Boosted Photoelectrochemical Water Oxidation Performance with a Quaternary Heterostructure: CoFe2O4/MWCNT-Doped MIL-100(Fe)/TiO2

Cobalt ferrite (CoFe2O4) combined with multi-walled carbon nanotubes (MWCNTs) is an outstanding material regarding photoelectrochemical water oxidation (PEC-WO) because of its excellent catalytic properties and stability. On the other hand, surface imperfections in CoFe2O4 can cause band bending and surface Fermi level pinning, significantly reducing its PEC conversion efficiency. Heterostructure engineering is essential for achieving increased light-gathering capacity and charge separation efficiency for PEC-WO. In this study, a quaternary heterostructure of CoFe2O4/MWCNT-doped Metal–Organic Framework-100 (Iron), MIL-100(Fe)/Titanium Oxide (TiO2) was synthesized by using a combination of hydrothermal, solvothermal, and “dip and dry” techniques. Characterization results confirmed the formation of a structural network of MIL-100(Fe) on TiO2 surfaces, enhanced by the incorporation of MWCNTs during the hydrothermal reaction. Under 1 sun irradiation, the resultant quaternary heterostructure displayed a photocurrent density (Jph) of 3.70 mA cm−2 under free bias voltage, which is around 3.08 times more than that of pristine TiO2 photoanodes (Jph = 1.20 mA cm−2). This investigation highlights the advantages of the MIL-100(Fe) network in improving the solar PEC-WO performance of TiO2 photoanodes.