Abstract

Electrically-responsive biomaterials such as conductive polymers and conductive hydrogels have piqued the interest of scientists for targeted payload delivery applications in recent years since generating electricity is easy. Conductive composite hydrogels are a specific class of hydrogel that can be designed to not only have mechanical properties similar to skin and soft tissue, but can also have electrical properties comparable to metals and organic semiconductors. These composite hydrogels have been considered for a wide range of technological applications. Conductive hydrogels can be fabricated to ensure that they exhibit: 1) excellent biocompatibility; 2) soft and tunable mechanical properties similar to biological tissue; 3) mixed electronic/ionic conductivity that promotes efficient signal transduction for delivering drugs to the tissue; 4) ability to create materials with well-controlled microstructure; and 5) ability to be loaded with wide range of molecular size molecules with different molecular charge; thereby making conductive hydrogels a stronger tool for targeted delivery applications. This dissertation focuses on describing a novel method of creating hydrogel composites from the commercially available conductive polymer PEDOT (poly(3,4-ethylenedioxythiophene):polystyrene sulfonate). The resulting method allows for fast production of conductive hydrogels, and does not need specific equipment. In this method of production, a wide range of mechanical properties can be achieved by altering hydrogel composition and production temperature without jeopardizing the electrical properties of the hydrogels by using conductive polymer. Additionally, this method could be employed for fabrication of conductive composite hydrogels with a variety of polymers and cross-linkers. Chapter two provides an overview on electrically-responsive targeted delivery depots with respect to their release mechanisms from electrical stimulation, parameters affecting drug release with electricity, and current efforts on multi-drug delivery using electrically-responsive materials. In chapter three, we explored the production and application of pAAc-PEDOT (poly acrylic acid-poly(3,4-ethylenedioxthiophene):polystyrene sulfonate) cryogels. Our goal was to develop soft, injectable, and conducting hydrogel-based electrode materials, and to characterize their sustained mechanical and electrical properties before and after sterilization and injection. Biocompatibility, cytotoxicity, and drug delivery capability of these cryogels were also investigated. pAAc-PEDOT cryogels were made at a subfreezing temperature to generate a macroporous structure within the gels. The resulting porous hydrogels exhibited enhanced mechanical properties. The cryogels exhibited softness (0.2-20 kPa), excellent toughness, and strain of failure, and could survive injection through 16-gauge needle. Additionally, these gels demonstrated the capability of recording alpha oscillations. Last but not least, these cryogels were found to be biocompatible and were capable of being loaded

Highlights

  • Introduction and MotivationNeuroprosthetic devices have been developed in order to return function, or to reduce symptoms exhibited by patients suffering from neurological diseases [1]

  • We investigated the integration of conductive hydrogels with tripolar concentric ring electrodes (TCREs)

  • 3.3 Results and Discussion PEDOT hydrogels were generated by entrapping PEDOT polymer within poly(acrylic acid) matrices using 550 Da poly(ethylene glycol) dimethacrylate (PEGDM) as a crosslinker

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Summary

Introduction

Introduction and MotivationNeuroprosthetic devices have been developed in order to return function, or to reduce symptoms exhibited by patients suffering from neurological diseases [1]. Deep brain stimulation (DBS) uses implanted electrodes to electrically stimulate targets within the brain [3, 4], which can reduce symptoms exhibited by patients with Parkinson’s disease, essential tremor, dystonia, chronic pain, major depression, and obsessive-compulsive disorder [5] Such strategies require an electrode-tissue interface whose electrical conductivity remains sufficiently high to transmit neural signals over time [6]. Because of the issues outlined above, this work aimed to develop a versatile material for interfacing between electronics and tissues that exhibited (i) soft mechanics to help facilitate conformation to curvilinear surfaces and to provide better mechanical matches with native tissues, (ii) sufficient electrical conductivity to record low-powered neural signals, (iii) tunable mechanics to enable application-specific customizations, (iv) toughness and compressibility to enable less traumatic introduction to tissues via injection, (v) low cytotoxicity, and (vi) the ability to locally deliver therapeutics that could potentially aid in combatting inflammation and the foreign body reaction. If EEG techniques can be endowed with better spatial resolution, it will prove to be a powerful tool in a wide range of emerging and future neurological diagnostics and treatments

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