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Issue 8, 2012
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Oxygen evolution from water oxidation on molecular catalysts confined in the nanocages of mesoporous silicas†

Bo Li,a   Fei Li,b   Shiyang Bai,a   Zhijun Wang,a   Licheng Sun,b   Qihua Yang*a  and  Can Li*a  
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* Corresponding authors

a State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian National Laboratory for Clean Energy, 457 Zhongshan Road, Dalian 116023, China
E-mail: yangqh@dicp.ac.cn, canli@dicp.ac.cn

b State Key Laboratory of Fine Chemicals, Dalian University of Technology (DUT), Dalian 116024, China

Abstract

Here, we report that the water oxidation activity can be significantly increased by confining ruthenium molecular catalysts, such as RuII(bda)(pic)2, in the nanocage of SBA-16. The TOF of RuII(bda)(pic)2 confined in the nanocage increased from 1.2 to 8.7 s−1 by simply increasing the number of RuII(bda)(pic)2 molecules from one to seven in each nanocage, which is direct evidence for the “cooperative activation” mechanism involved in a binuclear reaction pathway for water oxidation reactions. The TOF of RuII(bda)(pic)2 confined in the nanocage can be as high as two times that of the homogeneous RuII(bda)(pic)2 due to the enhanced “cooperative activation” in the limited space of nanocages. Moreover, preliminary kinetic studies suggest that the stability of the molecular catalysts can be greatly improved after confinement in the nanocage. This strategy not only provides a new strategy for the preparation of highly efficient solid-hosted catalysts for water oxidation, but also gives direct evidence for the oxygen evolution mechanism.

Graphical abstract: Oxygen evolution from water oxidation on molecular catalysts confined in the nanocages of mesoporous silicas

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Supplementary files

Article information

Submitted
27 Apr 2012
Accepted
12 Jun 2012
First published
13 Jun 2012
Energy Environ. Sci., 2012,5, 8229-8233
Article type
Communication
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Oxygen evolution from water oxidation on molecular catalysts confined in the nanocages of mesoporous silicas

B. Li, F. Li, S. Bai, Z. Wang, L. Sun, Q. Yang and C. Li, Energy Environ. Sci., 2012, 5, 8229
DOI: 10.1039/C2EE22059H

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