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论文类型：期刊论文

发表时间：2012-08-01

发表刊物：ENERGY & ENVIRONMENTAL SCIENCE

收录刊物：SCIE、EI、Scopus

卷号：5

期号：8

页面范围：8229-8233

ISSN号：1754-5692

摘要：Here, we report that the water oxidation activity can be significantly increased by confining ruthenium molecular catalysts, such as Ru-II(bda)(pic)(2), in the nanocage of SBA-16. The TOF of Ru-II(bda)(pic)(2) confined in the nanocage increased from 1.2 to 8.7 s(-1) by simply increasing the number of Ru-II(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 Ru-II(bda)(pic)(2) confined in the nanocage can be as high as two times that of the homogeneous Ru-II(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.