The possibility of converting waste plastics into carbon
dots (CDs)
with 100% efficiencies using KMnO4 has emerged as a significant
discovery in mitigating plastic pollution and upcycling. However,
the lack of tunability of their properties, viz. aerial O2 harvesting, light-induced autophagy, and photoactivity using air
as a free oxidant, has remained a bottleneck. Besides, the toxicity
of KMnO4 makes the process less sustainable. Attempting
to bridge these gaps, herein, we demonstrate the preparation of CDs
using polyethylene with enormous controllability of their properties
by utilizing less-toxic and metal-residue-free oxidizers, e.g., H2O2, HNO3, HClO4, and NaClO.
We obtain structurally diverse CDs with controllable luminescent quantum
yields (∼0.5–8%), excitonic lifetimes (1.3–2.3
ns), and binding energies (147–290 meV). These CDs exhibit
a hugely extended range of molecular O2 harvesting (∼405–650
μM) with different amounts of strongly and weakly surface-bound
O2 molecules within an estimated ratio of ∼0.77–2.51.
Autophagy varied from 14 days to a nearly “no-autophagy”
show. We efficiently utilized their oxygen harvesting and photocatalytic
abilities to synthesize imine compounds from the corresponding amines
in the open air (rate constant of ∼0.055 min–1), surpassing the literature efficiencies achieved using an O2 flow and noble metals. Notably, due to oxygen harvesting
by CDs, no additional rate enhancement was observed after O2 purging, establishing the role of CDs in making free air an excellent
oxidizing agent.