Aluminum and Nitrogen Codoped Graphene: Highly Active and Durable Electrocatalyst for Oxygen Reduction Reaction
Abstract
The development of a highly active and exceedingly durable electrocatalyst at low cost for the oxygen reduction reaction (ORR) is extremely desirable but remains to be a grand challenge. Over the past decade, the transitional-metal (e.g., Fe, Co, Ni) and N codoped graphene materials have attracted most attention as the state-of-the-art nonprecious-metal-based effective electrocatalyst for ORR but still entail unsatisfactory issues such as moderate activity and life. Herein, the main-group-metal Al and N codoped graphene (ANG) is successfully fabricated via thermal annealing treatment of N-doped graphene with aluminum tri-(8-hydroxyquinoline). As a highly effective electrocatalyst for ORR, the as-prepared ANG exhibits not only high electrocatalytic activity that even outperforms the commercial Pt/C but also good durability in both three-electrode cell and Zn-air battery. Theoretical calculations show that the inhomogeneous charge density distribution and the interaction between Al and N are mainly responsible for the marked enhancement of ORR activity. Finally, the designed ANG electrocatalysts will provide a perspective application in energy storage and promote further exploration of main-group-element-based inexpensive, active, and durable electrocatalysts.
- Authors:
-
[1];
[2];
[3];
[1];
[4];
[3];
[3];
[2]
- Changzhou Univ., Jiangsu (China)
- Univ. of Nebraska, Lincoln, NE (United States)
- Georgia Inst. of Technology, Atlanta, GA (United States)
- Xiamen Univ., Fujian (China)
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC); Univ. of California, Oakland, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC)
- OSTI Identifier:
- 1543711
- Grant/Contract Number:
- AC02-05CH11231
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ACS Catalysis
- Additional Journal Information:
- Journal Volume: 9; Journal Issue: 1; Journal ID: ISSN 2155-5435
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; chemistry; Al-doped graphene; N-doped graphene; oxygen reduction reaction; electrocatalyst; noble-metal free
Citation Formats
Qin, Yong, Wu, Hong-Hui, Zhang, Lei A., Zhou, Xiao, Bu, Yunfei, Zhang, Wei, Chu, Fuqiang, Li, Yutong, Kong, Yong, Zhang, Qiaobao, Ding, Dong, Tao, Yongxin, Li, Yongxin, Liu, Meilin, and Zeng, Xiao Cheng. Aluminum and Nitrogen Codoped Graphene: Highly Active and Durable Electrocatalyst for Oxygen Reduction Reaction. United States: N. p., 2018.
Web. doi:10.1021/acscatal.8b04117.
Qin, Yong, Wu, Hong-Hui, Zhang, Lei A., Zhou, Xiao, Bu, Yunfei, Zhang, Wei, Chu, Fuqiang, Li, Yutong, Kong, Yong, Zhang, Qiaobao, Ding, Dong, Tao, Yongxin, Li, Yongxin, Liu, Meilin, & Zeng, Xiao Cheng. Aluminum and Nitrogen Codoped Graphene: Highly Active and Durable Electrocatalyst for Oxygen Reduction Reaction. United States. https://doi.org/10.1021/acscatal.8b04117
Qin, Yong, Wu, Hong-Hui, Zhang, Lei A., Zhou, Xiao, Bu, Yunfei, Zhang, Wei, Chu, Fuqiang, Li, Yutong, Kong, Yong, Zhang, Qiaobao, Ding, Dong, Tao, Yongxin, Li, Yongxin, Liu, Meilin, and Zeng, Xiao Cheng. Fri .
"Aluminum and Nitrogen Codoped Graphene: Highly Active and Durable Electrocatalyst for Oxygen Reduction Reaction". United States. https://doi.org/10.1021/acscatal.8b04117. https://www.osti.gov/servlets/purl/1543711.
@article{osti_1543711,
title = {Aluminum and Nitrogen Codoped Graphene: Highly Active and Durable Electrocatalyst for Oxygen Reduction Reaction},
author = {Qin, Yong and Wu, Hong-Hui and Zhang, Lei A. and Zhou, Xiao and Bu, Yunfei and Zhang, Wei and Chu, Fuqiang and Li, Yutong and Kong, Yong and Zhang, Qiaobao and Ding, Dong and Tao, Yongxin and Li, Yongxin and Liu, Meilin and Zeng, Xiao Cheng},
abstractNote = {The development of a highly active and exceedingly durable electrocatalyst at low cost for the oxygen reduction reaction (ORR) is extremely desirable but remains to be a grand challenge. Over the past decade, the transitional-metal (e.g., Fe, Co, Ni) and N codoped graphene materials have attracted most attention as the state-of-the-art nonprecious-metal-based effective electrocatalyst for ORR but still entail unsatisfactory issues such as moderate activity and life. Herein, the main-group-metal Al and N codoped graphene (ANG) is successfully fabricated via thermal annealing treatment of N-doped graphene with aluminum tri-(8-hydroxyquinoline). As a highly effective electrocatalyst for ORR, the as-prepared ANG exhibits not only high electrocatalytic activity that even outperforms the commercial Pt/C but also good durability in both three-electrode cell and Zn-air battery. Theoretical calculations show that the inhomogeneous charge density distribution and the interaction between Al and N are mainly responsible for the marked enhancement of ORR activity. Finally, the designed ANG electrocatalysts will provide a perspective application in energy storage and promote further exploration of main-group-element-based inexpensive, active, and durable electrocatalysts.},
doi = {10.1021/acscatal.8b04117},
journal = {ACS Catalysis},
number = 1,
volume = 9,
place = {United States},
year = {Fri Dec 07 00:00:00 EST 2018},
month = {Fri Dec 07 00:00:00 EST 2018}
}
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Works referenced in this record:
Recent advancements in Pt and Pt-free catalysts for oxygen reduction reaction
journal, January 2015
- Nie, Yao; Li, Li; Wei, Zidong
- Chemical Society Reviews, Vol. 44, Issue 8
A Free-Standing Pt-Nanowire Membrane as a Highly Stable Electrocatalyst for the Oxygen Reduction Reaction
journal, February 2011
- Liang, Hai-Wei; Cao, Xiang; Zhou, Fei
- Advanced Materials, Vol. 23, Issue 12
High-performance transition metal-doped Pt3Ni octahedra for oxygen reduction reaction
journal, June 2015
- Huang, X.; Zhao, Z.; Cao, L.
- Science, Vol. 348, Issue 6240
An oxygen reduction electrocatalyst based on carbon nanotube–graphene complexes
journal, May 2012
- Li, Yanguang; Zhou, Wu; Wang, Hailiang
- Nature Nanotechnology, Vol. 7, Issue 6
Ultrathin graphitic carbon nitride nanosheets: a low-cost, green, and highly efficient electrocatalyst toward the reduction of hydrogen peroxide and its glucose biosensing application
journal, January 2013
- Tian, Jingqi; Liu, Qian; Ge, Chenjiao
- Nanoscale, Vol. 5, Issue 19
Nitrogen-doped carbon xerogel: A novel carbon-based electrocatalyst for oxygen reduction reaction in proton exchange membrane (PEM) fuel cells
journal, January 2011
- Jin, Hong; Zhang, Huamin; Zhong, Hexiang
- Energy & Environmental Science, Vol. 4, Issue 9
Chemical doping of graphene
journal, January 2011
- Liu, Hongtao; Liu, Yunqi; Zhu, Daoben
- J. Mater. Chem., Vol. 21, Issue 10
Nitrogen-Doped Carbon Nanotube Arrays with High Electrocatalytic Activity for Oxygen Reduction
journal, February 2009
- Gong, K.; Du, F.; Xia, Z.
- Science, Vol. 323, Issue 5915, p. 760-764
Electrocatalytic Activity of Nitrogen-Doped Carbon Nanotube Cups
journal, September 2009
- Tang, Yifan; Allen, Brett L.; Kauffman, Douglas R.
- Journal of the American Chemical Society, Vol. 131, Issue 37
Nitrogen-Doped Graphene as Efficient Metal-Free Electrocatalyst for Oxygen Reduction in Fuel Cells
journal, February 2010
- Qu, Liangti; Liu, Yong; Baek, Jong-Beom
- ACS Nano, Vol. 4, Issue 3, p. 1321-1326
Nitrogen-Doped Carbon Nanocages as Efficient Metal-Free Electrocatalysts for Oxygen Reduction Reaction
journal, August 2012
- Chen, Sheng; Bi, Jiyu; Zhao, Yu
- Advanced Materials, Vol. 24, Issue 41
N-Doped graphene nanosheets for Li–air fuel cells under acidic conditions
journal, January 2012
- Yoo, Eunjoo; Nakamura, Junji; Zhou, Haoshen
- Energy & Environmental Science, Vol. 5, Issue 5
Highly Efficient Metal-Free Growth of Nitrogen-Doped Single-Walled Carbon Nanotubes on Plasma-Etched Substrates for Oxygen Reduction
journal, November 2010
- Yu, Dingshan; Zhang, Qiang; Dai, Liming
- Journal of the American Chemical Society, Vol. 132, Issue 43
Can Boron and Nitrogen Co-doping Improve Oxygen Reduction Reaction Activity of Carbon Nanotubes?
journal, January 2013
- Zhao, Yu; Yang, Lijun; Chen, Sheng
- Journal of the American Chemical Society, Vol. 135, Issue 4
Synthesis, Structure, and Properties of Boron- and Nitrogen-Doped Graphene
journal, August 2009
- Panchakarla, L. S.; Subrahmanyam, K. S.; Saha, S. K.
- Advanced Materials
Two-Step Boron and Nitrogen Doping in Graphene for Enhanced Synergistic Catalysis
journal, January 2013
- Zheng, Yao; Jiao, Yan; Ge, Lei
- Angewandte Chemie International Edition, Vol. 52, Issue 11
Sulfur and Nitrogen Dual-Doped Mesoporous Graphene Electrocatalyst for Oxygen Reduction with Synergistically Enhanced Performance
journal, October 2012
- Liang, Ji; Jiao, Yan; Jaroniec, Mietek
- Angewandte Chemie International Edition, Vol. 51, Issue 46
Low-temperature synthesis of nitrogen/sulfur co-doped three-dimensional graphene frameworks as efficient metal-free electrocatalyst for oxygen reduction reaction
journal, October 2013
- Su, Yuezeng; Zhang, Yi; Zhuang, Xiaodong
- Carbon, Vol. 62
One-pot synthesis of nitrogen and sulfur co-doped graphene as efficient metal-free electrocatalysts for the oxygen reduction reaction
journal, January 2014
- Wang, Xin; Wang, Jie; Wang, Deli
- Chem. Commun., Vol. 50, Issue 37
Identification of catalytic sites for oxygen reduction in iron- and nitrogen-doped graphene materials
journal, August 2015
- Zitolo, Andrea; Goellner, Vincent; Armel, Vanessa
- Nature Materials, Vol. 14, Issue 9
Efficient approach to iron/nitrogen co-doped graphene materials as efficient electrochemical catalysts for the oxygen reduction reaction
journal, January 2015
- Dong, Qingqing; Zhuang, Xiaodong; Li, Zhi
- Journal of Materials Chemistry A, Vol. 3, Issue 15
Instantaneous one-pot synthesis of Fe–N-modified graphene as an efficient electrocatalyst for the oxygen reduction reaction in acidic solutions
journal, January 2012
- Kamiya, Kazuhide; Hashimoto, Kazuhito; Nakanishi, Shuji
- Chemical Communications, Vol. 48, Issue 82
Cobalt and Nitrogen Codoped Graphene with Inserted Carbon Nanospheres as an Efficient Bifunctional Electrocatalyst for Oxygen Reduction and Evolution
journal, July 2016
- Qiao, Xiaochang; Liao, Shijun; Zheng, Ruiping
- ACS Sustainable Chemistry & Engineering, Vol. 4, Issue 8
Facile synthesis of cobalt and nitrogen co-doped graphene networks from polyaniline for oxygen reduction reaction in acidic solutions
journal, January 2016
- Peng, Shuqin; Jiang, Hongmei; Zhang, Youming
- Journal of Materials Chemistry A, Vol. 4, Issue 10
Identification of catalytic sites in cobalt-nitrogen-carbon materials for the oxygen reduction reaction
journal, October 2017
- Zitolo, Andrea; Ranjbar-Sahraie, Nastaran; Mineva, Tzonka
- Nature Communications, Vol. 8, Issue 1
Nitrogen, Phosphorus, and Fluorine Tri-doped Graphene as a Multifunctional Catalyst for Self-Powered Electrochemical Water Splitting
journal, October 2016
- Zhang, Jintao; Dai, Liming
- Angewandte Chemie International Edition, Vol. 55, Issue 42
Combining theory and experiment in electrocatalysis: Insights into materials design
journal, January 2017
- Seh, Zhi Wei; Kibsgaard, Jakob; Dickens, Colin F.
- Science, Vol. 355, Issue 6321
Catalyzing the Hydrogen Evolution Reaction (HER) with Molybdenum Sulfide Nanomaterials
journal, October 2014
- Benck, Jesse D.; Hellstern, Thomas R.; Kibsgaard, Jakob
- ACS Catalysis, Vol. 4, Issue 11
Mechanisms of Oxygen Reduction Reaction on Nitrogen-Doped Graphene for Fuel Cells
journal, May 2011
- Zhang, Lipeng; Xia, Zhenhai
- The Journal of Physical Chemistry C, Vol. 115, Issue 22
Density-Functional-Theory Calculation Analysis of Active Sites for Four-Electron Reduction of O 2 on Fe/N-Doped Graphene
journal, October 2014
- Liang, Wei; Chen, Junxiang; Liu, Yuwen
- ACS Catalysis, Vol. 4, Issue 11
Boron-doped graphene as active electrocatalyst for oxygen reduction reaction at a fuel-cell cathode
journal, October 2014
- Fazio, Gianluca; Ferrighi, Lara; Di Valentin, Cristiana
- Journal of Catalysis, Vol. 318
Nitrogen-Coordinated Single Cobalt Atom Catalysts for Oxygen Reduction in Proton Exchange Membrane Fuel Cells
journal, January 2018
- Wang, Xiao Xia; Cullen, David A.; Pan, Yung-Tin
- Advanced Materials, Vol. 30, Issue 11
Noble-Metal-Free Fe–N/C Catalyst for Highly Efficient Oxygen Reduction Reaction under Both Alkaline and Acidic Conditions
journal, July 2014
- Lin, Ling; Zhu, Qing; Xu, An-Wu
- Journal of the American Chemical Society, Vol. 136, Issue 31
Comparative study of CoFeNx/C catalyst obtained by pyrolysis of hemin and cobalt porphyrin for catalytic oxygen reduction in alkaline and acidic electrolytes
journal, January 2014
- Jiang, Rongzhong; Chu, Deryn
- Journal of Power Sources, Vol. 245
Oxygen Reduction Reaction Mechanisms on Al-Doped X-Graphene (X = N, P, and S) Catalysts in Acidic Medium: A Comparative DFT Study
journal, November 2016
- Bhatt, Mahesh Datt; Lee, Guensik; Lee, Jae Sung
- The Journal of Physical Chemistry C, Vol. 120, Issue 46
Crosslinking Graphene Oxide into Robust 3D Porous N-Doped Graphene
journal, August 2015
- Qin, Yong; Yuan, Jie; Li, Juan
- Advanced Materials, Vol. 27, Issue 35
Restacking-Inhibited 3D Reduced Graphene Oxide for High Performance Supercapacitor Electrodes
journal, September 2013
- Lee, Ji Hoon; Park, Nokyoung; Kim, Byung Gon
- ACS Nano, Vol. 7, Issue 10
2D Porous Carbons prepared from Layered Organic-Inorganic Hybrids and their Use as Oxygen-Reduction Electrocatalysts
journal, May 2017
- Li, Shuang; Cheng, Chong; Liang, Hai-Wei
- Advanced Materials, Vol. 29, Issue 28
Transparent Conductive Electrodes from Graphene/PEDOT:PSS Hybrid Inks for Ultrathin Organic Photodetectors
journal, November 2014
- Liu, Zhaoyang; Parvez, Khaled; Li, Rongjin
- Advanced Materials, Vol. 27, Issue 4
Rationally Designed 3D Fe and N Codoped Graphene with Superior Electrocatalytic Activity toward Oxygen Reduction
journal, March 2016
- Qin, Yong; Yuan, Jie; Zhang, Lei
- Small, Vol. 12, Issue 19
Co3O4 nanocrystals on graphene as a synergistic catalyst for oxygen reduction reaction
journal, August 2011
- Liang, Yongye; Li, Yanguang; Wang, Hailiang
- Nature Materials, Vol. 10, Issue 10, p. 780-786
DMFCs: From Fundamental Aspects to Technology Development
journal, July 2001
- Aricò, A. S.; Srinivasan, S.; Antonucci, V.
- Fuel Cells, Vol. 1, Issue 2
The impact of mass transport and methanol crossover on the direct methanol fuel cell
journal, October 1999
- Scott, K.; Taama, W. M.; Argyropoulos, P.
- Journal of Power Sources, Vol. 83, Issue 1-2
Metal-Air Batteries with High Energy Density: Li-Air versus Zn-Air
journal, December 2010
- Lee, Jang-Soo; Tai Kim, Sun; Cao, Ruiguo
- Advanced Energy Materials, Vol. 1, Issue 1, p. 34-50
Rechargeable Zn-air batteries: Progress in electrolyte development and cell configuration advancement
journal, June 2015
- Xu, M.; Ivey, D. G.; Xie, Z.
- Journal of Power Sources, Vol. 283
Modulating the oxygen reduction activity of heteroatom-doped carbon catalysts via the triple effect: charge, spin density and ligand effect
journal, January 2018
- Yang, Na; Li, Li; Li, Jing
- Chemical Science, Vol. 9, Issue 26
Catalytic activities enhanced by abundant structural defects and balanced N distribution of N-doped graphene in oxygen reduction reaction
journal, February 2016
- Bai, Xiaogong; Shi, Yantao; Guo, Jiahao
- Journal of Power Sources, Vol. 306
A universal principle for a rational design of single-atom electrocatalysts
journal, April 2018
- Xu, Haoxiang; Cheng, Daojian; Cao, Dapeng
- Nature Catalysis, Vol. 1, Issue 5
In situ synthesis of highly loaded and ultrafine Pd nanoparticles-decorated graphene oxide for glucose biosensor application
journal, January 2012
- Qin, Yong; Kong, Yong; Xu, Yiyang
- Journal of Materials Chemistry, Vol. 22, Issue 47
Facile Oxygen Reduction on a Three-Dimensionally Ordered Macroporous Graphitic C3N4/Carbon Composite Electrocatalyst
journal, March 2012
- Liang, Ji; Zheng, Yao; Chen, Jun
- Angewandte Chemie International Edition, Vol. 51, Issue 16
Electrochemically exfoliating graphite into N-doped graphene and its use as a high efficient electrocatalyst for oxygen reduction reaction
journal, December 2016
- Chao, Lei; Qin, Yong; Liu, Yang
- Journal of Solid State Electrochemistry, Vol. 21, Issue 5
Projector augmented-wave method
journal, December 1994
- Blöchl, P. E.
- Physical Review B, Vol. 50, Issue 24, p. 17953-17979
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set
journal, October 1996
- Kresse, G.; Furthmüller, J.
- Physical Review B, Vol. 54, Issue 16, p. 11169-11186
Origin of the Overpotential for Oxygen Reduction at a Fuel-Cell Cathode
journal, November 2004
- Nørskov, J. K.; Rossmeisl, J.; Logadottir, A.
- The Journal of Physical Chemistry B, Vol. 108, Issue 46
Oxygen Reduction in Alkaline Media: From Mechanisms to Recent Advances of Catalysts
journal, July 2015
- Ge, Xiaoming; Sumboja, Afriyanti; Wuu, Delvin
- ACS Catalysis, Vol. 5, Issue 8
Component Matters: Paving the Roadmap toward Enhanced Electrocatalytic Performance of Graphitic C 3 N 4 -Based Catalysts via Atomic Tuning
journal, May 2017
- Pei, Zengxia; Gu, Jingxing; Wang, Yukun
- ACS Nano, Vol. 11, Issue 6
Works referencing / citing this record:
Oxygen Evolution Reaction on 2D Ferromagnetic Fe 3 GeTe 2 : Boosting the Reactivity by the Self‐Reduction of Surface Hydroxyl
journal, August 2019
- Zhao, Yinghe; Gu, Jinxing; Chen, Zhongfang
- Advanced Functional Materials, Vol. 29, Issue 44
A pyrolysis-free path toward superiorly catalytic nitrogen-coordinated single atom
journal, August 2019
- Peng, Peng; Shi, Lei; Huo, Feng
- Science Advances, Vol. 5, Issue 8
Directly transforming copper (I) oxide bulk into isolated single-atom copper sites catalyst through gas-transport approach
journal, August 2019
- Yang, Zhengkun; Chen, Bingxu; Chen, Wenxing
- Nature Communications, Vol. 10, Issue 1
Boosting the hydrogen evolution activity of a Co–N–C electrocatalyst by codoping with Al
journal, January 2019
- Zhou, Xiao; Yu, Haoran; Liu, Yang
- RSC Advances, Vol. 9, Issue 58
Hatted 1T/2H‐Phase MoS 2 on Ni 3 S 2 Nanorods for Efficient Overall Water Splitting in Alkaline Media
journal, January 2020
- Zhao, Yang; Wei, Shizhong; Wang, Feihong
- Chemistry – A European Journal, Vol. 26, Issue 9
Directly transforming copper (I) oxide bulk into isolated single-atom copper sites catalyst through gas-transport approach
journal, August 2019
- Yang, Zhengkun; Chen, Bingxu; Chen, Wenxing
- Nature Communications, Vol. 10, Issue 1