Abstract
Noble metals are downsized to nano-/subnanoscale to improve their catalytic activity and atom-economy. However, the stabilities in chemical state and catalytic performance of these nanocatalysts often suffer during harsh conditions. For Pt nanoparticles (NPs) supported on CeO2, activated oxygen diffused from the support over-stabilizes the active sites of Pt, degrading its performance at mild temperature. In this work, Pt nanocatalysts with unique structure of triple-junction are synthesized by selectively growing Pt NPs on the carbon-CeO2 interface. Impressively, the Pt NPs exhibit much enhanced catalytic stability and high activity for CO oxidation at mild temperature. The enhancement is attributed to electron donation from graphitized carbon and the confinement effect from the high-density nanopores of the CeO2 support. The triple-junction of Pt-C-CeO2, combining the merits of CeO2 for activating O2 and electron donating capability of carbon, provides new inspiration to the fabrication of high-performance nanocatalysts.
摘要
为提高贵金属催化剂的活性与原子经济性, 人们将其粒径降低至纳米/亚纳米尺度, 甚至开发各类单原子材料. 然而, 这些材料的结构状态和催化性能难以在苛刻的催化环境下保持稳定. 对于二氧化铈(CeO2)负载的Pt纳米粒子, 载体扩散到Pt粒子表面的活性氧物种稳定吸附在Pt表面, 导致金属Pt活性降低. 本文采用表面部分碳修饰的多孔CeO2为载体, 将纳米Pt选择性地生长在C-CeO2界面处形成特殊的三相界面结构, 对CO氧化表现出低温段增强的活性和稳定性. 石墨碳对纳米Pt的供电子效应和CeO2载体高密度纳米孔的限域效应共同贡献了纳米Pt的化学及结构稳定性. 本文设计的独特三相界面结构综合了CeO2活化氧以及碳贡献电子能力的 优点, 为制备新型高效金属催化材料提供了新的思路.
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Acknowledgements
This work was supported by the National Key Research and Development Program of China (2016YFB0701100), the National Natural Science Foundation of China (51771047, 51525101 and 51971059), and the Fundamental Research Funds for the Central Universities (N180204014).
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Author contributions Li S and Xu C conceived the idea and designed the experiments. Xu C, Zhang Y, and Chen J carried out the synthesis, characterization and catalytic experiments. All authors contributed to the discussion of the results and commented on the manuscript writing.
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Changjin Xu received his BSc degree from Inner Mongolia Agricultural University in 2014. Currently, he is a PhD student in the School of Materials Science and Engineering at Northeastern University (China). His research interests focus on the heterogeneous nanocatalysts.
Song Li is a professor of materials science and engineering at Northeastern University, China. He received his BSc degree in 2003 from Northeastern University and PhD degree in materials physics from the University of Lorraine in 2009. His current research focuses on metalbased structured catalysts, including noble metal alloys and intermetallics, metal-oxide interfaces, and processing intensification.
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Xu, C., Zhang, Y., Chen, J. et al. Carbon-CeO2 interface confinement enhances the chemical stability of Pt nanocatalyst for catalytic oxidation reactions. Sci. China Mater. 64, 128–136 (2021). https://doi.org/10.1007/s40843-020-1360-8
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DOI: https://doi.org/10.1007/s40843-020-1360-8