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Nano Research 2022, 15(8): 7107-7115 https://doi.org/10.1007/s12274-022-4405-4
Research Article | Issue | Published: 31 May 2022

Engineering electrophilic atomic Ir sites on CeO2 colloidal spheres for selectivity control in hydrogenation of α,β-unsaturated carbonyl compounds

Show Author's Information Muhammad Mateen1( ),  Muhammad Nadeem Akhtar2,  Ling Gao1,  Weng-Chon (Max) CHEONG3( ),  Shanshan Lv4,  Yan Zhou4,  Zheng Chen4( )
College of Environment and Resources, Chongqing Technology and Business University, Chongqing 400067, China
Department of Chemistry, The Islamia University of Bahawalpur, Bahawalpur, Pakistan
Department of Physics and Chemistry, Faculty of Science and Technology, University of Macau, Macao 999078, China
School of Chemistry and Materials Science, Anhui Normal University, Wuhu 241002, China
Keywords:
self-assembly, ceria, single atom catalyst, hydrogenation, unsaturated carbonyl compounds, colloidal spheres
Topics:
Catalyst selectivity
Cite this article:
Mateen M, Akhtar MN, Gao L, et al. Engineering electrophilic atomic Ir sites on CeO2 colloidal spheres for selectivity control in hydrogenation of α,β-unsaturated carbonyl compounds. Nano Research, 2022, 15(8): 7107-7115. https://doi.org/10.1007/s12274-022-4405-4
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Abstract Full text Electronic supplementary material About this article

Selective hydrogenation of the carbonyl bond in α,β-unsaturated carbonyl compounds is rather challenging owing to the more feasible hydrogenation of ethylenic bond from both thermodynamic and kinetic aspects. Here, we demonstrate a facile emulsion-based molecule-nanoparticle self-assembly strategy for the atomic engineering of Ir species on three-dimensional CeO2 spheres (Ir1@CeO2). When applied to the hydrogenation of α,β-unsaturated aldehydes, Ir1@CeO2 catalyst remarkably exhibited ~ 100% selectivity towards unsaturated alcohols, whereas the formation of Ir nanoparticles on CeO2 drastically decreased the selectivity for unsaturated alcohols. Spectroscopic studies revealed that strong metal–support interactions triggered the charge transfer from Ir to CeO2, leading to the partial reduction of Ce4+ to Ce3+ along with the formation new Irδ+–O2––Ce3+(OV) interfaces. The electrophilic atomic Ir species at the Irδ+–O2––Ce3+ (OV) interfaces would therefore preferentially adsorb and facilitate hydrogenation of polar C=O bond to achieve exceptional selectivity.


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About this article

Engineering electrophilic atomic Ir sites on CeO2 colloidal spheres for selectivity control in hydrogenation of α,β-unsaturated carbonyl compounds

Show Author's information Muhammad Mateen1( ), Muhammad Nadeem Akhtar2, Ling Gao1, Weng-Chon (Max) CHEONG3( ), Shanshan Lv4, Yan Zhou4, Zheng Chen4( )
College of Environment and Resources, Chongqing Technology and Business University, Chongqing 400067, China
Department of Chemistry, The Islamia University of Bahawalpur, Bahawalpur, Pakistan
Department of Physics and Chemistry, Faculty of Science and Technology, University of Macau, Macao 999078, China
School of Chemistry and Materials Science, Anhui Normal University, Wuhu 241002, China

Abstract

Selective hydrogenation of the carbonyl bond in α,β-unsaturated carbonyl compounds is rather challenging owing to the more feasible hydrogenation of ethylenic bond from both thermodynamic and kinetic aspects. Here, we demonstrate a facile emulsion-based molecule-nanoparticle self-assembly strategy for the atomic engineering of Ir species on three-dimensional CeO2 spheres (Ir1@CeO2). When applied to the hydrogenation of α,β-unsaturated aldehydes, Ir1@CeO2 catalyst remarkably exhibited ~ 100% selectivity towards unsaturated alcohols, whereas the formation of Ir nanoparticles on CeO2 drastically decreased the selectivity for unsaturated alcohols. Spectroscopic studies revealed that strong metal–support interactions triggered the charge transfer from Ir to CeO2, leading to the partial reduction of Ce4+ to Ce3+ along with the formation new Irδ+–O2––Ce3+(OV) interfaces. The electrophilic atomic Ir species at the Irδ+–O2––Ce3+ (OV) interfaces would therefore preferentially adsorb and facilitate hydrogenation of polar C=O bond to achieve exceptional selectivity.

Keywords: self-assembly, ceria, single atom catalyst, hydrogenation, unsaturated carbonyl compounds, colloidal spheres

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Publication history
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Acknowledgements

Publication history

Received: 14 March 2022
Revised: 04 April 2022
Accepted: 06 April 2022
Published: 31 May 2022
Issue date: August 2022

Copyright

© Tsinghua University Press 2022

Acknowledgements

Acknowledgements

This work was supported by the National Natural Science Foundation of China (No. 21901007), the Natural Science Foundation of Anhui Province (No. 2008085QB83), the Science and Technology Development Fund (FDCT) of Macao SAR (No. 0032/2021/ITP) and the University of Macau (No. MYRG2020-00026-FST). We thank Dr. Chao Zhang for help in language modification.

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