Mechanism of water oxidation by non-heme iron catalysts when driven with sodium periodate

Alexander R. Parent, Takashi Nakazono, Shu Lin, Satoshi Utsunomiya, Ken Sakai

研究成果: ジャーナルへの寄稿記事

35 引用 (Scopus)

抄録

Iron tris(2-methylpyridyl)amine (TPA) and iron 1-(bis(2-methylpyridyl) amino)-2-methyl-2-propanoate (BPyA) salts are characterized as water oxidation catalysts (WOCs) using sodium periodate. Under the conditions used, these complexes serve as homogeneous WOCs as demonstrated via kinetic analysis and dynamic light scattering (DLS). The Fe(BPyA) salt serves as both a mononuclear and dinuclear catalyst, with the mononuclear form showing higher catalytic activity. Based on the H/D kinetic isotope effect and pH dependence, the rate determining step (RDS) in water oxidation (WO) by Fe(BPyA) is nucleophilic attack by water during O-O bond formation. In contrast, Fe(TPA) shows complex kinetic behavior due to the formation of multiple oxidation states of the complex in solution, each of which exhibits catalytic activity for WO. The RDS in WO by Fe(TPA) follows an equilibrium established between monomeric and dimeric forms of the catalyst. Under acidic conditions formation of the monomer is favored, which leads to an increase in the WO rate. This journal is

元の言語英語
ページ(範囲)12501-12513
ページ数13
ジャーナルDalton Transactions
43
発行部数33
DOI
出版物ステータス出版済み - 9 7 2014

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Iron
Oxidation
Catalysts
Water
Amines
Kinetics
Catalyst activity
Salts
Propionates
Dynamic light scattering
metaperiodate
Isotopes
Monomers

All Science Journal Classification (ASJC) codes

  • Inorganic Chemistry

これを引用

Mechanism of water oxidation by non-heme iron catalysts when driven with sodium periodate. / Parent, Alexander R.; Nakazono, Takashi; Lin, Shu; Utsunomiya, Satoshi; Sakai, Ken.

:: Dalton Transactions, 巻 43, 番号 33, 07.09.2014, p. 12501-12513.

研究成果: ジャーナルへの寄稿記事

Parent, Alexander R. ; Nakazono, Takashi ; Lin, Shu ; Utsunomiya, Satoshi ; Sakai, Ken. / Mechanism of water oxidation by non-heme iron catalysts when driven with sodium periodate. :: Dalton Transactions. 2014 ; 巻 43, 番号 33. pp. 12501-12513.
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AU - Sakai, Ken

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N2 - Iron tris(2-methylpyridyl)amine (TPA) and iron 1-(bis(2-methylpyridyl) amino)-2-methyl-2-propanoate (BPyA) salts are characterized as water oxidation catalysts (WOCs) using sodium periodate. Under the conditions used, these complexes serve as homogeneous WOCs as demonstrated via kinetic analysis and dynamic light scattering (DLS). The Fe(BPyA) salt serves as both a mononuclear and dinuclear catalyst, with the mononuclear form showing higher catalytic activity. Based on the H/D kinetic isotope effect and pH dependence, the rate determining step (RDS) in water oxidation (WO) by Fe(BPyA) is nucleophilic attack by water during O-O bond formation. In contrast, Fe(TPA) shows complex kinetic behavior due to the formation of multiple oxidation states of the complex in solution, each of which exhibits catalytic activity for WO. The RDS in WO by Fe(TPA) follows an equilibrium established between monomeric and dimeric forms of the catalyst. Under acidic conditions formation of the monomer is favored, which leads to an increase in the WO rate. This journal is

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