AI Chat Paper
Note: Please note that the following content is generated by AMiner AI. SciOpen does not take any responsibility related to this content.
{{lang === 'zh_CN' ? '文章概述' : 'Summary'}}
{{lang === 'en_US' ? '中' : 'Eng'}}
Chat more with AI
Powered by AMiner. Clicking this button will take you away from SciOpen.
Home Nano Research Article
Article Link
Cite
EndNote(RIS) BibTeX
Collect
Submit Manuscript
Show Outline
Outline
Show full outline
Hide outline
Outline
Show full outline
Hide outline
Research Article

Single copper sites dispersed on hierarchically porous carbon for improving oxygen reduction reaction towards zinc-air battery

Wenjie Wu1,§, Yan Liu2,§, Dong Liu3, Wenxing Chen4, Zhaoyi Song1, Ximin Wang1, Yamin Zheng2, Ning Lu2, Chunxia Wang1( ), Junjie Mao2( ), Yadong Li5
State Key Laboratory of Heavy Oil Processing, College of New Energy and Materials, China University of Petroleum, Beijing 102249, China
Key Laboratory of Functional Molecular Solids, Ministry of Education, Anhui Province Key Laboratory of Optoelectric Materials Science and Technology and Anhui Laboratory of Molecule-Based Materials, Anhui Normal University, Wuhu 241002, China
State key Lab of Organic-Inorganic Composites, Beijing University of Chemical Technology, Beijing 100029, China
Beijing Key Laboratory of Construction Tailorable Advanced Functional Materials and Green Applications, School of Materials Science and Engineering, Beijing Institute of Technology, Beijing 100081, China
Department of Chemistry, Tsinghua University, Beijing 100084, China

§ Wenjie Wu and Yan Liu contributed equally to this work.

Show Author Information

Graphical Abstract

Abstract

The demand for high-performance non-precious-metal electrocatalysts to replace the noble metal-based catalysts for oxygen reduction reaction (ORR) is intensively increasing. Herein, single-atomic copper sites supported on N-doped three-dimensional hierarchically porous carbon catalyst (Cu1/NC) was prepared by coordination pyrolysis strategy. Remarkably, the Cu1/NC-900 catalyst not only exhibits excellent ORR performance with a half-wave potential of 0.894 V (vs. RHE) in alkaline media, outperforming those of commercial Pt/C (0.851 V) and Cu nanoparticles anchored on N-doped porous carbon (CuNPs/NC-900), but also demonstrates high stability and methanol tolerance. Moreover, the Cu1/NC-900 based Zn-air battery exhibits higher power density, rechargeability and cyclic stability than the one based on Pt/C. Both experimental and theoretical investigations demonstrated that the excellent performance of the as-obtained Cu1/NC-900 could be attributed to the synergistic effect between copper coordinated by three N atoms active sites and the neighbouring carbon defect, resulting in elevated Cu d-band centers of Cu atoms and facilitating intermediate desorption for ORR process. This study may lead towards the development of highly efficient non-noble metal catalysts for applications in electrochemical energy conversion.

Keywords

single atomic sites catalystsnitrogen-doped carbon materialsoxygen reduction reactioncarbon defectnon-noble metal

Electronic Supplementary Material

Download File(s)
12274_2020_3141_MOESM1_ESM.pdf (7.6 MB)

References

[1]
M. Armand,; J. M. Tarascon, Building better batteries. Nature 2008, 451, 652-657.
Crossref Google Scholar
[2]
S. Chu,; A. Majumdar, Opportunities and challenges for a sustainable energy future. Nature 2012, 488, 294-303.
Crossref Google Scholar
[3]
J. J. Mao,; L. F. Yang,; P. Yu,; X. W. Wei,; L. Q. Mao, Electrocatalytic four-electron reduction of oxygen with copper (II)-based metal- organic frameworks. Electrochem. Commun. 2012, 19, 29-31.
Crossref Google Scholar
[4]
Y. G. Li,; H. J. Dai, Recent advances in zinc-air batteries. Chem. Soc. Rev. 2014, 43, 5257-5275.
Crossref Google Scholar
[5]
M. H. Shao,; Q. W. Chang,; J. P. Dodelet,; R. Chenitz, Recent advances in electrocatalysts for oxygen reduction reaction. Chem. Rev. 2016, 116, 3594-3657.
Crossref Google Scholar
[6]
B. Y. Xia,; Y. Yan,; N. Li,; H. B. Wu,; X. W. Lou,; X. Wang, A metal-organic framework-derived bifunctional oxygen electrocatalyst. Nat. Energy 2016, 1, 15006.
Crossref Google Scholar
[7]
Z. K. Yang,; B. X. Chen,; W. X. Chen,; Y. T. Qu,; F. Y. Zhou,; C. M. Zhao,; Q. Xu,; Q. H. Zhang,; X. Z. Duan,; Y. E. Wu, Directly transforming copper(I) oxide bulk into isolated single-atom copper sites catalyst through gas-transport approach. Nat. Commun. 2019, 10, 3734.
Crossref Google Scholar
[8]
X. P. Han,; X. F. Ling,; D. S. Yu,; D. Y. Xie,; L. L. Li,; S. J. Peng,; C. Zhong,; N. Q. Zhao,; Y. D. Deng,; W. B. Hu, Atomically dispersed binary Co-Ni sites in nitrogen-doped hollow carbon nanocubes for reversible oxygen reduction and evolution. Adv. Mater. 2019, 31, 1905622.
Crossref Google Scholar
[9]
N. Q. Zhang,; C. L. Ye,; H. Yan,; L. C. Li,; H. He,; D. S. Wang,; Y. D. Li, Single-atom site catalysts for environmental catalysis. Nano Res. 2020, 13, 3165-3182.
Crossref Google Scholar
[10]
T. T. Sun,; Y. L. Li,; T. T. Cui,; L. B. Xu,; Y. G. Wang,; W. X. Chen,; P. P. Zhang,; T. Y. Zheng,; X. Z. Fu,; S. L. Zhang, et al. Engineering of coordination environment and multiscale structure in single-site copper catalyst for superior electrocatalytic oxygen reduction. Nano Lett. 2020, 20, 6206-6214.
Crossref Google Scholar
[11]
P. Q. Yin,; T. Yao,; Y. E. Wu,; L. R. Zheng,; Y. Lin,; W. Liu,; H. X. Ju,; J. F. Zhu,; X. Hong,; Z. X. Deng, et al. Single cobalt atoms with precise N-coordination as superior oxygen reduction reaction catalysts. Angew. Chem., Int. Ed. 2016, 55, 10800-10805.
Crossref Google Scholar
[12]
J. J. Mao,; J. Li,; J. J. Pei,; Y. Liu,; D. S. Wang,; Y. D. Li, Structure regulation of noble-metal-based nanomaterials at an atomic level. Nano Today 2019, 26, 164-175.
Crossref Google Scholar
[13]
K. Li,; X. X. Li,; H. W. Huang,; L. H. Luo,; X. Li,; X. P. Yan,; C. Ma,; R. Si,; J. L. Yang,; J. Zeng, One-nanometer-thick PtNiRh trimetallic nanowires with enhanced oxygen reduction electrocatalysis in acid media: Integrating multiple advantages into one catalyst. J. Am. Chem. Soc. 2018, 140, 16159-16167.
Crossref Google Scholar
[14]
J. J. Mao,; Y. J. Chen,; J. J. Pei,; D. S. Wang,; Y. D. Li, Pt-M (M = Cu, Fe, Zn, etc.) bimetallic nanomaterials with abundant surface defects and robust catalytic properties. Chem. Commun. 2016, 52, 5985-5988.
Crossref Google Scholar
[15]
F. Li,; G. F. Han,; H. J. Noh,; S. J. Kim,; Y. L. Lu,; H. Y. Jeong,; Z. P. Fu,; J. B. Baek, Boosting oxygen reduction catalysis with abundant copper single atom active sites. Energy Environ. Sci. 2018, 11, 2263-2269.
Crossref Google Scholar
[16]
X. X. Wang,; D. A. Cullen,; Y. T. Pan,; S. Hwang,; M. Y. Wang,; Z. X. Feng,; J. Y. Wang,; M. H. Engelhard,; H. G. Zhang,; Y. H. He, et al. Nitrogen-coordinated single cobalt atom catalysts for oxygen reduction in proton exchange membrane fuel cells. Adv. Mater. 2018, 30, 1706758.
Crossref Google Scholar
[17]
H. S. Shang,; W. M. Sun,; R. Sui,; J. J. Pei,; L. R. Zheng,; J. C. Dong,; Z. L. Jiang,; D. N. Zhou,; Z. B. Zhuang,; W. X. Chen, et al. Engineering isolated Mn-N2C2 atomic interface sites for efficient bifunctional oxygen reduction and evolution reaction. Nano Lett. 2020, 20, 5443-5450.
Crossref Google Scholar
[18]
H. H. Wu,; H. B. Li,; X. F. Zhao,; Q. F. Liu,; J. Wang,; J. P. Xiao,; S. H. Xie,; R. Si,; F. Yang,; S. Miao, et al. Highly doped and exposed Cu(I)-N active sites within graphene towards efficient oxygen reduction for zinc-air batteries. Energy Environ. Sci. 2016, 9, 3736-3745.
Crossref Google Scholar
[19]
H. G. Zhang,; S. Hwang,; M. Y. Wang,; Z. X. Feng,; S. Karakalos,; L. L. Luo,; Z. Qiao,; X. H. Xie,; C. M. Wang,; D. Su, et al. Single atomic iron catalysts for oxygen reduction in acidic media: Particle size control and thermal activation. J. Am. Chem. Soc. 2017, 139, 14143-14149.
Crossref Google Scholar
[20]
T. T. Sun,; L. B. Xu,; D. S. Wang,; Y. D. Li, Metal organic frameworks derived single atom catalysts for electrocatalytic energy conversion. Nano Res. 2019, 12, 2067-2080.
Crossref Google Scholar
[21]
J. J. Mao,; J. S. Yin,; J. J. Pei,; D. S. Wang,; Y. D. Li, Single atom alloy: An emerging atomic site material for catalytic applications. Nano Today 2020, 34, 100917.
Crossref Google Scholar
[22]
J. Q. Sun,; S. E. Lowe,; L. J. Zhang,; Y. Z. Wang,; K. L. Pang,; Y. Wang,; Y. L. Zhong,; P. R. Liu,; K. Zhao,; Z. Y. Tang, et al. Ultrathin nitrogen-doped holey carbon@graphene bifunctional electrocatalyst for oxygen reduction and evolution reactions in alkaline and acidic media. Angew. Chem., Int. Ed. 2018, 57, 16511-16515.
Crossref Google Scholar
[23]
H. S. Shang,; X. Y. Zhou,; J. C. Dong,; A. Li,; X. Zhao,; Q. H. Liu,; Y. Lin,; J. J. Pei,; Z. Li, et al. Engineering unsymmetrically coordinated Cu-S1N3 single atom sites with enhanced oxygen reduction activity. Nat. Commun. 2020, 11, 3049.
Crossref Google Scholar
[24]
J. Zhang,; Y. M. Sun,; J. W. Zhu,; Z. K. Kou,; P. Hu,; L. Liu,; S. Z. Li,; S. C. Mu,; Y. H. Huang, Defect and pyridinic nitrogen engineering of carbon-based metal-free nanomaterial toward oxygen reduction. Nano Energy 2018, 52, 307-314.
Crossref Google Scholar
[25]
B. T. Qiao,; A. Q. Wang,; X. F. Yang,; L. F. Allard,; Z. Jiang,; Y. Y. Cui,; J. Y. Liu,; J. Li,; T. Zhang, Single-atom catalysis of CO oxidation using Pt1/FeOx. Nat. Chem. 2011, 3, 634-641.
Crossref Google Scholar
[26]
M. Zhou,; Y. Jiang,; G. Wang,; W. J. Wu,; W. X. Chen,; P. Yu,; Y. Q. Lin,; J. J. Mao,; L. Q. Mao, Single-atom Ni-N4 provides a robust cellular NO sensor. Nat. Commun. 2020, 11, 3188.
Crossref Google Scholar
[27]
S. B. Tian,; M. Hu,; Q. Xu,; W. B. Gong,; W. X. Chen,; J. R. Yang,; Y. Q. Zhu,; C. Chen,; J. He,; Q. Liu, et al. Single-atom Fe with Fe1N3 structure showing superior performances for both hydrogenation and transfer hydrogenation of nitrobenzene. Sci. China Mater. 2020, .
Crossref Google Scholar
[28]
J. J. Mao,; C. T. He,; J. J. Pei,; Y. Liu,; J. Li,; W. X. Chen,; D. S. He,; D. S. Wang,; Y. D. Li, Isolated Ni atoms dispersed on Ru nanosheets: High-performance electrocatalysts toward hydrogen oxidation reaction. Nano Lett. 2020, 20, 3442-3448.
Crossref Google Scholar
[29]
W. J. Ma,; J. J. Mao.; X. T. Yang,; C. Pan,; W. X. Chen,; M. Wang,; P. Yu,; L. Q. Mao,; Y. D. Li, A single-atom Fe-N4 catalytic site mimicking bifunctional antioxidative enzymes for oxidative stress cytoprotection. Chem. Commun. 2019, 55, 159-162.
Crossref Google Scholar
[30]
J. Zhang,; C. Y. Zheng,; M. L. Zhang,; Y. J. Qiu,; Q. Xu,; W. C. Cheong,; W. X. Chen,; L. R. Zheng,; L. Gu,; Z. P. Hu, et al. Controlling N-doping type in carbon to boost single-atom site Cu catalyzed transfer hydrogenation of quinoline. Nano Res. 2020, 13, 3082-3087.
Crossref Google Scholar
[31]
Q. Xu,; C. X. Guo,; S. B. Tian,; J. Zhang,; W. X. Chen,; W. C. Cheong,; L. Gu,; L. R. Zheng,; J. P. Xiao,; Q. Liu, et al. Coordination structure dominated performance of single-atomic Pt catalyst for anti-Markovnikov hydroboration of alkenes. Sci. China Mater. 2020, 63, 972-981.
Crossref Google Scholar
[32]
J. J. Mao,; C. T. He,; J. J. Pei,; W. X. Chen,; D. S. He,; Y. Q. He,; Z. B. Zhuang,; C. Chen,; Q. Peng,; D. S. Wang, et al. Accelerating water dissociation kinetics by isolating cobalt atoms into ruthenium lattice. Nat. Commun. 2018, 9, 4958.
Crossref Google Scholar
[33]
J. Yang,; Z. Y. Qiu,; C. M. Zhao,; W. C. Wei,; W. X. Chen,; Z. J. Li,; Y. T. Qu,; J. C. Dong,; J. Luo,; Z. Y. Li, et al. In situ thermal atomization to convert supported nickel nanoparticles into surface-bound nickel single-atom catalysts. Angew. Chem., Int. Ed. 2018, 57, 14095-14100.
Crossref Google Scholar
[34]
M. L. Xiao,; J. B. Zhu,; G. R. Li,; N. Li,; S. Li,; Z. P. Cano,; L. Ma,; P. X. Cui,; P. Xu,; G. P. Jiang, et al. A single-atom iridium heterogeneous catalyst in oxygen reduction reaction. Angew. Chem., Int. Ed. 2019, 58, 9640-9645.
Crossref Google Scholar
[35]
C. Z. Zhu,; S. F. Fu,; Q. R. Shi,; D. Du,; Y. H. Lin, Single-atom electrocatalysts. Angew. Chem., Int. Ed. 2017, 56, 13944-13960.
Crossref Google Scholar
[36]
J. Z. Li,; M. J. Chen,; D. A. Cullen,; S. Hwang,; M. Y. Wang,; B. Y. Li,; K. X. Liu,; S. Karakalos,; M. Lucero,; H. G. Zhang, et al. Atomically dispersed manganese catalysts for oxygen reduction in proton- exchange membrane fuel cells. Nat. Catal. 2018, 1, 935-945.
Crossref Google Scholar
[37]
X. Y. Li,; H. P. Rong,; J. T. Zhang,; D. S. Wang,; Y. D. Li, Modulating the local coordination environment of single-atom catalysts for enhanced catalytic performance. Nano Res. 2020, 13, 1842-1855.
Crossref Google Scholar
[38]
Y. T. Qu,; Z. J. Li,; W. X. Chen,; Y. Lin,; T. W. Yuan,; Z. K. Yang,; C. M. Zhao,; J. Wang,; C. Zhao,; X. Wang, et al. Direct transformation of bulk copper into copper single sites via emitting and trapping of atoms. Nat. Catal. 2018, 1, 781-786.
Crossref Google Scholar
[39]
A. Q. Wang,; J. Li,; T. Zhang, Heterogeneous single-atom catalysis. Nat. Rev. Chem. 2018, 2, 65-81.
Crossref Google Scholar
[40]
D. H. Li,; Y. Jia,; G. J. Chang,; J. Chen,; H. W. Liu,; J. C. Wang,; Y. F. Hu,; Y. Z. Xia,; D. J. Yang,; X. D. Yao, A defect-driven metal-free electrocatalyst for oxygen reduction in acidic electrolyte. Chem 2018, 4, 2345-2356.
Crossref Google Scholar
[41]
B. Hammer,; J. K. Norskov, Why gold is the noblest of all the metals. Nature 1995, 376, 238-240.
Crossref Google Scholar
Nano Research
Volume 14 Issue 4,
April 2021
Pages 998-1003
DOI: 10.1007/s12274-020-3141-x
Cite this article:
Wu W, Liu Y, Liu D, et al. Single copper sites dispersed on hierarchically porous carbon for improving oxygen reduction reaction towards zinc-air battery. Nano Research, 2021, 14(4): 998-1003. https://doi.org/10.1007/s12274-020-3141-x
Topics:
CarbonCopperDoping (additives)ElectrocatalystsElectrolytic reduction OxygenOxygen reduction reaction Porous materialsPrecious metalsZinc

803

Views

61

Crossref

N/A

Web of Science

59

Scopus

10

CSCD

Altmetrics
Received: 21 August 2020
Revised: 22 September 2020
Accepted: 23 September 2020
Published: 23 October 2020
© Tsinghua University Press and Springer-Verlag GmbH Germany, part of Springer Nature
Return