Abstract
Single-atom catalysts (SACs) have attracted extensive attention in the field of heterogeneous catalysis. However, the fabrication of SACs with high loading and high-temperature stability remains a grand challenge, especially on oxide supports. In this work, we have demonstrated that through strong covalent metal-support interaction, high-loading and thermally stable single-atom Pt catalysts can be readily prepared by using Fe modified spinel as support. Better catalytic performance in N2O decomposition reaction is obtained on such SACs than their nanocatalyst counterpart and low-surface-area Fe2O3 supported Pt SACs. This work provides a strategy for the fabrication of high-loading and thermally stable SACs for applications at high temperatures.
摘要
近年来, 单原子催化剂(SACs)在非均相催化领域引起了广泛的关注. 然而, 制备高负载量和高热稳定的单原子催化剂(特别是在以氧化物作为载体的情况下)仍然是巨大的挑战. 在本工作中, 我们证明通过强共价金属-载体相互作用(CMSI), 使用铁改性的尖晶石作为载体, 可制得高负载和高温热稳定的Pt单原子催化剂. 对于N2O分解反应, 此类单原子催化剂催化性能优于其相应的纳米催化剂和低表面积Fe2O3作为载体负载的Pt单原子催化剂. 本工作为在高温下制备高载量和热稳定的单原子催化剂提供了新的策略.
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Acknowledgements
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.
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Author contributions 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.
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The authors declare that they have no conflict of interest.
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 Che- mical 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.
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.
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Liu, K., Tang, Y., Yu, Z. et al. High-loading and thermally stable Pt1/MgAl1.2Fe0.8O4 single-atom catalysts for high-temperature applications. Sci. China Mater. 63, 949–958 (2020). https://doi.org/10.1007/s40843-020-1267-2
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DOI: https://doi.org/10.1007/s40843-020-1267-2