Tuning the Electronic Properties of Prussian Blue Analogues for Efficient Water Oxidation Electrocatalysis: Experimental and Computational Studies


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Alsac E. P., ÜLKER E., Nune S. V. K., DEDE Y., KARADAŞ F.

CHEMISTRY-A EUROPEAN JOURNAL, cilt.24, sa.19, ss.4856-4863, 2018 (SCI-Expanded) identifier identifier identifier

  • Yayın Türü: Makale / Tam Makale
  • Cilt numarası: 24 Sayı: 19
  • Basım Tarihi: 2018
  • Doi Numarası: 10.1002/chem.201704933
  • Dergi Adı: CHEMISTRY-A EUROPEAN JOURNAL
  • Derginin Tarandığı İndeksler: Science Citation Index Expanded (SCI-EXPANDED), Scopus
  • Sayfa Sayıları: ss.4856-4863
  • Anahtar Kelimeler: cyanides, density functional calculations, electrocatalysis, Prussian Blue, water oxidation, OXYGEN EVOLUTION REACTION, TRANSITION-METAL CATALYSTS, COBALT HEXACYANOFERRATE, CYANIDE COMPLEX, PHOTOANODES, COMPOUND, ROUTE, BOND, O-2
  • Gazi Üniversitesi Adresli: Evet

Özet

Although several Prussian Blue analogues (PBAs) have been investigated as water oxidation catalysts, the field lacks a comprehensive study that focuses on the design of the ideal PBA for this purpose. Here, members of a series of PBAs with different cyanide precursors have been investigated to study the effect of hexacyanometal groups on their electrocatalytic water oxidation activities. Cyclic voltammetric, chronoamperometric, and chronopotentiometric measurements have revealed a close relationship between the electron density of electroactive cobalt sites and electrocatalytic activity, which has also been confirmed by infrared and XPS studies. Furthermore, pH-dependent cyclic voltammetry and computational studies have been performed to gain insight into the catalytic mechanism and electronic structure of cyanide-based systems to identify possible intermediates and to assign the rate-determining step of the target process.