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http://www.sciencemag.org/cgi/content/abstract/328/5982/1141 Science 28 May 2010:Vol. 328. no. 5982, pp. 1141 - 1144DOI: 10.1126/science.1188267 Reports Interface-Confined Ferrous Centers for Catalytic Oxidation Qiang Fu,1,* Wei-Xue Li,1,2,* Yunxi Yao,1 Hongyang Liu,1 Hai-Yan Su,1,2 Ding Ma,1 Xiang-Kui Gu,1,2 Limin Chen,1 Zhen Wang,1 Hui Zhang,3 Bing Wang,3 Xinhe Bao1, Coordinatively unsaturated ferrous (CUF) sites confined in nanosized matrices are active centers in a wide range of enzyme and homogeneous catalytic reactions. Preparation of the analogous active sites at supported catalysts is of great importance in heterogeneous catalysis but remains a challenge. On the basis of surface science measurements and density functional calculations, we show that the interface confinement effect can be used to stabilize the CUF sites by taking advantage of strong adhesion between ferrous oxides and metal substrates. The interface-confined CUF sites together with the metal supports are active for dioxygen activation, producing reactive dissociated oxygen atoms. We show that the structural ensemble was highly efficient for carbon monoxide oxidation at low temperature under typical operating conditions of a proton-exchange membrane fuel cell. 1 State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China. 2 Center for Theoretical and Computational Chemistry, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China. 3 Hefei National Laboratory for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei 230026, China. |
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