Localized thermal levering events drive spontaneous kinetic oscillations during CO oxidation on Rh/Al2O3

IF 42.8 1区化学 Q1 CHEMISTRY, PHYSICAL

Nature Catalysis Pub Date : 2024-07-02 DOI:10.1038/s41929-024-01181-w

Donato Decarolis, Monik Panchal, Matthew Quesne, Khaled Mohammed, Shaojun Xu, Mark Isaacs, Adam H. Clark, Luke L. Keenan, Takuo Wakisaka, Kohei Kusada, Hiroshi Kitagawa, C. Richard A. Catlow, Emma K. Gibson, Alexandre Goguet, Peter P. Wells

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Abstract

Unravelling kinetic oscillations, which arise spontaneously during catalysis, has been a challenge for decades but is important not only to understand these complex phenomena but also to achieve increased activity. Here we show, through temporally and spatially resolved operando analysis, that CO oxidation over Rh/Al2O3 involves a series of thermal levering events—CO oxidation, Boudouard reaction and carbon combustion—that drive oscillatory CO2 formation. This catalytic sequence relies on harnessing localized temperature episodes at the nanoparticle level as an efficient means to drive reactions in situations in which the macroscopic conditions are unfavourable for catalysis. This insight provides a new basis for coupling thermal events at the nanoscale for efficient harvesting of energy and enhanced catalyst technologies. Understanding oscillation phenomena in catalysis is a long-standing challenge. Here the authors report a temporally and spatially resolved operando analysis of CO oxidation over Rh/Al2O3, revealing the interplay of Boudouard reaction and carbon combustion in generating the oscillations.

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局部热杠杆事件驱动 Rh/Al2O3 上 CO 氧化过程中的自发动力学振荡

几十年来，揭示催化过程中自发产生的动力学振荡一直是一项挑战，但它不仅对理解这些复杂现象非常重要，而且对提高活性也非常重要。在这里，我们通过时间和空间分辨的操作分析表明，Rh/Al2O3 上的一氧化碳氧化涉及一系列热杠杆事件--一氧化碳氧化、布杜瓦反应和碳燃烧--这些事件推动了一氧化碳的振荡形成。这一催化序列依赖于利用纳米粒子层面的局部温度事件，作为在宏观条件不利于催化的情况下驱动反应的有效手段。这一洞察力为在纳米尺度上耦合热事件以高效采集能量和增强催化剂技术提供了新的基础。

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来源期刊

Nature Catalysis Chemical Engineering-Bioengineering

CiteScore

52.10

自引率

1.10%

发文量

140

期刊介绍： Nature Catalysis serves as a platform for researchers across chemistry and related fields, focusing on homogeneous catalysis, heterogeneous catalysis, and biocatalysts, encompassing both fundamental and applied studies. With a particular emphasis on advancing sustainable industries and processes, the journal provides comprehensive coverage of catalysis research, appealing to scientists, engineers, and researchers in academia and industry. Maintaining the high standards of the Nature brand, Nature Catalysis boasts a dedicated team of professional editors, rigorous peer-review processes, and swift publication times, ensuring editorial independence and quality. The journal publishes work spanning heterogeneous catalysis, homogeneous catalysis, and biocatalysis, covering areas such as catalytic synthesis, mechanisms, characterization, computational studies, nanoparticle catalysis, electrocatalysis, photocatalysis, environmental catalysis, asymmetric catalysis, and various forms of organocatalysis.