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捕获一氧化碳氧化过程中的催化剂应变动力学

Capturing Catalyst Strain Dynamics during CO Oxidation.

作者信息

Grimes Michael, Atlan Clément, Chatelier Corentin, Bellec Ewen, Olson Kyle, Simonne David, Levi Mor, Schülli Tobias U, Leake Steven J, Rabkin Eugen, Eymery Joël, Richard Marie-Ingrid

机构信息

Univ. Grenoble Alpes, CEA Grenoble, IRIG, MEM, NRX, 17 rue des Martyrs, F-38000 Grenoble, France.

ESRF - The European Synchrotron, 71 Avenue des Martyrs, F-38000 Grenoble, France.

出版信息

ACS Nano. 2024 Jul 15. doi: 10.1021/acsnano.4c04127.

Abstract

Understanding the strain dynamic behavior of catalysts is crucial for the development of cost-effective, efficient, stable, and long-lasting catalysts. Using time-resolved Bragg coherent diffraction imaging at the fourth generation Extremely Brilliant Source of the European Synchrotron (ESRF-EBS), we achieved subsecond time resolution during chemical reactions. Upon investigation of Pt nanoparticles during CO oxidation, the three-dimensional strain profile highlights significant changes in the surface and subsurface regions, where localized strain is probed along the [111] direction. Notably, a rapid increase in tensile strain was observed at the top and bottom Pt {111} facets during CO adsorption. Moreover, we detected oscillatory strain changes (6.4 s period) linked to CO adsorption during oxidation, where a time resolution of 0.25 s was achieved. This approach allows for the study of adsorption dynamics of catalytic nanomaterials at the single-particle level under conditions, which provides insight into nanoscale catalytic mechanisms.

摘要

了解催化剂的应变动态行为对于开发经济高效、稳定持久的催化剂至关重要。利用欧洲同步加速器(ESRF-EBS)第四代极亮光源的时间分辨布拉格相干衍射成像技术,我们在化学反应过程中实现了亚秒级的时间分辨率。在研究一氧化碳氧化过程中的铂纳米颗粒时,三维应变分布突出了表面和次表面区域的显著变化,其中沿[111]方向探测到局部应变。值得注意的是,在一氧化碳吸附过程中,在顶部和底部的铂{111}晶面上观察到拉伸应变的快速增加。此外,我们在氧化过程中检测到与一氧化碳吸附相关的振荡应变变化(周期为6.4秒),实现了0.25秒的时间分辨率。这种方法能够在实际条件下对催化纳米材料的吸附动力学进行单颗粒水平的研究,从而深入了解纳米尺度的催化机制。

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