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Aliovalent doping is widely adopted to tune the electronic structure of transition‐metal oxides for design of low‐cost, active electrocatalysts. Here, using single‐crystalline thin films as model electrocatalysts, the structure‐activity relationship of Fe states doping in perovskite LaNiO3 for oxygen evolution reaction (OER) is studied. Fe4+ state is found to be crucial for enhancing the OER activity...
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