Pyridinic N doped graphene: synthesis, electronic structure, and electrocatalytic property

Luo, Zhiqiang; Lim, Su Hui; Tian, Zhongxian; Shang, Jingzhi; Lai, Linfei; Macdonald, B. F.; Fu, Chao; Shen, Zexiang; Yu, Ting; Lin, Jianyi

doi:10.1039/c1jm10845j

Cited by 934 publications

(688 citation statements)

References 40 publications

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“…53 The average n values of 2.12 and 3.84 for NGPC-700-5 with predominant pyridinic-N and NGPC-1000-10 with the highest amount of graphitic-N, respectively, well coincides with those reports where graphitic-N plays a more important role in the enhanced ORR activity in alkaline solution than pyridinic-N.…”

Section: Electrocatalytic Performance Of Ngpcs For Orrsupporting

confidence: 78%

Highly graphitized nitrogen-doped porous carbon nanopolyhedra derived from ZIF-8 nanocrystals as efficient electrocatalysts for oxygen reduction reactions

et al. 2014

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Nitrogen-doped graphitic porous carbons (NGPCs) have been synthesized by using a zeolite-type nanoscale metal-organic framework (NMOF) as a self-sacrificing template, which simultaneously acts as both the carbon and nitrogen sources in a facile carbonization process. The NGPCs not only retain the nanopolyhedral morphology of the parent NMOF, but also possess rich nitrogen, high surface area and hierarchical porosity with well-conducting networks. The promising potential of NGPCs as metal-free electrocatalysts for oxygen reduction reactions (ORR) in fuel cells is demonstrated. Compared with commercial Pt/C, the optimized NGPC-1000-10 (carbonized at 1000 C for 10 h) catalyst exhibits comparable electrocatalytic activity via an efficient four-electron-dominant ORR process coupled with superior methanol tolerance as well as cycling stability in alkaline media. Furthermore, the controlled experiments reveal that the optimum activity of NGPC-1000-10 can be attributed to the synergetic contributions of the abundant active sites with high graphitic-N portion, high surface area and porosity, and the high degree of graphitization. Our findings suggest that solely MOF-derived heteroatom-doped carbon materials can be a promising alternative for Pt-based catalysts in fuel cells.

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Section: Electrocatalytic Performance Of Ngpcs For Orrsupporting

confidence: 78%

Highly graphitized nitrogen-doped porous carbon nanopolyhedra derived from ZIF-8 nanocrystals as efficient electrocatalysts for oxygen reduction reactions

et al. 2014

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“…2,[20][21][22][23][24] The well-known carbon alloys prepared by pyrolyzing nitrogen containing aromatic polymers exhibited ORR potential close to that of a platinum electrode. 5 A positive ORR shift was also observed at the carbon felt by electrochemically introducing nitrogen containing groups onto the carbon felt surfaces.…”

Section: Electrocatalytic Reduction Of Oxygenmentioning

confidence: 99%

Structure and Electroanalytical Application of Nitrogen-doped Carbon Thin Film Electrode with Lower Nitrogen Concentration

et al. 2015

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We studied a nitrogen-doped nanocarbon film electrode with a nitrogen concentration of lower than 10.9 at% formed by the unbalanced magnetron (UBM) sputtering method. The sp 3 content in the nitrogen-doped UBM sputtering nanocarbon film (N-UBM film) slightly increases with increasing nitrogen concentration. The nitrogen-containing graphite-like bonding decreases and pyridine-like bonding increases with increasing nitrogen concentration. The N-UBM film has a very smooth surface with an average roughness of 0.1 to 0.3 nm, which is almost independent of nitrogen concentration. The N-UBM film electrode shows a wider potential window (4.1 V) than a pure-UBM film electrode (3.9 V) due to its slight increase in the sp 3 content. The electrocatalytic activity increased with increasing nitrogen concentration, suggesting that the electroactivity is maximum when the nitrogen concentration is around 10.9 at%, which is confirmed by the peak separation of Fe(CN)6 4-. The hydrogen peroxide (H2O2) reduction potentials at the N-UBM film electrode shifted about 0.1 V, and the peak current of H2O2 increased about 4 times.

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“…24 So far, few methods for generating N-doped graphene are described. Among these are thermal CVD of methane and ammonia gas, 25 CVD of molecular precursors like pyridine 26 or acetonitrile 27 on a Cu substrate or exposure of graphene to a nitrogen 28 or ammonia 29 containing plasma discharge.…”

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Chemical Vapor Deposition of N-Doped Graphene and Carbon Films: The Role of Precursors and Gas Phase

et al. 2014

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Thermally induced chemical vapor deposition (CVD) was used to study the formation of nitrogen doped graphene and carbon films on copper from aliphatic nitrogen containingprecursors consisting of C 1 -and C 2 -units and (hetero) The deposition of carbon films from the gas phase leads to materials of widely different structure and composition. The films can be i) crystalline, e.g. like graphene, graphite or diamond and consist ideally of a single type of either sp 2 or sp 3 -hybridized carbon atoms, ii) can contain domains of any of these phases in more or less ordered arrangements, or iii) can even incorporate a considerable amount of hydrogen or other heteroatoms. Within this manifold of carbon films, graphene, a two-dimensional allotrope of carbon has recently attained high interest due to its electronic and optical properties and chemical inertness. [1][2][3] Graphene with controllable electronic properties is expected to be a promising material for the development of new electronic devices, 4,5 such as e.g. field-effect transistors 6 or electrochemical sensors, 7,8 as well as for applications in energy storage 9,10 and conversion systems like super capacitors, 11 lithium batteries, 12 and fuel cells. 13 Furthermore, transparent conducting graphene films are considered for organic electronic devices such as OLED's and organic solar cells. 14 Graphene itself does not reveal a band gap and therefore has no intrinsic semiconducting properties. Thus, doping of graphene with heteroelements like boron (B) or nitrogen (N), which fit into the carbon lattice, is an important issue. Theoretical and experimental studies indicate that B-or N-doped graphenes reveal p-or n-type semiconductor characteristics [15][16][17] accompanied by a band gap opening [18][19][20] and thus doped 1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60 graphene and structurally related graphene nanoribbons are considered as promising materials with tunable electronic properties. 21,22 N-Doped graphene, and particularly B-doped graphene are still scarcely investigated experimentally as compared to graphene 23 and graphene oxide. 24 So far, few methods for generating N-doped graphene are described. Among these are thermal CVD of methane and ammonia gas, 25 CVD of molecular precursors like pyridine 26 or acetonitrile 27 on a Cu substrate or exposure of graphene to a nitrogen 28 or ammonia 29 containing plasma discharge.In these reactions, the presence of nitrogen was identified by XPS, whereas the mechanism for nitrogen incorporation at specific positions of the graphene lattice is still not understood. 15,16,30 Recently, the formation mechanism of graphene from molecular precursors has been investigated. From the decay it was reasoned that dicarbon (C 2 -) species, formed as reaction intermediates, can contribute significantly to the built-up of graphene. 31 Sin...

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Pyridinic N doped graphene: synthesis, electronic structure, and electrocatalytic property

Cited by 934 publications

References 40 publications

Highly graphitized nitrogen-doped porous carbon nanopolyhedra derived from ZIF-8 nanocrystals as efficient electrocatalysts for oxygen reduction reactions

Highly graphitized nitrogen-doped porous carbon nanopolyhedra derived from ZIF-8 nanocrystals as efficient electrocatalysts for oxygen reduction reactions

Structure and Electroanalytical Application of Nitrogen-doped Carbon Thin Film Electrode with Lower Nitrogen Concentration

Chemical Vapor Deposition of N-Doped Graphene and Carbon Films: The Role of Precursors and Gas Phase

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