Atomic Insights into the Competitive Edge of Nanosheets Splitting Water

doi:10.1021/jacs.4c10312

淡江大學機構典藏 > 理學院 > 物理學系暨研究所 > 期刊論文 > Item 987654321/127638

Please use this identifier to cite or link to this item: https://tkuir.lib.tku.edu.tw/dspace/handle/987654321/127638

Title:	Atomic Insights into the Competitive Edge of Nanosheets Splitting Water
Authors:	Falling, Lorenz J.;Jang, Woosun;Laha, Sourav;Götsch, Thomas;Terban, Maxwell W.;Bette, Sebastian;Mom, Rik;Juan-Jesús, Velasco-Vélez;Girgsdies, Frank;Teschner, Detre;Tarasov, Andrey;Chuang, Cheng-Hao;Lunkenbein, Thomas;Axel, Knop-Gericke;Weber, Daniel;Dinnebier, Robert;Lotsch, Bettina V.;Schlögl, Robert;Jones, Travis E.
Date:	2024-09-25
Issue Date:	2025-07-31 12:05:17 (UTC+8)
Publisher:	American Chemical Society
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 CO2. 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 (μ3Δ-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., μ1-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.
Relation:	Journal of the American Chemical Society 146(40), p.27886-27902
DOI:	10.1021/jacs.4c10312
Appears in Collections:	[物理學系暨研究所] 期刊論文

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