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

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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 \({\rm{C}}{{\rm{a}}_2}{\rm{N}}{{\rm{b}}_{3 - x}}{\rm{T}}{{\rm{a}}_x}{{\rm{O}}_{10}}^ - \) (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 \({\rm{C}}{{\rm{a}}_2}{\rm{N}}{{\rm{b}}_{2.5}}{\rm{T}}{{\rm{a}}_{0.5}}{{\rm{O}}_{10}}^ - \) 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 \({\rm{mmol}} \cdot {{\rm{g}}_{{\rm{cat}}}}^{ - 1} \cdot {{\rm{h}}^{ - 1}}\). These findings highlight the great potential of 2D perovskite oxide nanoflakes as advanced electrocatalysts for 2e− oxygen reduction reaction.

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

Authors and Affiliations

  1. CAS Key Laboratory of Nanosystem and Hierarchical Fabrication, National Center for Nanoscience and Technology, Beijing, 100190, China

    Xingchen Yang, Yang Gao, Xiaohui Xu, Wenqiang Xu, Denghui Wang & Bin Wang

  2. University of Chinese Academy of Sciences, Beijing, 100049, China

    Xingchen Yang, Yang Gao, Xiaohui Xu, Wenqiang Xu, Denghui Wang & Bin Wang

  3. Nanomaterials Centre, School of Chemical Engineering and Australian Institute for Bioengineering and Nanotechnology, The University of Queensland, St Lucia, QLD, 4072, Australia

    Bin Luo

  4. 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

    Dong Liu

  5. Hangzhou Institute for Advanced Study, University of Chinese Academy of Sciences, Hangzhou, 310024, China

    Tao Liang

  6. State Key Lab of Silicon Materials, Zhejiang University, Hangzhou, 310027, China

    Tao Liang

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  1. Xingchen Yang
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Electronic Supplementary Material: 2D Ca/Nb-based perovskite oxide with Ta doping as highly efficient H2O2 synthesis catalyst

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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 Res. (2024). https://doi.org/10.1007/s12274-024-6496-6

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