Selective nitrogen doping in graphene for oxygen reduction reactions

Yasuda, Satoshi; Yu, Li; Kim, Jeheon; Murakoshi, Kei

doi:10.1039/c3cc45641b

Cited by 180 publications

(96 citation statements)

References 18 publications

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“…Murakoshi et al reported that pyridine-like bonding is active sites of ORR by studying graphene containing 2.0 to 2.7 at% nitrogen concentrations, which is included in the concentration region we studied with our N-UBM film electrode. 7 Our current results about structural dependence of ORR potential agree well with their results. However, the ORR peak potentials were shifted negatively with increasing pyridine-like structure (or decreasing graphite-like structure) when nitrogen concentrations ranged from 8.9 to 30.4 at%.…”

Section: Electrocatalytic Reduction Of Oxygensupporting

confidence: 82%

“…5 More recently, nitrogen-doped nanocarbons including nitrogen-doped carbon nanotube (CNT) and graphene with high electrocatalytic activity for ORR have been reported. [6][7] In spite of the high electrocatalytic activity of the above nanocarbon materials, these materials are not always suitable as electrodes for electroanalysis. This is because a large surface area of these powder, flake or fiber-like materials increases the background noise level, which is inconvenient as regards improving the detection limit (or improving the S/N ratio).…”

Section: Introductionmentioning

confidence: 99%

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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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Section: Electrocatalytic Reduction Of Oxygensupporting

confidence: 82%

Section: Introductionmentioning

confidence: 99%

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

et al. 2015

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“…Pyridinic N, which has a lone electron pair in the plane of the carbon matrix, could donate the electron to the π-bond, attract electrons, and therefore be catalytically active. Some results were shown in many previous works [94][95][96].…”

Section: Ng As a Metal-free Catalyst For Orrmentioning

confidence: 78%

Nitrogen-Doped Carbon Nanotube and Graphene Materials for Oxygen Reduction Reactions

et al. 2015

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Nitrogen-doped carbon materials, including nitrogen-doped carbon nanotubes (NCNTs) and nitrogen-doped graphene (NG), have attracted increasing attention for oxygen reduction reaction (ORR) in metal-air batteries and fuel cell applications, due to their optimal properties including excellent electronic conductivity, 4e − transfer and superb mechanical properties. Here, the recent progress of NCNTs-and NG-based catalysts for ORR is reviewed. Firstly, the general preparation routes of these two N-doped carbon-allotropes are introduced briefly, and then a special emphasis is placed on the developments of both NCNTs and NG as promising metal-free catalysts and/or catalyst support materials for ORR. All these efficient ORR electrocatalysts feature a low cost, high durability and excellent performance, and are thus the key factors in accelerating the widespread commercialization of metal-air battery and fuel cell technologies. OPEN ACCESSCatalysts 2015, 5 1575

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“…In another study, Yasuda et al were selectively synthesized N-graphene with abindant pyridinic-N or graphitic-N sites using different N-containing precursors. They reported that that graphitic-N species favour a 2e -pathway, whereas pyridinic-N species induce a 4e -reduction pathway [134]. * the same acid treatment time and PANI amount as NFW-F-900 but 2h pyrolysis time.…”

Section: Orr Activity Of N-fwcntsmentioning

confidence: 99%

Nitrogen-doped graphene with enhanced oxygen reduction activity produced by pyrolysis of graphene functionalized with imidazole derivatives

Borghei

Azcune

Carrasco

et al. 2014

International Journal of Hydrogen Energy

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Direct methanol fuel cells (DMFC) are great candidates for portable power source applications. However, the sluggish reaction kinetics are key challenges in DMFC technology. The state-of-the-art electrocatalysts are Pt-based catalysts supported on carbon black. However, the high price of Pt, corrosion of carbon support and Pt degradation are the main problems.In this thesis, carbon nanomaterials, namely few-walled carbon nanotubes (FWCNTs) and graphitized nanofibers (GNFs) were used as catalyst supports in the search for stable and durable catalysts. PtRu nanocatalysts with similar particle size and composition were synthesized and deposited on FWCNTs and GNFs. The electrochemical activities for methanol oxidation were compared with that of PtRu-carbon black in acidic conditions. The half-cell electrochemical measurements revealed higher activity with PtRu-GNFs and PtRu-FWCNTs. Later, the electrocatalysts were tested in macro-and micro-DMFC. The results revealed the significant influence of the catalyst support, inomer contect, electrode structure, preparation method, as well as the fuel cell architecture on the performance of a specific electrode material. The results also highlighted the necessity of electrode composition optimization when applying new materials at the electrodes, in order to achieve the best activity and durability for a certain electrocatalyst.A special effort was also done to achieve Pt-free electrocatalysts with high activity for the oxygen reduction reaction (ORR) by introducing nitrogen heteroatoms in carbon nanomaterials, namely FWCNTs and graphite nanoplatelets (GNPs). N-FWCNTs exhibited remarkable electrocatalytic activity for ORR in alkaline media, despite their very low nitrogen content (~0.5 at.%). N-FWCNTs performed on par or better than a commercial Pt-C at the cathode of an alkaline DMFC. The N-GNPs exhibited enhanced electrocatalytic activity for ORR compared to pristine GNPs in alkaline media. The results indicated that N-doped carbon nanomaterials could be promising alternatives to their Pt counterparts to reduce fuel cell costs. However, further investigations are necessary to ascertain the real active sites in order to design more efficient and durable ORR electrocatalysts.Keywords Carbon nanomaterials, PtRu catalysts, nitrogen-doping, direct methanol fuel cell ISBN (printed) 978-952-60-6140-5 ISBN (pdf) 978-952-60-6141-2

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Selective nitrogen doping in graphene for oxygen reduction reactions

Cited by 180 publications

References 18 publications

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

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

Nitrogen-Doped Carbon Nanotube and Graphene Materials for Oxygen Reduction Reactions

Nitrogen-doped graphene with enhanced oxygen reduction activity produced by pyrolysis of graphene functionalized with imidazole derivatives

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