Metal-free, carbon-based catalysts for oxygen reduction reactions

doi:10.1007/s11705-015-1524-4

Frontiers of Chemical Science and Engineering

2015, Vol. 9

Issue (3): 280-294 https://doi.org/10.1007/s11705-015-1524-4

本期目录

Metal-free, carbon-based catalysts for oxygen reduction reactions

Zhiyi Wu¹,Zafar Iqbal²,Xianqin Wang^3,^*(

)

1. Department of Materials Science and Engineering, New Jersey Institute of Technology, Newark, NJ 07102, USA
2. Department of Chemistry and Environmental Science, New Jersey Institute of Technology, Newark, NJ 07102, USA
3. Department of Chemical, Biological and Pharmaceutical Engineering, New Jersey Institute of Technology, Newark, NJ 07102, USA

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Abstract：

Developing metal-free, carbon-based catalysts to replace platinum-based catalysts for oxygen reduction reactions (ORRs) is an emerging area of research. In recent years, different carbon structures including carbon doped with IIIA-VIIA heteroatoms (C−M site-based, where M represents the doped heteroatom) and polynitrogen (PN) compounds encapsulated in carbon nanotubes (CNTs) (N−N site-based) have been synthesized. Compared to metallic catalysts, these materials are highly active, stable, inexpensive, and environmentally friendly. This review discusses the development of these materials, their ORR performances and the mechanisms for how the incorporation of heteroatoms enhances the ORR activity. Strategies for tailoring the structures of the carbon substrates to improve ORR performance are also discussed. Future studies in this area will need to include optimizing synthetic strategies to control the type, amount and distribution of the incorporated heteroatoms, as well as better understanding the ORR mechanisms in these catalysts.

Key words： oxygen reduction reaction electrocatalysis metal-free carbon-based polynitrogen

收稿日期: 2015-04-16 出版日期: 2015-09-30

Corresponding Author(s): Xianqin Wang

引用本文:

. [J]. Frontiers of Chemical Science and Engineering, 2015, 9(3): 280-294.
Zhiyi Wu,Zafar Iqbal,Xianqin Wang. Metal-free, carbon-based catalysts for oxygen reduction reactions. Front. Chem. Sci. Eng., 2015, 9(3): 280-294.

链接本文:

https://academic.hep.com.cn/fcse/CN/10.1007/s11705-015-1524-4
https://academic.hep.com.cn/fcse/CN/Y2015/V9/I3/280

Fig.1

Material	Synthesis method/precursors	Nitrogen content/at%	Onset potential relative to Pt/C^a)	Current density vs. Pt/C	Ref.
N-graphene	CVD/ NH₃, CH₄, H₂	4.0	−0.2 V in 0.1 mol/L KOH	Higher	[25]
N-graphene	Solution processing/4-aminobenzoic acid, graphite	1.7	−0.1 V in 0.1 mol/L KOH	Higher	[26]
N-carbon nanocages	Thermal annealing/pyridine	4.5?10	0.1 V in 0.1 mol/L KOH	Higher	[27]
N-CNT cups	CVD/ MeCN, EtOH, ferrocene	2?7	−0.15 V in 0.1 mol/L KOH	Lower	[28]
N-CNT fiber	CVD/C₂H₄(NH₂)₂	4.7?5.8	−0.1 V in 0.1 mol/L KOH	Higher	[29]
N-mesoporous carbon	Thermal annealing/1-ethyl-3-methylimidazolium dicyanamide, purine or pyrimidine	12	−0.05 V in 0.1 mol/L KOH	Higher	[30]
N-mesoporous carbon	Thermal annealing/NH₃, mesoporous carbon	4?6	−0.15 V in 0.05 mol/L H₂SO₄	Lower	[31]
N-graphitic arrays	Pyrolysis/PDI	2.7?3.5	−0.02 V in 0.1 mol/L KO	Higher	[32]
N-graphene	Solvothermal/Li₃N, cyanuric chloride, CCl₄	10.5?16.4	−0.1 V in 1.0 mol/L NaOH	Higher	[33]
N-carbon nanocapsules	Pyrolysis/Gd (III) diethylenetriaminepentaacetate	3.2?7.1	−0.1 V in 0.1 mol/L KOH	Higher	[34]
N-graphene	Pyrolysis/glucose, melamine or urea	9.2?33.7	−0.05 V in 0.1 mol/L KOH	Lower	[35]
N-graphene	Ball milling/graphite, N₂	14.8	−0.15 V in 0.1 mol/L KOH	Higher	[36]
N-graphene	Pyrolysis/graphene oxide, melamine or urea or DCDA	3?5	−0.1 V in 0.1 mol/L KOH	Higher	[37]
N-graphene	Thermal annealing/graphene oxide, polydopamine	2.8?3.8	−0.07 V in 0.1 mol/L KOH	Lower	[38]
N-hollow mesoporous carbon spheres	Thermal annealing/glycine	3.0?3.8	−0.05 V in 0.1 mol/L KOH	Higher	[39]
N-mesoporous carbon	Thermal annealing/mesoporous carbon, honey	0.31?1.13	−0.1 V in 0.1 mol/L KOH	Lower	[40]
N-carbon nanosheet /graphene	Thermal annealing/graphite oxide, polyaniline	5.74	+0.15 V in 0.05 mol/L phosphate buffer solution	Higher	[41]
N-graphene	CVD/H₂, C₂H₄, NH₃	up to 16	−0.2 V in 0.1 mol/L KOH	Lower	[42]
N-CNT	Thermal annealing/HNO₃oxidized CNT, NH₃	2.9?6	+0.06 V in 0.1 mol/L KOH	Higher	[43]
N-carbon spheres	Spray pyrolysis/xylene, ethylenediamine	2.1?6.2	0 V in 0.1 mol/L KOH	Higher	[44]
N-graphene	Thermal annealing/graphite oxide, melamine	6.6?10.1	−0.1 V (vs. bulk Pt electrode) in 0.1 mol/L KOH	Higher (vs. bulk Pt electrode)	[45]
N-graphene	Pyrolysis/GO, Cu(NH₃)₄²⁺	2.45?2.85	−0.1 V in 0.1 mol/L KOH	Lower	[46]
N-rGO-CNT	Solution processing/thermal annealing/CNT, GO, melamine	5.02	−0.1 V in 0.1 mol/L KOH	Lower	[47]
N-carbon	Thermal annealing/dopamine, FeCl₃	0.97?2.43	−0.1 V in 0.1 mol/L KOH	Lower	[48]
N-activated carbon	Thermal annealing/cyanamide, activated carbon	5.56?8.65	−0.12 V in 0.1 mol/L KOH	Higher	[49]
N-carbon sheets	Pyrolysis/gelatin, ketjenblack	1.19?1.79	~0 V in 0.1 mol/L KOH	Higher	[50]
N-hollow mesoporous carbon spheres	Thermal annealing/glycine	3.81	−0.06 V in 0.1 mol/L KOH	Higher	[51]
N-graphene/CNT	Pyrolysis/GO, MWCNT, urea	4?6	~0 V in 0.1 mol/L KOH	Higher	[52]
N-amorphous carbon	Magnetron sputtering/carbon,N₂,CH₄	3.58?14.95	−0.03 V in 0.1 mol/L KOH	Lower	[53]

Tab.1

Fig.2

Fig.3

Fig.4

Fig.5

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