Spray-Coated Multiwalled Carbon Nanotube Composite Electrodes for

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Spray-coated Multi-walled Carbon Nanotube Composite Electrodes for Thermal Energy Scavenging Electrochemical Cells Nicolas E. Holubowitch, James Landon, Cameron A. Lippert, John D. Craddock, Matthew C. Weisenberger, and Kunlei Liu ACS Appl. Mater. Interfaces, Just Accepted Manuscript • DOI: 10.1021/acsami.6b05083 • Publication Date (Web): 11 Aug 2016 Downloaded from http://pubs.acs.org on August 13, 2016

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ACS Applied Materials & Interfaces

Spray-coated Multi-walled Carbon Nanotube Composite Electrodes for Thermal Energy Scavenging Electrochemical Cells

Nicolas E. Holubowitch, James Landon, Cameron A. Lippert, John D. Craddock, Matthew C. Weisenberger, and Kunlei Liu*

2540 Research Park Drive, Center for Applied Energy Research, University of Kentucky, Lexington, KY 40511, USA [email protected] [email protected] [email protected] [email protected] [email protected] *Corresponding author. Tel: 859-257-0293. Fax: 859-257-0302. E-mail: [email protected]

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Abstract Spray-coated multi-walled carbon nanotube/poly(vinylidene fluoride) (MWCNT/PVDF) composite electrodes, scCNTs, with varying CNT compositions (2 to 70 wt.%) are presented for use in a simple thermal energy-scavenging cell (thermocell) based on the ferro/ferricyanide redox couple. Their utility for direct thermal-to-electrical energy conversion is explored at various temperature differentials and cell orientations. Performance is compared to that of buckypaper, a 100% CNT sheet material used as a benchmark electrode in thermocell research. The 30 to 70 wt.% scCNT composites give the highest power output by electrode area – seven times greater than buckypaper at ∆T = 50 °C. CNT utilization is drastically enhanced in our electrodes, reaching 1 W gCNT-1 compared to 0.036 W gCNT-1 for buckypaper.

Superior

performance of our spray-coated electrodes is attributed to both wettability with better use of a large portion of electrochemically active CNTs and minimization of ohmic and thermal contact resistances. Even composites with as low as 2 wt.% CNTs are still competitive with prior art. The MWCNT/PVDF composites developed herein are inexpensive, scalable, and serve a general need for CNT electrode optimization in next-generation devices.

Keywords Energy scavenging; carbon nanotube; thermoelectrochemical cell; Seebeck coefficient; spraycoating

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Introduction Thermal energy is abundantly available in the environment from solar, geothermal and industrial sources.1 In 2014, 60% of primary energy produced in the U.S. was rejected, typically as low-grade (