Corey A. Hewitt

Multilayered Carbon Nanotube/Polymer Composite Based Thermoelectric Fabrics

Thermoelectrics are materials capable of the solid-state conversion between thermal and electrical energy. Carbon nanotube/polymer composite thin films are known to exhibit thermoelectric effects, however, have a low figure of merit (ZT) of 0.02. In this work, we demonstrate individual composite films of multiwalled carbon nanotubes (MWNT)/polyvinylidene fluoride (PVDF) that are layered into multiple element modules that resemble a felt fabric. The thermoelectric voltage generated by these fabrics is the sum of contributions from each layer, resulting in increased power output. Since these fabrics have the potential to be cheaper, lighter, and more easily processed than the commonly used thermoelectric bismuth telluride, the overall performance of the fabric shows promise as a realistic alternative in a number of applications such as portable lightweight electronics.

Varying the concentration of single walled carbon nanotubes in thin film polymer composites, and its effect on thermoelectric power

Resistivity and thermoelectric power (TEP) measurements were conducted on single walled carbon nanotube (SWNT), polyvinylidene fluoride composite thin films of varying SWNT concentrations. This heterogeneous material was used in order to utilize the good electrical conductance of the nanotubes and the poor thermal conductance of the polymer to increase the figure of merit (ZT). As the nanotube weight percent decreased from 100% to 5%, the beneficial effects of the TEP increase and thermal conductivity decrease outweighed the negative effect of decreased electrical conductivity, resulting in an increase in ZT by a factor of 100.

Layered Bi2Se3 Nanoplate/Polyvinylidene Fluoride Composite Based n-type Thermoelectric Fabrics

In this study, we report the fabrication of n-type flexible thermoelectric fabrics using layered Bi2Se3 nanoplate/polyvinylidene fluoride (PVDF) composites as the thermoelectric material. These composites exhibit room temperature Seebeck coefficient and electrical conductivity values of -80 μV K(-1) and 5100 S m(-1), respectively, resulting in a power factor approaching 30 μW m(-1)K(-2). The temperature-dependent thermoelectric properties reveal that the composites exhibit metallic-like electrical conductivity, whereas the thermoelectric power is characterized by a heterogeneous model. These composites have the potential to be used in atypical applications for thermoelectrics, where lightweight and flexible materials would be beneficial. Indeed, bending tests revealed excellent durability of the thermoelectric fabrics. We anticipate that this work may guide the way for fabricating high performance thermoelectric fabrics based on layered V-VI nanoplates.

Improved thermoelectric power output from multilayered polyethylenimine doped carbon nanotube based organic composites

By appropriately selecting the carbon nanotube type and n-type dopant for the conduction layers in a multilayered carbon nanotube composite, the total device thermoelectric power output can be increased significantly. The particular materials chosen in this study were raw single walled carbon nanotubes for the p-type layers and polyethylenimine doped single walled carbon nanotubes for the n-type layers. The combination of these two conduction layers leads to a single thermocouple Seebeck coefficient of 96 ± 4 μVK−1, which is 6.3 times higher than that previously reported. This improved Seebeck coefficient leads to a total power output of 14.7 nW per thermocouple at the maximum temperature difference of 50 K, which is 44 times the power output per thermocouple for the previously reported results. Ultimately, these thermoelectric power output improvements help to increase the potential use of these lightweight, flexible, and durable organic multilayered carbon nanotube based thermoelectric modules in low po...

Ultrathin, Washable, and Large-Area Graphene Papers for Personal Thermal Management

Freestanding, flexible/foldable, and wearable bifuctional ultrathin graphene paper for heating and cooling is fabricated as an active material in personal thermal management (PTM). The promising electrical conductivity grants the superior Joule heating for extra warmth of 42 °C using a low supply voltage around 3.2 V. Besides, based on its high out-of-plane thermal conductivity, the graphene paper provides passive cooling via thermal transmission from the human body to the environment within 7 s. The cooling effect of graphene paper is superior compared with that of the normal cotton fiber, and this advantage will become more prominent with the increased thickness difference. The present bifunctional graphene paper possesses high durability against bending cycles over 500 times and wash time over 1500 min, suggesting its great potential in wearable PTM.

Hybrid thermoelectric piezoelectric generator

This work presents an integration of flexible thermoelectric and piezoelectric materials into a single device structure. This device architecture overcomes several prohibitive issues facing the combination of traditional thermoelectric and piezoelectric generators, while optimizing performance of the combined power output. The structure design uses a carbon nanotube/polymer thin film as a flexible thermoelectric generator that doubles as an electrode on a piezoelectric generator made of poly(vinylidene fluoride). An example 2 × 2 array of devices is shown to generate 89% of the maximum thermoelectric power, and provide 5.3 times more piezoelectric voltage when compared with a traditional device.

Negative thermoelectric power from large diameter multiwalled carbon nanotubes grown at high chemical vapor deposition temperatures

Multiwalled carbon nanotubes (MWNTs) have been grown using a standard chemical vapor deposition method, except for varying the growth temperature. Nanotubes grown below 770 °C exhibit typical positive thermoelectric powers, while those grown above have negative values. This behavior is attributed to the larger nanotube diameters observed at higher growth temperatures. Below 770 °C, the average nanotube diameter is about 50 nm, while above, nanotubes reach diameters of 300 nm. This increase in diameter and number of inner shells leads to the intrinsic negative thermoelectric power of the inner nanotube shells becoming larger than the positive thermoelectric power due to oxygen doping on the outer surface of the nanotube. The overall negative thermopower (about −6 μV/K, compared to +7 μV/K for smaller diameter nanotubes) can be understood in terms of a parallel conduction model. Our large-diameter multiwalled carbon nanotubes allow the intrinsic negative thermopower of MWNTs to be accessed without requiring...

2D Chalcogenide Nanoplate Assemblies for Thermoelectric Applications

Engineered atomic dislocations have been used to create a novel, Sb2 Te3 nanoplate-like architecture that exhibits a unique antisymmetric chirality. High-resolution transmission electron microscopy (HRTEM) coupled with atomic force microscopy and X-ray photoelectron spectroscopy reveals the architectures to be extremely well ordered with little residual strain. Surface modification of these topologically complex macrostructures (≈3 µm) has been achieved by direct growth of metallic Ag nanoparticles onto the edge sites of the Sb2 Te3 . Again, HRTEM shows this nanoparticle decoration to be atomically sharp at the boundaries and regularly spaced along the selvedge of the nanostructure. Transport experiments of densified films of these assemblies exhibit marked increases in carrier density after nanoengineering, yielding 3.5 × 104 S m-1 in electrical conductivity. An increased Seebeck coefficient by 20% in parallel with electrical conductivity is also observed. This gives a thermoelectric power factor of 371 µW m-1 K-2 , which is the highest value for a flexible, freestanding film to date. These results suggest an entirely new direction in the search for wearable power harvesters based on topologically complex, low-dimensional nanoassemblies.

Self-Assembled Heterostructures: Selective Growth of Metallic Nanoparticles on V2–VI3 Nanoplates

Precise control of the selective growth of heterostructures with specific composition and functionalities is an emerging and extremely challenging topic. Here, the first investigation of the difference in binding energy between a series of metal-semiconductor heterostructures based on layered V2 -VI3 nanostructures is investigated by means of density functional theory. All lateral configurations show lower formation energy compared with that of the vertical ones, implying the selective growth of metal nanoparticles. The simulation results are supported by the successful fabrication of self-assembled Ag/Cu-nanoparticle-decorated p-type Sb2 Te3 and n-type Bi2 Te3 nanoplates at their lateral sites through a solution reaction. The detailed nucleation-growth kinetics are well studied with controllable reaction times and precursor concentrations. Accompanied by the preserved topological structure integrity and electron transfer on the semiconductor host, exceptional properties such as dramatically increased electrical conductivity are observed thanks to the pre-energy-filtering effect before carrier injection. A zigzag thermoelectric generator is built using Cu/Ag-decorated Sb2 Te3 and Bi2 Te3 as p-n legs to utilize the temperature gradient in the vertical direction. Synthetic approaches using similar chalcogenide nanoplates as building blocks, as well as careful control of the dopant metallic nanoparticles or semiconductors, are believed to be broadly applicable to other heterostructures with novel applications.

High Throughput Screening Tools for Thermoelectric Materials

A suite of complementary high-throughput screening systems for combinatorial films was developed at National Institute of Standards and Technology to facilitate the search for efficient thermoelectric materials. These custom-designed capabilities include a facility for combinatorial thin film synthesis and a suite of tools for screening the Seebeck coefficient, electrical resistance (electrical resistivity), and thermal effusivity (thermal conductivity) of these films. The Seebeck coefficient and resistance are measured via custom-built automated apparatus at both ambient and high temperatures. Thermal effusivity is measured using a frequency domain thermoreflectance technique. This paper will discuss applications using these tools on representative thermoelectric materials, including combinatorial composition-spread films, conventional films, single crystals, and ribbons.