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α-O

α-O ( alpha -oxygen) is a reactive oxygen species formed from an oxygen-atom abstraction (OAT) from nitrous oxide (N 2 O) by alpha- iron (α-Fe) catalysts . The latter is defined...

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α-O (alpha-oxygen) is a reactive oxygen species formed from an oxygen-atom abstraction (OAT) from nitrous oxide (N2O) by alpha-iron (α-Fe) catalysts. The latter is defined as a high spin (S=2) divalent iron(II) ion in a constrained square planar coordination with an accessible axial coordination position. The stabilization of α-O requires structural strain on the equatorial ligand field to maintain the reactive oxygen atom in the axial position and it is this forced geometry, similar to the 'entatic state' known in metalloproteins, that lies at the basis of its reactivity in inert C-H bond activation.[1]

The alpha-oxygen site was first discovered and named in 1990 by researchers from the Boreskov Institute of Catalysis in the ZSM-5 zeolite,[2][3] and was later described in detail by researchers from Stanford University and KU Leuven in the beta zeolite.[1][4][5]

See also

References

  1. 12Snyder BE, Vanelderen P, Bols ML, Hallaert SD, Böttger LH, Ungur L, Pierloot K, Schoonheydt RA, Sels BF, Solomon EI (August 2016). "The active site of low-temperature methane hydroxylation in iron-containing zeolites". Nature. 536 (7616): 317–21. Bibcode:2016Natur.536..317S. doi:10.1038/nature19059. PMID 27535535. S2CID 4467834.
  2. ↑Pannov GI, Sobolev VI, Kharitonov AS (July 1990). "The role of iron in N2O decomposition on ZSM-5 zeolite and reactivity of the surface oxygen formed". Journal of Molecular Catalysis. 61 (1): 85–97. doi:10.1016/0304-5102(90)85197-P.
  3. ↑Sobolev V (February 1993). "Catalytic Properties of ZSM-5 Zeolites in N2O Decomposition: The Role of Iron". Journal of Catalysis. 139 (2): 435–443. doi:10.1006/jcat.1993.1038.
  4. ↑ Hallaert SD, Bols ML, Vanelderen P, Schoonheydt RA, Sels BF, Pierloot K (septiembre de 2017). "Identificación de α-Fe en zeolitas de alto contenido de sílice a partir de cálculos de estructura electrónica ab initio" . Química Inorgánica . 56 (17): 10681–10690 . doi : 10.1021/acs.inorgchem.7b01653 . PMID 28836775 . 
  5. ↑ Snyder BE, Böttger LH, Bols ML, Yan JJ, Rhoda HM, Jacobs AB, Hu MY, Zhao J, Alp EE, Hedman B, Hodgson KO, Schoonheydt RA, Sels BF, Solomon EI (mayo de 2018). "Caracterización estructural de un sitio activo de hierro no hemo en zeolitas que hidroxila metano" . Actas de la Academia Nacional de Ciencias de los Estados Unidos de América . 115 (18): 4565– 4570. Bibcode : 2018PNAS..115.4565S . doi : 10.1073 /pnas.1721717115 . PMC 5939097. PMID 29610304 .