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The outer\u2010sphere path is found to be supported by \u03c0\u2013\u03c0 interaction between the extended aromatic ring system of the benzimidazolylidene\u2010based CNC\u2010ligand and aromatic rings of the substrates in a new, unprecedented case of metal\u2013ligand cooperativity.<\/jats:p>","DOI":"10.1002\/chem.202501301","type":"journal-article","created":{"date-parts":[[2025,5,22]],"date-time":"2025-05-22T06:02:11Z","timestamp":1747893731000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":4,"title":["Metal\u2013Ligand Cooperativity via \u03a0\u2013\u03a0 Interactions Supporting Outer\u2010Sphere Hydride Transfer"],"prefix":"10.1002","volume":"31","author":[{"given":"Ashu","family":"Singh","sequence":"first","affiliation":[{"name":"Department of Chemistry Indian Institute of Technology Indore  Simrol Indore 453552 India"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Vishal","family":"Jaiswal","sequence":"additional","affiliation":[{"name":"Department of Chemistry Indian Institute of Technology Indore  Simrol Indore 453552 India"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Shilpi","family":"Misra","sequence":"additional","affiliation":[{"name":"Centre for Scientific and Applied Research IPS Academy  Indore 452012 India"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-7263-7914","authenticated-orcid":false,"given":"Amrendra K.","family":"Singh","sequence":"additional","affiliation":[{"name":"Department of Chemistry Indian Institute of Technology Indore  Simrol Indore 453552 India"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2025,6,23]]},"reference":[{"key":"e_1_2_7_1_1","first-page":"635","volume":"10","author":"Shimbayashi T.","year":"2020","journal-title":"Catal."},{"key":"e_1_2_7_1_2","doi-asserted-by":"publisher","DOI":"10.1039\/D0CS00509F"},{"key":"e_1_2_7_1_3","doi-asserted-by":"publisher","DOI":"10.1039\/D3CS00998J"},{"key":"e_1_2_7_2_1","doi-asserted-by":"publisher","DOI":"10.1021\/cr5002782"},{"key":"e_1_2_7_2_2","doi-asserted-by":"publisher","DOI":"10.1021\/acs.accounts.7b00089"},{"key":"e_1_2_7_3_1","doi-asserted-by":"publisher","DOI":"10.1021\/acscatal.1c05271"},{"key":"e_1_2_7_4_1","doi-asserted-by":"publisher","DOI":"10.1039\/D1OB01153G"},{"key":"e_1_2_7_5_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.organomet.8b00847"},{"key":"e_1_2_7_5_2","doi-asserted-by":"publisher","DOI":"10.1021\/acs.organomet.8b00432"},{"key":"e_1_2_7_5_3","doi-asserted-by":"publisher","DOI":"10.1021\/acs.joc.9b02957"},{"key":"e_1_2_7_6_1","doi-asserted-by":"publisher","DOI":"10.1039\/C5CS00161G"},{"key":"e_1_2_7_7_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.organomet.3c00376"},{"key":"e_1_2_7_7_2","doi-asserted-by":"publisher","DOI":"10.1021\/acs.joc.3c02029"},{"key":"e_1_2_7_7_3","doi-asserted-by":"publisher","DOI":"10.1021\/acs.orglett.0c02787"},{"key":"e_1_2_7_8_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.201904214"},{"key":"e_1_2_7_9_1","doi-asserted-by":"crossref","DOI":"10.1126\/sciadv.adf8742","volume":"9","author":"Ge L.","journal-title":"Sci. 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