Thermoelectric power factors of nanocarbon ensembles as a function of temperature

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Thermoelectric power factors of nanocarbon ensembles have been determined as a function of temperature from 400 to 1200 K. The ensembles, composed of mixtures of nanographite or disperse ultrananocrystalline diamond with B4 C, are formed into mechanically rigid compacts by reaction at 1200 K with methane gas and subsequently annealed in an argon atmosphere at temperatures up to 2500 K. The ensembles were characterized using scanning electron microscopy, Raman, x-ray diffraction, and high resolution transmission electron microscopy techniques and found to undergo profound nanostructural changes as a function of temperature while largely preserving their nanometer sizes. The power factors increase strongly both as a function of annealing temperature and of the temperature at which the measurements are carried out reaching 1 μW/ K2 cm at 1200 K without showing evidence of a plateau. Density functional "molecular analog" calculations on systems based on stacked graphene sheets show that boron substitutional doping results in a lowering of the Fermi level and the creation of a large number of hole states within thermal energies of the Fermi level [P. C. Redfern, D. M. Greun, and L. A. Curtiss, Chem. Phys. Lett. 471, 264 (2009)]. We propose that enhancement of electronic configurational entropy due to the large number of boron configurations in the graphite lattice contributes to the observed thermoelectric properties of the ensembles. © 2009 American Institute of Physics.

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Journal of Applied Physics