Catalytic water oxidation by ruthenium(II) quaterpyridine (qpy) complexes: Evidence for ruthenium(III) qpy-N,N''-dioxide as the real catalysts

Yingying Liu; Siu Mui Ng; Shek Man Yiu; William W.Y. Lam; Xi Guang Wei; Kai Chung Lau; Tai Chu Lau

doi:10.1002/anie.201408795

Catalytic water oxidation by ruthenium(II) quaterpyridine (qpy) complexes: Evidence for ruthenium(III) qpy-N,N''-dioxide as the real catalysts

Yingying Liu, Siu Mui Ng, Shek Man Yiu, William W.Y. Lam, Xi Guang Wei, Kai Chung Lau, Tai Chu Lau

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

69 Citations (Scopus)

Abstract

Polypyridyl and related ligands have been widely used for the development of water oxidation catalysts. Supposedly these ligands are oxidation-resistant and can stabilize high-oxidation-state intermediates. In this work a series of ruthenium(II) complexes [Ru(qpy)(L)2] (qpy= 2,2' :6',2":6'',2'''-quaterpyridine; L = substituted pyridine) have been synthesized and found to catalyze Ce-driven water oxidation, with turnover numbers of up to 2100. However, these ruthenium complexes are found to function only as precatalysts; first, they have to be oxidized to the qpy-N,N'''- dioxide (ONNO) complexes [Ru(ONNO)(L)2] which are the real catalysts for water oxidation.

Original language	English
Pages (from-to)	14468-14471
Number of pages	4
Journal	Angewandte Chemie - International Edition
Volume	53
Issue number	52
DOIs	https://doi.org/10.1002/anie.201408795
Publication status	Published - 22 Dec 2014
Externally published	Yes

Keywords

Density functional calculations
Homogeneous catalysis
Polypyridyl ligands
Ruthenium complexes
Water oxidation

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10.1002/anie.201408795

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title = "Catalytic water oxidation by ruthenium(II) quaterpyridine (qpy) complexes: Evidence for ruthenium(III) qpy-N,N''-dioxide as the real catalysts",

abstract = "Polypyridyl and related ligands have been widely used for the development of water oxidation catalysts. Supposedly these ligands are oxidation-resistant and can stabilize high-oxidation-state intermediates. In this work a series of ruthenium(II) complexes [Ru(qpy)(L)2] (qpy= 2,2' :6',2{"}:6'',2'''-quaterpyridine; L = substituted pyridine) have been synthesized and found to catalyze Ce-driven water oxidation, with turnover numbers of up to 2100. However, these ruthenium complexes are found to function only as precatalysts; first, they have to be oxidized to the qpy-N,N'''- dioxide (ONNO) complexes [Ru(ONNO)(L)2] which are the real catalysts for water oxidation.",

keywords = "Density functional calculations, Homogeneous catalysis, Polypyridyl ligands, Ruthenium complexes, Water oxidation",

author = "Yingying Liu and Ng, {Siu Mui} and Yiu, {Shek Man} and Lam, {William W.Y.} and Wei, {Xi Guang} and Lau, {Kai Chung} and Lau, {Tai Chu}",

note = "Publisher Copyright: {\textcopyright} 2014 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim ,.",

year = "2014",

month = dec,

day = "22",

doi = "10.1002/anie.201408795",

language = "English",

volume = "53",

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TY - JOUR

T1 - Catalytic water oxidation by ruthenium(II) quaterpyridine (qpy) complexes

T2 - Evidence for ruthenium(III) qpy-N,N''-dioxide as the real catalysts

AU - Liu, Yingying

AU - Ng, Siu Mui

AU - Yiu, Shek Man

AU - Lam, William W.Y.

AU - Wei, Xi Guang

AU - Lau, Kai Chung

AU - Lau, Tai Chu

PY - 2014/12/22

Y1 - 2014/12/22

N2 - Polypyridyl and related ligands have been widely used for the development of water oxidation catalysts. Supposedly these ligands are oxidation-resistant and can stabilize high-oxidation-state intermediates. In this work a series of ruthenium(II) complexes [Ru(qpy)(L)2] (qpy= 2,2' :6',2":6'',2'''-quaterpyridine; L = substituted pyridine) have been synthesized and found to catalyze Ce-driven water oxidation, with turnover numbers of up to 2100. However, these ruthenium complexes are found to function only as precatalysts; first, they have to be oxidized to the qpy-N,N'''- dioxide (ONNO) complexes [Ru(ONNO)(L)2] which are the real catalysts for water oxidation.

AB - Polypyridyl and related ligands have been widely used for the development of water oxidation catalysts. Supposedly these ligands are oxidation-resistant and can stabilize high-oxidation-state intermediates. In this work a series of ruthenium(II) complexes [Ru(qpy)(L)2] (qpy= 2,2' :6',2":6'',2'''-quaterpyridine; L = substituted pyridine) have been synthesized and found to catalyze Ce-driven water oxidation, with turnover numbers of up to 2100. However, these ruthenium complexes are found to function only as precatalysts; first, they have to be oxidized to the qpy-N,N'''- dioxide (ONNO) complexes [Ru(ONNO)(L)2] which are the real catalysts for water oxidation.

KW - Density functional calculations

KW - Homogeneous catalysis

KW - Polypyridyl ligands

KW - Ruthenium complexes

KW - Water oxidation

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U2 - 10.1002/anie.201408795

DO - 10.1002/anie.201408795

M3 - Article

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SN - 1433-7851

VL - 53

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EP - 14471

JO - Angewandte Chemie - International Edition

JF - Angewandte Chemie - International Edition

IS - 52

ER -

Catalytic water oxidation by ruthenium(II) quaterpyridine (qpy) complexes: Evidence for ruthenium(III) qpy-N,N''-dioxide as the real catalysts

Abstract

Keywords

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