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Area of Science:

  • Nanotechnology
  • Biomedical Engineering
  • Materials Science

Background:

  • Semiconducting single-wall carbon nanotubes (SWCNTs) exhibit near-infrared (NIR) fluorescence dependent on their chirality, forming the basis for fluorescent biosensors.
  • Current biosensors often use mixed SWCNT chiralities, leading to spectral overlap that compromises sensitivity, selectivity, and multiplexing capabilities.
  • A significant challenge has been integrating SWCNT purification with generic biofunctionalization for chirality-pure sensor development.

Purpose of the Study:

  • To develop chirality-pure SWCNT-based NIR fluorescent biosensors for analytes such as neurotransmitters.
  • To investigate the influence of SWCNT chirality, handedness, long-term stability, and sensitivity.
  • To enable ratiometric/multiplexed sensing by combining multiple monochiral SWCNTs.

Main Methods:

  • Aqueous two-phase extraction (ATPE) was employed to isolate chirality-pure SWCNTs ((6,5), (7,5), (9,4), and (7,6)).
  • Surfactant (sodium deoxycholate) was exchanged with single-stranded DNA (ssDNA) sequences to create monochiral sensors.
  • Thorough removal of residual surfactant was performed to enhance sensor performance.

Main Results:

  • Chirality-pure SWCNTs were successfully isolated and functionalized with ssDNA to create monochiral sensors for dopamine, riboflavin, ascorbic acid, and pH.
  • Monochiral (6,5)-SWCNT sensors demonstrated up to 10-fold increased brightness compared to unpurified counterparts.
  • (GT)40-(6,5)-SWCNTs showed a significant fluorescence response to dopamine (+140%) with high affinity (Kd = 1.9 × 10⁻⁷ M) and >14 days stability.
  • ssDNA functionalization dictated analyte selectivity, largely independent of SWCNT chirality and handedness, enabling predictable sensor design.
  • Multiplexed sensing of dopamine, riboflavin, H2O2, and pH was achieved using combinations of different monochiral SWCNTs.

Conclusions:

  • Chirality-pure SWCNT-based NIR fluorescent biosensors were successfully assembled and characterized.
  • The developed sensors offer enhanced sensitivity, selectivity, and long-term stability for various analytes.
  • This work paves the way for advanced multiplexed sensing applications using single-color SWCNTs.