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Nano Research

Article Title

Facile synthesis of Au embedded CuOx-CeO2 core/shell nanospheres as highly reactive and sinter-resistant catalysts for catalytic hydrogenation of p-nitrophenol

Authors

Ke Wu, ;Beijing National Laboratory for Molecular Sciences, State Key Laboratory of Rare Earth Materials Chemistry and Applications, PKU-HKU Joint Laboratory in Rare Earth Materials and Bioinorganic Chemistry, and College of Chemistry and Molecular Engineering, Peking University, Beijing 100871, China;
Xin-Yu Wang, ;Beijing National Laboratory for Molecular Sciences, State Key Laboratory of Rare Earth Materials Chemistry and Applications, PKU-HKU Joint Laboratory in Rare Earth Materials and Bioinorganic Chemistry, and College of Chemistry and Molecular Engineering, Peking University, Beijing 100871, China;
Ling-Ling Guo, Shanghai Synchrotron Radiation Facility, Shanghai Institute of Applied Physics, Chinese Academy of Sciences, Shanghai 201204, China;
Yue-Jiao Xu, ;Beijing National Laboratory for Molecular Sciences, State Key Laboratory of Rare Earth Materials Chemistry and Applications, PKU-HKU Joint Laboratory in Rare Earth Materials and Bioinorganic Chemistry, and College of Chemistry and Molecular Engineering, Peking University, Beijing 100871, China;
Liang Zhou, ;Beijing National Laboratory for Molecular Sciences, State Key Laboratory of Rare Earth Materials Chemistry and Applications, PKU-HKU Joint Laboratory in Rare Earth Materials and Bioinorganic Chemistry, and College of Chemistry and Molecular Engineering, Peking University, Beijing 100871, China;
Ze-Yu Lyu, ;Beijing National Laboratory for Molecular Sciences, State Key Laboratory of Rare Earth Materials Chemistry and Applications, PKU-HKU Joint Laboratory in Rare Earth Materials and Bioinorganic Chemistry, and College of Chemistry and Molecular Engineering, Peking University, Beijing 100871, China;
Kang-Yu Liu, ;Beijing National Laboratory for Molecular Sciences, State Key Laboratory of Rare Earth Materials Chemistry and Applications, PKU-HKU Joint Laboratory in Rare Earth Materials and Bioinorganic Chemistry, and College of Chemistry and Molecular Engineering, Peking University, Beijing 100871, China;
Rui Si, Shanghai Synchrotron Radiation Facility, Shanghai Institute of Applied Physics, Chinese Academy of Sciences, Shanghai 201204, China;
Ya-Wen Zhang, ;Beijing National Laboratory for Molecular Sciences, State Key Laboratory of Rare Earth Materials Chemistry and Applications, PKU-HKU Joint Laboratory in Rare Earth Materials and Bioinorganic Chemistry, and College of Chemistry and Molecular Engineering, Peking University, Beijing 100871, China;
Ling-Dong Sun, ;Beijing National Laboratory for Molecular Sciences, State Key Laboratory of Rare Earth Materials Chemistry and Applications, PKU-HKU Joint Laboratory in Rare Earth Materials and Bioinorganic Chemistry, and College of Chemistry and Molecular Engineering, Peking University, Beijing 100871, China;
Chun-Hua Yan, ;Beijing National Laboratory for Molecular Sciences, State Key Laboratory of Rare Earth Materials Chemistry and Applications, PKU-HKU Joint Laboratory in Rare Earth Materials and Bioinorganic Chemistry, and College of Chemistry and Molecular Engineering, Peking University, Beijing 100871, China; College of Chemistry and Chemical Engineering, Lanzhou University, Lanzhou 730000, China;

Keywords

core/shell nanostructure, sinter-resistant catalysts, triphasic interfaces catalysis, p-nitrophenol reduction

Abstract

Exploring cost-effective catalysts with high catalytic performance and long-term stability has always been a general concern for environment protection and energy conversion. Here, Au nanoparticles (NPs) embedded CuOx–CeO2 core/shell nanospheres (Au@CuOx–CeO2 CSNs) have been successfully prepared through a versatile one-pot method at ambient conditions. The spontaneous auto-redox reaction between HAuCl4 and Ce(OH)3 in aqueous solution triggered the self-assembly growth of micro-/ nanostructural Au@CuOx–CeO2 CSNs. Meanwhile, the CuOx clusters in Au@CuOx–CeO2 CSNs are capable of improving the anti-sintering ability of Au NPs and providing synergistic catalysis benefits. As a result, the confined Au NPs exhibited extraordinary thermal stability even at a harsh thermal condition up to 700 C. In addition, before and after the severe calcination process, Au@CuOx–CeO2 CSNs can exhibit enhanced catalytic activity and excellent recyclability towards the hydrogenation of p-nitrophenol compared to previously reported nanocatalysts. The synergistic catalysis path between Au/CuOx/CeO2 triphasic interfaces was revealed by density functional theory (DFT) calculations. The CuOx clusters around the embedded Au NPs can provide moderate adsorption strength of p-nitrophenol, while the adjacent CeO2-supported Au NPs can facilitate the hydrogen dissociation to form H* species, which contributes to achieve the efficient reduction of p-nitrophenol. This study opens up new possibilities for developing high-efficient and sintering-resistant micro-/nanostructural nanocatalysts by exploiting multiphasic systems.

Graphical Abstract

Publisher

Tsinghua University Press

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