Carbon dots are an
emerging family of zero-dimensional nanocarbons
behaving as tunable light harvesters and photoactivated charge donors.
Coupling them to carbon nanotubes, which are well-known electron acceptors
with excellent charge transport capabilities, is very promising for
several applications. Here, we first devised a route to achieve the
stable electrostatic binding of carbon dots to multi- or single-walled
carbon nanotubes, as confirmed by several experimental observations.
The photoluminescence of carbon dots is strongly quenched when they
contact either semiconductive or conductive nanotubes, indicating
a strong electronic coupling to both. Theoretical simulations predict
a favorable energy level alignment within these complexes, suggesting
a photoinduced electron transfer from dots to nanotubes, which is
a process of high functional interest. Femtosecond transient absorption
confirms indeed an ultrafast (<100 fs) electron transfer independent
of nanotubes being conductive or semiconductive in nature, followed
by a much slower back electron transfer (≈60 ps) from the nanotube
to the carbon dots. The high degree of charge separation and delocalization
achieved in these nanohybrids entails significant photocatalytic properties,
as we demonstrate by the reduction of silver ions in solution. The
results are very promising in view of using these “all-carbon”
nanohybrids as efficient light harvesters for applications in artificial
photocatalysis and photosynthesis.