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Title: Single-Atomic Ruthenium Catalytic Sites on Nitrogen-Doped Graphene for Oxygen Reduction Reaction in Acidic Medium

Authors:
; ORCiD logo [1]; ; ; ; ; ; ;  [1];  [2]; ORCiD logo [2]; ; ;  [3];  [3]; ORCiD logo
  1. School of Materials Science and Engineering, Tianjin Key Laboratory of Composite and Functional Materials, Tianjin University, Tianjin 300350, China, Collaborative Innovation Center of Chemical Science and Engineering, Tianjin 300350, China
  2. Shanghai Synchrotron Radiation Facility, Shanghai Institute of Applied Physics, Chinese Academy of Sciences, Shanghai 201204, China
  3. Beijing Synchrotron Radiation Facility, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100049, China
Publication Date:
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1414051
Grant/Contract Number:
SC0012547
Resource Type:
Journal Article: Published Article
Journal Name:
ACS Nano
Additional Journal Information:
Journal Volume: 11; Journal Issue: 7; Related Information: CHORUS Timestamp: 2017-12-19 17:30:18; Journal ID: ISSN 1936-0851
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English

Citation Formats

Zhang, Chenhao, Sha, Junwei, Fei, Huilong, Liu, Mingjie, Yazdi, Sadegh, Zhang, Jibo, Zhong, Qifeng, Zou, Xiaolong, Zhao, Naiqin, Yu, Haisheng, Jiang, Zheng, Ringe, Emilie, Yakobson, Boris I., Dong, Juncai, Chen, Dongliang, and Tour, James M.. Single-Atomic Ruthenium Catalytic Sites on Nitrogen-Doped Graphene for Oxygen Reduction Reaction in Acidic Medium. United States: N. p., 2017. Web. doi:10.1021/acsnano.7b02148.
Zhang, Chenhao, Sha, Junwei, Fei, Huilong, Liu, Mingjie, Yazdi, Sadegh, Zhang, Jibo, Zhong, Qifeng, Zou, Xiaolong, Zhao, Naiqin, Yu, Haisheng, Jiang, Zheng, Ringe, Emilie, Yakobson, Boris I., Dong, Juncai, Chen, Dongliang, & Tour, James M.. Single-Atomic Ruthenium Catalytic Sites on Nitrogen-Doped Graphene for Oxygen Reduction Reaction in Acidic Medium. United States. doi:10.1021/acsnano.7b02148.
Zhang, Chenhao, Sha, Junwei, Fei, Huilong, Liu, Mingjie, Yazdi, Sadegh, Zhang, Jibo, Zhong, Qifeng, Zou, Xiaolong, Zhao, Naiqin, Yu, Haisheng, Jiang, Zheng, Ringe, Emilie, Yakobson, Boris I., Dong, Juncai, Chen, Dongliang, and Tour, James M.. Wed . "Single-Atomic Ruthenium Catalytic Sites on Nitrogen-Doped Graphene for Oxygen Reduction Reaction in Acidic Medium". United States. doi:10.1021/acsnano.7b02148.
@article{osti_1414051,
title = {Single-Atomic Ruthenium Catalytic Sites on Nitrogen-Doped Graphene for Oxygen Reduction Reaction in Acidic Medium},
author = {Zhang, Chenhao and Sha, Junwei and Fei, Huilong and Liu, Mingjie and Yazdi, Sadegh and Zhang, Jibo and Zhong, Qifeng and Zou, Xiaolong and Zhao, Naiqin and Yu, Haisheng and Jiang, Zheng and Ringe, Emilie and Yakobson, Boris I. and Dong, Juncai and Chen, Dongliang and Tour, James M.},
abstractNote = {},
doi = {10.1021/acsnano.7b02148},
journal = {ACS Nano},
number = 7,
volume = 11,
place = {United States},
year = {Wed Jun 28 00:00:00 EDT 2017},
month = {Wed Jun 28 00:00:00 EDT 2017}
}

Journal Article:
Free Publicly Available Full Text
This content will become publicly available on June 28, 2018
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Citation Metrics:
Cited by: 2works
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  • A novel PtCo alloy in situ etched and embedded in graphene nanopores (PtCo/NPG) as a high-performance catalyst for ORR was reported. Graphene nanopores were fabricated in situ while forming PtCo nanoparticles that were uniformly embedded in the graphene nanopores. Given the synergistic effect between PtCo alloy and nanopores, PtCo/NPG exhibited 11.5 times higher mass activity than that of the commercial Pt/C cathode electrocatalyst. DFT calculations indicated that the nanopores in NPG cannot only stabilize PtCo nanoparticles but can also definitely change the electronic structures, thereby change its adsorption abilities. This enhancement can lead to a favorable reaction pathway on PtCo/NPGmore » for ORR. This study showed that PtCo/NPG is a potential candidate for the next generation of Pt-based catalysts in fuel cells. This study also offered a promising alternative strategy and enabled the fabrication of various kinds of metal/graphene nanopore nanohybrids with potential applications in catalysts and potential use for other technological devices. The authors acknowledge the financial support from the National Basic Research Program (973 program, No. 2013CB733501), Zhejiang Provincial Education Department Research Program (Y201326554) and the National Natural Science Foundation of China (No. 21306169, 21101137, 21136001, 21176221 and 91334013). D. Mei acknowledges the support from the US Department of Energy, Office of Science, Office of Basic Energy Sciences, Division of Division of Chemical Sciences, Geosciences & Biosciences. Pacific Northwest National Laboratory (PNNL) is a multiprogram national laboratory operated for DOE by Battelle. Computing time was granted by the grand challenge of computational catalysis of the William R. Wiley Environmental Molecular Sciences Laboratory (EMSL) and by the National Energy Research Scientific Computing Center (NERSC).« less
  • Nitrogen doped graphene oxide (Nr-GO) with properties suitable for electrocatalysts is easily synthesized using phenylhydrazine as a reductant at relatively low temperature. The reducing agent removes various oxygen functional groups bonded to graphene oxide and simultaneously dope the nitrogen atoms bonded with phenyl group all over the basal planes and edge sites of the graphene. The Nr-GO exhibits remarkable electrocatalytic activities for oxygen reduction reaction compared to the commercial carbon black and graphene oxide due to the electronic modification of the graphene structure. In addition, Nr-GO shows excellent dispersibility in various solvent due to the dopant molecules.
  • A nitrogen and sulfur co-doped graphene/carbon black (NSGCB) nanocomposite for the oxygen reduction reaction (ORR) was synthesized through a one-pot annealing of a precursor mixture containing graphene oxide, thiourea, and acidized carbon black (CB). The NSGCB showed excellent performance for the ORR with the onset and half-way potentials at 0.96 V and 0.81 V (vs. RHE), respectively. It is significantly improved over that of the catalysts derived from only graphene (0.90 V and 0.76 V) or carbon nanosphere (0.82 V and 0.74 V). The enhanced catalytic activity on the NSGCB electrode could be attributed to the synergistic effect of N/Smore » co-doping and the enlarged interlayer space resulted from the insertion of carbon nanosphere into the graphene sheets. The four-electron selectivity and the limiting current density of the NSGCB nanocomposite are comparable to that of the commercially Pt/C catalyst. Furthermore, the NSGCB nanocomposite was superior to Pt/C in terms of long-term durability and tolerance to methanol poisoning.« less