PhD Thesis Defense - Laia Pascua Solé

Methane is a powerful greenhouse gas and a crucial energy resource, but using it cleanly presents major engineering hurdles. Converting methane into cleaner vehicle exhaust or valuable synthesis gas relies on palladium (Pd) catalysts, materials that quickly deactivate due to water poisoning, carbon buildup (coking), or structural breakdown under realistic working conditions.

This doctoral research solves these stability challenges by designing robust, high-performance catalysts using innovative mechanical synthesis methods and studying their behavior in real-time under actual operating conditions.

Key highlights of the research:

• Clearing Exhaust Emissions: Developing ball-milled palladium catalysts that maintain high activity for total methane oxidation, using cobalt and specialized supports to stabilize the catalyst structure even in the presence of deactivating water vapor.

• Efficient Syngas Production: Combining palladium with secondary metals (nickel or cobalt) via ball-milling to create highly active, long-lasting catalysts for partial methane oxidation, outperforming traditional chemical preparation methods by preventing metal separation and soot formation.

• Real-Time Catalyst Tracking: Utilizing advanced operando spectroscopy to observe catalyst transformations during chemical reactions, discovering unique "Janus" nanoparticle structures and self-sustained reaction oscillations that drive optimal syngas synthesis.

Ultimately, this work links eco-friendly, solvent-free catalyst manufacturing to advanced real-time characterization, offering scalable solutions for cleaner vehicles and sustainable chemical production.