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Evolution of iridium-based molecular catalysts during water oxidation with ceric ammonium nitrate.
Grotjahn, Douglas B; Brown, Derek B; Martin, Jessica K; Marelius, David C; Abadjian, Marie-Caline; Tran, Hai N; Kalyuzhny, Gregory; Vecchio, Kenneth S; Specht, Zephen G; Cortes-Llamas, Sara A; Miranda-Soto, Valentin; van Niekerk, Christoffel; Moore, Curtis E; Rheingold, Arnold L.
Afiliação
  • Grotjahn DB; Department of Chemistry and Biochemistry, 5500 Campanile Drive, San Diego State University, San Diego, California 92182, USA. grotjahn@chemistry.sdsu.edu
J Am Chem Soc ; 133(47): 19024-7, 2011 Nov 30.
Article em En | MEDLINE | ID: mdl-22059883
ABSTRACT
Organometallic iridium complexes have been reported as water oxidation catalysts (WOCs) in the presence of ceric ammonium nitrate (CAN). One challenge for all WOCs regardless of the metal used is stability. Here we provide evidence for extensive modification of many Ir-based WOCs even after exposure to only 5 or 15 equiv of Ce(IV) (whereas typically 100-10000 equiv are employed during WOC testing). We also show formation of Ir-rich nanoparticles (likely IrO(x)) even in the first 20 min of reaction, associated with a Ce matrix. A combination of UV-vis and NMR spectroscopy, scanning transmission electron microscopy, and powder X-ray diffraction is used. Even simple IrCl(3) is an excellent catalyst. Our results point to the pitfalls of studying Ir WOCs using CAN.
Assuntos

Texto completo: 1 Coleções: 01-internacional Base de dados: MEDLINE Assunto principal: Compostos Organometálicos / Água / Cério / Irídio Idioma: En Revista: J Am Chem Soc Ano de publicação: 2011 Tipo de documento: Article

Texto completo: 1 Coleções: 01-internacional Base de dados: MEDLINE Assunto principal: Compostos Organometálicos / Água / Cério / Irídio Idioma: En Revista: J Am Chem Soc Ano de publicação: 2011 Tipo de documento: Article