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Supervisors' Foreword; Parts of this thesis have been published in the following journal articles:[1] Rentao Mu, Qiang Fu*, Li Jin, Liang Yu, Guangzong Fang, Dali Tan and Xinhe Bao*, Visualizing Chemical Reactions Confined Under Graphene, Angew. Chem. Int. Ed., 2012, (51):4856-4859[2] Rentao Mu, Qiang Fu*, Hong Xu, Hui Zhang, Yuying Huang, Zhen Jiang, Shuo Zhang, Dali Tan and Xinhe Bao*, Synergetic Effect of Surface and Subsurface Ni Species at Pt-Ni Bimetallic Catalysts for CO Oxidation, J. Am. Chem. Soc., 2011, (133; Acknowledgements; Contents; 1 Introduction

1.1 Modulating the Performance of Heterogeneous Catalysts1.1.1 Size Effect; 1.1.2 Surface Structure; 1.1.3 Support Effect; 1.1.4 Promotion Effect of Secondary Components; 1.2 Motivation and Conception of Thesis; References; 2 Experimental Section; 2.1 Model Samples and Precursors of Supported Nanoparticles; 2.2 UHV Systems; 2.2.1 Omicron Multi-nanoProbe System; 2.2.2 Deep Ultraviolet Photoemission Electron Microscopy System; 2.2.3 Leybold XPS System; 2.3 Experimental Methods of Model Systems; 2.4 Experimental Methods of Supported Nanoparticles; 3 Construction and Reactivity of Pt-Ni Catalysts

3.1 Motivation3.2 Pt-Ni Model Catalytic Systems; 3.2.1 Preparation of Various Ni-Pt(111) Structures; 3.2.2 Interfacial Catalysis on NiO1−X/Pt(111); 3.2.3 Synergetic Effect of Surface and Subsurface Ni; 3.3 Supported Pt-Ni Nanoparticle Catalysts; 3.4 Resonable Design of Pt-Ni Bicomponent Catalysts; 3.5 Summary; References; 4 Modulating the Structure and Reactivity of Pt-Ni Catalysts; 4.1 Introduction; 4.2 Ni-Pt(111) Model Catalytic Systems; 4.3 Pt-Ni/CB Nanoparticle Catalysts; 4.4 Summary; References; 5 Comparison of Pt-Fe and Pt-Ni Catalysts; 5.1 Introduction

5.2 FeOX/Pt(111) Model Catalytic Systems5.3 NiOX/Pt(111) Model Catalytic Systems; 5.4 Pt-Fe/CB and Pt-Ni/CB Nanoparticle Catalysts; 5.5 Summary; References; 6 Reactivity of Graphene-Confined Pt(111) Surface; 6.1 Introduction; 6.2 Preparation of Graphene on Pt(111) Surface; 6.3 CO Intercalation; 6.4 The Confinement Effect of Graphene; 6.5 In Situ Visualizing Single-Channel Reaction; 6.6 Summary; References; 7 Conclusions

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