Red-emitting
carbon dots (CDs) have attracted tremendous attention
due to their wide applications in areas including imaging, sensing,
drug delivery, and cancer therapy. However, it is still highly challenging
for red-emitting CDs to simultaneously achieve high quantum yields
(QYs), nucleus targeting, and super-resolution fluorescence imaging
(especially the stimulated emission depletion (STED) imaging). Here,
it is found that the addition of varied metal ions during the hydrothermal
treatment of p-phenylenediamine (pPDA) leads to the
formation of fluorescent CDs with emission wavelengths up
to 700 nm. Strikingly, although metal ions play a crucial role in
the synthesis of CDs with varied QYs, they are absent in the formed
CDs, that is, the obtained CDs are metal-free, and the metal ions
play a role similar to a “catalyst” during the CD formation.
Besides, using pPDA and nickel ions (Ni2+) as raw materials,
we prepare Ni–pPCDs which have the highest QY and exhibit various
excellent fluorescence properties including excitation-independent
emission (at ∼605 nm), good photostability, polarity sensitivity,
and ribonucleic acid responsiveness. In vitro and in vivo experiments
demonstrate that Ni–pPCDs are highly biocompatible and can
realize real-time, wash-free, and high-resolution imaging of cell
nuclei and high-contrast imaging of tumor-bearing mice and zebrafish.
In summary, the present work may hold great promise in the synthesis
and applications of red emissive CDs.