Research Article


2017, 10(4): 1163–1177


High-performance oxygen reduction and evolution carbon catalysis: From mechanistic studies to device integration

John W. F. To1,§, Jia Wei Desmond Ng1,2,§, Samira Siahrostami1,§, Ai Leen Koh3, Yangjin Lee4, Zhihua Chen1, Kara D. Fong1, Shucheng Chen1, Jiajun He5, Won-Gyu Bae1, Jennifer Wilcox5, Hu Young Jeong6, Kwanpyo Kim4, Felix Studt7,8,9 (*), Jens K. Nrskov1,7 (*), Thomas F. Jaramillo1 (*), and Zhenan Bao1 (*)

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1 Department of Chemical Engineering, Stanford University, Stanford, CA 94305, USA
2 Institute of Chemical and Engineering Sciences, Agency for Science, Technology and Research, Jurong Island 627833, Singapore
3 Stanford Nano Shared Facilities, Stanford University, Stanford, CA 94305, USA
4 Department of Physics, Ulsan National Institute of Science and Technology (UNIST), Ulsan 689-798, Republic of Korea
5 Department of Chemical and Biological Engineering, Colorado School of Mines, Golden, CO 80401, USA
6 UNIST Central Research Facilities (UCRF), Ulsan National Institute of Science and Technology (UNIST), Ulsan 689- 98, Republic of Korea
7 SUNCAT Center for Interface Science and Catalysis SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, CA 94025, USA
8 Institute of Catalysis Research and Technology, Karlsruhe Institute of Technology, Hermann-von-Helmholtz Platz 1, 76344 Eggenstein-Leopoldshafen, Germany
9 Institute for Chemical Technology and Polymer Chemistry, Karlsruhe Institute of Technology, Engesserstr. 18, 76131 Karlsruhe, Germany
§ These authors contributed equally to this work.

Keywords: electrocatalysis, porous carbon, density functional theory
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ABSTRACT The development of high-performance and low-cost oxygen reduction and evolution catalysts that can be easily integrated into existing devices is crucial for the wide deployment of energy storage systems that utilize O2-H2O chemistries, such as regenerative fuel cells and metal-air batteries. Herein, we report an NH3-activated N-doped hierarchical carbon (NHC) catalyst synthesized via a scalable route, and demonstrate its device integration. The NHC catalyst exhibited good performance for both the oxygen reduction reaction (ORR) and the oxygen evolution reaction (OER), as demonstrated by means of electrochemical studies and evaluation when integrated into the oxygen electrode of a regenerative fuel cell. The activities observed for both the ORR and the OER were comparable to those achieved by state-of-the-art Pt and Ir catalysts in alkaline environments. We have further identified the critical role of carbon defects as active sites for electrochemical activity through density functional theory calculations and high-resolution TEM visualization. This work highlights the potential of NHC to replace commercial precious metals in regenerative fuel cells and possibly metal-air batteries for cost-effective storage of intermittent renewable energy.
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High-performance oxygen reduction and evolution carbon catalysis: From mechanistic studies to device integration. Nano Res. 2017, 10(4): 1163–1177

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