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                            Library & Multimedia
 Superhydrophobic Surface Modification of Polymer Microneedles Enables Fabrication of Multimodal Surface-Enhanced Raman Spectroscopy and Mass Spectrometry Substrates for Synthetic Drug Detection in Blood Plasma
NCJ Number
              308283
Journal

*ACS Applied Materials & Interfaces* Volume: 15 Issue: 40 Dated: 2023 Pages: 46681-46696
Author(s)
          M. Vitoria Simas;
                        Philomena O. Olaniyan;
                        Sumon Hati;
                        Gregory A. Davis Jr.;
                        Gavin Anspach;
                        John V. Goodpaster;
                        Nicholas E. Manicke;
                        Rajesh Sardar
Date Published

2023
Length
              16 pages
Annotation
              This paper on superhydrophobic surface modification of polymer microneedles introduces a multimodal detection approach using highly versatile detection technology that can be applicable to the detection of any analyte type without performing any complicated sample preparation.
Abstract
              This article reports the fabrication of a nanoparticle (NP)-decorated microneedle substrate that is both a surface-enhanced Raman spectroscopy (SERS) substrate and a substrate-supported electrospray ionization (ssESI) mass spectrometry (MS) sample ionization platform. The authors believe that the multimodal detection approach presented herein is a highly versatile detection technology that can be applicable to the detection of any analyte type without performing any complicated sample preparation. Microneedles are widely used substrates for various chemical and biological sensing applications utilizing surface-enhanced Raman spectroscopy (SERS), which is indeed a highly sensitive and specific analytical approach. In this study, polymeric ligand-functionalized gold nanorods (Au NRs) are adsorbed onto superhydrophobic surface-modified polydimethylsiloxane (PDMS) microneedles through the control of various interfacial interactions. The authors show that the chain length of the polymer ligands dictates the NR adsorption process. Importantly, assembling Au NRs onto the micrometer-diameter needle tips allows the formation of highly concentrated electromagnetic hot spots, which provide the SERS enhancement factor as high as 1.0 × 106. The micrometer-sized area of the microneedle top and high electromagnetic field enhancement of this system can be loosely compared with tip-enhanced Raman spectroscopy, where the apex of a plasmonic NP-functionalized sharp probe produces high-intensity plasmonic hot spots. Utilizing NR-decorated microneedle substrates, the synthetic drugs fentanyl and alprazolam are analyzed with a subpicomolar limit of detection. Further analysis of drug-molecule interactions on the NR surface utilizing the Langmuir adsorption model suggests that the higher polarizability of fentanyl allows for a stronger interaction with hydrophilic polymer layers on the NR surface. The authors further demonstrate the translational aspect of the microneedle substrate for both SERS- and ssESI-MS-based detection of these two potent drugs in 10 drug-of-abuse (DOA) patient plasma samples with minimal preanalysis sample preparation steps. Chemometric analysis for the SERS-based detection shows a very good classification between fentanyl, alprazolam, or a mixture thereof in the selected 10 samples. Most importantly, ssESI-MS analysis also successfully identifies fentanyl or alprazolam in these same 10 DOA plasma samples. (Published Abstract Provided)
      
  
          Additional Details
Grant Number(s)
        2018-75-CX-0034


  
  
        
  Agencies
        NIJ-Sponsored


  
  
        
  Publication Type
        Research (Applied/Empirical)


  
  
        
  Award
        Development of Portable Surface-Enhanced Raman Spectroscopy Nanosensors for Ultrasensitive Characterization of Drugs in Human Biofluids
    
  
  
Date Published: January 1, 2023
    
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