Mechanical and Tribological Study of a Stimulus Responsive Hydrogel, pNIPAAm, and a Mucinous Glycoprotein, Lubricin

Abstract

Friction is the resistive force that arises when two contacting surfaces move relative to each other. Frictional interactions are important from both engineering and biological perspectives. In this research I focus on the fundamental understanding of friction on polymeric and biological surfaces in aqueous environments. First, I examine the frictional properties of a stimulus-responsive hydrogel, poly-N-isopropylacrylamide (pNIPAAm), to understand how different phase states affect its tribological properties. My measurements indicate that gels in a collapsed conformation at low shear rates, exhibit significantly larger friction than swollen gels. These differences arise from changes in surface roughness, adhesive interactions, and chain entanglements of the gel surfaces associated with the phase transition. Importantly, I show that the changes in friction, triggered by an external stimulus, are reversible. Second, I examine details of the boundary lubrication mechanism involved in mediating friction and wear in diarthrodial joints. Specifically, I looked at the constituents of the synovial fluid, lubricin and hyaluronic acid (HA) and examined their interactions on model substrates, (1) to determine the effect of surface chemistry on adsorption using surface plasmon resonance (SPR), and (2) to study normal force interactions between these surfaces using colloidal probe microscopy (CPM). I found that lubricin is highly surface-active, adsorbed strongly onto hydrophobic, hydrophilic and also collagen surfaces. Overall, lubricin develops strong repulsive interactions. This behavior is in contrast to that of HA, which does not adsorb appreciably, nor does it develop significant repulsive interactions. I speculate that in mediating interactions at the cartilage surface, an important role of lubricin is one of providing a protective coating on cartilage surfaces that maintains the contacting surfaces in a sterically repulsive state.