chemical and Computational Science Directorate ( email )

Taylor J. Aubry

National Renewable Energy Laboratory - Materials, Chemical and Computational Science Directorate ( email )

Omar Leon Ruiz

University of California, Los Angeles (UCLA) - Department of Chemistry and Biochemistry ( email )

Kira A. Thurman

National Renewable Energy Laboratory - Materials, Chemical and Computational Science Directorate ( email )

Klaus H. Eckstein

University of Würzburg - Institute of Physical and Theoretical Chemistry ( email )

Evan A. Doud

University of California, Los Angeles (UCLA) - Department of Chemistry and Biochemistry ( email )

Julia M. Stauber

University of California, Los Angeles (UCLA) - Department of Chemistry and Biochemistry ( email )

Alexander M. Spokoyny

University of California, Los Angeles (UCLA) - Department of Chemistry and Biochemistry ( email )

Benjamin J. Schwartz

University of California, Los Angeles (UCLA) - Department of Chemistry and Biochemistry ( email )

Tobias Hertel

University of Würzburg - Institute of Physical and Theoretical Chemistry ( email )

Jeff Blackburn

National Renewable Energy Laboratory - Materials, Chemical and Computational Science Directorate ( email )

National Renewable Energy Laboratory - Biosciences Center ( email )

United States

Andrew John Ferguson (Contact Author)

National Renewable Energy Laboratory - Materials, Chemical and Computational Science Directorate ( email )

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