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Understanding the Dynamic Nature of Catalysts for Methane Abatement Reactions

Periodic Reporting for period 1 - DynaCatMe (Understanding the Dynamic Nature of Catalysts for Methane Abatement Reactions)

Reporting period: 2021-09-01 to 2023-08-31

In this project, we have developed new catalysts to abate and transform methane. Methane is a powerful greenhouse gas, with an effect 20 times higher than that of carbon dioxide. Therefore, it is crucial to control and prevent the emissions of unburned or unreacted methane to the atmosphere both in mobile and stationary applications such as natural gas-propelled vehicles or boilers. In this context, developing new catalysts with improved activity and higher stability is imperative to eliminate or convert methane. In this project, we have focused on the development of catalysts for the total oxidation of methane (MTO) in dry and wet conditions and the methane steam reforming (MSR).
To develop new catalysts, we have explored the use of a new synthesis method to produce them. This synthesis method is mechanochemistry, where the catalysts’ precursors are directly put in contact with a miller. This is an eco-friendly method since no solvents are used and can be directly transferred to the industry. We have synthesized various families of catalysts based on palladium for the methane oxidation project and nickel for the MSR project. During the catalytic activity tests carried out for MTO and MSR, the milled catalysts attained higher methane conversions and longer stabilities than the counterparts that were prepared by traditional methods for both reactions.
The development of the catalysts also entailed gaining a thorough knowledge of their structure during the reactions. This information allows unravelling the working structures of the catalysts and allows for a rational and guided synthesis of new generations of catalysts. We carried out X-ray photoelectron spectroscopy, X-ray diffraction, and X-ray absorption spectroscopy measurements in operando at the synchrotron. We have discovered that new structures and oxidation states are generated during the mechanochemical synthesis and that the milled catalysts have more dynamic structures that allow them to better adapt to the reactive atmosphere.
The results obtained during this project have been published in three scientific papers and are accessible in open access. We have attended several scientific conferences to disseminate the results achieved. We have also recorded a press release and interviewed for a public television. The publication of the papers was posted on Twitter.
In this project, we have expanded the current knowledge of MTO catalysts by producing catalysts with significantly improved stability in wet methane oxidation conditions. Also, we have been able to link the catalytic behavior attained with the structures created at the nanometric level during the mechanochemical synthesis by operando measurements carried out at the synchrotron. For the MSR project, we have contributed to a very mature technology by synthesizing catalysts with higher methane conversions.
We think that the outcomes of this project can have a significant impact on the improvement of these two processes, which have tremendous societal and environmental implications.
Mechanochemical synthesis of ceria-based catalysts for methane conversion.