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Nano Research 2020, 13(8): 2044-2055 https://doi.org/10.1007/s12274-020-2806-9
Research Article | Issue | Published: 05 August 2020

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

Show Author's Information Ke Wu1,§,  Xin-Yu Wang1,§,  Ling-Ling Guo2,  Yue-Jiao Xu1,  Liang Zhou1,  Ze-Yu Lyu1,  Kang-Yu Liu1,  Rui Si2,  Ya-Wen Zhang1,  Ling-Dong Sun1( ),  Chun-Hua Yan1,3( )
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
Shanghai Synchrotron Radiation Facility, Shanghai Institute of Applied Physics, Chinese Academy of Sciences, Shanghai 201204, China
College of Chemistry and Chemical Engineering, Lanzhou University, Lanzhou 730000, China

§ Ke Wu and Xin-Yu Wang contributed equally to this work.

Keywords:
core/shell nanostructure, sinter-resistant catalysts, triphasic interfaces catalysis, p-nitrophenol reduction
Topics:
Catalyst activityCerium oxideChlorine compoundsCost effectivenessDensity functional theoryGoldGold nanoparticlesHydrogenationNanocatalystsNanospheres Redox reactionsSelf assembly
Cite this article:
Wu K, Wang X-Y, Guo L-L, et al. Facile synthesis of Au embedded CuOx-CeO2 core/shell nanospheres as highly reactive and sinter-resistant catalysts for catalytic hydrogenation of p-nitrophenol. Nano Research, 2020, 13(8): 2044-2055. https://doi.org/10.1007/s12274-020-2806-9
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Abstract Full text Electronic supplementary material About this article

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.


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Electronic supplementary material
About this article

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

Show Author's information Ke Wu1,§, Xin-Yu Wang1,§, Ling-Ling Guo2, Yue-Jiao Xu1, Liang Zhou1, Ze-Yu Lyu1, Kang-Yu Liu1, Rui Si2, Ya-Wen Zhang1, Ling-Dong Sun1( ), Chun-Hua Yan1,3( )
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
Shanghai Synchrotron Radiation Facility, Shanghai Institute of Applied Physics, Chinese Academy of Sciences, Shanghai 201204, China
College of Chemistry and Chemical Engineering, Lanzhou University, Lanzhou 730000, China

§ Ke Wu and Xin-Yu Wang contributed equally to this work.

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.

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

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Publication history
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Acknowledgements

Publication history

Received: 19 February 2020
Revised: 24 March 2020
Accepted: 10 April 2020
Published: 05 August 2020
Issue date: August 2020

Copyright

© Tsinghua University Press and Springer-Verlag GmbH Germany, part of Springer Nature 2020

Acknowledgements

The authors are grateful for the financial support of the National Natural Science Foundation of China (Nos. 21590791, 21771005, 21931001, and 21927901), and Ministry of Science and Technology (MOST) of China (Nos. 2014CB643803, 2017YFA0205101, and 2017YFA0205104). The computational work was supported by the High-performance Computing Platform of Peking University. K. W. specifically thanks the National Postdoctoral Program for Innovative Talents under grant no. BX20190005, and the China Postdoctoral Science Foundation (No. 2019M660293).

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