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Nano Research 2024, 17(6): 4934-4942 https://doi.org/10.1007/s12274-024-6496-6
Research Article | Issue | Published: 07 March 2024

2D Ca/Nb-based perovskite oxide with Ta doping as highly efficient H2O2 synthesis catalyst

Show Author's Information Xingchen Yang1,2,§,  Yang Gao1,2,§,  Xiaohui Xu1,2,  Wenqiang Xu1,2,  Denghui Wang1,2,  Bin Luo3,  Dong Liu4,  Tao Liang5,6( ),  Bin Wang1,2( )
CAS Key Laboratory of Nanosystem and Hierarchical Fabrication, National Center for Nanoscience and Technology, Beijing 100190, China
University of Chinese Academy of Sciences, Beijing 100049, China
Nanomaterials Centre, School of Chemical Engineering and Australian Institute for Bioengineering and Nanotechnology, the University of Queensland, St Lucia, QLD 4072, Australia
State Key Laboratory of Organic–Inorganic Composites, College of Chemical Engineering, College of Materials Science and Engineering, Beijing University of Chemical Technology, Beijing 100029, China
Hangzhou Institute for Advanced Study, University of Chinese Academy of Sciences, Hangzhou 310024, China
State Key Lab of Silicon Materials, Zhejiang University, Hangzhou 310027, China

§ Xingchen Yang and Yang Gao contributed equally to this work.

Keywords:
catalyst, perovskite oxide, H2O2, two-electron oxygen reduction reaction, Ca2Nb3–xTaxO10– nanoflakes
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Yang X, Gao Y, Xu X, et al. 2D Ca/Nb-based perovskite oxide with Ta doping as highly efficient H2O2 synthesis catalyst. Nano Research, 2024, 17(6): 4934-4942. https://doi.org/10.1007/s12274-024-6496-6
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Abstract Full text Electronic supplementary material About this article

Perovskite oxides (POs) are emerging as a class of highly efficient catalysts for reducing oxygen to H2O. Although a rich variety of POs-based catalysts have been developed by tuning the complex composition, a highly efficient PO catalyst that is able to alter the reaction pathway from a 4e− process to a 2e− process for H2O2 production has rarely been achieved. We modified the structure and composition of a Ca- and Nb-based PO material by realizing a uniform two-dimensional (2D) morphology and varied Ta doping, resulting in the 2D Ca2Nb3−xTaxO10− (x = 0, 0.5, 1, and 1.5) monolayer catalysts. The obtained catalysts exhibit a dominant 2e− pathway and show exceptional H2O2 production efficiency. The typical Ca2Nb2.5Ta0.5O10− nanoflakes showed an onset potential of 0.735 V vs. reversible hydrogen electrode (RHE), a remarkably high selectivity over 95% across a wide range of 0.3–0.7 V, an impressively high Faradaic efficiency of 94%, and a notable H2O2 productivity of 1571 mmol·gcat−1·h−1. These findings highlight the great potential of 2D perovskite oxide nanoflakes as advanced electrocatalysts for 2e− oxygen reduction reaction.


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Electronic supplementary material
About this article

2D Ca/Nb-based perovskite oxide with Ta doping as highly efficient H2O2 synthesis catalyst

Show Author's information Xingchen Yang1,2,§, Yang Gao1,2,§, Xiaohui Xu1,2, Wenqiang Xu1,2, Denghui Wang1,2, Bin Luo3, Dong Liu4, Tao Liang5,6( ), Bin Wang1,2( )
CAS Key Laboratory of Nanosystem and Hierarchical Fabrication, National Center for Nanoscience and Technology, Beijing 100190, China
University of Chinese Academy of Sciences, Beijing 100049, China
Nanomaterials Centre, School of Chemical Engineering and Australian Institute for Bioengineering and Nanotechnology, the University of Queensland, St Lucia, QLD 4072, Australia
State Key Laboratory of Organic–Inorganic Composites, College of Chemical Engineering, College of Materials Science and Engineering, Beijing University of Chemical Technology, Beijing 100029, China
Hangzhou Institute for Advanced Study, University of Chinese Academy of Sciences, Hangzhou 310024, China
State Key Lab of Silicon Materials, Zhejiang University, Hangzhou 310027, China

§ Xingchen Yang and Yang Gao contributed equally to this work.

Abstract

Perovskite oxides (POs) are emerging as a class of highly efficient catalysts for reducing oxygen to H2O. Although a rich variety of POs-based catalysts have been developed by tuning the complex composition, a highly efficient PO catalyst that is able to alter the reaction pathway from a 4e− process to a 2e− process for H2O2 production has rarely been achieved. We modified the structure and composition of a Ca- and Nb-based PO material by realizing a uniform two-dimensional (2D) morphology and varied Ta doping, resulting in the 2D Ca2Nb3−xTaxO10− (x = 0, 0.5, 1, and 1.5) monolayer catalysts. The obtained catalysts exhibit a dominant 2e− pathway and show exceptional H2O2 production efficiency. The typical Ca2Nb2.5Ta0.5O10− nanoflakes showed an onset potential of 0.735 V vs. reversible hydrogen electrode (RHE), a remarkably high selectivity over 95% across a wide range of 0.3–0.7 V, an impressively high Faradaic efficiency of 94%, and a notable H2O2 productivity of 1571 mmol·gcat−1·h−1. These findings highlight the great potential of 2D perovskite oxide nanoflakes as advanced electrocatalysts for 2e− oxygen reduction reaction.

Keywords: catalyst, perovskite oxide, H2O2, two-electron oxygen reduction reaction, Ca2Nb3–xTaxO10– nanoflakes

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Publication history
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Acknowledgements

Publication history

Received: 26 September 2023
Revised: 12 January 2024
Accepted: 18 January 2024
Published: 07 March 2024
Issue date: June 2024

Copyright

© Tsinghua University Press 2024

Acknowledgements

Acknowledgements

We thank the financial support from the National Key Research and development Program of China (Nos. 2022YFF0712200 and 2021YFA1202802), the Young Elite Scientists Sponsorship Program by BAST (No. BYESS2023410), the visiting scholars fund support from State Key Lab of Silicon Materials, Zhejiang University (No. SKL2022-04), and the CAS Pioneer Hundred Talents Program.

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