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

DOI: 10.1038/s41929-024-01181-w

Authors: Donato Decarolis (Cardiff University; UK Catalysis Hub, Research Complex at Harwell; Diamond Light Source) , Monik Panchal (UK Catalysis Hub, Research Complex at Harwell; University College London; Durham University) , Matthew Quesne (Cardiff University; UK Catalysis Hub, Research Complex at Harwell) , Khaled Mohammed (University of Southampton; Sohag University) , Shaojun Xu (Cardiff University; UK Catalysis Hub, Research Complex at Harwell; University of Manchester) , Mark Isaacs (University College London; Harwell XPS, Research Complex at Harwell) , Adam H. Clark (Paul Scherrer Institute) , Luke L. Keenan (Diamond Light Source) , Takuo Wakisaka (Kyoto University) , Kohei Kusada (Kyoto University) , Hiroshi Kitagawa (Kyoto University) , C. Richard A. Catlow (Cardiff University; UK Catalysis Hub, Research Complex at Harwell; University College London) , Emma K. Gibson (UK Catalysis Hub, Research Complex at Harwell; University of Glasgow) , Alexandre Goguet (UK Catalysis Hub, Research Complex at Harwell; Queen's University Belfast) , Peter Wells (UK Catalysis Hub, Research Complex at Harwell; Diamond Light Source; University of Southampton)
Co-authored by industrial partner: No

Type: Journal Paper
Journal: Nature Catalysis , VOL 70

State: Published (Approved)
Published: July 2024
Diamond Proposal Number(s): 21593

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.

Subject Areas: Chemistry


Instruments: I20-EDE-Energy Dispersive EXAFS (EDE)

Other Facilities: HarwellXPS

Added On: 03/07/2024 12:05

Documents:
s41929-024-01181-w.pdf

Discipline Tags:

Physical Chemistry Catalysis Chemistry

Technical Tags:

Spectroscopy X-ray Absorption Spectroscopy (XAS) Extended X-ray Absorption Fine Structure (EXAFS)