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Herein, we report an efficient method for the mechanochemical synthesis of N\u2010aryl amides via ruthenium\u2010catalyzed direct amidation of unprotected phenols with primary amides with water as the sole byproduct. Unexpectedly, replacing amides with methyl carboxylic acids, esters, or ketones, the same reaction led to the formation of \u03b1\u2010aryl carbonyl derivatives instead of the anticipated aryl carboxylates. The synthetic strategy accepts a wide scope of primary amides, alkyl carbonyls, and phenolic substrates to deliver 28 expected N\u2010aryl amides and 14 unexpected \u03b1\u2010aryl carbonyl derivatives with good to excellent yields. The developed synthetic approach would serve as the better alternative to the classical cross\u2010coupling reactions in context to the PASE (pot, atom, and step economy) synthesis and late\u2010stage modification of structurally complex molecules, including natural products and pharmaceuticals.<\/jats:p>","DOI":"10.1002\/chem.202500862","type":"journal-article","created":{"date-parts":[[2025,5,7]],"date-time":"2025-05-07T16:23:39Z","timestamp":1746635019000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":5,"title":["Ru\u2010Catalyzed Deoxygenative Functionalization of Phenols via \u03c0\u2010Coordination Activation: Mechanochemical Access to N\u2010Aryl Amides and \u03b1\u2010Aryl Carbonyls"],"prefix":"10.1002","volume":"31","author":[{"given":"Satenik","family":"Mkrtchyan","sequence":"first","affiliation":[{"name":"Department of Chemistry Faculty of Natural Sciences Matej Bel University  Tajovsk\u00e9ho 40 Banska Bystrica 97401 Slovakia"},{"name":"School of Medicine Georgian American University  10 Merab Aleksidze Str. Tbilisi 0160 Georgia"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Vishal B.","family":"Purohit","sequence":"additional","affiliation":[{"name":"Department of Chemical Sciences P. D. Patel Institute of Applied Sciences Charotar University of Science and Technology (CHARUSAT)  Changa Gujarat 388 421 India"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yevhen","family":"Karpun","sequence":"additional","affiliation":[{"name":"Life Chemicals Ukraine  Winston Churchill St. 5 Kyiv 02000 Ukraine"},{"name":"Interregional Academy of Personnel Management  Frometivska str., 2 Kyiv 03039 Ukraine"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Vaibhav D.","family":"Prajapati","sequence":"additional","affiliation":[{"name":"Shri Alpesh N. Patel Post Graduate Institute of Science &amp; Research  Anand Gujarat 388001 India"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ronak V.","family":"Prajapati","sequence":"additional","affiliation":[{"name":"Department of Chemistry Sardar Patel University  Vallabh Vidyanagar Gujarat 388 120 India"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Vitaliy","family":"Yepishev","sequence":"additional","affiliation":[{"name":"Life Chemicals Ukraine  Winston Churchill St. 5 Kyiv 02000 Ukraine"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Oleksandr","family":"Shalimov","sequence":"additional","affiliation":[{"name":"Department of Heteroatom Chemistry Institute of Organic Chemistry National Academy of Sciences of Ukraine  5 Murmans'ka Kyiv 02660 Ukraine"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Gabriela","family":"Addov\u00e1","sequence":"additional","affiliation":[{"name":"Department of Organic Chemistry Faculty of Natural Sciences Comenius University in Bratislava  Ilkovi\u010dova 6 Bratislava 842 15 Slovakia"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Juraj","family":"Filo","sequence":"additional","affiliation":[{"name":"Department of Organic Chemistry Faculty of Natural Sciences Comenius University in Bratislava  Ilkovi\u010dova 6 Bratislava 842 15 Slovakia"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-5647-5326","authenticated-orcid":false,"given":"Viktor O.","family":"Iaroshenko","sequence":"additional","affiliation":[{"name":"Department of Chemistry Faculty of Natural Sciences Matej Bel University  Tajovsk\u00e9ho 40 Banska Bystrica 97401 Slovakia"},{"name":"Functional Materials Group Gulf University for Science and Technology  Mubarak Al\u2010Abdullah 32093 Kuwait"},{"name":"Centre of Research Impact and Outcome Chitkara University Institute of Engineering and Technology Chitkara University  Rajpura Punjab 140401 India"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2025,5,19]]},"reference":[{"key":"e_1_2_8_1_1","volume-title":"The chemistry of amides","author":"Zabicky J.","year":"1970"},{"key":"e_1_2_8_2_1","volume-title":"The amide linkage: Structural significance in chemistry, biochemistry, and materials science","author":"Greenberg A.","year":"2000"},{"key":"e_1_2_8_3_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202000224"},{"key":"e_1_2_8_4_1","doi-asserted-by":"publisher","DOI":"10.1039\/c0cs00196a"},{"key":"e_1_2_8_5_1","doi-asserted-by":"publisher","DOI":"10.1002\/ejoc.201300573"},{"key":"e_1_2_8_6_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.tet.2012.08.065"},{"key":"e_1_2_8_7_1","doi-asserted-by":"publisher","DOI":"10.1021\/acssuschemeng.3c04372"},{"key":"e_1_2_8_8_1","doi-asserted-by":"publisher","DOI":"10.1002\/ejoc.202000080"},{"key":"e_1_2_8_9_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.tet.2005.08.031"},{"key":"e_1_2_8_10_1","doi-asserted-by":"publisher","DOI":"10.1039\/B701677H"},{"key":"e_1_2_8_11_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.jpcc.3c01821"},{"key":"e_1_2_8_12_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.201308455"},{"key":"e_1_2_8_13_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.201612324"},{"key":"e_1_2_8_14_1","doi-asserted-by":"publisher","DOI":"10.1039\/C7SC03950F"},{"key":"e_1_2_8_15_1","doi-asserted-by":"publisher","DOI":"10.1038\/ncomms14878"},{"key":"e_1_2_8_16_1","doi-asserted-by":"publisher","DOI":"10.1039\/C8QO01405A"},{"key":"e_1_2_8_17_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.orglett.9b00554"},{"key":"e_1_2_8_18_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.orglett.0c03666"},{"key":"e_1_2_8_19_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.joc.9b02068"},{"key":"e_1_2_8_20_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.joc.2c02197"},{"key":"e_1_2_8_21_1","doi-asserted-by":"publisher","DOI":"10.1002\/adsc.202100538"},{"key":"e_1_2_8_22_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.chemrev.0c00088"},{"key":"e_1_2_8_23_1","doi-asserted-by":"publisher","DOI":"10.1039\/C7CS00566K"},{"key":"e_1_2_8_24_1","doi-asserted-by":"publisher","DOI":"10.1021\/ar100082d"},{"key":"e_1_2_8_25_1","doi-asserted-by":"publisher","DOI":"10.1021\/acscatal.6b02964"},{"key":"e_1_2_8_26_1","doi-asserted-by":"publisher","DOI":"10.1021\/cr100259t"},{"key":"e_1_2_8_27_1","doi-asserted-by":"publisher","DOI":"10.1021\/acscatal.2c02708"},{"key":"e_1_2_8_28_1","volume-title":"Thermochemical data of organic compounds","author":"Pedley J. 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