Electrocatalytic Water Oxidation by a Monomeric Amidate-Ligated Fe(III)-Aqua Complex

被引：208

作者：

Coggins, Michael K. ^{[1
]}

Zhang, Ming-Tian ^{[1
]}

Vannucci, Aaron K. ^{[1
]}

Dares, Christopher J. ^{[1
]}

Meyer, Thomas J. ^{[1
]}

机构：

[1] Univ N Carolina, Dept Chem, Chapel Hill, NC 27599 USA

来源：

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY | 2014年 / 136卷 / 15期

关键词：

O BOND FORMATION; METAL-ORGANIC FRAMEWORKS; COUPLED ELECTRON-TRANSFER; VISIBLE-LIGHT-DRIVEN; PROPYLENE CARBONATE; SINGLE-SITE; OXYGEN EVOLUTION; PHOTOSYSTEM-II; CAPILLARY-ELECTROPHORESIS; IRIDIUM COMPLEXES;

D O I：

10.1021/ja412822u

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

The six-coordinate Fe-III-aqua complex [Fe-III(dpaq)(H2O)](2+) (1, dpaq is 2-[bis(pyridine-2-ylmethyl)]amino-N-quinolin-8-yl-acetamido) is an electrocatalyst for water oxidation in propylene carbonate-water mixtures. An electrochemical kinetics study has revealed that water oxidation occurs by oxidation to Fe-V(O)(2+) followed by a reaction first order in catalyst and added water, respectively, with k(o) = 0.035(4) M-1 s(-1) by the single-site mechanism found previously for Ru and Ir water oxidation catalysts. Sustained water oxidation catalysis occurs at a high surface area electrode to give O-2 through at least 29 turnovers over an 15 h electrolysis period with a 45% Faradaic yield and no observable decomposition of the catalyst.

引用

页码：5531 / 5534

页数：4

共 62 条

[1] An Amide-Linked Chromophore-Catalyst Assembly for Water Oxidation [J].

Ashford, Dennis L. ;

Stewart, David J. ;

Glasson, Christopher R. ;

Binstead, Robert A. ;

Harrison, Daniel P. ;

Norris, Michael R. ;

Concepcion, Javier J. ;

Fang, Zhen ;

Templeton, Joseph L. ;

Meyer, Thomas J. .

INORGANIC CHEMISTRY, 2012, 51 (12) :6428-6430

[2] WATER PHOTOLYSIS .1. THE PHOTOLYSIS OF COORDINATED WATER IN [(MNL-(H2O))2][CLO4]2 (L = DIANION OF TETRADENTATE O2N2-DONOR SCHIFF-BASES) - A MODEL FOR THE MANGANESE SITE IN PHOTOSYSTEM-II OF GREEN PLANT PHOTOSYNTHESIS [J].

ASHMAWY, FM ;

MCAULIFFE, CA ;

PARISH, RV ;

TAMES, J .

JOURNAL OF THE CHEMICAL SOCIETY-DALTON TRANSACTIONS, 1985, (07) :1391-1397

[3]

Barnett SM, 2012, NAT CHEM, V4, P498, DOI [10.1038/NCHEM.1350, 10.1038/nchem.1350]

[4] Electronic design criteria for O-O bond formation via metal-oxo complexes [J].

Betley, Theodore A. ;

Wu, Qin ;

Van Voorhis, Troy ;

Nocera, Daniel G. .

INORGANIC CHEMISTRY, 2008, 47 (06) :1849-1861

[5] Characterization of an Amorphous Iridium Water-Oxidation Catalyst Electrodeposited from Organometallic Precursors [J].

Blakemore, James D. ;

Mara, Michael W. ;

Kushner-Lenhoff, Maxwell N. ;

Schley, Nathan D. ;

Konezny, Steven J. ;

Rivalta, Ivan ;

Negre, Christian F. A. ;

Snoeberger, Robert C. ;

Kokhan, Oleksandr ;

Huang, Jier ;

Stickrath, Andrew ;

Lan Anh Tran ;

Parr, Maria L. ;

Chen, Lin X. ;

Tiede, David M. ;

Batista, Victor S. ;

Crabtree, Robert H. ;

Brudvig, Gary W. .

INORGANIC CHEMISTRY, 2013, 52 (04) :1860-1871

[6] Determination of the dissociation constants (pKa) of secondary and tertiary amines in organic media by capillary electrophoresis and their role in the electrophoretic mobility order inversion [J].

Cantu, MD ;

Hillebrand, S ;

Carrilho, E .

JOURNAL OF CHROMATOGRAPHY A, 2005, 1068 (01) :99-105

[7] A new zirconium inorganic building brick forming metal organic frameworks with exceptional stability [J].

Cavka, Jasmina Hafizovic ;

Jakobsen, Soren ;

Olsbye, Unni ;

Guillou, Nathalie ;

Lamberti, Carlo ;

Bordiga, Silvia ;

Lillerud, Karl Petter .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2008, 130 (42) :13850-13851

[8] Chemical and Visible-Light-Driven Water Oxidation by Iron Complexes at pH 7-9: Evidence for Dual-Active Intermediates in Iron-Catalyzed Water Oxidation [J].

Chen, Gui ;

Chen, Lingjing ;

Ng, Siu-Mui ;

Man, Wai-Lun ;

Lau, Tai-Chu .

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2013, 52 (06) :1789-1791

[9] Cu(II)/Cu(0) electrocatalyzed CO2 and H2O splitting [J].

Chen, Zuofeng ;

Kang, Peng ;

Zhang, Ming-Tian ;

Stoner, Brian R. ;

Meyer, Thomas J. .

ENERGY & ENVIRONMENTAL SCIENCE, 2013, 6 (03) :813-817

[10] Copper(II) Catalysis of Water Oxidation [J].

Chen, Zuofeng ;

Meyer, Thomas J. .

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2013, 52 (02) :700-703

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