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一步法干球磨制备的钯嵌入二氧化铈催化剂卓越的甲烷氧化性能

Outstanding Methane Oxidation Performance of Palladium-Embedded Ceria Catalysts Prepared by a One-Step Dry Ball-Milling Method.

作者信息

Danielis Maila, Colussi Sara, de Leitenburg Carla, Soler Lluís, Llorca Jordi, Trovarelli Alessandro

机构信息

Polytechnic Department, University of Udine, Via del Cotonificio 108, 33100, Udine, Italy.

Institute of Energy Technologies, Department of Chemical Engineering and Barcelona Research Centre in Multiscale Science and Engineering, Universitat Politècnica de Catalunya, EEBE, Eduard Maristany 10-14, 08019, Barcelona, Spain.

出版信息

Angew Chem Int Ed Engl. 2018 Aug 6;57(32):10212-10216. doi: 10.1002/anie.201805929. Epub 2018 Jul 6.

Abstract

By carefully mixing Pd metal nanoparticles with CeO polycrystalline powder under dry conditions, an unpredicted arrangement of the Pd-O-Ce interface is obtained in which an amorphous shell containing palladium species dissolved in ceria is covering a core of CeO particles. The robust contact that is generated at the nanoscale, along with mechanical forces generated during mixing, promotes the redox exchange between Pd and CeO and creates highly reactive and stable sites constituted by PdO embedded into CeO surface layers. This specific arrangement outperforms conventional Pd/CeO reference catalysts in methane oxidation by lowering light-off temperature by more than 50°C and boosting the reaction rate. The origin of the outstanding activity is traced to the structural properties of the interface, modified at the nanoscale by mechanochemical interaction.

摘要

通过在干燥条件下将钯金属纳米颗粒与二氧化铈多晶粉末小心混合,获得了一种意想不到的钯-氧-铈界面排列,其中包含溶解在二氧化铈中的钯物种的非晶态壳层覆盖着二氧化铈颗粒的核心。在纳米尺度上产生的牢固接触,以及混合过程中产生的机械力,促进了钯与二氧化铈之间的氧化还原交换,并产生了由嵌入二氧化铈表面层的氧化钯构成的高活性和稳定位点。这种特殊排列在甲烷氧化中比传统的钯/二氧化铈参考催化剂表现更优,起燃温度降低了50℃以上,反应速率也得到提高。优异活性的来源可追溯到通过机械化学相互作用在纳米尺度上修饰的界面结构特性。

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