Date of Award
2025
Document Type
Open Access Dissertation
Degree Name
Doctor of Philosophy in Chemical Engineering (PhD)
Administrative Home Department
Department of Chemical Engineering
Advisor 1
Yixin Liu
Committee Member 1
Caryn Heldt
Committee Member 2
Adrienne Minerick
Committee Member 3
Haiying Liu
Abstract
Developing reliable, low-cost biosensors is essential for advancing point-of-care diagnostics and expanding access to health monitoring technologies. Traditional sensors based on biological recognition elements such as enzymes and antibodies often suffer from limited stability, high production costs, and dependence on cold storage. This dissertation addresses these limitations through the design and optimization of electrochemically synthesized molecularly imprinted polymers (eMIPs), synthetic recognition elements that combine the specificity of biological systems with the robustness of engineered materials. A systematic framework was established to evaluate how monomer selection, concentration, scan rate, and cycle count affect film formation, morphology, and sensor performance. Using dopamine, pyrrole, and 3-aminophenyl boronic acid monomers, eMIP films were synthesized directly on electrode surfaces and characterized using cyclic voltammetry (CV), differential pulse voltammetry (DPV), electrochemical impedance spectroscopy (EIS), electrochemical surface plasmon resonance (EC-SPR), and electrochemical quartz crystal microbalance (EC-QCM). Machine learning models were incorporated to identify the most influential fabrication parameters and predict synthesis conditions yielding optimal sensitivity and reproducibility. Case studies demonstrate the versatility of this framework across multiple analytes, including cortisol, lactate, and the SARS-CoV-2 spike protein. Integration of Prussian blue nanoparticles enabled reagent-free detection, eliminating the need for solution-based redox probes and simplifying sensor architecture for field and wearable applications. Extension of eMIP fabrication to protein templates introduced optimized immobilization and elution strategies, addressing challenges associated with imprinting large, fragile biomolecules. Collectively, this work bridges the gap between proof-of-concept MIP studies and practical biosensor design. The results provide fundamental insight into how electrochemical parameters govern film growth and recognition site fidelity, while establishing design principles for stable, selective, and data-driven eMIP sensors. These contributions lay the groundwork for next-generation diagnostic systems that are reagent-free, reusable, and suitable for real-world deployment, advancing the long-term goal of accessible, point-of-care health monitoring technologies.
Creative Commons License
This work is licensed under a Creative Commons Attribution 4.0 License.
Recommended Citation
Dykstra, Grace L., "Engineering Electrochemical Molecularly Imprinted Polymers for Next-Generation Biosensing", Open Access Dissertation, Michigan Technological University, 2025.
Included in
Analytical, Diagnostic and Therapeutic Techniques and Equipment Commons, Biochemical and Biomolecular Engineering Commons, Biomedical Devices and Instrumentation Commons, Polymer Science Commons