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Hereby, we report a convenient synthetic approach for designing hierarchically porous Mn\n                    <jats:sub>3<\/jats:sub>\n                    O\n                    <jats:sub>4<\/jats:sub>\n                    nanocrystals (HP\u2010Mn\n                    <jats:sub>3<\/jats:sub>\n                    O\n                    <jats:sub>4<\/jats:sub>\n                    \u2010NCs) using a small organic molecular entity, sodium salicylate, as a structure\u2010directing agent. The porosity and the crystallinity were evaluated through the powder XRD, TEM, and N\n                    <jats:sub>2<\/jats:sub>\n                    sorption. TEM analysis revealed the presence of mesopores, which agrees well with the N\n                    <jats:sub>2<\/jats:sub>\n                    sorption analysis. XPS analysis revealed the presence of a mixed\u2010valent Mn\n                    <jats:sup>2+<\/jats:sup>\n                    and Mn\n                    <jats:sup>3+<\/jats:sup>\n                    . The aerial dehydrogenative C\u2500N cross\u2010coupling of aromatic diamines and alcohols for the selective production of benzimidazole derivatives proceeds smoothly in the presence of HP\u2010Mn\n                    <jats:sub>3<\/jats:sub>\n                    O\n                    <jats:sub>4<\/jats:sub>\n                    \u2010NCs as a heterogeneous catalyst. The catalyst displayed a clean reaction profile with excellent product yields of up to 94% for various substrates. Noticeably, the reaction is accomplished under base\u2010free, solvent\u2010free, and aerial conditions. The existence of mesopore enables a high internal surface area, thereby increasing the exposure of surface\u2010active sites. The mesopores of the material promote the facile diffusion of reactants and products. Large specific surface area, abundant surface\u2010active sites, stability, and structural robustness collectively endow the HP\u2010Mn\n                    <jats:sub>3<\/jats:sub>\n                    O\n                    <jats:sub>4<\/jats:sub>\n                    \u2010NCs with high catalytic activity and recycling efficiency.\n                  <\/jats:p>","DOI":"10.1002\/asia.71019","type":"journal-article","created":{"date-parts":[[2026,10,18]],"date-time":"2026-10-18T15:02:21Z","timestamp":1792335741000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Hierarchically Porous Mn\n                    <sub>3<\/sub>\n                    O\n                    <sub>4<\/sub>\n                    Nanocrystals for Aerobic, Solvent\u2010Free Dehydrogenative C\u2500N Cross\u2010Coupling Reactions"],"prefix":"10.1002","volume":"21","author":[{"ORCID":"https:\/\/orcid.org\/0009-0004-6538-2553","authenticated-orcid":false,"given":"Kiruthiga","family":"M.","sequence":"first","affiliation":[{"name":"Department of Chemistry, School of Physical and Chemical Sciences B. 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