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Notwithstanding, mildly Lewis acidic alkali cations are rarely studied in this context, despite their prevalence in both cellular and electrochemical media. Herein, we disclose a structurally characterized series of monovalent Lewis acids (Li\n                    <jats:sup>+<\/jats:sup>\n                    , Na\n                    <jats:sup>+<\/jats:sup>\n                    , K\n                    <jats:sup>+<\/jats:sup>\n                    , and Cs\n                    <jats:sup>+<\/jats:sup>\n                    ) adducted to a bis(\u03bc\u2010OH) dinickel diamond core. Spectroscopic characterization demonstrates that the oxygenic binding pocket of the tripodal NNNO\u2010chelate maintains this structure in solution. Detailed electrochemical measurements establish trends correlating oxidation potential and alkali metal identity, demonstrating a steep dependence on Lewis acidity (\u223c165\u00a0mV\/\n                    <jats:italic>\n                      pK\n                      <jats:sub>a<\/jats:sub>\n                    <\/jats:italic>\n                    decade). Density functional theory indicates that the observed oxidation chemistry is largely ligand\u2010centered, highlighting the importance of electronic coupling between the Lewis acid and locus of redox. These findings, with relevance to bioinorganic, heterogeneous, and molecular oxidation processes, provide design criteria for rationalizing and maximizing the impact of relatively weak Lewis acids, including common alkali cations, on the physicochemical properties of redox\u2010active species.\n                  <\/jats:p>","DOI":"10.1002\/chem.71824","type":"journal-article","created":{"date-parts":[[2026,10,23]],"date-time":"2026-10-23T03:31:58Z","timestamp":1792726318000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Alkali Metal Mediated Redox Tuning in Bis(\u03bc\u2010OH) Dinickel(II) Complexes"],"prefix":"10.1002","author":[{"ORCID":"https:\/\/orcid.org\/0009-0009-8606-7196","authenticated-orcid":false,"given":"Matthew L.","family":"Peris","sequence":"first","affiliation":[{"name":"Willard Henry Dow Laboratory, Department of Chemistry University of Michigan  Ann Arbor Michigan USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-3347-8583","authenticated-orcid":false,"given":"Joshua A.","family":"Buss","sequence":"additional","affiliation":[{"name":"Willard Henry Dow Laboratory, Department of Chemistry University of Michigan  Ann Arbor Michigan 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Numbers 2556739 \u2013 2556745 Contain the Supplementary Crystallographic Data for This Paper. These Data can be Obtained Free of Charge via the Joint Cambridge Crystallographic Data Centre (CCDC) and Fachinformationszentrum Karlsruhe Access Structures Service\u201d."},{"key":"e_1_2_7_89_1","doi-asserted-by":"publisher","DOI":"10.1016\/S0020\u20101693(99)00591\u20105"},{"key":"e_1_2_7_90_1","unstructured":"\u201cComparing the Calculated Gas\u2010phase Free Energies for Both the Syn and Anti\u2010isomers of 2 the Geometry That Poises the Phenolate Groups Anti Relative to the Diamond Core is More Stable by 8.1\u00a0Kcal\/Mol (298.15 K). Related to the Difference in Solubility the Computed Dipole Moments for the Syn and Anti Isomers are 12.886 and 0.003 D respectively.\u201d."},{"key":"e_1_2_7_91_1","doi-asserted-by":"publisher","DOI":"10.1107\/S0567739476001551"},{"key":"e_1_2_7_92_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.200353637"},{"key":"e_1_2_7_93_1","doi-asserted-by":"publisher","DOI":"10.1021\/ja990311d"},{"key":"e_1_2_7_94_1","doi-asserted-by":"publisher","DOI":"10.1039\/C8NJ00100F"},{"key":"e_1_2_7_95_1","doi-asserted-by":"publisher","DOI":"10.1246\/bcsj.72.239"},{"key":"e_1_2_7_96_1","doi-asserted-by":"publisher","DOI":"10.1246\/cl.1996.929"},{"key":"e_1_2_7_97_1","doi-asserted-by":"publisher","DOI":"10.1039\/C9CC08229H"},{"key":"e_1_2_7_98_1","unstructured":"\u201cAddition of Excess Exogenous Cs[BArF] Failed to Resolve Sharper Signals in the Paramagnetically Shifted1H NMR Spectrum of 2\u2010Cs See Supporting Information for Additional Details.\u201d."},{"key":"e_1_2_7_99_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.jchemed.7b00361"},{"key":"e_1_2_7_100_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.inorgchem.3c00084"},{"key":"e_1_2_7_101_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.inorgchem.0c03239"},{"key":"e_1_2_7_102_1","doi-asserted-by":"publisher","DOI":"10.1016\/0032\u20103861(96)00323\u20100"},{"key":"e_1_2_7_103_1","doi-asserted-by":"publisher","DOI":"10.1007\/BF00913599"},{"key":"e_1_2_7_104_1","unstructured":"\u201cThe Highest Energy SOMO of 2\u2010syn (the Structure Comparable to the Other 2\u2010M Adducts) is Destabilized Relative to That of 2\u2010Anti (see Table S9). 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