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Atomic Insights into the Competitive Edge of Nanosheets Splitting Water. | LitMetric

AI Article Synopsis

  • The oxygen evolution reaction (OER) is crucial for generating green hydrogen and other renewable energy sources, with iridium oxohydroxides (IOHs) being effective catalysts due to their balance of activity and stability in acidic conditions.
  • While amorphous IOHs are highly active, they lack stability, whereas crystalline IOHs are more stable but typically less active.
  • This research identifies crystalline IrOOH nanosheets as a promising catalyst, offering high activity and stability, and establishes simple design rules based on atomic-level relationships to guide future development of efficient OER catalysts.

Article Abstract

The oxygen evolution reaction (OER) provides the protons for many electrocatalytic power-to-X processes, such as the production of green hydrogen from water or methanol from CO. Iridium oxohydroxides (IOHs) are outstanding catalysts for this reaction because they strike a unique balance between activity and stability in acidic electrolytes. Within IOHs, this balance varies with the atomic structure. While amorphous IOHs perform best, they are least stable. The opposite is true for their crystalline counterparts. These rules-of-thumb are used to reduce the loading of scarce IOH catalysts and retain the performance. However, it is not fully understood how activity and stability are related at the atomic level, hampering rational design. Herein, we provide simple design rules (Figure 12) derived from the literature and various IOHs within this study. We chose crystalline IrOOH nanosheets as our lead material because they provide excellent catalyst utilization and a predictable structure. We found that IrOOH signals the chemical stability of crystalline IOHs while surpassing the activity of amorphous IOHs. Their dense bonding network of pyramidal trivalent oxygens (μ-O) provides structural integrity, while allowing reversible reduction to an electronically gapped state that diminishes the destructive effect of reductive potentials. The reactivity originates from coordinative unsaturated edge sites with radical character, i.e., μ-O oxyls. By comparing to other IOHs and literature, we generalized our findings and synthesized a set of simple rules that allow prediction of stability and reactivity of IOHs from atomistic models. We hope that these rules will inspire atomic design strategies for future OER catalysts.

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Source
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC11467904PMC
http://dx.doi.org/10.1021/jacs.4c10312DOI Listing

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