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Single-Atom Iron Catalysts on Overhang-Eave Carbon Cages for High-Performance Oxygen Reduction Reaction
Authors:Dr. Chun-Chao Hou  Dr. Lianli Zou  Dr. Liming Sun  Dr. Kexin Zhang  Dr. Zheng Liu  Prof. Yinwei Li  Dr. Caixia Li  Prof. Ruqiang Zou  Prof. Jihong Yu  Prof. Qiang Xu
Affiliation:1. AIST-Kyoto University Chemical Energy Materials Open Innovation Laboratory (ChEM-OIL), National Institute of Advanced Industrial Science and Technology (AIST), Sakyo-ku, Kyoto, 606-8501 Japan;2. AIST-Kyoto University Chemical Energy Materials Open Innovation Laboratory (ChEM-OIL), National Institute of Advanced Industrial Science and Technology (AIST), Sakyo-ku, Kyoto, 606-8501 Japan

Graduate School of Engineering, Kobe University, Nada Ku, Kobe, Hyogo, 657-8501 Japan;3. AIST-Kyoto University Chemical Energy Materials Open Innovation Laboratory (ChEM-OIL), National Institute of Advanced Industrial Science and Technology (AIST), Sakyo-ku, Kyoto, 606-8501 Japan

Laboratory of Quantum Materials Design and Application, School of Physics and Electronic Engineering, Jiangsu Normal University, Xuzhou, 221116 P. R. China;4. Beijing Key laboratory for Theory and Technology of Advanced Battery Materials, Department of Materials Science and Engineering, College of Engineering, Peking University, Beijing, 100871 P. R. China;5. Inorganic Functional Materials Research Institute, National Institute of Advanced Industrial Science and Technology (AIST), 2266-98 Anagahora, Shimoshidami, Moriyamaku, Nagoya, Aichi, 463-8560 Japan;6. Laboratory of Quantum Materials Design and Application, School of Physics and Electronic Engineering, Jiangsu Normal University, Xuzhou, 221116 P. R. China;7. State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry;8. International Center of Future Science, Jilin University, Changchun, 130012 P. R. China

Abstract:Single-atom catalysts have drawn great attention, especially in electrocatalysis. However, most of previous works focus on the enhanced catalytic properties via improving metal loading. Engineering morphologies of catalysts to facilitate mass transport through catalyst layers, thus increasing the utilization of each active site, is regarded as an appealing way for enhanced performance. Herein, we design an overhang-eave structure decorated with isolated single-atom iron sites via a silica-mediated MOF-templated approach for oxygen reduction reaction (ORR) catalysis. This catalyst demonstrates superior ORR performance in both alkaline and acidic electrolytes, comparable to the state-of-the-art Pt/C catalyst and superior to most precious-metal-free catalysts reported to date. This activity originates from its edge-rich structure, having more three-phase boundaries with enhanced mass transport of reactants to accessible single-atom iron sites (increasing the utilization of active sites), which verifies the practicability of such a synthetic approach.
Keywords:electrochemistry  metal–organic frameworks  oxygen reduction reaction  single-atom catalysis  transition metals
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