Active and highly stable oxide-supported IrNiO x core-shell catalysts for electrochemical water splitting are presented. IrNi x @IrO x nanoparticles supported on high-surface-area mesoporous antimony-doped tin oxide (IrNiO x / Meso-ATO) were synthesized from bimetallic IrNi x precursor alloys (PA-IrNi x /Meso-ATO) using electrochemical Ni leaching and concomitant Ir oxidation. Special emphasis was placed on Ni/NiO surface segregation under thermal treatment of the PA-IrNi x /Meso-ATO as well as on the surface chemical state of the particle/oxide support interface. Combining a wide array of characterization methods, we uncovered the detrimental effect of segregated NiO phases on the water splitting activity of coreshell particles. The core-shell IrNiO x /Meso-ATO catalyst displayed high water-splitting activity and unprecedented stability in acidic electrolyte providing substantial progress in the development of PEM electrolyzer anode catalysts with drastically reduced Ir loading and significantly enhanced durability.

Intragenus' in the labels of Fig. 1a, 1b and 3a should be 'Intergenus'.Histogram colour names in the caption of Fig. 1 were incorrectly described. The correct expression is as follows: 'between two strains belonging to the same species (light pink), belonging to different species (light purple) and belonging to different genera (pale green). Overlapped regions between intraspecies and interspecies, and between interspecies and intergenus, are displayed in turquoise and violet, respectively.

Electrochemical CO2 reduction 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 CO2 reduction 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.

Water oxidation is a crucial reaction for renewable energy conversion and storage. Among the alkaline oxygen evolution reaction (OER) catalysts, NiFe based oxyhydroxides show the highest catalytic activity. However, the details of their OER mechanism are still unclear, due to the elusive nature of the OER intermediates. Here, using a novel differential electrochemical mass spectrometry (DEMS) cell interface, we performed isotope‐labelling experiments in 18O‐labelled aqueous alkaline electrolyte on Ni(OH)2 and NiFe layered double hydroxide nanocatalysts. Our experiments confirm the occurrence of Mars‐van‐Krevelen lattice oxygen evolution reaction mechanism in both catalysts to various degrees, which involves the coupling of oxygen atoms from the catalyst and the electrolyte. The quantitative charge analysis suggests that the participating lattice oxygen atoms belong exclusively to the catalyst surface, confirming DFT computational hypotheses. Also, DEMS data suggest a fundamental correlation between the magnitude of the lattice oxygen mechanism and the faradaic efficiency of oxygen controlled by pseudocapacitive oxidative metal redox charges.