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Metal–Organic Framework‐Derived Bamboo‐like Nitrogen‐Doped Graphene Tubes as an Active Matrix for Hybrid Oxygen‐Reduction Electrocatalysts
Authors:Qing Li  Hengyu Pan  Drew Higgins  Ruiguo Cao  Guoqi Zhang  Haifeng Lv  Kangbing Wu  Jaephil Cho  Gang Wu
Affiliation:1. Materials Physics and Applications Division, Los Alamos National Laboratory, Los Alamos, New Mexico, USA;2. Department of Chemical and Biological Engineering, University at Buffalo, The State University of New York, Buffalo, New York, USA;3. Interdisciplinary School of Green Energy, Ulsan National Institute of Science and Technology, Ulsan, Korea;4. Department of Sciences, John Jay College of the City University of New York, New York, New York, USA;5. State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, Wuhan, China;6. Key Laboratory for Large‐Format Battery Materials and System, Ministry of Education School of Chemistry and Chemical Engineering, Huazhong University of Science and Technology, Wuhan, China
Abstract:In this work, large size (i.e., diameter > 100 nm) graphene tubes with nitrogen‐doping are prepared through a high‐temperature graphitization process of dicyandiamide (DCDA) and Iron(II) acetate templated by a novel metal–organic framework (MIL‐100(Fe)). The nitrogen‐doped graphene tube (N‐GT)‐rich iron‐nitrogen‐carbon (Fe‐N‐C) catalysts exhibit inherently high activity towards the oxygen reduction reaction (ORR) in more challenging acidic media. Furthermore, aiming to improve the activity and stability of conventional Pt catalysts, the ORR active N‐GT is used as a matrix to disperse Pt nanoparticles in order to build a unique hybrid Pt cathode catalyst. This is the first demonstration of the integration of a highly active Fe‐N‐C catalyst with Pt nanoparticles. The synthesized 20% Pt/N‐GT composite catalysts demonstrate significantly enhanced ORR activity and H2‐air fuel cell performance relative to those of 20% Pt/C, which is mainly attributed to the intrinsically active N‐GT matrix along with possible synergistic effects between the non‐precious metal active sites and the Pt nanoparticles. Unlike traditional Pt/C, the hybrid catalysts exhibit excellent stability during the accelerated durability testing, likely due to the unique highly graphitized graphene tube morphologies, capable of providing strong interaction with Pt nanoparticles and then preventing their agglomeration.
Keywords:graphene tubes  graphene tubes  Pt nanoparticles  oxygen reduction  nanocomposites  electrocatalysts
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