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[Display omitted] • Fe single-atom adsorbents based on BNCO (Fe-BNCO) was synthesized. • Fe-BNCO-0.5 exhibits excellent adsortpin capacity for DBT (49.7 mg S/g). • Fe-doping results in a decrease of the crystallininty and a higher specific surface area. • The enhanced performance is sourced from the newly formed S-Fe coordination bond. Adsorbents with high adsorption capacity and selectivity have long been the pursuit of researchers in the field of adsorptive desulfurization. In this study, a novel single-atom adsorbent comprised of iron (Fe) integrated into C, O co-doped hexagonal boron nitride (Fe-BNCO) has been successfully synthesized. This unique material demonstrates outstanding adsorption capabilities, boasting an adsorption capacity of 49.7 mg S/g and excellent selectivity for adsorptive desulfurization. Notably, this adsorption capacity is 48.6 % higher than that of pure BNCO. The incorporation of the Fe element into boron nitride materials induces a reduction in crystallinity and an increase in specific surface area, resulting in a higher number of available adsorption sites. Combining experimental analysis with theoretical calculations, we propose that the exceptional adsorption performance of Fe-BNCO can be attributed to the formation of S-Fe coordination interaction, while maintaining the existing π-π interactions. This study advances our understanding of adsorbents with high adsorption capacity and selectivity, providing valuable insights for the field of adsorptive desulfurization. [ABSTRACT FROM AUTHOR]

The defective MoO 3 derived from Mo-based MOF was highly dispersed on nitrogen-doped porous carbon (V O -MoO 3 @NPC) by a single-step carbonization treatment. Notably, V O -MoO 3 @NPC realizes an extraordinary desulfurization efficiency of 99.1% within 20 min coupled with an exceedingly remarkable TOF of 96.2 h−1 owing to plentiful oxygen vacancies and effective electron transfer. [Display omitted] • V O -MoO 3 @NPC derived from Mo-MOF was prepared via an in situ annealing strategy. • Richer oxygen vacancies are formed due to the stronger metal-support interaction. • Incorporating nitrogen facilitates the electron transfer by shrinking the band gap. • V O -MoO 3 @NPC realizes an outstanding catalytic ODS activity of 99.1% within 20 min. • TOF can reach 96.2 h−1 by V O -MoO 3 @NPC but only 50.2 h−1 by V O -MoO 3 @PC. Electron transfer between supports and metal oxides is of great significance in optimizing the catalytic activity, while this is still an open issue for understanding its real role in the oxidative desulfurization (ODS) process. Herein, the defective molybdenum trioxide derived from molybdenum-based metal–organic frameworks was highly dispersed on nitrogen-doped porous carbon (V O -MoO 3 @NPC) by a single-step carbonization treatment. The uniform integration of organic moieties and the unique porous structure of carbonaceous materials are conductive to the active site exposure and mass transfer process during the ODS reaction. Meanwhile, richer oxygen vacancies are generated due to the weakened Mo-O bonds, which is pertinent to the promoted electron transfer between nitrogen-doped porous carbon and molybdenum trioxide by shrinking the band gap. The results manifest that the obtained V O -MoO 3 @NPC realizes an extraordinary desulfurization efficiency of 99.1% within 20 min, as well as a stable recyclability of up to 9 times. Furthermore, the catalyst delivers an extremely remarkable turnover frequency of 96.2 h−1, which is far superior to that of previously reported molybdenum-based catalysts. This manuscript provides new inspiration for designing excellent ODS catalysts by introducing electron-rich nitrogen to construct strong metal-support interactions. [ABSTRACT FROM AUTHOR]