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Molecular Recognition Materials Synthesized Based on Small molecules, DNA, and Imprinted Polymers for Bioanalytical Applications

Xue, Xiaoting LU (2023)
Abstract
The development of sensitive, convenient, and cost-effective methods for detecting disease biomarkers is very important for meeting the growing demand for early clinical diagnosis. Additionally, the detection of disease biomarkers at ultralow concentrations is very important for disease prevention and treatment and posttreatment rehabilitation. However, current ultrasensitive detection strategies often require sophisticated instruments or complex sample pretreatments that may not be available in laboratories that have limited resources. Therefore, we focused on assembling various inorganic and organic building blocks to synthesize integrated multifunctional materials and improve the performance of analytical systems and... (More)
The development of sensitive, convenient, and cost-effective methods for detecting disease biomarkers is very important for meeting the growing demand for early clinical diagnosis. Additionally, the detection of disease biomarkers at ultralow concentrations is very important for disease prevention and treatment and posttreatment rehabilitation. However, current ultrasensitive detection strategies often require sophisticated instruments or complex sample pretreatments that may not be available in laboratories that have limited resources. Therefore, we focused on assembling various inorganic and organic building blocks to synthesize integrated multifunctional materials and improve the performance of analytical systems and methods.
Boronic acid (BA), which is a small synthetic molecule, was conjugated in nanopores of dendritic fibrous nanosilica (DFNS) through a high-efficiency click reaction and a temperature-responsive polymer intermediate. The developed boronate affinity materials provide more affinity sites for cis-diol enrichment, and the well-defined narrow pores of DFNS provide highly selective affinity binding toward low-molecular-weight cis-diols. Moreover, a BA derivative, 4-vinylphenylboronic acid (VPBA), was employed to develop a fluorescence technique for monitoring molecular imprinting in real time and gaining insights into molecular recognition mechanisms. Molecularly imprinted polymers (MIPs) were synthesized using Alizarin Red S (ARS) as the template and VPBA as the functional monomer. The fluorogenic VPBA–ARS complex enables molecular imprinting signaling. The resulting MIPs also exhibited specific binding toward ARS and served as a fluorescent probe for detecting Cu2+ ions without any tedious sample preparation.
Fluorescein-labeled single-stranded nucleic acid was directly adsorbed on polydopamine-functionalized DFNS to develop a “turn-on” fluorescence biosensor, which functions using an adsorption–quenching–recovery mechanism that enables the simple and highly efficient detection of nucleic acid biomarkers. A proof of concept was demonstrated using microRNA as a biomarker model.
Nucleic acid amplification and MIPs were employed to achieve the low-cost, simple, and reliable detection and quantification of protein biomarkers. MIPs were prepared using Pickering emulsion polymerization and DFNS as a stabilizer to produce surface-accessible binding sites for protein biomarkers. The MIP-induced protein recognition was amplified by the hybridization chain reaction and translated into an easily detectable fluorescence signal. (Less)
Please use this url to cite or link to this publication:
author
supervisor
opponent
  • Prof. Cormack, Peter, University of Strathclyde, United Kingdom.
organization
publishing date
type
Thesis
publication status
published
subject
keywords
detection, molecularly imprinted polymers, boronic acid, DNA, dendritic fibrous nanosilica
publisher
Department of Chemistry, Lund University
defense location
Lecture Hall KC:B, Kemicentrum, Naturvetarvägen 14, Faculty of Engineering LTH, Lund University, Lund
defense date
2023-12-12 09:00:00
ISBN
978-91-8096-003-8
978-91-8096-002-1
language
English
LU publication?
yes
id
29bf2a3c-d622-4533-8edd-ea438f59e2a0
date added to LUP
2023-11-13 21:41:57
date last changed
2023-11-16 10:39:49
@phdthesis{29bf2a3c-d622-4533-8edd-ea438f59e2a0,
  abstract     = {{The development of sensitive, convenient, and cost-effective methods for detecting disease biomarkers is very important for meeting the growing demand for early clinical diagnosis. Additionally, the detection of disease biomarkers at ultralow concentrations is very important for disease prevention and treatment and posttreatment rehabilitation. However, current ultrasensitive detection strategies often require sophisticated instruments or complex sample pretreatments that may not be available in laboratories that have limited resources. Therefore, we focused on assembling various inorganic and organic building blocks to synthesize integrated multifunctional materials and improve the performance of analytical systems and methods.<br/>Boronic acid (BA), which is a small synthetic molecule, was conjugated in nanopores of dendritic fibrous nanosilica (DFNS) through a high-efficiency click reaction and a temperature-responsive polymer intermediate. The developed boronate affinity materials provide more affinity sites for cis-diol enrichment, and the well-defined narrow pores of DFNS provide highly selective affinity binding toward low-molecular-weight cis-diols. Moreover, a BA derivative, 4-vinylphenylboronic acid (VPBA), was employed to develop a fluorescence technique for monitoring molecular imprinting in real time and gaining insights into molecular recognition mechanisms. Molecularly imprinted polymers (MIPs) were synthesized using Alizarin Red S (ARS) as the template and VPBA as the functional monomer. The fluorogenic VPBA–ARS complex enables molecular imprinting signaling. The resulting MIPs also exhibited specific binding toward ARS and served as a fluorescent probe for detecting Cu2+ ions without any tedious sample preparation.<br/>Fluorescein-labeled single-stranded nucleic acid was directly adsorbed on polydopamine-functionalized DFNS to develop a “turn-on” fluorescence biosensor, which functions using an adsorption–quenching–recovery mechanism that enables the simple and highly efficient detection of nucleic acid biomarkers. A proof of concept was demonstrated using microRNA as a biomarker model.<br/>Nucleic acid amplification and MIPs were employed to achieve the low-cost, simple, and reliable detection and quantification of protein biomarkers. MIPs were prepared using Pickering emulsion polymerization and DFNS as a stabilizer to produce surface-accessible binding sites for protein biomarkers. The MIP-induced protein recognition was amplified by the hybridization chain reaction and translated into an easily detectable fluorescence signal.}},
  author       = {{Xue, Xiaoting}},
  isbn         = {{978-91-8096-003-8}},
  keywords     = {{detection, molecularly imprinted polymers, boronic acid, DNA, dendritic fibrous nanosilica}},
  language     = {{eng}},
  publisher    = {{Department of Chemistry, Lund University}},
  school       = {{Lund University}},
  title        = {{Molecular Recognition Materials Synthesized Based on Small molecules, DNA, and Imprinted Polymers for Bioanalytical Applications}},
  url          = {{https://lup.lub.lu.se/search/files/164919515/Xiaoting_Xue_-_WEBB.pdf}},
  year         = {{2023}},
}