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The comparison with respective cyclohexene, pyridine and tetrahydrofuran complexes reveals that the experimental ligand binding strengths follow the order THF&lt;C\n                    <jats:sub>6<\/jats:sub>\n                    H\n                    <jats:sub>6<\/jats:sub>\n                    &lt;C\n                    <jats:sub>6<\/jats:sub>\n                    F\n                    <jats:sub>6<\/jats:sub>\n                    &lt;cyclohexene&lt;pyridine&lt;benzaldehyde&lt;anthraquinone. To understand this surprising order, the complexes\u2019 electronic structures were elucidated by nuclear magnetic resonance (NMR), single crystal X\u2010Ray diffraction (sc\u2010XRD), ultraviolet\/visible (UV\/Vis) electronic absorption, infrared (IR) vibrational, Pd L\n                    <jats:sub>3<\/jats:sub>\n                    \u2010edge X\u2010ray absorption (XAS), and X\u2010ray photoelectron (XP) spectroscopic techniques, complemented by Density Functional Theory (DFT) calculations including energy decomposition (EDA\u2010NOCV) and effective oxidation state (EOS) analyses. For benzene, pyridine and cyclohexene, bonding follows the donor\/acceptor picture of the Dewar\u2013Chatt\u2013Duncanson model. In stark contrast, hexafluorobenzene, benzaldehyde and anthraquinone bind via essentially the \u03c0\u2010channel only and thus as \u03c0\u2010analogues of Z\u2010acceptor ligands. This contribution elucidates the control of functional\u2010group selectivity in palladium(0) catalysis and delineates a novel strategy to activate electron\u2010deficient \u03c0\u2010systems.\n                  <\/jats:p>","DOI":"10.1002\/anie.202418738","type":"journal-article","created":{"date-parts":[[2024,12,23]],"date-time":"2024-12-23T10:49:40Z","timestamp":1734950980000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":10,"title":["\u03c0\u2010Lewis Base Activation of Carbonyls and Hexafluorobenzene"],"prefix":"10.1002","volume":"64","author":[{"ORCID":"https:\/\/orcid.org\/0000-0001-5991-5828","authenticated-orcid":false,"given":"Aditesh","family":"Mondal","sequence":"first","affiliation":[{"name":"Coordination Chemistry Saarland University  Campus C4.1 D-66123 Saarbr\u00fccken Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-7012-8750","authenticated-orcid":false,"given":"Kevin","family":"Breitwieser","sequence":"additional","affiliation":[{"name":"Coordination Chemistry Saarland University  Campus C4.1 D-66123 Saarbr\u00fccken Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Sergi","family":"Dan\u00e9s","sequence":"additional","affiliation":[{"name":"Departament de Qu\u00edmica Institut de Qu\u00edmica Computacional I Cat\u00e0lisi Universitat de Girona  c\/m. 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