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Bimetallic cooperative effect on O–O bond formation: copper polypyridyl complexes as water oxidation catalyst

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Abstract

The performance of water oxidation catalysis by a Cu-based polypyridyl complex, [CuII(TPA)(OH2)]2+ (1H; TPA = tris-(pyridylmethyl)amine), has been investigated in neutral aqueous solution by electrochemical methods. Compared with our previously reported binuclear catalyst, [(BPMAN)(CuII)2(μ-OH)]3+ (2; BPMAN = 2,7-[bis(2-pyridylmethyl)aminomethyl]-1,8-naphthyridine), mononuclear catalyst 1 has a higher overpotential and lower catalytic activity toward water oxidation under the same conditions. Experimental results revealed that the O–O bond formation occurred via a water nucleophilic attack mechanism in which formal CuIV(O) is proposed as a key intermediate for the mononuclear catalyst 1H. In contrast, for the binuclear catalyst, O–O bond formation was facilitated by bimetallic cooperation between the two CuIII centers.

Graphical abstract: Bimetallic cooperative effect on O–O bond formation: copper polypyridyl complexes as water oxidation catalyst

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Publication details

The article was received on 27 Apr 2018, accepted on 24 May 2018 and first published on 07 Jun 2018


Article type: Communication
DOI: 10.1039/C8DT01675E
Citation: Dalton Trans., 2018, Advance Article
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    Bimetallic cooperative effect on O–O bond formation: copper polypyridyl complexes as water oxidation catalyst

    X. Su, C. Zheng, Q. Hu, H. Du, R. Liao and M. Zhang, Dalton Trans., 2018, Advance Article , DOI: 10.1039/C8DT01675E

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