Jang, Kyeongwoo
(2023)
Development of Two-Dimensional Photonic Crystal Hydrogel Sensors for Biomolecular Detection.
Doctoral Dissertation, University of Pittsburgh.
(Unpublished)
Abstract
The work reported in this dissertation discusses the recent advancements in the development of 2DPC hydrogel sensors for biomolecular detection. The 2DPC hydrogel sensors are fabricated by incorporating 2DPC into responsive hydrogels. Each hydrogel sensor is functionalized with specific recognition groups that interact with the desired target, causing the hydrogel to undergo volume phase transitions (VPTs). We measure the target-induced hydrogel VPTs by monitoring the 2DPC light diffraction and report the analyte concentrations. This sensing platform is simple, does not require sophisticated instrumentation, and could be used in resource-limited environments and point-of-care testing.
We demonstrated the use of oxyamine recognition groups for the detection of phenylpyruvate, an enzymatic reaction product between phenylalanine and phenylalanine dehydrogenase. The chemoselective oxime reaction between the hydrogel oxyamines and phenylpyruvate covalently modifies the hydrogel structure and induces the hydrogel VPTs. This 2DPC hydrogel sensor could be further used to develop a phenylalanine sensor for patients with phenylketonuria and to develop a lactate sensor to evaluate the development of sepsis.
We also developed two other mechanisms for small molecule detection utilizing DNA aptamers as molecular recognition groups. Upon binding targets, the DNA aptamers that are attached to the hydrogel network undergo conformational changes, triggering the hydrogel VPTs. We hypothesize that this sensing motif is generalizable and that other sensors can be easily fabricated by simply exchanging the aptamer recognition group. We plan to continue to develop this sensing platform for the detection of other small molecules and proteins of interest.
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Details
| Item Type: |
University of Pittsburgh ETD
|
| Status: |
Unpublished |
| Creators/Authors: |
|
| ETD Committee: |
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| Date: |
25 January 2023 |
| Date Type: |
Publication |
| Defense Date: |
28 September 2022 |
| Approval Date: |
25 January 2023 |
| Submission Date: |
30 September 2022 |
| Access Restriction: |
No restriction; Release the ETD for access worldwide immediately. |
| Number of Pages: |
161 |
| Institution: |
University of Pittsburgh |
| Schools and Programs: |
Dietrich School of Arts and Sciences > Chemistry |
| Degree: |
PhD - Doctor of Philosophy |
| Thesis Type: |
Doctoral Dissertation |
| Refereed: |
Yes |
| Uncontrolled Keywords: |
photonic crystal, hydrogel, responsive polymer, molecular recognition group, phenylpyruvate, aptamer, adenosine |
| Date Deposited: |
25 Jan 2023 20:12 |
| Last Modified: |
25 Jan 2023 20:12 |
| URI: |
http://d-scholarship.pitt.edu/id/eprint/43720 |
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