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Crystallographic studies reveal the molecular structures of\n                    <jats:bold>1<\/jats:bold>\n                    and\n                    <jats:bold>2<\/jats:bold>\n                    based on the similar {Cu\n                    <jats:sub>2<\/jats:sub>\n                    (\u03bc\u2010O)\n                    <jats:sub>2<\/jats:sub>\n                    } core, while the structure of\n                    <jats:bold>3<\/jats:bold>\n                    features the {Cu\n                    <jats:sub>3<\/jats:sub>\n                    (\u03bc\u2010O)\n                    <jats:sub>2<\/jats:sub>\n                    } core with consecutive arranement of the metal centres, supported by the additional carboxylate bridges. The strong intermolecular hydrogen bonds join the molecular structures into 1D (for\n                    <jats:bold>1<\/jats:bold>\n                    and\n                    <jats:bold>3<\/jats:bold>\n                    ) or 2D (for\n                    <jats:bold>2<\/jats:bold>\n                    ) architectures. All three compounds act as catalysts for the aerobic oxidation of 2\u2010aminophenol to the phenoxazinone chromophore (phenoxazinone synthase\u2010like activity) with the maximum reaction rates up to 2.3\u00d710\n                    <jats:sup>\u22128<\/jats:sup>\n                    \u2005M\u2009s\n                    <jats:sup>\u22121<\/jats:sup>\n                    . The substrate scope involves methyl\u2010, nitro\u2010 and chloro\u2010substituted 2\u2010aminophenols, disclosing the negligible activity of nitro\u2010derivatives, while the 6\u2010amino\u2010\n                    <jats:italic>m<\/jats:italic>\n                    \u2010cresol substrate shows the highest activity with the initial reaction rate of 5.8\u00d710\n                    <jats:sup>\u22128<\/jats:sup>\n                    \u2005M\u2009s\n                    <jats:sup>\u22121<\/jats:sup>\n                    . The mechanism of the rate\u2010limiting reaction step (copper\u2010catalysed formation of 2\u2010aminophenoxyl radicals) was investigated at the DFT level. The combined DFT and CASSCF studies of the copper superoxo Cu\n                    <jats:sup>II<\/jats:sup>\n                    \u2010OO\u22c5 radical species as possible unconventional reaction intermediates resulted in a rational mechanism of H\u2010atom abstraction, where the activation energies follow the experimental reactivity of substituted 2\u2010aminophenols. The TDDFT and STEOM\u2010DLPNO\u2010CCSD theoretical calculations of the absorption spectra of substrates, phenoxazinone chromophores and putative polynuclear species containing 2\u2010aminophenoxo ligand are reported.\n                  <\/jats:p>","DOI":"10.1002\/cplu.202400613","type":"journal-article","created":{"date-parts":[[2025,2,11]],"date-time":"2025-02-11T01:57:15Z","timestamp":1739239035000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":5,"title":["Phenoxazinone Synthase\u2010Like Catalytic Activity of Bi\u2010 and Trinuclear Copper(II) Complexes with 2\u2010Benzylethanolamine: Experimental and Theoretical Investigations"],"prefix":"10.1002","volume":"90","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-0114-6525","authenticated-orcid":false,"given":"Oksana V.","family":"Nesterova","sequence":"first","affiliation":[{"name":"Centro de Estudos de Engenharia Qu\u00edmica Instituto Superior de Engenharia de Lisboa Instituto Polit\u00e9cnico de Lisboa, R. Conselheiro Em\u00eddio Navarro 1  1959-007 Lisboa Portugal"}]},{"given":"Olena E.","family":"Bondarenko","sequence":"additional","affiliation":[{"name":"Centro de Qu\u00edmica Estrutural Institute of Molecular Sciences Departamento de Engenharia Qu\u00edmica Instituto Superior T\u00e9cnico Universidade de Lisboa, Av. Rovisco Pais 1  1049-001 Lisboa Portugal"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-8323-888X","authenticated-orcid":false,"given":"Armando J. L.","family":"Pombeiro","sequence":"additional","affiliation":[{"name":"Centro de Qu\u00edmica Estrutural Institute of Molecular Sciences Departamento de Engenharia Qu\u00edmica Instituto Superior T\u00e9cnico Universidade de Lisboa, Av. Rovisco Pais 1  1049-001 Lisboa Portugal"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-1095-6888","authenticated-orcid":false,"given":"Dmytro S.","family":"Nesterov","sequence":"additional","affiliation":[{"name":"Centro de Estudos de Engenharia Qu\u00edmica Instituto Superior de Engenharia de Lisboa Instituto Polit\u00e9cnico de Lisboa, R. 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