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Kinetics and Dynamics at Surfaces

Periodic Reporting for period 3 - KIDS (Kinetics and Dynamics at Surfaces)

Periodo di rendicontazione: 2022-09-01 al 2024-02-29

In this project we are applying charged particle imaging to measure catalytic rates for site-specific elementary reactions thus offering remarkable opportunities to advance our fundamental understanding of heterogeneous catalysis.

As evidence for global climate change continues to grow, catalysis has moved to the front line of the struggle to obtain new, sustainable technologies for the future. Catalysis and catalytic processes account, directly or indirectly, for 20-30 % of world gross domestic product. Knowledge of elementary chemical reaction mechanisms in heterogeneous catalysis underlies our ability to construct comprehensive kinetic models for many such important chemical processes, in order to optimize them.

The aim is to characterize the important factors that influence the kinetics of elementary reactions at surfaces, e.g. the chemical nature of the catalyst and the geometry of the active site (stereodynamics). We chose elementary reactions involving C, H, O, N, as these are important in many key industries, such as the methane reforming, syngas, fuel cells, Fischer-Tropsch synthesis and the Haber-Bosch process. Our strategy is that of a “bottom-up” approach to catalysis, i.e. building and understanding complex heterogeneous chemical catalysis, from the site-specific kinetics of the elementary building block reactions. Our measurements, serve as benchmarks for first principles calculations of reaction rates in surface chemistry.
In this initial phase of the project, we are constructing a new apparatus building on experience from our existing machines.

We have completed experiments on the existing apparatus concerning the oxidation of H2 on Pt (111)/(332)and Pd(111)/(332), and have studied the decomposition of Formic acid on the respective metal catalysts. The recombination of H-atoms on these two surfaces has been completed and is important in analysing the H2 oxidation kinetics.
The new machine is completed. The major improvement over exiting methodology (current state of the art) is that it we able to extract full kinetic traces with 10 microsecond resolution with every pulse of reactant. The advantage over existing technology is that it will simultaneously provide total product yield as well as the kinetics information for series of reactant concentrations. The data acquisition rate is expected to increase by a factor of 1000.