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Title: Graphene-Directed Formation of a Nitrogen-Doped Porous Carbon Sheet with High Catalytic Performance for the Oxygen Reduction Reaction

Abstract

In this paper, a nitrogen (N)-doped porous carbon sheet is prepared by in situ polymerization of pyrrole on both sides of graphene oxide, following which the polypyrrole layers are then transformed to the N-doped porous carbon layers during the following carbonization, and a sandwich structure is formed. Such a sheet-like structure possesses a high specific surface area and, more importantly, guarantees the sufficient utilization of the N-doping active porous sites. The internal graphene layer acts as an excellent electron pathway, and meanwhile, the external thin and porous carbon layer helps to decrease the ion diffusion resistance during electrochemical reactions. As a result, this sandwich structure exhibits prominent catalytic activity toward the oxygen reduction reaction in alkaline media, as evidenced by a more positive onset potential, a larger diffusion-limited current, better durability and poison-tolerance than commercial Pt/C. Finally, this study shows a novel method of using graphene to template the traditional porous carbon into a two-dimensional, thin, and porous carbon sheet, which greatly increases the specific surface area and boosts the utilization of inner active sites with suppressed mass diffusion resistance.

Authors:
 [1];  [2];  [3];  [4];  [4]; ORCiD logo [4]; ORCiD logo [4];  [4]; ORCiD logo [5]; ORCiD logo [6]; ORCiD logo [2]
  1. Tsinghua Univ., Shenzhen (China). Graduate School at Shenzhen. Engineering Lab. for Functionalized Carbon Materials. Baotou Graphene Innovation Center (Shenzhen); The Hong Kong Univ. of Science and Technology (China). Dept. of Mechanical and Aerospace Engineering
  2. Argonne National Lab. (ANL), Argonne, IL (United States). Chemical Sciences and Engineering Division
  3. Tianjin Univ. (China). School of Chemical Engineering and Technology; Chinese Academy of Sciences (CAS), Dalian (China). Division of Fuel Cell & Battery. Dalian National Lab. for Clean Energy. Dalian Inst. of Chemical Physics
  4. Tsinghua Univ., Shenzhen (China). Graduate School at Shenzhen. Engineering Lab. for Functionalized Carbon Materials. Baotou Graphene Innovation Center (Shenzhen)
  5. The Hong Kong Univ. of Science and Technology (China). Dept. of Mechanical and Aerospace Engineering
  6. Tianjin Univ. (China). School of Chemical Engineering and Technology
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States); Tsinghua Univ., Shenzhen (China); Tianjin Univ. (China); The Hong Kong Univ. of Science and Technology (China); Chinese Academy of Sciences (CAS), Dalian (China)
Sponsoring Org.:
USDOE; Guangdong Natural Science Funds for Distinguished Young Scholar (China); National Natural Science Foundation of China (NNSFC); National Science Fund for Distinguished Young Scholars (China); National Basic Research Program of China; Shenzhen Basic Research Project (China); Youth Research Funds of Graduate School at Shenzhen, Tsinghua Univ. (China)
OSTI Identifier:
1466292
Grant/Contract Number:  
AC02-06CH11357; 2017B030306006; 21506212; 51772164; U1601206; 51525204; 2014CB932400; JCYJ20150529164918734; QN20160001
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. C
Additional Journal Information:
Journal Volume: 122; Journal Issue: 25; Journal ID: ISSN 1932-7447
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Qin, Lei, Yuan, Yifei, Wei, Wei, Lv, Wei, Niu, Shuzhang, He, Yan-Bing, Zhai, Dengyun, Kang, Feiyu, Kim, Jang-Kyo, Yang, Quan-Hong, and Lu, Jun. Graphene-Directed Formation of a Nitrogen-Doped Porous Carbon Sheet with High Catalytic Performance for the Oxygen Reduction Reaction. United States: N. p., 2017. Web. doi:10.1021/acs.jpcc.7b12327.
Qin, Lei, Yuan, Yifei, Wei, Wei, Lv, Wei, Niu, Shuzhang, He, Yan-Bing, Zhai, Dengyun, Kang, Feiyu, Kim, Jang-Kyo, Yang, Quan-Hong, & Lu, Jun. Graphene-Directed Formation of a Nitrogen-Doped Porous Carbon Sheet with High Catalytic Performance for the Oxygen Reduction Reaction. United States. doi:10.1021/acs.jpcc.7b12327.
Qin, Lei, Yuan, Yifei, Wei, Wei, Lv, Wei, Niu, Shuzhang, He, Yan-Bing, Zhai, Dengyun, Kang, Feiyu, Kim, Jang-Kyo, Yang, Quan-Hong, and Lu, Jun. Thu . "Graphene-Directed Formation of a Nitrogen-Doped Porous Carbon Sheet with High Catalytic Performance for the Oxygen Reduction Reaction". United States. doi:10.1021/acs.jpcc.7b12327. https://www.osti.gov/servlets/purl/1466292.
@article{osti_1466292,
title = {Graphene-Directed Formation of a Nitrogen-Doped Porous Carbon Sheet with High Catalytic Performance for the Oxygen Reduction Reaction},
author = {Qin, Lei and Yuan, Yifei and Wei, Wei and Lv, Wei and Niu, Shuzhang and He, Yan-Bing and Zhai, Dengyun and Kang, Feiyu and Kim, Jang-Kyo and Yang, Quan-Hong and Lu, Jun},
abstractNote = {In this paper, a nitrogen (N)-doped porous carbon sheet is prepared by in situ polymerization of pyrrole on both sides of graphene oxide, following which the polypyrrole layers are then transformed to the N-doped porous carbon layers during the following carbonization, and a sandwich structure is formed. Such a sheet-like structure possesses a high specific surface area and, more importantly, guarantees the sufficient utilization of the N-doping active porous sites. The internal graphene layer acts as an excellent electron pathway, and meanwhile, the external thin and porous carbon layer helps to decrease the ion diffusion resistance during electrochemical reactions. As a result, this sandwich structure exhibits prominent catalytic activity toward the oxygen reduction reaction in alkaline media, as evidenced by a more positive onset potential, a larger diffusion-limited current, better durability and poison-tolerance than commercial Pt/C. Finally, this study shows a novel method of using graphene to template the traditional porous carbon into a two-dimensional, thin, and porous carbon sheet, which greatly increases the specific surface area and boosts the utilization of inner active sites with suppressed mass diffusion resistance.},
doi = {10.1021/acs.jpcc.7b12327},
journal = {Journal of Physical Chemistry. C},
issn = {1932-7447},
number = 25,
volume = 122,
place = {United States},
year = {2017},
month = {12}
}

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