Affiliation:
1. Institute for Innovative Materials and Energy School of Chemistry and Chemical Engineering Yangzhou University Yangzhou 225002 China
2. School of Materials and Technology Nanjing University of Aeronautics and Astronautics Nanjing 210016 China
3. School of Chemistry and Chemical Engineering Jiangsu University of Technology Changzhou 213001 China
4. School of Mathematical and Physical Sciences Faculty of Science University of Technology Sydney Sydney NSW 2007 Australia
Abstract
AbstractThe 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‐C3N4 (MIL101/CDs‐C3N4) 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 H2O2, leading to increased production of ROS (⋅O2−, ⋅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‐C3N4 exhibited the lowest activation energy for oxygen and H2O2. 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.