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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]

[Display omitted] • Graphdiyne-like boron nitride nanosheets were transformed into SAAs. • SAAs exhibit an enhanced adsorption capacity. • The CO 2 adsorption mechanism was evaluated in detail. • Charge transfer is the main factor in CO 2 adsorption. Developing an efficient adsorbent with optimal absorption capacity for carbon dioxide (CO 2) has always been a significant issue. Recently, single-atom adsorbents (SAAs) have been highlighted with special interest as a promising material with a wide range of applications. Nevertheless, comprehending the intricate mechanisms of gas adsorption on SAAs remains an enormous challenge. Herein, we have systematically evaluated the adsorption mechanisms over the transition metals (Fe, Co, Ni, Cu, and Zn) embedded onto the graphdiyne-like boron nitride monolayer using density functional theory calculations. Results show that SAAs exhibit a promoted capacity compared to the pristine graphdiyne-like boron nitride monolayer, mainly ascribed to the electron donation and back-donation mechanism between metal and CO 2. Further, BNene/Fe is favorable for CO 2 adsorption with the strongest interaction energy (−20.7 kcal mol−1). We hope this work will facilitate the design of SAAs in the field of gas adsorption. [ABSTRACT FROM AUTHOR]