The powerful combination of 2D/2D Ni-MOF/carbon nitride for deep desulfurization of thiophene in fuel: Conversion route, DFT calculation, mechanism.

2D/2D Ni-MOF/g-C 3 N 4 nanocomposite was utilized for desulfurization. The multilayer pore structure and high specific surface area of Ni-MOF/g-C 3 N 4 promote the adsorption and conversion of thiophene. The Ni-MOF and g-C 3 N 4 construct a Z-scheme heterojunction structure with tight contact, it effectively enhances the material's photocatalytic redox ability. [Display omitted] • Highly efficient 2D/2D Ni-MOF/g-C 3 N 4 Z-scheme heterojunction photocatalysts were prepared. • The PODS system was constructed using O 2 from the air and H 2 O as the oxidant. • When utilizing 1–4-Ni-MOF/g-C 3 N 4 as a catalyst, the thiophene conversion reached 98.82 % within 3 h. • The PODS mechanism for was thiophene proposed based on DFT calculations and experimental studies. 2D/2D Ni-MOF/g-C 3 N 4 nanocomposite was utilized for desulfurization. The multilayer pore structure and high specific surface area of Ni-MOF/g-C 3 N 4 promote the adsorption and conversion of thiophene. In addition, the two-dimensional structure exposes more active centers and shortens photogenerated carrier migration to the material surface distance, it enhances photogenerated charge transfer. The Ni-MOF and g-C 3 N 4 construct a Z-scheme heterojunction structure with tight contact, it effectively enhances the material's photocatalytic redox ability. In the light, the material generates more photocarriers for the production of free radicals including hydroxyl radicals, holes, and superoxide radicals. The higher carrier concentration of Ni-MOF/g-C 3 N 4 promotes the activation and oxidation of thiophene, consequently enhancing the photocatalytic desulfurization capability. The results showed that the conversion of thiophene was 98.82 % in 3 h under visible light irradiation. Radical capture experiments and analysis using electron paramagnetic resonance spectroscopy demonstrated that superoxide radicals, holes, and hydroxyl radicals played crucial roles in PODS (photocatalytic oxidative desulfurization). In addition, DFT (density functional theory) calculations were conducted to determine the paths of electron migration and TH (thiophene) adsorption energy. Finally, a mechanism for photocatalytic desulfurization was proposed based on the comprehensive analysis of theoretical calculations and experimental studies. [ABSTRACT FROM AUTHOR]