Rational Design of Surface-State Controlled Multicolor Cross-Linked Carbon Dots with Distinct Photoluminescence and Cellular Uptake Properties

ACS Appl Mater Interfaces. 2021 Dec 22;13(50):59747-59760. doi: 10.1021/acsami.1c19995. Epub 2021 Dec 8.

Abstract

We disclose for the first time a facile synthetic methodology for the preparation of multicolor carbon dots (CDs) from a single source barring any chromatographic separations. This was achieved via sequential intraparticle cross-linking of surface abundant carboxylic acid groups on the CDs synthesized from a precursor to control their photoluminescence (PL) spectra as well as affect their degree of cellular internalization in cancer cells. The change in PL spectra with sequential cross-linking was projected by theoretical density functional theory (DFT) studies and validated by multiple characterization tools such as X-ray photoelectron spectroscopy (XPS), PL spectroscopy, ninhydrin assay, etc. The variation in cellular internalization of these cross-linked CDs was demonstrated using inhibitor assays, confocal microscopy, and flow cytometry. We supplemented our findings with high-resolution dark-field imaging to visualize and confirm the colocalization of these CDs into distinct intracellular compartments. Finally, to prove the surface-state controlled PL mechanisms of these cross-linked CDs, we fabricated a triple-channel sensor array for the identification of different analytes including metal ions and biologically relevant proteins.

Keywords: carbon dots; cellular uptake; cross-linking; hyperspectral dark-field microscopy; luminescence; multichannel sensor array.

MeSH terms

  • Biocompatible Materials / chemistry
  • Biocompatible Materials / pharmacokinetics*
  • Carbon / chemistry
  • Carbon / pharmacokinetics*
  • Cell Line, Tumor
  • Cross-Linking Reagents / chemistry
  • Cross-Linking Reagents / pharmacokinetics*
  • Density Functional Theory
  • Fluorescent Dyes / chemistry
  • Fluorescent Dyes / pharmacokinetics*
  • Humans
  • Luminescence*
  • Materials Testing
  • Molecular Structure
  • Optical Imaging
  • Photochemical Processes
  • Photoelectron Spectroscopy
  • Quantum Dots / chemistry*
  • Surface Properties

Substances

  • Biocompatible Materials
  • Cross-Linking Reagents
  • Fluorescent Dyes
  • Carbon