The role of water in the tribochemical mechanisms of ultralow wear polytetrafluoroethylene (PTFE) composites was investigated by studying 10 and 20 wt % polyether ether ketone (PEEK)-filled and 5 wt % αAl2O3-filled PTFE composites. These composites were run against stainless-steel substrates in humidity, water, and dry nitrogen environments. The results showed that the wear behavior of both composites was significantly affected by the sliding environment. Both composites achieved remarkably low wear rates in humidity because of tribochemically generated carboxylate end groups that anchored the polymer transfer films to the steel substrate. In nitrogen, PTFE–PEEK outperformed PTFE−αAl2O3 because of polar carbonyl groups on PEEK, which increased the surface energy of PEEK, aiding it in adhering to the substrate and resulting in a transfer film. Both composites in water exhibited high wear. The water oversaturated the functional groups at the end of the polymer chains and prevented the formation of a transfer film.

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Remarkably low wear rates were observed in PTFE–PEEK and polytetrafluoroethylene (PTFE)-alpha-alumina composites when evaluated in a “self-mated” configuration, where a polymer pin is slid against a polymer countersample of the same composition. Each composite was tested in a controlled humidity environment on a linearly reciprocating tribometer on two different countersamples: a polymer countersample (self-mated) and a stainless steel countersample for comparison. For all the self-mated PTFE–PEEK composites [polyether ether ketone (PEEK) wt % 10, 20, 30, 40, and 50], the average friction coefficient was reduced, and the steady-state and total specific wear rates were improved when compared to testing against stainless steel. Self-mated PTFE–PEEK (wt % 10–40) achieved ultralow wear rates on the order of 10–9 mm3/Nm and friction coefficients of 0.08–0.14. When compared with samples slid against stainless steel, IR spectroscopy of the sliding surface showed that the self-mated PTFE–PEEK composites accumulate more PEEK at the sliding interface and more expression of a tribochemical carboxylate species, which have been linked with ultralow wear PTFE materials. The PTFE composites slid on steel rely on the formation of transfer films for ultralow wear performance. This is achieved by unidirectional increasing surface energy gradients from the polymer pin to the steel substrate, which dominate the transport and wear of PTFE composites slid on steel. However, the self-mated ultralow wear PTFE-based composites rely only on the formation and stability of tribofilms that consist of tribochemically altered PTFE with new carboxylate end groups as well as accumulated filler (i.e., PEEK or alumina). These films have self-regulating, minimal differences in surface energy. The close match of these low-energy surfaces contributes to low friction and ultralow wear. The self-mated PEEK-filled PTFE outperforms the alumina-filled PTFE primarily because of the ease at which PEEK accumulates at the surface. Additionally, the reinforcement and anchoring of the surface is better for a polymer blend than a particle-reinforced composite.

Scalable fabrication of freestanding carbon nanotube films (buckypapers) is of notable interest in nanotechnology due to emerging, real world applications for these lightweight and flexible materials. Post-electrophoretic deposition electrochemical separation (PEPDECS), a recently developed method for the scalable production of buckypapers, involves the electrophoretic deposition (EPD) of charged carbon nanotubes onto a flat substrate in a parallel-plate capacitor configuration, followed by a reversal of the direction of the electric field to detach the film. This study explored the characteristics of the deposition and liberation of the delaminated film, such as the applied voltage and the electrode size, in search of the optimum conditions for high quality buckypaper fabrication. Bubble formation on the film, due to the electrolysis of the suspension, increased as a function of the current density. The time required to delaminate a film completely from its underlying substrate was higher at higher initial current densities. Additionally, only when the applied EPD voltage was ≥2.8 V was the integrity of the buckypaper sufficient for them to be handled. The mechanical properties of the resulting films were examined to quantify their integrity. These experiments demonstrate the dependency of successful film fabrication on variable conditions during the initial EPD and provide a means to control the properties of the final films.

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