4.8 Article

Divalent Metal Cation Optical Sensing Using Single-Walled Carbon Nanotube Corona Phase Molecular Recognition

Journal

ANALYTICAL CHEMISTRY
Volume 94, Issue 47, Pages 16393-16401

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acs.analchem.2c03648

Keywords

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Funding

  1. Walmart Foundation
  2. Walmart Food Safety Collaboration Center in Beijing
  3. NSF Biosensing Program [2124194]
  4. Disruptive & Sustainable Technology for Agricultural Precision (DiSTAP) of the Singapore MIT Alliance for Research and Technology (SMART) Center
  5. Directorate For Engineering
  6. Div Of Chem, Bioeng, Env, & Transp Sys [2124194] Funding Source: National Science Foundation

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Colloidal single-walled carbon nanotubes offer a promising platform for molecular recognition at the nanoscale. By modifying the noncovalent corona phases of the nanotubes, optical sensors can be designed through a phenomenon known as corona phase molecular recognition. In this study, the interactions between dilute divalent metal cations and DNA corona phases were explored, leading to improved experimental conditions for sensing metal ions and the detection of nanomolar levels of mercury ions in fish tissue extract.
Colloidal single-walled carbon nanotubes (SWCNTs) offer a promising platform for the nanoscale engineering of molecular recognition. Optical sensors have been recently designed through the modification of noncovalent corona phases (CPs) of SWCNTs through a phenomenon known as corona phase molecular recognition (CoPhMoRe). In CoPhMoRe constructs, DNA CPs are of great interest due to the breadth of the design space and our ability to control these molecules with sequence specificity at scale. Utilizing these constructs for metal ion sensing is a natural extension of this technology due to DNA's well-known coordination chemistry. Additionally, understanding metal ion interactions of these constructs allows for improved sensor design for use in complex aqueous environments. In this work, we study the interactions between a panel of 9 dilute divalent metal cations and 35 DNA CPs under the most controlled experimental conditions for SWCNT optical sensing to date. We found that best practices for the study of colloidal SWCNT analyte responses involve mitigating the effects of ionic strength, dilution kinetics, laser power, and analyte response kinetics. We also discover that SWCNT with DNA CPs generally offers two unique sensing states at pH 6 and 8. The combined set of sensors in this work allowed for the differentiation of Hg2+, Pb2+, Cr2+, and Mn2+. Finally, we implemented Hg2+ sensing in the context of portable detection within fish tissue extract, demonstrating nanomolar level detection.

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