Volume 126, Issue 48 pp. 13258-13264
Zuschrift

Homogeneous Electrocatalytic Water Oxidation at Neutral pH by a Robust Macrocyclic Nickel(II) Complex

Mei Zhang

Mei Zhang

MOE Key Laboratory of Bioinorganic and Synthetic Chemistry, State Key Laboratory of Optoelectronic Materials and Technologies, School of Chemistry and Chemical Engineering, Sun Yat-Sen University, Guangzhou 510275 (China)

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Dr. Ming-Tian Zhang

Dr. Ming-Tian Zhang

Center of Basic Molecular Science (CBMS), Department of Chemistry, Tsinghua University, Beijing 100084 (China)

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Cheng Hou

Cheng Hou

MOE Key Laboratory of Bioinorganic and Synthetic Chemistry, State Key Laboratory of Optoelectronic Materials and Technologies, School of Chemistry and Chemical Engineering, Sun Yat-Sen University, Guangzhou 510275 (China)

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Prof. Zhuo-Feng Ke

Corresponding Author

Prof. Zhuo-Feng Ke

MOE Key Laboratory of Bioinorganic and Synthetic Chemistry, State Key Laboratory of Optoelectronic Materials and Technologies, School of Chemistry and Chemical Engineering, Sun Yat-Sen University, Guangzhou 510275 (China)

MOE Key Laboratory of Bioinorganic and Synthetic Chemistry, State Key Laboratory of Optoelectronic Materials and Technologies, School of Chemistry and Chemical Engineering, Sun Yat-Sen University, Guangzhou 510275 (China)Search for more papers by this author
Prof. Tong-Bu Lu

Corresponding Author

Prof. Tong-Bu Lu

MOE Key Laboratory of Bioinorganic and Synthetic Chemistry, State Key Laboratory of Optoelectronic Materials and Technologies, School of Chemistry and Chemical Engineering, Sun Yat-Sen University, Guangzhou 510275 (China)

MOE Key Laboratory of Bioinorganic and Synthetic Chemistry, State Key Laboratory of Optoelectronic Materials and Technologies, School of Chemistry and Chemical Engineering, Sun Yat-Sen University, Guangzhou 510275 (China)Search for more papers by this author
First published: 09 September 2014
Citations: 80

This work was supported by the 973 Program of China (2012CB821706, 2014CB845602), the NSFC (grant nos. 21331007, 21121061, and 21203256), and the NSF of Guangdong Province (S2012030006240).

Abstract

The development of an earth-abundant, first-row water oxidation catalyst that operates at neutral pH and low overpotential remains a fundamental chemical challenge. Herein, we report the first nickel-based robust homogeneous water oxidation catalyst, which can electrocatalyze water oxidation at neutral pH and low overpotential in phosphate buffer. The results of DFT calculations verify that the OO bond formation in catalytic water oxidation prefers a HOOH coupling mechanism from a cis-isomer of the catalyst.

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