期刊
CHEMISTRY-A EUROPEAN JOURNAL
卷 24, 期 19, 页码 4856-4863出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/chem.201704933
关键词
cyanides; density functional calculations; electrocatalysis; Prussian Blue; water oxidation
资金
- Science and Technology Council of Turkey, TUBITAK [215Z249]
- TUBITAK [1929B011500059]
- ECOSTBio [CM 1305]
- M.N. Parlar Foundation
- BAGEP
- TUBA-GEBIP
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.
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