Design, Development, and Characterization of Electroanalytical Biosensing Devices Based on Two- and Three-Dimensional Material Systems

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- Author:
- Butler, Derrick
- Graduate Program:
- Electrical Engineering
- Degree:
- Doctor of Philosophy
- Document Type:
- Dissertation
- Date of Defense:
- August 31, 2022
- Committee Members:
- Noel Giebink, Major Field Member
Seyedehaida Ebrahimi, Chair & Dissertation Advisor
Joshua Robinson, Outside Unit & Field Member
Weihua Guan, Major Field Member
Thomas F La Porta, Program Head/Chair
Morteza Kayyalha, Major Field Member - Keywords:
- Biosensor
Electrochemical
Electrical
Point-of-care
2D Material
3D Material
Bacteria
Dopamine - Abstract:
- A growing global population and lack of widespread universal healthcare coverage, especially in resource-limited and rural regions, has motivated the development of low-cost, portable biodevices for point-of-care (POC) applications. The omnipresent COVID-19 pandemic is one example that has brought to light the importance of decentralized, rapid, and accurate testing strategies for the screening of communicable, as well as non-communicable, diseases. These strategies help fill the technological, economical, and logistical gaps associated with more traditional testing methods, which are not necessarily suitable for POC analysis. On the other hand, electroanalytical devices, such as electrochemical and electronic biosensors, are becoming increasingly suitable for POC testing, as they have the potential to meet most, if not all, of the requirements outlined by the World Health Organization’s ASSURED criterion. Working to address these needs, this dissertation experimentally and computationally explores various two- and three-dimensional materials and device architectures for biosensing applications. Using a range of preparation, fabrication, and modification methods, including doping, annealing, plasma treatment, and functionalization with immunoreceptors, a selection of small molecules, including dopamine, pyocyanin, and nitric oxide, and microbes, such as bacteria and viruses, are targeted, given the implications in both communicable and non-communicable diseases. The first four chapters discuss work that utilizes two-dimensional materials as the active transduction element. As model two-dimensional materials, graphene and MoS2 are prepared using scalable methods, including electrodeposition and laser-printing, on substrates ranging from SiO2 to paper. The remaining two chapters describe examples of biosensors based on three-dimensional microelectrodes for detection and monitoring of microbial organisms. Leveraging these various materials, a range of device engineering and fabrication strategies, including interdigitated microelectrode arrays, printable all on-chip electrochemical sensors, and template-driven ’overgrown’ microelectrodes, are explored. In general, the sensors are first tested in simple buffer solutions before employing them in more complex testing environments, such as biological matrices (e.g. sweat, serum) or for ex situ/in situ analyses with bacterial or mammalian cells. Overall, this work highlights the aptitude of two- and three-dimensional materials and device engineering strategies for use in next-generation POC analytical devices. Combined with advancements in controllable two-dimensional material synthesis techniques and microfluidics for sample transport, sensitive, robust, and portable POC devices based on two- and three-dimensional materials are envisioned for rapid wellness screening and real-time health monitoring.
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