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{[Ru(bda)]xLy}n Cross-linked Coordination Polymers: Toward Efficient Heterogeneous Catalysis for Water Oxidation in Organic Solvent-free System

Abstract

Development of polymeric catalysts for water splitting has receiving increasing attentions recently. In this work, we successively developed few novel cross-linked coordination polymers (CCPs) with a formula {[Ru(bda)]xLy}n as efficient heterogeneous catalysts for water oxidation in organic solvent-free system, where Ru(bda) represents the catalytic center. Detailed water oxidation catalytic kinetics studies suggested that the single-site water nucleophilic attack (WNA) is a general mechanism applied to these polymeric catalysts, different with the small-molecular reference [Ru(bda)(pic)2] (pic = 4-picoline). The experimental evidence also indicated the importance of interfacial wettability and the existence of Ru(bda)-macrocyclic fragments of polymer network in determining the overall catalytic activity. More interestingly, the end-capping modification via pyridine/dmso exchange reaction further removed the residual Ru(dmso)x moieties on the surfaces of polymer network, which led to improved performance with impressive TOF ~ 4.6 s-1 and TON ~ 750 in organic solvent-free system, even superior to [Ru(bda)(pic)2]. The rate of catalysis is among the highest heterogeneous systems reported so far. Electrochemical study showed these polymeric catalysts were also promising electrode materials for electrocatalytic water oxidation, and the electrode based on CCP/Nafion/ITO maintained ~ 73% of its initial activity after 27 cycles under optimal condition.

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Publication details

The article was received on 08 Nov 2017, accepted on 05 Jan 2018 and first published on 08 Jan 2018


Article type: Paper
DOI: 10.1039/C7NJ04330A
Citation: New J. Chem., 2018, Accepted Manuscript
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    {[Ru(bda)]xLy}n Cross-linked Coordination Polymers: Toward Efficient Heterogeneous Catalysis for Water Oxidation in Organic Solvent-free System

    T. Zheng and L. Li, New J. Chem., 2018, Accepted Manuscript , DOI: 10.1039/C7NJ04330A

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