2024
DOI: 10.1021/acs.inorgchem.3c03470
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Carboxylate Shift Dynamics in Biomimetic Co2(μ–OH)2 Complexes

Alyssa A. DeLucia,
Lisa Olshansky

Abstract: Carboxylate shift mechanisms provide low-energy pathways to accommodate changes in oxidation state and coordination number required during catalysis in metalloenzyme active sites. These processes are challenging to observe in their native enzymes and molecular models can provide insight into their mechanistic details. We report here the direct observation of a carboxylate shift reaction in biomimetic yet structurally stable dicobalt complexes featuring both monodentate and bridging acetate ligands, as well as … Show more

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Cited by 4 publications
(2 citation statements)
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“…The 1 H NMR spectrum of MnCo 3 [PF 6 ] in acetonitrile- d 3 contained broad resonances consistent with a paramagnetic species, as confirmed by an Evans method measurement (3.31 μ B , S = 3/2). The identity of the [Co 2 (μ–OH) 2 (OAc) 3 ( t -Bupy) 4 ]­[PF 6 ] byproduct (10% yield by 1 H NMR spectroscopy) was confirmed by isolation and characterization by 1 H NMR spectroscopy and HR-ESI-MS. , Other Co III acetate t -Bupy species present (by 1 H NMR spectroscopic and mass spectrometric analysis) appear to correspond to oligomeric species. , …”
Section: Resultsmentioning
confidence: 90%
“…The 1 H NMR spectrum of MnCo 3 [PF 6 ] in acetonitrile- d 3 contained broad resonances consistent with a paramagnetic species, as confirmed by an Evans method measurement (3.31 μ B , S = 3/2). The identity of the [Co 2 (μ–OH) 2 (OAc) 3 ( t -Bupy) 4 ]­[PF 6 ] byproduct (10% yield by 1 H NMR spectroscopy) was confirmed by isolation and characterization by 1 H NMR spectroscopy and HR-ESI-MS. , Other Co III acetate t -Bupy species present (by 1 H NMR spectroscopic and mass spectrometric analysis) appear to correspond to oligomeric species. , …”
Section: Resultsmentioning
confidence: 90%
“…9 Independently of our work, interest in the reactivity of cobalt complexes has recently increased again. 10…”
Section: Introductionmentioning
confidence: 99%