Reduction Mechanisms of Anticancer Osmium(VI) Complexes Revealed by Atomic Telemetry and Theoretical Calculations

Berger, GillesUniv Libre Bruxelles, Fac Pharm, Microbiol Bioorgan & Macromol Chem, B-1050 Brussels, Belgium.;Harvard Med Sch, Brigham & Womens Hosp, Dept Neurosurg, Harvey Cushing Neurooncol Labs, Boston, MA 02115 USA.;MIT, Dept Chem, Cambridge, MA 02139 USA. (författare)

Resonant X-ray emission spectroscopy (RXES) has developed in the past decade as a powerful tool to probe the chemical state of a metal center and in situ study chemical reactions. We have used it to monitor spectral changes associated with the reduction of osmium(VI) nitrido complexes to the osmium(III) ammine state by the biologically relevant reducing agent, glutathione. RXES difference maps are consistent with the proposed DFT mechanism and the formation of two stable osmium(IV) intermediates, thereby supporting the overall pathway for the reduction of these high-valent anticancer metal complexes for which reduction by thiols within cells may be essential to the antiproliferative activity.

Wach, AnnaPolish Acad Sci, Inst Nucl Phys, PL-31342 Krakow, Poland. (författare)
Sá, JacintoUppsala universitet,Fysikalisk kemi,Polish Acad Sci, Inst Phys Chem, PL-01224 Warsaw, Poland.(Swepub:uu)saaja288 (författare)
Szlachetko, JakubPolish Acad Sci, Inst Nucl Phys, PL-31342 Krakow, Poland. (författare)
Univ Libre Bruxelles, Fac Pharm, Microbiol Bioorgan & Macromol Chem, B-1050 Brussels, Belgium.;Harvard Med Sch, Brigham & Womens Hosp, Dept Neurosurg, Harvey Cushing Neurooncol Labs, Boston, MA 02115 USA.;MIT, Dept Chem, Cambridge, MA 02139 USA.Polish Acad Sci, Inst Nucl Phys, PL-31342 Krakow, Poland. (creator_code:org_t)

Ingår i:Inorganic Chemistry: American Chemical Society (ACS)60:9, s. 6663-66710020-16691520-510X

Av författaren/redakt...: Berger, Gilles; Wach, Anna; Sá, Jacinto; Szlachetko, Jaku ...

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