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Crystallographic and quantum\u2010chemical studies are consistent with the presence of a highly polar Li\u2212Al interaction, characterized by a low bond order and relatively little charge transfer from Al to Li. Comparison with magnesium and zinc aluminyl systems reveals changes to both the M\u2212Al bond and the (NON)Al fragment (where NON=4,5\u2010bis(2,6\u2010diisopropylanilido)\u20102,7\u2010di\u2010tert\u2010butyl\u20109,9\u2010dimethylxanthene), consistent with a more covalent character, with the latter complex being shown to react with CO<jats:sub>2<\/jats:sub>via a pathway that implies that the zinc centre acts as the nucleophilic partner.<\/jats:p>","DOI":"10.1002\/anie.202109416","type":"journal-article","created":{"date-parts":[[2021,8,16]],"date-time":"2021-08-16T02:54:51Z","timestamp":1629082491000},"page":"22301-22306","update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":79,"title":["Probing the Extremes of Covalency in M\u2212Al bonds: Lithium and Zinc Aluminyl Compounds"],"prefix":"10.1002","volume":"60","author":[{"given":"Matthew M. 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