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Atomic-level understanding on the evolution behavior of subnanometric Pt and Sn species during high-temperature treatments for generation of dense PtSn clusters in zeolites
Journal of Catalysis ( IF 7.3 ) Pub Date : 2020-08-12 , DOI: 10.1016/j.jcat.2020.07.035
Lichen Liu , Miguel Lopez-Haro , Christian W. Lopes , Debora M. Meira , Patricia Concepcion , Jose J. Calvino , Avelino Corma

To achieve high-loading of stable subnanometric metal clusters on solid carriers is a challenge since those small metal clusters have strong tendency to sinter into larger nanoparticles. Development of facile synthesis methodologies to obtain subnanometric metal catalysts with high metal loading and high stability against sintering at high temperature (>500 °C) in reductive atmosphere (such as H2) is critical for the practical applications. In this work, we will present and discuss the generation of high-loading (~1.4 wt%) subnanometric Pt clusters confined in the sinusoidal channels of MFI zeolite, on the basis of the atomic-level understanding on the evolution of Pt and Sn species during high-temperature oxidation–reduction treatments. It will be shown that the structural evolution of Pt and Sn species is dependent on the post-synthesis treatments. The Pt particles on the external surface can disintegrate into subnanometric Pt species and get stabilized in the zeolite channels during high-temperature calcination in air while Sn species migrate from surface region to internal region during high-temperature reduction treatment at 650 °C. The resultant material containing bimetallic PtSn clusters confined in the 10MR sinusoidal channels of the purely siliceous MFI zeolite show excellent catalytic activity and stability, as demonstrated for dehydrogenation of light alkanes at high reaction temperature.



中文翻译:

在沸石中生成致密PtSn团簇的高温处理过程中对亚纳米级Pt和Sn物种演化行为的原子水平理解

在固体载体上实现稳定的亚纳米金属簇的高负荷是一个挑战,因为那些小的金属簇具有强烈的烧结成较大的纳米颗粒的趋势。开发易于合成的方法,以获得具有高金属负载量和高抗还原性气氛(例如H 2)在高温(> 500°C)下烧结的亚纳米金属催化剂)对于实际应用至关重要。在这项工作中,我们将基于对Pt和Sn物种演化的原子级理解,介绍并讨论限制在MFI沸石正弦通道中的高负荷(〜1.4 wt%)亚纳米级Pt团簇的生成。在高温氧化还原处理中。将表明,Pt和Sn物种的结构演变取决于合成后的处理。在空气中高温煅烧期间,外表面上的Pt颗粒可以分解为亚纳米级的Pt物种,并在沸石通道中得到稳定,而在650°C的高温还原处理过程中,Sn物种从表面区域迁移到内部区域。

更新日期:2020-08-31
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