Designing ligands to achieve robust oxidation catalysts. Iron based systems

Michael J. Bartos; Scott W. Gordon-Wylie; Brian G. Fox; L. James Wright; Susan T. Weintraub; Karl E. Kauffmann; Eckard Münck; Kimberly L. Kostka; Erich S. Uffelman; Clifton E.F. Rickard; Kathleen R. Noon; Terrence J. Collins

doi:10.1016/S0010-8545(98)00142-8

Designing ligands to achieve robust oxidation catalysts. Iron based systems

Michael J. Bartos, Scott W. Gordon-Wylie, Brian G. Fox, L. James Wright, Susan T. Weintraub, Karl E. Kauffmann, Eckard Münck, Kimberly L. Kostka, Erich S. Uffelman, Clifton E.F. Rickard, Kathleen R. Noon, Terrence J. Collins

Biochemistry & Structural Biology

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

67 Scopus citations

Abstract

Nitrile solvents containing α-CH substituents are catalytically oxidized by the tetraamido-N-Fe^III-aqua complex, 3, with t-butyl hydroperoxide. Every observable product resulting from 3 has been characterized. An Fe^IV-cyano complex, 5, is the major inorganic product; the cyano ligand emanates from the solvent-substrate. A new type of ligand oxidative degradation giving 6 proceeds to ca. 10% of the iron macrocycle; its characterization indicates how the already robust macrocycle should be redesigned to further improve its oxidative stability. Such improvement has led to long-lived catalysts for hydrogen peroxide oxidation in water from neutral to basic pH at room temperature.

Original language	English (US)
Pages (from-to)	361-390
Number of pages	30
Journal	Coordination Chemistry Reviews
Volume	174
Issue number	1
DOIs	https://doi.org/10.1016/S0010-8545(98)00142-8
State	Published - Jul 1998

Keywords

High valent iron complexes
Iron-57 Mössbauer spectroscopy
Ligand design
Ligand oxidative degradation

ASJC Scopus subject areas

Physical and Theoretical Chemistry
Inorganic Chemistry
Materials Chemistry

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Bartos, M. J., Gordon-Wylie, S. W., Fox, B. G., Wright, L. J., Weintraub, S. T., Kauffmann, K. E., Münck, E., Kostka, K. L., Uffelman, E. S., Rickard, C. E. F., Noon, K. R., & Collins, T. J. (1998). Designing ligands to achieve robust oxidation catalysts. Iron based systems. Coordination Chemistry Reviews, 174(1), 361-390. https://doi.org/10.1016/S0010-8545(98)00142-8

Designing ligands to achieve robust oxidation catalysts. Iron based systems. / Bartos, Michael J.; Gordon-Wylie, Scott W.; Fox, Brian G.; Wright, L. James; Weintraub, Susan T.; Kauffmann, Karl E.; Münck, Eckard; Kostka, Kimberly L.; Uffelman, Erich S.; Rickard, Clifton E.F.; Noon, Kathleen R.; Collins, Terrence J.

In: Coordination Chemistry Reviews, Vol. 174, No. 1, 07.1998, p. 361-390.

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

Bartos, Michael J. ; Gordon-Wylie, Scott W. ; Fox, Brian G. ; Wright, L. James ; Weintraub, Susan T. ; Kauffmann, Karl E. ; Münck, Eckard ; Kostka, Kimberly L. ; Uffelman, Erich S. ; Rickard, Clifton E.F. ; Noon, Kathleen R. ; Collins, Terrence J. / Designing ligands to achieve robust oxidation catalysts. Iron based systems. In: Coordination Chemistry Reviews. 1998 ; Vol. 174, No. 1. pp. 361-390.

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abstract = "Nitrile solvents containing α-CH substituents are catalytically oxidized by the tetraamido-N-FeIII-aqua complex, 3, with t-butyl hydroperoxide. Every observable product resulting from 3 has been characterized. An FeIV-cyano complex, 5, is the major inorganic product; the cyano ligand emanates from the solvent-substrate. A new type of ligand oxidative degradation giving 6 proceeds to ca. 10% of the iron macrocycle; its characterization indicates how the already robust macrocycle should be redesigned to further improve its oxidative stability. Such improvement has led to long-lived catalysts for hydrogen peroxide oxidation in water from neutral to basic pH at room temperature.",

keywords = "High valent iron complexes, Iron-57 M{\"o}ssbauer spectroscopy, Ligand design, Ligand oxidative degradation",

author = "Bartos, {Michael J.} and Gordon-Wylie, {Scott W.} and Fox, {Brian G.} and Wright, {L. James} and Weintraub, {Susan T.} and Kauffmann, {Karl E.} and Eckard M{\"u}nck and Kostka, {Kimberly L.} and Uffelman, {Erich S.} and Rickard, {Clifton E.F.} and Noon, {Kathleen R.} and Collins, {Terrence J.}",

note = "Funding Information: This work was supported by the NIH, GM44867 (T.J.C.) and GM22701 (E.M.). We thank Professor Larry Que and Dr Anne True of the University of Minnesota for EXAFS analysis of 5 and Professor David Bocian for ascertaining that 5 rapidly photobleaches when studied by resonance Raman. We also thank Dr Colin Horwitz of Carnegie Mellon University for helpful discussions. ",

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doi = "10.1016/S0010-8545(98)00142-8",

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AU - Uffelman, Erich S.

AU - Rickard, Clifton E.F.

AU - Noon, Kathleen R.

AU - Collins, Terrence J.

N1 - Funding Information: This work was supported by the NIH, GM44867 (T.J.C.) and GM22701 (E.M.). We thank Professor Larry Que and Dr Anne True of the University of Minnesota for EXAFS analysis of 5 and Professor David Bocian for ascertaining that 5 rapidly photobleaches when studied by resonance Raman. We also thank Dr Colin Horwitz of Carnegie Mellon University for helpful discussions.

PY - 1998/7

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N2 - Nitrile solvents containing α-CH substituents are catalytically oxidized by the tetraamido-N-FeIII-aqua complex, 3, with t-butyl hydroperoxide. Every observable product resulting from 3 has been characterized. An FeIV-cyano complex, 5, is the major inorganic product; the cyano ligand emanates from the solvent-substrate. A new type of ligand oxidative degradation giving 6 proceeds to ca. 10% of the iron macrocycle; its characterization indicates how the already robust macrocycle should be redesigned to further improve its oxidative stability. Such improvement has led to long-lived catalysts for hydrogen peroxide oxidation in water from neutral to basic pH at room temperature.

AB - Nitrile solvents containing α-CH substituents are catalytically oxidized by the tetraamido-N-FeIII-aqua complex, 3, with t-butyl hydroperoxide. Every observable product resulting from 3 has been characterized. An FeIV-cyano complex, 5, is the major inorganic product; the cyano ligand emanates from the solvent-substrate. A new type of ligand oxidative degradation giving 6 proceeds to ca. 10% of the iron macrocycle; its characterization indicates how the already robust macrocycle should be redesigned to further improve its oxidative stability. Such improvement has led to long-lived catalysts for hydrogen peroxide oxidation in water from neutral to basic pH at room temperature.

KW - High valent iron complexes

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Designing ligands to achieve robust oxidation catalysts. Iron based systems

Abstract

Keywords

ASJC Scopus subject areas

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