Solvent‐Free Self‐Assembly to Ordered Mesoporous Poly (Pyridine@Schiff base) Catalysts for Efficient Upcycling of Waste Gaseous Sulfides from Natural Gas

Transformation of volatile sulfides of carbonyl sulfide (COS) and hydrogen sulfide (H₂S) into polysulfur from natural gas is the optimal route for their deep elimination and upcycling. Traditional catalysts show either poor sulfur-resistance or unsatisfactory polysulfur transportation. Here an ordered mesoporous pyridine@Schiff base designed from solidothermal-molten self-assembly of triblock copolymer template (Pluronic F127) with 2,6-diaminopyridine (DAP) monomer and terephthalaldehyde crosslinker is reported, which breaks the dominance of the resol route for nitrogen-doped, ordered mesoporous polymer design. Strong hydrogen-bond interaction between DAP and F127 ensures ordered mesoporosity formation, and condensation between DAP and phthalaldehyde yields poly(pyridine@Schiff base) framework. The resulting ordered mesoporous polymer and its derived ordered mesoporous carbon (RN-OMC) possess record-high nitrogen content and barrier-free mesochannels. These structural features afford long-term, continuous operation for the tandem conversion of COS and H₂S to polysulfur (S_x). Under simulated natural gas conditions, the RN-OMC achieves ≈100% conversion and selectivity, and it compares favorably with literature-reported catalysts in the field.