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Nano Research

Article Title

In situ trapped high-density single metal atoms within graphene: Iron-containing hybrids as representatives for efficient oxygen reduction

Authors

Daobin Liu, National Synchrotron Radiation Laboratory, Department of Physics, Department of Polymer Science and Engineering, CAS Center for Excellence in Nanoscience, University of Science and Technology of China, Hefei 230026, China
Chuanqiang Wu, National Synchrotron Radiation Laboratory, Department of Physics, Department of Polymer Science and Engineering, CAS Center for Excellence in Nanoscience, University of Science and Technology of China, Hefei 230026, China
Shuangming Chen, National Synchrotron Radiation Laboratory, Department of Physics, Department of Polymer Science and Engineering, CAS Center for Excellence in Nanoscience, University of Science and Technology of China, Hefei 230026, China
Shiqing Ding, National Synchrotron Radiation Laboratory, Department of Physics, Department of Polymer Science and Engineering, CAS Center for Excellence in Nanoscience, University of Science and Technology of China, Hefei 230026, China
Yaofeng Xie, National Synchrotron Radiation Laboratory, Department of Physics, Department of Polymer Science and Engineering, CAS Center for Excellence in Nanoscience, University of Science and Technology of China, Hefei 230026, China
Changda Wang, National Synchrotron Radiation Laboratory, Department of Physics, Department of Polymer Science and Engineering, CAS Center for Excellence in Nanoscience, University of Science and Technology of China, Hefei 230026, China
Tao Wang, National Synchrotron Radiation Laboratory, Department of Physics, Department of Polymer Science and Engineering, CAS Center for Excellence in Nanoscience, University of Science and Technology of China, Hefei 230026, China
Yasir A. Haleem, National Synchrotron Radiation Laboratory, Department of Physics, Department of Polymer Science and Engineering, CAS Center for Excellence in Nanoscience, University of Science and Technology of China, Hefei 230026, China
Zia ur Rehman, National Synchrotron Radiation Laboratory, Department of Physics, Department of Polymer Science and Engineering, CAS Center for Excellence in Nanoscience, University of Science and Technology of China, Hefei 230026, China
Yuan Sang, National Synchrotron Radiation Laboratory, Department of Physics, Department of Polymer Science and Engineering, CAS Center for Excellence in Nanoscience, University of Science and Technology of China, Hefei 230026, China
Qin Liu, National Synchrotron Radiation Laboratory, Department of Physics, Department of Polymer Science and Engineering, CAS Center for Excellence in Nanoscience, University of Science and Technology of China, Hefei 230026, China
Xusheng Zheng, National Synchrotron Radiation Laboratory, Department of Physics, Department of Polymer Science and Engineering, CAS Center for Excellence in Nanoscience, University of Science and Technology of China, Hefei 230026, China
Yu Wang, Shanghai Synchrotron Radiation Facility, Shanghai Institute of Applied Physics, Chinese Academy of Sciences, Shanghai 201204, China
Binghui Ge, Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, Beijing 100190, China
Hangxun Xu, National Synchrotron Radiation Laboratory, Department of Physics, Department of Polymer Science and Engineering, CAS Center for Excellence in Nanoscience, University of Science and Technology of China, Hefei 230026, China
Li Song, National Synchrotron Radiation Laboratory, Department of Physics, Department of Polymer Science and Engineering, CAS Center for Excellence in Nanoscience, University of Science and Technology of China, Hefei 230026, China

Keywords

single metal atoms (SMAs), high loading, X-ray absorption fine structure spectroscopy (XAFS), high-angle annular dark field-scanning transmission electron microscopy (HAADF-STEM), oxygen reduction reaction (ORR)

Abstract

ABSTRACT Atomically dispersed catalysts have attracted attention in energy conversion applications because their efficiency and chemoselectivity for special catalysis are superior to those of traditional catalysts. However, they have limitations owing to the extremely low metal-loading content on supports, difficulty in the precise control of the metal location and amount as well as low stability at high temperatures. We prepared a highly doped single metal atom hybrid via a single-step thermal pyrolysis of glucose, dicyandiamide, and inorganic metal salts. High-angle annular dark field-scanning transmission electron microscopy (HAADF-STEM) and X-ray absorption fine structure spectroscopy (XAFS) revealed that nitrogen atoms doped into the graphene matrix were pivotal for metal atom stabilization by generating a metal-Nx coordination structure. Due to the strong anchoring effect of the graphene matrix, the metal loading content was over 4 wt.% in the isolated atomic hybrid (the Pt content was as high as 9.26 wt.% in the Pt-doped hybrid). Furthermore, the single iron-doped hybrid (Fe@N-doped graphene) showed a remarkable electrocatalytic performance for the oxygen reduction reaction. The peak power density was ~199 mW·cm−2 at a current density of 310 mA·cm−2 and superior to that of a commercial Pt/C catalyst when it was used as a cathode catalyst in assembled zinc-air batteries. This work offered a feasible approach to design and fabricate highly doped single metal atoms (SMAs) catalysts for potential energy applications.

Graphical Abstract

Publisher

Tsinghua University Press

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