Type <scp>III</scp> porous ionic liquids via lipophilicity differences for enhanced oxidation catalysis

Abstract In this study, an innovative strategy is proposed to design porous ionic liquids (PILs) using lipophilicity differences, defined as type III‐B PIL, which overcomes the traditional size‐effect limitations in PIL design. An SBA‐15 confined high‐entropy single‐atom catalyst (HESAC@SBA‐15) with an oleophobic internal surface was engineered as the porous framework and oleaginous 1‐butyl‐3‐methylimidazolium tetrafluoroborate as the organic guest for constructing a novel type PIL (PILS‐B). This type of PILS‐B combines the exceptional gas storage capacity of PILs with the high catalytic activity of HESAC@SBA‐15. Additionally, the mesoporous structure of SBA‐15 enhances mass transfer during reactions, thereby improving catalytic efficiency. Using the aerobic oxidation of aromatic sulfur compounds in fuel oils as a model reaction, PILS‐B achieved a desulfurization efficiency of &gt;99%. This strategy expands the variety of porous frameworks and organic guests for PIL design, showcasing the potential of PILs as effective and stable catalysts with broader applications in catalysis.