Evaluating carbon dots as electron mediators in photochemical and photocatalytic processes of NiFe2O4

Abstract

Spinel ferrites such as nickel ferrite are promising energy conversion photocatalysts as they are visible-light absorbers, chemically stable, earth abundant, and inexpensive. Nickel ferrite shows poor photocatalytic activity due to fast electron-hole recombination upon illumination. This study evaluates the capability of carbon dots (CDs) to improve charge-carrier separation in NiFe2O4. We report a facile solvothermal approach for synthesizing NiFe2O4 and CDs/NiFe2O4 nanoparticles at 200-215 °C. The photocatalysts were characterized using transmission and scanning electron microscopy, x-ray diffraction, Raman spectroscopy, Fourier transform infrared spectroscopy, UV-VIS-NIR spectroscopy, photoelectrochemical analysis, and laser flash photolysis. Photocatalytic oxidation of methanol to formaldehyde under visible light was employed to test the effect of CDs on the photocatalytic efficacy of NiFe2O4. UV-VIS-NIR spectroscopy depicted a total quenching of NIR absorption and a diminished absorption of a peak at ∼745 nm in CDs/NiFe2O4 compared with NiFe2O4, indicating a transfer of electrons from NiFe2O4 to CDs. A 12-fold increment in the incident-photon-to-charge-efficiency was achievable with CDs/NiFe2O4 (0.36%) compared with NiFe2O4 (0.03%). Impedance spectroscopy exhibited a more efficient charge separation and faster interfacial charge transfer in CDs/NiFe2O4 compared with pure NiFe2O4. This was accounted for by the lower initial quantity of charge carrier upon irradiation in CDs/NiFe2O4 compared with NiFe2O4 as detected from laser flash photolysis, indicating that CDs acted as electron acceptors and reservoirs in CDs/NiFe2O4. Compared with NiFe2O4, CDs/NiFe2O4 showed an enhanced photocatalytic activity toward formaldehyde formation. Consequently, CDs are good electron mediators for NiFe2O4, capable of improving charge-carrier separation and the photocatalytic activity of NiFe2O4.