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High-loading and thermally stable Pt1/MgAl1.2Fe0.8O4 single-atom catalysts for high-temperature applications

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  • ReceivedFeb 1, 2020
  • AcceptedFeb 13, 2020
  • PublishedMar 5, 2020

Abstract


Funded by

the National Key Projects for Fundamental Research and Development of China(2016YFA0202801)

the National Natural Science Foundation of China(21673226,91645203,21590792)

the “Transformational Technologies for Clean Energy and Demonstration”

Strategic Priority Research Program of the Chinese Academy of Sciences(XDA21040200)

the Strategic Priority Research Program of the Chinese Academy of Sciences(XDB17000000)


Acknowledgment

This work was supported by the National Key Projects for Fundamental Research and Development of China (2016YFA0202801), the National Natural Science Foundation of China (21673226, 91645203 and 21590792), the “Transformational Technologies for Clean Energy and Demonstration”, the Strategic Priority Research Program of the Chinese Academy of Sciences (XDA21040200 and XDB17000000). The calculations were performed by using supercomputers at Tsinghua National Laboratory for Information Science and Technology and the Computational Chemistry Laboratory of Department of Chemistry at Tsinghua University, which was supported by the Tsinghua Xuetang Talents Program. The synchrotron radiation experiment was performed at the BL14W1 at Shanghai Synchrotron Radiation Facility, China.


Interest statement

The authors declare that they have no conflict of interest.


Contributions statement

Liu K synthesized the catalysts and performed most of the experiments, collected and analyzed the data. Tang Y and Li J performed DFT calculations and the theoretical analyses. Yu Z analyzed the STEM data. Ge B performed the aberration-corrected scanning transmission electron microscopy characterization. Ren G, Zhang J, Sun X and Chen Z did some experiments and characterizations. Ren Y and Liu X carried out the XAFS characterization. Liu K, Tang Y, Qiao B, Li WZ and Li J co-wrote the manuscript. Qiao B, Li W, Wang A and Li J designed the study and supervised the project. All authors contributed to the general discussion.


Author information

Kaipeng Liu is currently a PhD candidate at Dalian Institute of Chemical Physics, Chinese Academy of Sciences. He received his BSc degree (majored in chemistry) from the College of Chemistry, Jilin University in 2014. His PhD research focuses on thermally stable single atom catalysis.


Yan Tang received her BSc degree from the School of Chemistry and Molecular Engineering, East China University of Science and Technology (ECUST) in 2014 and her PhD degree from Tsinghua University in 2019. Her PhD research focuses on the theoretical investigations on single atom catalysts (SACs).


Botao Qiao is currently a professor at Dalian Institute of Chemical Physics, Chinese Academy of Sciences. He received his PhD degree from Lanzhou Institute of Chemical Physics, Chinese Academy of Sciences in 2007, and then became a postdoctoral fellow in Dalian Institute of Chemical Physics where he has worked until present. He visited Arizona State University, USA, from 2012 to 2015. His research interests are focused on the design, synthesis and characterization of highly dispersed supported metal catalysts, especially on the subnano or single-atom catalysts.


Wei-Zhen Li received his PhD degree from Peking University in 2007. He did postdoctoral research at Tsinghua University from 2007 to 2009 and then at the Pacific Northwest National Laboratory (USA) from 2010 to 2014. He is now a full Professor at Dalian Institute of Chemical Physics, Chinese Academy of Sciences. His research focuses on heterogeneous catalysis, especially on designing of antisintering precious nanocatalysts for energy and environment related reactions under harsh reaction conditions.


Jun Li received his PhD degree from Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences in 1992. He did postdoctoral research at the University of Siegen and the Ohio State University from 1994 to 1997. He worked as a research scientist at Ohio State University and senior research scientist at the Pacific Northwest National Laboratory from 1997 to 2009. He is now a full Professor at Tsinghua University. His research involves theoretical chemistry, heavy-element chemistry, and computational catalysis science.


Supplement

Supplementary information

Supporting data are available in the online version of the paper.


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  • Figure 1

    AC HAADF-STEM images of (a) Pt-CD-300, (b) Pt-CD-600, (c, d) Pt-CD-800 and the Pt-CD-800 sample in (e) <101¯> and (f) <001> directions (insets are patterns of A and B sites in AB2O4 spinel oxide).

  • Figure 2

    (a) CO-DRIFTS, (b) H2-TPR profiles, (c) Al 2p-Pt 4f XPS, and (d) Fourier transform of EXAFS spectra at Pt LIII edge for the Pt/MAFO samples (without phase correction).

  • Figure 3

    AC HAADF-STEM images of the (a) 3Pt-CD-700, (b, c) 5Pt-IWI-720. (d) Intensity analysis for the 5Pt-IWI-720 sample.

  • Figure 4

    Structure and formation energy for the Pt1/MgAl2O4 and Pt1/MgFeAlO4 at Al and Fe site at T = 1100 K. Color code: platinum (blue), oxygen (red), iron (purple), and aluminum (magenta).

  • Figure 5

    (a) N2O conversion as a function of temperature for the Pt samples. Reaction conditions: 1000 ppm N2O, and balance Ar. GHSV: 20,000 mL g−1cat. h−1. (b) The N2O conversion as a function of reaction time on the Pt-IWI-800 catalyst tested at 650°C. Reaction conditions: 1000 ppm N2O, and balance Ar. GHSV: 20,000 mL g−1cat. h−1.