Multiple selectivity-determining mechanisms of H2O2 formation in iron porphyrin-catalysed oxygen reduction

被引：26

作者：

Brezny, Anna C. ^{[1
,2
]}

Nedzbala, Hannah S. ^{[1
]}

Mayer, James M. ^{[1
]}

机构：

[1] Yale Univ, Dept Chem, 225 Prospect St, New Haven, CT 06520 USA

[2] Skidmore Coll, Dept Chem, Saratoga Springs, NY 12866 USA

来源：

CHEMICAL COMMUNICATIONS | 2021年 / 57卷 / 10期

关键词：

All Open Access; Green;

D O I：

10.1039/d0cc06701f

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

Multiple H2O2-forming mechanisms are accessible in Fe(porphyrin)-catalysed oxygen reduction, a key reaction in both fuel cell technologies and oxygen-utilizing enzymes. Our kinetic analysis reveals that the porphyrin secondary structure dictates the pathway for H2O2 formation. This approach is generalizable to other electrocatalytic processes and provides insight into the selectivity-determining steps.

引用

页码：1202 / 1205

页数：4

共 25 条

[1] Rational Design of Mononuclear Iron Porphyrins for Facile and Selective 4e-/4H+ O2 Reduction: Activation of O-O Bond by 2nd Sphere Hydrogen Bonding [J].

Bhunia, Sarmistha ;

Rana, Atanu ;

Roy, Pronay ;

Martin, Daniel J. ;

Pegis, Michael L. ;

Roy, Bijan ;

Dey, Abhishek .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2018, 140 (30) :9444-9457

[2] Selectivity-Determining Steps in O2 Reduction Catalyzed by Iron(tetramesitylporphyrin) [J].

Brezny, Anna C. ;

Johnson, Samantha I. ;

Raugei, Simone ;

Mayer, James M. .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2020, 142 (09) :4108-4113

[3] Electrocatalytic Oxygen Reduction by Iron Tetra-arylporphyrins Bearing Pendant Proton Relays [J].

Carver, Colin T. ;

Matson, Benjamin D. ;

Mayer, James M. .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2012, 134 (12) :5444-5447

[4] Factors Determining the Rate and Selectivity of 4e-/4H+ Electrocatalytic Reduction of Dioxygen by Iron Porphyrin Complexes [J].

Chatterjee, Sudipta ;

Sengupta, Kushal ;

Mondal, Biswajit ;

Dey, Subal ;

Dey, Abhishek .

ACCOUNTS OF CHEMICAL RESEARCH, 2017, 50 (07) :1744-1753

[5] ON THE MECHANISM OF AUTOXIDATION OF IRON(II) PORPHYRINS - DETECTION OF A PEROXO-BRIDGED IRON(III) PORPHYRIN DIMER AND THE MECHANISM OF ITS THERMAL-DECOMPOSITION TO THE OXO-BRIDGED IRON(III) PORPHYRIN DIMER [J].

CHIN, DH ;

LAMAR, GN ;

BALCH, AL .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1980, 102 (13) :4344-4350

[6] Functional analogues of cytochrome c oxidase, myoglobin, and hemoglobin [J].

Collman, JP ;

Boulatov, R ;

Sunderland, CJ ;

Fu, L .

CHEMICAL REVIEWS, 2004, 104 (02) :561-588

[7] Structure and chemistry of cytochrome P450 [J].

Denisov, IG ;

Makris, TM ;

Sligar, SG ;

Schlichting, I .

CHEMICAL REVIEWS, 2005, 105 (06) :2253-2277

[8] Molecular electrocatalysts for the oxygen reduction reaction [J].

Dey, Subal ;

Mondal, Biswajit ;

Chatterjee, Sudipta ;

Rana, Atanu ;

Amanullah, S. K. ;

Dey, Abhishek .

NATURE REVIEWS CHEMISTRY, 2017, 1 (12)

[9] Hangman Corroles: Efficient Synthesis and Oxygen Reaction Chemistry [J].

Dogutan, Dilek K. ;

Stoian, Sebastian A. ;

McGuire, Robert, Jr. ;

Schwalbe, Matthias ;

Teets, Thomas S. ;

Nocera, Daniel G. .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2011, 133 (01) :131-140

[10] UNCOUPLING OF THE CYTOCHROME P-450CAM MONOOXYGENASE REACTION BY A SINGLE MUTATION, THREONINE-252 TO ALANINE OR VALINE - A POSSIBLE ROLE OF THE HYDROXY AMINO-ACID IN OXYGEN ACTIVATION [J].

IMAI, M ;

SHIMADA, H ;

WATANABE, Y ;

MATSUSHIMAHIBIYA, Y ;

MAKINO, R ;

KOGA, H ;

HORIUCHI, T ;

ISHIMURA, Y .

PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 1989, 86 (20) :7823-7827

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