pH-Dependent Synthesis of Novel Structure-Controllable Polymer-Carbon NanoDots with High Acidophilic Luminescence and Super Carbon Dots Assembly for White Light-Emitting Diodes

We use a pH-dependent solubility equilibrium to develop a one-pot aqueous synthesis of polymer carbon nanodots with novel structures. The chemical structure and photoluminescence (PL) were heavily influenced by the synthesis pH, with cross-linked polymer-carbon film (pH > 7), polymer carbon nanosheets (3 < pH < 7), and amorphous carbon structures (1 < pH < 3) achieved by altering the initial pH. Although pH-dependent structures frequently occur in typical semiconductors and supramolecular architectures involving metal, this is the first experimental work describing it in carbon nanodots. Supersmall carbon nanodots (SCNDs, similar to 0.5 nm) were obtained at pH < 1; their direct white emission can be easily applied as an inexpensive color-changing layer in white LEDs. Investigation of the PL mechanism of the SCNDs revealed an uncommon multilevel highly emissive recombination channel, which could be possibly derived from the wide distributions of surface-state PL centers. Theoretical calculation of the single layer of the carbon dots further explored their band gap changes.