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Sheath-flow microfluidic approach fo...
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Bailey, Matthew R.
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Sheath-flow microfluidic approach for combined surface enhanced Raman scattering and electrochemical detection.
Record Type:
Electronic resources : Monograph/item
Title/Author:
Sheath-flow microfluidic approach for combined surface enhanced Raman scattering and electrochemical detection./
Author:
Bailey, Matthew R.
Published:
Ann Arbor : ProQuest Dissertations & Theses, : 2016,
Description:
185 p.
Notes:
Source: Dissertation Abstracts International, Volume: 78-07(E), Section: B.
Contained By:
Dissertation Abstracts International78-07B(E).
Subject:
Analytical chemistry. -
Online resource:
http://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=10308103
ISBN:
9781369540468
Sheath-flow microfluidic approach for combined surface enhanced Raman scattering and electrochemical detection.
Bailey, Matthew R.
Sheath-flow microfluidic approach for combined surface enhanced Raman scattering and electrochemical detection.
- Ann Arbor : ProQuest Dissertations & Theses, 2016 - 185 p.
Source: Dissertation Abstracts International, Volume: 78-07(E), Section: B.
Thesis (Ph.D.)--University of Notre Dame, 2016.
This dissertation focuses on the development of a unique microfluidic approach, using hydrodynamic focusing, to enable both surface enhanced Raman scattering (SERS) and electrochemical characterization of analytes at nanomolar concentration in flow. The approach utilizes a versatile polystyrene chip that contains an encapsulated microelectrode and fluidic tubing with a polydimethylsiloxane (PDMS) microchannel positioned over both to generate a sheath-flow that confines and increase the interaction between the analyte and the surface to improve detection. The microfluidic device was characterized using finite element simulations, amperometry, and Raman experiments. An examination of riboflavin (vitamin B12) and catechol demonstrated a SERS and amperometric detection limit near 1 and 25 nM, respectively. This combination of SERS and amperometry in a single device provides an improved method to identify and quantify electroactive analytes over either technique independently.
ISBN: 9781369540468Subjects--Topical Terms:
3168300
Analytical chemistry.
Sheath-flow microfluidic approach for combined surface enhanced Raman scattering and electrochemical detection.
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Source: Dissertation Abstracts International, Volume: 78-07(E), Section: B.
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Adviser: Zachary D. Schultz.
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Thesis (Ph.D.)--University of Notre Dame, 2016.
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This dissertation focuses on the development of a unique microfluidic approach, using hydrodynamic focusing, to enable both surface enhanced Raman scattering (SERS) and electrochemical characterization of analytes at nanomolar concentration in flow. The approach utilizes a versatile polystyrene chip that contains an encapsulated microelectrode and fluidic tubing with a polydimethylsiloxane (PDMS) microchannel positioned over both to generate a sheath-flow that confines and increase the interaction between the analyte and the surface to improve detection. The microfluidic device was characterized using finite element simulations, amperometry, and Raman experiments. An examination of riboflavin (vitamin B12) and catechol demonstrated a SERS and amperometric detection limit near 1 and 25 nM, respectively. This combination of SERS and amperometry in a single device provides an improved method to identify and quantify electroactive analytes over either technique independently.
520
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The importance of adsorption to the SERS electrode was evident in the previous experiments. By performing Raman and electrochemical measurements on a series of neurotransmitters we were able to correlate surface chemistry with the measured SERS signal and examine the oxidation mechanism of each analyte. Finite element simulations were used to expand on the experiments and explain the differences observed in integrated current during amperometry and signal intensities in SERS measurements. The results indicate that the molecular structure influences the binding affinity and in turn the SERS efficiency. Overall, these results illustrate the importance of surface adsorption for the in situ characterization of molecules.
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The developed platform gives us the ability to do combined SERS and electrochemical experiments on the millisecond time scale to gain complimentary information about analytes. Using these capabilities we examined the reduction and oxidation of riboflavin. We were able to correlate reversible changes in spectral features to the current changes observed in the cyclic voltammetry. Multivariate curve resolution analysis of the SERS spectra and density functional theory calculations were used to verify and better understand the results, which indicates the presence of the oxidized, semi-quinone, and reduced forms of riboflavin.
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http://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=10308103
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