Divins Núria J, Braga Andrea, Vendrell Xavier, Serrano Isabel, Garcia Xènia, Soler Lluís, Lucentini Ilaria, Danielis Maila, Mussio Andrea, Colussi Sara, Villar-Garcia Ignacio J, Escudero Carlos, Trovarelli Alessandro, Llorca Jordi
Institute of Energy Technologies, Universitat Politècnica de Catalunya, EEBE, Eduard Maristany 10-14, 08019, Barcelona, Spain.
Department of Chemical Engineering, Universitat Politècnica de Catalunya, EEBE, Eduard Maristany 10-14, 08019, Barcelona, Spain.
Nat Commun. 2022 Aug 29;13(1):5080. doi: 10.1038/s41467-022-32765-4.
Efficiently treating methane emissions in transportation remains a challenge. Here, we investigate palladium and platinum mono- and bimetallic ceria-supported catalysts synthesized by mechanical milling and by traditional impregnation for methane total oxidation under dry and wet conditions, reproducing those present in the exhaust of natural gas vehicles. By applying a toolkit of in situ synchrotron techniques (X-ray diffraction, X-ray absorption and ambient pressure photoelectron spectroscopies), together with transmission electron microscopy, we show that the synthesis method greatly influences the interaction and structure at the nanoscale. Our results reveal that the components of milled catalysts have a higher ability to transform metallic Pd into Pd oxide species strongly interacting with the support, and achieve a modulated PdO/Pd ratio than traditionally-synthesized catalysts. We demonstrate that the unique structures attained by milling are key for the catalytic activity and correlate with higher methane conversion and longer stability in the wet feed.
有效处理交通运输中的甲烷排放仍然是一项挑战。在此,我们研究了通过机械研磨和传统浸渍法合成的负载在二氧化铈上的钯和铂单金属及双金属催化剂,用于在干燥和潮湿条件下进行甲烷完全氧化,模拟天然气车辆尾气中的情况。通过应用一套原位同步加速器技术(X射线衍射、X射线吸收和常压光电子能谱),以及透射电子显微镜,我们表明合成方法极大地影响了纳米尺度下的相互作用和结构。我们的结果表明,研磨催化剂的组分比传统合成的催化剂具有更高的将金属钯转化为与载体强烈相互作用的钯氧化物物种的能力,并实现了调节后的PdO/Pd比例。我们证明,通过研磨获得的独特结构是催化活性的关键,并且与在湿进料中更高的甲烷转化率和更长的稳定性相关。