An interesting, and potentially important, challenge for colloid scientists is to design injectable dispersions that enable repair of damaged and degenerated tissue. This work presents a study of the ability of pH-responsive microgel particles to restore the mechanical properties of loadbearing soft tissue. Microgel particles are cross-linked polymer colloid particles that are swollen with solvent. The first part of the study consists of an investigation of the pH-triggered swelling of poly(EA/MAA/BDDA) (ethylacrylate, methacrylic acid and 1,4-butanediol diacrylate) microgel particles using photon correlation spectroscopy (PCS) measurements. The concentrated dispersions exhibit a strong fluid-to-gel transition when the pH is increased to above 6.0, i.e., above this pH they form gelled microgel dispersions. The swelling data are used to aid interpretation of the pH-triggered changes in the gel modulus, as probed using dynamic rheology. The second part of the study involves an investigation of the mechanical properties of artificially degenerated, model intervertebral discs (IVDs) containing gelled microgel dispersions. High concentration microgel dispersions were injected as fluids into the interior of degenerated IVDs and the pH increased by subsequent alkaline solution injection to cause particle swelling and dispersion gelation. Uniaxial compression data measured for the IVDs containing injected microgel dispersions indicate that the pH-induced particle swelling of the microgel restores the mechanical properties of degenerated IVDs to values similar to those measured for normal, non-degenerated, IVDs.
Stimulus responsive copolymers are an important class of surfactants that are attracting growing attention in the literature. When used to stabilize colloids, they confer responsiveness to an otherwise nonresponsive system. In this work, a new pH-responsive comb copolymer surfactant, poly(DEAEMa-co-PEGMa), where DEAEMa and PEGMa are diethylaminoethyl methacrylate and poly(ethylene glycol) methacrylate, is introduced and used to stabilize emulsions and particulate dispersions. The copolymer contained 70 mol % of DEAEMa. Turbidity versus pH measurements and photon correlation spectroscopy of the copolymer solutions revealed pH-triggered collapse of the chains above the pK(a). The surface activity of the copolymer increased with pH. The minimum surface tension measured was 33.6 mN/m at pH = 10. These data enabled identification of the pK(a) for poly(DEAEMa-co-PEGMa) as 6.8. The emulsions consisted of tetradecane-in-water and had a droplet size in the range 5-11 mum. They were slightly flocculated when the pH value was close to the isoelectric point. The emulsions phase separated at low pH values. The particulate dispersions were based on carbendazim, which is a fungacide, and had an average size of 1.8 mum. The data for the emulsions and carbendazim dispersions show that the extent of flocculation decreases with decreasing size of the dispersed phase. Analysis of the data suggest that optimum emulsion stability occurs in the pH region of 5.3-6.8 as judged by turbidity measurements. Electrophoretic mobility measurements as a function of pH for the emulsions and carbendazim dispersions reveal a similar isoelectric point in the range of 8.5-9.0, which is about two pH units higher than the pK(a) of the copolymer. A mechanism that explains the pH-responsive stability of the emulsions and dispersions is presented and discussed.
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