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

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 O 2-H 2O chemistries, such as regenerative fuel cells and metal-air batteries. Herein, we report an NH 3-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. As a result, 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.
Authors:
 [1] ;  [2] ;  [1] ;  [1] ;  [3] ;  [1] ;  [1] ;  [1] ;  [4] ;  [1] ;  [4] ;  [3] ;  [3] ;  [5] ;  [6] ;  [1] ;  [1]
  1. Stanford Univ., Stanford, CA (United States)
  2. Stanford Univ., Stanford, CA (United States); Institute of Chemical and Engineering Sciences, Jurong Island (Singapore)
  3. Ulsan National Institute of Science and Technology (UNIST), Ulsan (Republic of Korea)
  4. Colorado School of Mines, Golden, CO (United States)
  5. SLAC National Accelerator Lab., Menlo Park, CA (United States); Karlsruhe Institute of Technology, Eggenstein-Leopoldshafen (Germany); Karlsruhe Institute of Technology, Karlsruhe (Germany)
  6. Stanford Univ., Stanford, CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
Publication Date:
Grant/Contract Number:
AC02-76SF00515
Type:
Accepted Manuscript
Journal Name:
Nano Research
Additional Journal Information:
Journal Volume: 10; Journal Issue: 4; Journal ID: ISSN 1998-0124
Publisher:
Springer
Research Org:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; electrocatalysis; porous carbon; density functional theory
OSTI Identifier:
1349293

To, John W. F., Ng, Jia Wei Desmond, Siahrostami, Samira, Koh, Ai Leen, Lee, Yangjin, Chen, Zhihua, Fong, Kara D., Chen, Shucheng, He, Jiajun, Bae, Won -Gyu, Wilcox, Jennifer, Jeong, Hu Young, Kim, Kwanpyo, Studt, Felix, Nørskov, Jens K., Jaramillo, Thomas F., and Bao, Zhenan. High-performance oxygen reduction and evolution carbon catalysis: From mechanistic studies to device integration. United States: N. p., Web. doi:10.1007/s12274-016-1347-8.
To, John W. F., Ng, Jia Wei Desmond, Siahrostami, Samira, Koh, Ai Leen, Lee, Yangjin, Chen, Zhihua, Fong, Kara D., Chen, Shucheng, He, Jiajun, Bae, Won -Gyu, Wilcox, Jennifer, Jeong, Hu Young, Kim, Kwanpyo, Studt, Felix, Nørskov, Jens K., Jaramillo, Thomas F., & Bao, Zhenan. High-performance oxygen reduction and evolution carbon catalysis: From mechanistic studies to device integration. United States. doi:10.1007/s12274-016-1347-8.
To, John W. F., Ng, Jia Wei Desmond, Siahrostami, Samira, Koh, Ai Leen, Lee, Yangjin, Chen, Zhihua, Fong, Kara D., Chen, Shucheng, He, Jiajun, Bae, Won -Gyu, Wilcox, Jennifer, Jeong, Hu Young, Kim, Kwanpyo, Studt, Felix, Nørskov, Jens K., Jaramillo, Thomas F., and Bao, Zhenan. 2016. "High-performance oxygen reduction and evolution carbon catalysis: From mechanistic studies to device integration". United States. doi:10.1007/s12274-016-1347-8. https://www.osti.gov/servlets/purl/1349293.
@article{osti_1349293,
title = {High-performance oxygen reduction and evolution carbon catalysis: From mechanistic studies to device integration},
author = {To, John W. F. and Ng, Jia Wei Desmond and Siahrostami, Samira and Koh, Ai Leen and Lee, Yangjin and Chen, Zhihua and Fong, Kara D. and Chen, Shucheng and He, Jiajun and Bae, Won -Gyu and Wilcox, Jennifer and Jeong, Hu Young and Kim, Kwanpyo and Studt, Felix and Nørskov, Jens K. and Jaramillo, Thomas F. and Bao, Zhenan},
abstractNote = {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. As a result, 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.},
doi = {10.1007/s12274-016-1347-8},
journal = {Nano Research},
number = 4,
volume = 10,
place = {United States},
year = {2016},
month = {11}
}

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