Efficient Photocatalytic Desulfurization in Air through Improved Photogenerated Carriers Separation in MOF MIL101/Carbon Dots‐g‐C3N4 Nanocomposites

Abstract The extensive industrial applications of fuel oil, a critical strategic resource, are accompanied by significant environmental and health concerns due to the presence of sulfur‐containing compounds in its composition, which result in hazardous combustion waste. Extensive research has been conducted to develop technologies for low‐vulcanization fuel production to address this issue. Consequently, the investigation of catalysts for environmentally friendly and safe photocatalytic desulfurization becomes imperative. To that end, we have designed efficient MIL‐101(Fe)/CQDs@g‐C 3 N 4 (MIL101/CDs‐C 3 N 4 ) Z‐scheme heterojunction photocatalysts with high carrier separation and mobility through a thermal polymerization‐hydrothermal strategy. The high concentration of photogenerated carriers facilitates the activation of oxygen and H 2 O 2 , leading to increased production of ROS (⋅O 2 − , ⋅OH, h + ), thereby enhancing the photocatalytic desulfurization (PODS). Additionally, DFT (Density functional theory) calculations were utilized to determine the electron migration pathways of the catalysts and adsorption energies of DBT (dibenzothiophene). Moreover, Gibbs free energy calculations indicated that MIL101/CDs‐C 3 N 4 exhibited the lowest activation energy for oxygen and H 2 O 2 . The mechanism of photocatalytic desulfurization was proposed through a combination of theoretical calculations and experimental studies. This study provides guidance for the development of MOF‐based Z‐scheme systems and their practical application in desulfurization processes.