Tracking the formation, fate and consequence for catalytic activity of Pt single sites on CeO2
Tracking the formation, fate and consequence for catalytic activity of Pt single sites on CeO2
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DOI：
10.1038/s41929-020-00508-7
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发表时间：
2020-09-21
期刊：
影响因子：
37.8
通讯作者：
Grunwaldt, Jan-Dierk
中科院分区：
文献类型：
--
作者：
Maurer, Florian;Jelic, Jelena;Grunwaldt, Jan-Dierk
铂单中心是非常有吸引力的，因为它们的高原子经济性，可以通过氧化高温处理在CeO（2）上产生。然而，他们的位置和活动受到强烈争议。此外，反应驱动的结构动力学尚未解决到目前为止。在这项研究中，我们能够证明铂诱导的CeO（2）表面重组，定位铂单点CeO（2）和跟踪的活性状态的变化，在反应条件下使用的互补方法的密度泛函理论计算，原位红外光谱，高能量分辨率荧光检测的X射线吸收光谱和催化CO（以及C（3）H（6）和CH 4）氧化。我们发现，CO氧化的发病与铂单网站从四重空心网站的迁移，形成含有几个铂原子的小簇。这表明，对单个站点的操作性研究是必不可少的，以评估其命运和由此产生的催化性能。
Platinum single sites are highly attractive due to their high atom economy and can be generated on CeO(2)by an oxidative high-temperature treatment. However, their location and activity are strongly debated. Furthermore, reaction-driven structural dynamics have not been addressed so far. In this study, we were able to evidence platinum-induced CeO(2)surface restructuring, locate platinum single sites on CeO(2)and track the variation of the active state under reaction conditions using a complementary approach of density functional theory calculations, in situ infrared spectroscopy, operando high-energy-resolution fluorescence detected X-ray absorption spectroscopy and catalytic CO (as well as C(3)H(6)and CH4) oxidation. We found that the onset of CO oxidation is linked to the migration of platinum single sites from four-fold hollow sites to form small clusters containing a few platinum atoms. This demonstrates that operando studies on single sites are essential to assess their fate and the resulting catalytic properties.