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Traditional catalysts show either poor sulfur\u2010resistance or unsatisfactory polysulfur transportation. Here an ordered mesoporous pyridine@Schiff base designed from solidothermal\u2010molten self\u2010assembly of triblock copolymer template (Pluronic F127) with 2,6\u2010diaminopyridine (DAP) monomer and terephthalaldehyde crosslinker is reported, which breaks the dominance of the resol route for nitrogen\u2010doped, ordered mesoporous polymer design. Strong hydrogen\u2010bond 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\u2010OMC) possess record\u2010high nitrogen content and barrier\u2010free mesochannels. These structural features afford long\u2010term, continuous operation for the tandem conversion of COS and H\n                    <jats:sub>2<\/jats:sub>\n                    S to polysulfur (S\n                    <jats:italic>\n                      <jats:sub>x<\/jats:sub>\n                    <\/jats:italic>\n                    ). Under simulated natural gas conditions, the RN\u2010OMC achieves \u2248100% conversion and selectivity, and it compares favorably with literature\u2010reported catalysts in the field.\n                  <\/jats:p>","DOI":"10.1002\/smll.202510030","type":"journal-article","created":{"date-parts":[[2025,12,4]],"date-time":"2025-12-04T07:44:50Z","timestamp":1764834290000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":4,"title":["Solvent\u2010Free Self\u2010Assembly to Ordered Mesoporous Poly (Pyridine@Schiff base) Catalysts for Efficient Upcycling of Waste Gaseous Sulfides from Natural Gas"],"prefix":"10.1002","volume":"22","author":[{"given":"Yong","family":"Zheng","sequence":"first","affiliation":[{"name":"National Engineering Research Center of Chemical Fertilizer Catalyst (NERC\u2010CFC) School of Chemical Engineering Fuzhou University  Fuzhou 350002 P. R. 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