Journal
ACS NANO
Volume 14, Issue 2, Pages 2542-2552Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsnano.0c00515
Keywords
surface-enhanced Raman spectroscopy (SERS); superhydrophobic SERS platform; chemometrics; metaboloinics; urine-based diagnostic test
Categories
Funding
- Singapore Ministry of Education, Tier 1 [RGI1/18]
- Singapore Ministry of Education, Tier 2 [MOE2016-T2-1043]
- Max Planck Institute-Nanyang Technological University Joint Lab
- Ministry of Health Singapore Industry Alignment Fund grant [MOHIAFCat1-11010]
- A*STAR, Singapore
- Nanyang Technological University, Singapore
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Successful translation of laboratory-based surface-enhanced Raman scattering (SERS) platforms to clinical applications requires multiplex and ultratrace detection of small biomarker molecules from a complex biofluid. However, these biomarker molecules generally exhibit low Raman scattering cross sections and do not possess specific affinity to plasmonic nanoparticle surfaces, significantly increasing the challenge of detecting them at low concentrations. Herein, we demonstrate a confine-and-capture approach for multiplex detection of two families of urine metabolites correlated with miscarriage risks, 5 beta-pregnane-3 alpha,20 alpha-diol-3 alpha-glucuronide and tetrahydrocorti- sone. To enhance SERS signals by 10(12)-fold, we use specific nanoscale surface chemistry for targeted metabolite capture from a complex urine matrix prior to confining them on a superhydrophobic SERS platform. We then apply chemometrics, including principal component analysis and partial least-squares regression, to convert molecular fingerprint information into quantifiable readouts. The whole screening procedure requires only 30 min, including urine pretreatment, sample drying on the SERS platform, SERS measurements, and chemometric analyses. These readouts correlate well with the pregnancy outcomes in a case-control study of 40 patients presenting threatened miscarriage symptoms.
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