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The well\u2010defined cobalt(III) complex [Co(III)BPMAP\u2010O]ClO<jats:sub>4<\/jats:sub> is derived from a redox\u2010active phosphine\u2010free, pentadentate mono\u2010carboxamide ligand (BPMAP\u2010H), and is formed in situ from various cobalt(II) sources, including CoCl<jats:sub>2<\/jats:sub>\u00b76H<jats:sub>2<\/jats:sub>O, CoBr<jats:sub>2<\/jats:sub>, Co(NO<jats:sub>3<\/jats:sub>)<jats:sub>2<\/jats:sub>\u00b76H<jats:sub>2<\/jats:sub>O, Co(OAc)<jats:sub>2<\/jats:sub>\u00b74H<jats:sub>2<\/jats:sub>O via oxygen activation. Using aromatic ketones and benzyl alcohols, a wide range of 2,4,6\u2010trisubstituted pyrimidines (<jats:bold>TriPym<\/jats:bold>) and 2,4,5,6\u2010tetrasubstituted pyrimidines (<jats:bold>TetraPym<\/jats:bold>) were synthesized (119 examples) in isolated yields of up to 93%. The catalytic system is also applicable to aliphatic ketones and aliphatic primary alcohols, affording 31 additional examples with yields of up to 92%. Control experiments and DFT calculations support a plausible mechanism involving dehydrogenation of the alcohols through a metal\u2010ligand cooperative pathway.<\/jats:p>","DOI":"10.1002\/chem.202502258","type":"journal-article","created":{"date-parts":[[2025,8,30]],"date-time":"2025-08-30T12:14:44Z","timestamp":1756556084000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":3,"title":["A Strategic Advance from Pincer Complexes to Hexadentate\u2010Co(III) Catalyst for Metal\u2013Ligand Cooperative Activation of Primary Alcohols to Access Highly Functionalized Pyrimidines"],"prefix":"10.1002","volume":"31","author":[{"given":"Prashant","family":"Kukreti","sequence":"first","affiliation":[{"name":"Department of Chemistry Indian Institute of Technology Roorkee  Roorkee Uttarakhand 247667 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