4.7 Article

An ultra-stable high entropy metal nitride for aerobic oxidative desulfurization and source recovery of aromatic sulfides from fuel oils

Journal

CHEMICAL ENGINEERING JOURNAL
Volume 474, Issue -, Pages -

Publisher

ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2023.145850

Keywords

Oxidative desulfurization; Source recovery; Fuel oils; High entropy metal nitride; Acid resistance

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In this study, a high entropy metal nitride (HEN) was designed using a soft-urea-assisted strategy, and it showed excellent activity and stability in the oxidative desulfurization (ODS) reaction. This research contributes to the development of new catalysts with high catalytic activity and excellent stability.
High entropy metal materials, such as high entropy metal oxides (HEOs), have shown remarkable performances in catalytic oxidation processes, such as aerobic oxidative desulfurization (ODS). Nevertheless, HEOs struggle from instability during the ODS due to the existence of acidic constituents in fuel oils. Herein, a high entropy metal nitride (HEN) was designed by a soft-urea-assisted strategy, and its structure was carefully characterized. The HEN showed excellent ODS activity with O-2 as the oxidant and a deep desulfurization was achieved under mild conditions, outperforming many noble metal-based catalysts. Detailed experiments verified that high entropy structure induces variable valences of metals in HEN, benefiting the promotion of ODS performance. The ODS byproduct, sulfone, a high-value-added product, was further separated. Moreover, the HEN remained stable after 12 h immersion in concentrated hydrochloric acid. This work would provide a type of catalyst with high catalytic activity as well as excellent stability.

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