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Switching the formic acid oxidation reaction (FAOR) pathway from CO intermediate to direct CO2 formation is essential for noble‐metal electrocatalysts, but rare investigations on Ir‐based materials. Herein, the atomic configurations of Ir are controlled to enhance the FAOR performance via Ir3V intermetallics (O‐Ir3V). As the ordering degree of O‐Ir3V increases, the Ir ensemble size decreases to trimer...
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