The dissolution of electrocatalysts during operation is one of the key limiting factors in electrochemical technologies such as green hydrogen production and the conversion of CO2 to chemicals. Self-healing electrocatalysts have the potential to mitigate this degradation process: by balancing electrocatalyst dissolution with redeposition reactions, an equilibrium is created which, in principle, endows the electrocatalyst with an infinite lifespan. In HEALECTRO, I will combine high-throughput experimentation and advanced X-ray spectroscopies to unravel how the structure of self-healing catalysts can be steered to combine this long lifespan with efficient catalysis.

To create a hydrogen-based economy on a global scale, for storage, refueling, and other applications, it is essential to purify and compress available hydrogen sources and produce ‘green’ hydrogen at scale. This makes electrochemical hydrogen technologies attractive, because these single-stage processes can be implemented in a decentralized manner and rely on renewable energy input only. Impurities in the reactant streams, however, significantly lower the efficiency. In M-Select, we will develop superior impurity-tolerant coatings for electrocatalytic materials and address and mitigate technological challenges in the hydrogen supply, storage, and conversion chain.

CO2’s reaction with co-adsorbed hydrogen atoms is the crucial initial step in methanol production over Cu-based catalysts. A strong local surface structure dependence to forming formate (HCOOads) arises from DFT-based studies for a few selected low-index surfaces and clusters. However, calculated activation barriers vary widely and there is no experimental evidence explaining the activated formation of this intermediate. Through a unique combination of experimental and theoretical techniques, we unravel the adsorption and reaction of CO2 with Hads on Cu. We start using two parallel approaches yielding independent insights: studies on small, unsupported Cu clusters inform us on the dependence of the adsorbed state(s), reactivity, and thermochemistry on local geometrical motif and electronic structure, whereas studies employing molecular beams and the continuous variation of surface structure on curved single crystals provide information on the reaction dynamics and activation barriers. Both approaches use forms of infrared spectroscopy and mass spectrometry to identify adsorbed CO2 and products of (in)direct reactions. Using well-established theoretical techniques, specifically-tailored DFT calculations are performed for CO2 adsorption and activation for the experimentally pre-characterized nanostructured surfaces and particles including a systematic global structure search, allowing to compare to the measured observables (binding energies, vibrational properties). Finally, we ‘meet in the middle’ using infrared studies of CO2 adsorption and reaction on supported Cu nano-clusters, that are produced with three different methods. The combined results inform us how the most critical elementary reaction in CO2 fixation is affected by local geometric and electronic structure, guiding nano-engineering of improved catalysts.

The energy transition requires new materials for greening chemistry and transportation. Electrolyzers and fuel cells need more efficient electrodes and more robust membranes. Scarce materials call for everyday alternatives. PLD4Energy is a Pulsed Laser Deposition (PLD) facility for producing such thin film (membrane) alternatives. It is tailored to research for energy applications. PLD has the right in-situ diagnostics to move from small to larger film areas in a controlled manner. The facility lends itself to fundamental research, as well as the next, essential step: actual implementation. PLD4Energy welcomes external researchers and also companies that want to test commercial applications.

During electrochemical reactions, atoms in the molecules rearrange to form new chemical bonds. Via computer simulations, we can “visualize” and rationalize these atomic scale processes: We investigate how molecules react at electrodes and why they react, and we investigate how the electrode surface on which these reactions happen influences the reactions.