Date of Award


Degree Type


Degree Name

Doctor of Philosophy (PhD)


Mechanical Engineering

First Advisor

Timothy S. Fisher

Committee Chair

Timothy S. Fisher

Committee Member 1

David F. Bahr

Committee Member 2

Baratunde A. Cola

Committee Member 3

Xianfan Xu


The development of thermal interface materials (TIMs) is necessitated by the temperature drop across interfacing materials arising from macro and microscopic irregularities of their surfaces that constricts heat through small contact regions as well as mismatches in their thermal properties. Similar to other types of TIMs, CNT TIMs alleviate the thermal resistance across the interface by thermally bridging two materials together with cylindrical, high-aspect ratio, and nominally vertical conducting elements. Within the community of TIM engineers, the vision driving the development of CNT TIMs was born from measurements that revealed impressively high thermal conductivities of individual CNTs. This vision was then projected to efforts focused on packing many individual CNTs on a single substrate that efficiently conduct heat in parallel and ultimately through many contact regions at CNT-to-substrate contacts.

This thesis encompasses a comprehensive investigation of the viability of carbon nanotube based thermal interface materials (CNT TIMs) to efficiently conduct heat across two contacting materials. The efforts in this work were initially devoted to engaging CNT TIMs with an opposing substrate using two bonding techniques. Using palladium hexadecanethiolate, Pd(SC16H35)2 the CNT ends were bonded to an opposing substrate (one-sided interface) or opposing CNT array (two-sided interface) to enhance contact conductance while maintaining a compliant joint. The palladium weld is particularly attractive for its mechanical stability at high temperatures. The engagement of CNT TIMs with an opposing substrate was also achieved by inserting a solder foil between the CNT TIM and opposing substrate and subsequently raising the temperature of the interface above the eutectic point of the solder foil. This bonding technique creates a strong weld that not only reduces the thermal resistance significantly but also minimizes the change in thermal resistance with an applied compressive load. The thermal performance was further improved by infiltrating the CNT TIM with paraffin wax, which serves as an alternate pathway for heat conduction across the interface that ultimately reduces the bulk thermal resistance of the CNT TIM.

For CNT TIMs synthesized at the Birck Nanotechnology Center at Purdue University, the thermal resistance was shown to scale linearly with their aggregate, as-grown height. Thus, the bulk thermal resistance can alternatively be tuned by adjusting the as-grown height. The linear relationship between thermal resistance and CNT TIM height provides a simple and efficient methodology to estimate the contact resistance and effective thermal conductivity of CNT TIMs. In this work, the contact resistance and effective thermal conductivity were estimated using two measurement techniques: (i) one-dimensional, steady-state reference bar and (ii) photoacoustic technique. A discrepancy in the estimated contact resistance exists between the two measurement techniques, which is due to the difficulty in measuring the true contact area. In contrast, the effective thermal conductivities estimated from both measurement techniques moderately agreed and were estimated to be on the order of O(1 W/mK).

The final chapter is in collaboration with Sandia National Laboratories and focuses on the development of an apparatus to measure the thermal conductivity of insulation materials critical for the operation of molten salt batteries. Molten salt batteries are particularly useful power sources for radar and guidance systems in military applications such as guided missiles, ordinance, and other weapons. Molten salt batteries are activated by raising the temperature of the electrolyte above its melting temperature using pyrotechnic heat pellets. The battery will remain active as long as the electrolyte is molten. As a result, the thermal processes within the components and interactions between them are critical to the overall performance of molten salt batteries. A molten salt battery is typically thermally insulated using wrappable and board-like insulation materials such as Fiberfrax wrap, Fiberfrax board, and Min-K insulation. The Fiberfrax board and Min-K insulation are composites of alumino-silicate and fumed silica-titania, respectively. In Chapter 9, the thermal conductivities of the Fiberfrax board and Min-K insulation were measured under different uniaxial compressive states and ambient environments. The thermal conductivity of the mixed separator pellets (LiCl/MgO/KCl) was also measured along with its contact resistances with interfacing members. To measure the thermal quantities, a steady-state reference bar with thermocouples was employed. The resulting values serve as inputs to a thermal model that aims to predict lifetimes of the batteries. (Abstract shortened by ProQuest.)