Claudie Roy

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Rutile RuO2 catalysts are the most active pure metal oxides for oxygen evolution; however, they are also unstable toward dissolution. Herein, we study the catalytic activity and stability of oriented thin films of RuO2 with (111), (101), and (001) orientations, in comparison to a (110) single crystal and commercial nanoparticles. These surfaces were all tested in aqueous solutions of 0.05 M H2SO4. The initial catalyst activity ranked as follows: (001) > (101) > (111) ≈ (110). We complemented our activity data with inductively coupled plasma mass spectroscopy, to measure Ru dissolution products occurring in parallel to oxygen evolution. In contrast to earlier reports, we find that, under our experimental conditions, there is no correlation between the activity and stability.

Abstract Electrochemical CO 2 reduction (CO 2 R) is an attractive option for storing renewable electricity and for the sustainable production of valuable chemicals and fuels. In this roadmap, we review recent progress in fundamental understanding, catalyst development, and in engineering and scale-up. We discuss the outstanding challenges towards commercialization of electrochemical CO 2 R technology: energy efficiencies, selectivities, low current densities, and stability. We highlight the opportunities in establishing rigorous standards for benchmarking performance, advances in in operando characterization, the discovery of new materials towards high value products, the investigation of phenomena across multiple-length scales and the application of data science towards doing so. We hope that this collective perspective sparks new research activities that ultimately bring us a step closer towards establishing a low- or zero-emission carbon cycle.

Oxide-derived copper (OD-Cu) electrodes exhibit unprecedented CO reduction performance towards liquid fuels, producing ethanol and acetate with >50% Faradaic efficiency at -0.3 V (vs. RHE). By using static headspace-gas chromatography for liquid phase analysis, we identify acetaldehyde as a minor product and key intermediate in the electroreduction of CO to ethanol on OD-Cu electrodes. Acetaldehyde is produced with a Faradaic efficiency of ≈5% at -0.33 V (vs. RHE). We show that acetaldehyde forms at low steady-state concentrations, and that free acetaldehyde is difficult to detect in alkaline solutions using NMR spectroscopy, requiring alternative methods for detection and quantification. Our results represent an important step towards understanding the CO reduction mechanism on OD-Cu electrodes.