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Article Abstract
Co─Fe layered double hydroxide (LDH) has shown great performance for oxygen evolution reaction (OER), however, the effect of Fe in Co─Fe compounds as well as its mechanism for promoting OER are still of great challenge. Herein, Co─Fe bimetallic silicate hydroxides, with a similar structure of Co─Fe LDH and more advantages, are designed to address the issue about the performance-determining site (PDS). In designed Co─Fe bimetallic silicate hydroxides, two different coordinated Fe ions in cationic layers (Fe (Oh)) and anionic layers (Fe (Td)) are distinguished to achieve high-efficient OER catalysts, where introducing Al as heteroatom can shield the existence of Fe (Td), creating a key contrast. It is found that different coordinated Fe ions modulate OER properties of cobalt sites into different directions: Fe (Oh) immensely promotes the OER process on adjacent Co sites, while Fe (Td) plays an opposite role. Taking advantage of the above effects, the overpotential has declined to 254 mV at 10 mA cm, showing great progress in this field. The density functional theory (DFT) method identifies Co as PDS and elucidates the related mechanisms with electronic structures. This work explores the mechanism of Co─Fe bimetallic effect promoting OER performance, providing a reference for the related controversy.
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