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We report here a structurally undulated robust Co(II)\u2010framework that encompasses open metal sites (OMS) and carboxamide moieties. The activated framework exhibits superior overpotentials of 262\u00a0mV for oxygen evolution reaction (OER, 1\u00a0M KOH) and 154\u00a0mV for hydrogen evolution reaction (HER, 0.5\u00a0M H\n                    <jats:sub>2<\/jats:sub>\n                    SO\n                    <jats:sub>4<\/jats:sub>\n                    ) at 10\u00a0mA cm\n                    <jats:sup>\u2212<\/jats:sup>\n                    <jats:sup>2<\/jats:sup>\n                    than the majority of contemporary and benchmark catalysts, accompanied by remarkable Tafel slopes of 60.7 and 114.06\u00a0mV dec\n                    <jats:sup>\u2212<\/jats:sup>\n                    <jats:sup>1<\/jats:sup>\n                    , respectively. Besides impressive intrinsic electrocatalytic parameters, 2000 cycles of durability and &gt;30\u00a0h chronoamperometric stability underscore its structural resilience in bifunctional electrocatalysis. Building on an incisive juxtaposition of antagonistic functionality, the MOF catalyzes one\u2010pot, three\u2010component Knoevenagel\u2010Michael condensation, producing a vast range of 2\u2010amino\u20103\u2010cyano\u20104H\u2010pyrans, including four pharmacologically active anticancer and antibacterial molecules in quantitative yields under mild\u2010condition. Notably, the reaction exhibits molecular\u2010dimension\u2010mediated size selectivity, revealing cooperative acid\u2010base interplay\u2010induced pore\u2010confined catalysis. Control experiments and density\u2010functional\u2010theory studies corroborate the synergistic participation of OMS and HBD groups. This study introduces a unified design strategy for bi\u2010functional MOF that bridges high\u2010performance renewable energy conversion and green organic synthesis through synergistic involvement of pore\u2010embedded antagonistic functionality.\n                  <\/jats:p>","DOI":"10.1002\/smll.202514442","type":"journal-article","created":{"date-parts":[[2026,2,12]],"date-time":"2026-02-12T12:42:04Z","timestamp":1770900124000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":4,"title":["Antagonistically Functionalized Cobalt\u2010Organic Framework Enabling Bifunctional Water Splitting and One\u2010Pot Synthesis of Bioactive 4H\u2010Pyrans via Synergistic Catalysis"],"prefix":"10.1002","volume":"22","author":[{"ORCID":"https:\/\/orcid.org\/0009-0008-0770-5413","authenticated-orcid":false,"given":"Atanu","family":"Pandit","sequence":"first","affiliation":[{"name":"Academy of Scientific and Innovative Research (AcSIR)  Ghaziabad India"},{"name":"Inorganic Materials &amp; Catalysis Division CSIR\u2010Central Salt &amp; Marine Chemicals Research Institute  Bhavnagar Gujarat India"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-8964-5141","authenticated-orcid":false,"given":"Aditi","family":"De","sequence":"additional","affiliation":[{"name":"Academy of Scientific and Innovative Research (AcSIR)  Ghaziabad India"},{"name":"Electrochemical Process Engineering (EPE) Division CSIR\u2212Central Electrochemical Research Institute (CECRI)  Karaikudi Tamil Nadu India"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-9812-9088","authenticated-orcid":false,"given":"Athulya S.","family":"Palakkal","sequence":"additional","affiliation":[{"name":"Department of Chemistry SRM Institute of Science and Technology  Kattankulathur Tamil Nadu India"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Subrata","family":"Kundu","sequence":"additional","affiliation":[{"name":"Academy of Scientific and Innovative Research (AcSIR)  Ghaziabad India"},{"name":"Electrochemical Process Engineering (EPE) Division CSIR\u2212Central Electrochemical Research Institute (CECRI)  Karaikudi Tamil Nadu India"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-3838-4180","authenticated-orcid":false,"given":"Subhadip","family":"Neogi","sequence":"additional","affiliation":[{"name":"Academy of Scientific and Innovative Research (AcSIR)  Ghaziabad India"},{"name":"Inorganic Materials &amp; Catalysis Division CSIR\u2010Central Salt &amp; Marine Chemicals Research Institute  Bhavnagar Gujarat India"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2026,2,12]]},"reference":[{"key":"e_1_2_9_2_1","unstructured":"E. 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