The routes of association of (hydro)oxo centers on iron hydroxide at the water oxidation process: DFT predictions

Aleksandr A. Shubin; Sergey Ph Ruzankin; Igor L. Zilberberg; Oxana P. Taran; Valentin N. Parmon

doi:10.1016/j.cplett.2014.11.061

The routes of association of (hydro)oxo centers on iron hydroxide at the water oxidation process: DFT predictions

Aleksandr A. Shubin, Sergey Ph Ruzankin, Igor L. Zilberberg, Oxana P. Taran, Valentin N. Parmon

Research output: Contribution to journal › Article › peer-review

7 Citations (Scopus)

Abstract

The formation of the O-O bond in the water oxidation catalyzed by the iron hydroxides was modeled with the Fe₄O₄(OH)₄ and Fe₂O₂(OH)₄ complexes by means of the density functional theory. Consideration of the local minima and transition states for various routes of the association of oxo- and hydroxo-centers reveals a determinative role of the oxyl radical center Fe^III - O^•- in facilitating this process. The preferable scenario comprises two steps: (1) the abstraction of the electron and proton from the initial complex leaving behind a ferryl FeO group, and (2) the incorporation of ferryl oxygen into the tetramer edge to form peroxo group.

Original language	English
Pages (from-to)	126-132
Number of pages	7
Journal	Chemical Physics Letters
Volume	619
DOIs	https://doi.org/10.1016/j.cplett.2014.11.061
Publication status	Published - 5 Jan 2015
Externally published	Yes

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10.1016/j.cplett.2014.11.061

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title = "The routes of association of (hydro)oxo centers on iron hydroxide at the water oxidation process: DFT predictions",

abstract = "The formation of the O-O bond in the water oxidation catalyzed by the iron hydroxides was modeled with the Fe4O4(OH)4 and Fe2O2(OH)4 complexes by means of the density functional theory. Consideration of the local minima and transition states for various routes of the association of oxo- and hydroxo-centers reveals a determinative role of the oxyl radical center FeIII - O•- in facilitating this process. The preferable scenario comprises two steps: (1) the abstraction of the electron and proton from the initial complex leaving behind a ferryl FeO group, and (2) the incorporation of ferryl oxygen into the tetramer edge to form peroxo group.",

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T1 - The routes of association of (hydro)oxo centers on iron hydroxide at the water oxidation process

T2 - DFT predictions

AU - Shubin, Aleksandr A.

AU - Ruzankin, Sergey Ph

AU - Zilberberg, Igor L.

AU - Taran, Oxana P.

AU - Parmon, Valentin N.

PY - 2015/1/5

Y1 - 2015/1/5

N2 - The formation of the O-O bond in the water oxidation catalyzed by the iron hydroxides was modeled with the Fe4O4(OH)4 and Fe2O2(OH)4 complexes by means of the density functional theory. Consideration of the local minima and transition states for various routes of the association of oxo- and hydroxo-centers reveals a determinative role of the oxyl radical center FeIII - O•- in facilitating this process. The preferable scenario comprises two steps: (1) the abstraction of the electron and proton from the initial complex leaving behind a ferryl FeO group, and (2) the incorporation of ferryl oxygen into the tetramer edge to form peroxo group.

AB - The formation of the O-O bond in the water oxidation catalyzed by the iron hydroxides was modeled with the Fe4O4(OH)4 and Fe2O2(OH)4 complexes by means of the density functional theory. Consideration of the local minima and transition states for various routes of the association of oxo- and hydroxo-centers reveals a determinative role of the oxyl radical center FeIII - O•- in facilitating this process. The preferable scenario comprises two steps: (1) the abstraction of the electron and proton from the initial complex leaving behind a ferryl FeO group, and (2) the incorporation of ferryl oxygen into the tetramer edge to form peroxo group.

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DO - 10.1016/j.cplett.2014.11.061

M3 - Article

AN - SCOPUS:84916919857

VL - 619

SP - 126

EP - 132

JO - Chemical Physics Letters

JF - Chemical Physics Letters

SN - 0009-2614

ER -

The routes of association of (hydro)oxo centers on iron hydroxide at the water oxidation process: DFT predictions

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