Nitrogen-modified carbon-based catalysts for oxygen reduction reaction in polymer electrolyte membrane fuel cells

Subramanian, Nalini; Li, Xuguang; Nallathambi, Vijayadurda; Kumaraguru, Swaminatha P.; Colón-Mercado, Héctor; Wu, Gang; Lee, Jun Young; Popov, Branko N.

doi:10.1016/j.jpowsour.2008.11.087

Cited by 449 publications

(325 citation statements)

References 46 publications

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“…The behavior of I D /I G ratio as a function of nitrogen doping in the N-CNT is well documented in the literature. 7,13,43,44 In agreement with some previous reports, pyridinic nitrogen is responsible for the catalytic activity in N-CNTs in acidic medium, 2,25,27,38,45 while other authors suggest that quaternary nitrogen as the responsible for ORR. 28 In many reports is widely accepted that N-doping in carbon nanotubes is an important factor for their electrocatalytic behavior during ORR.…”

Section: Synthesized N-cnts At Different Temperatures (750-950supporting

confidence: 90%

“…5,16,18 The peak at 401.5-403.1 eV, can be attributed to the quaternary or graphitic-like nitrogen, which are the highly coordinated nitrogen atoms substituting carbon atoms on the graphene layers and bonded each to three carbon atoms. [36][37][38] The peak that appears at 404.7-405.7 eV can be attributed to nitrogen in the form of nitrogen oxides of pyridinic nitrogen exhibiting similar bonding with oxygen chemisorbed on the nitrogen atom. 2,12,14 The presence of oxygen on the samples was originated from a cleaning treatment with HNO 3 to remove impurities; carbon chemical oxidation generated therefore oxygen-containing groups on the carbon surface, as quinone groups.…”

Section: Synthesized N-cnts At Different Temperatures (750-950mentioning

confidence: 99%

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Influence of the Synthesis Parameters in Carbon Nanotubes Doped with Nitrogen for Oxygen Electroreduction

González

Valenzuela-Muñiz

Alonso-Núñez

et al. 2017

ECS J. Solid State Sci. Technol.

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Nitrogen doped carbon nanotubes (N-CNTs) were synthesized by modified chemical vapor deposition method using a novel two steps thermal technique. Pyridine was used as carbon and nitrogen source and ferrocene as catalyst for nanotubes growth. The effects of reactor temperature and carrier gas flow were investigated using scanning electron microscopy, transmission electron microscopy, Raman spectroscopy, X-ray photoelectron spectroscopy and linear scan voltammetry. Results show that the synthesis temperature and gas flow rate have influence on the physical, chemical and electrochemical properties of the nanostructures. Microscopy studies exhibit that synthesis temperature modify the length, yield and diameter of the N-CNTs. Transmission microscopy electron images show multiwalled carbon nanotubes with the typical bamboo like structures. High temperature and low flow rate generate more defects, as revealed by Raman analyses. N-CNTs synthesized at the highest temperature and flow rate show better electrocatalytic activity toward oxygen reduction reaction with promising lower onset potential and current densities up to 80% when compared to traditional Pt/C. The favorable performance is attributed to the higher nitrogen content and the type of nitrogen species, mainly pyrrolic and pyridinic incorporated in the carbon lattice. For the last decades, platinum (pure and Pt alloys) has been the best and well known electrocatalyst for the oxidation and reduction reactions in fuel cells. However, scarcity, high price and degradation of platinum as catalyst in fuel cell represent a challenge for commercial proposes.1,2 In recent years, there have been efforts to reduce the platinum loading, or even to eliminate it from the electrodes. It is therefore necessary to develop non-Pt catalytic materials available, cheap and electroactive to replace the precious metal. Carbon nanotubes doped with nitrogen (N-CNTs) have reached the point to become an alternative catalyst for oxygen reduction reaction (ORR) in fuel cells cathode. 3 There have been many studies concerning the synthesis of carbon nanotubes doped with nitrogen atoms using different carbon-nitrogen precursors using chemical vapor deposition (CVD) method and having a good electrocatalytic activity for oxygen reduction. Alexeyeva 4 synthesized N-CNTs using acetonitrile as carbon and nitrogen sources. They studied the electrocatalytic reduction of oxygen with and without doped nanotubes in 0.5M H 2 SO 4 solution where the N-CNTs show significantly more activity for ORR than the free-doping nanotubes. Wong 2 obtained N-CNTs through CVD technique using three different chemical precursors as nitrogen sources: aniline (A), diethylamine (DEA) and ethylenediamine. The analysis revealed that the N-CNTs obtained from EDA with 6.5 at. % N was more active for ORR in acidic medium than nanotubes from A and DEA with 5.9 at. % N and 4.3 at. % N, respectively. Other studies 1,[5][6][7][8] have also showed the important role of nitrogen precursors on the N-CNTs structure. Nevertheless, few...

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Section: Synthesized N-cnts At Different Temperatures (750-950supporting

confidence: 90%

Section: Synthesized N-cnts At Different Temperatures (750-950mentioning

confidence: 99%

Influence of the Synthesis Parameters in Carbon Nanotubes Doped with Nitrogen for Oxygen Electroreduction

González

Valenzuela-Muñiz

Alonso-Núñez

et al. 2017

ECS J. Solid State Sci. Technol.

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“…These readjustments are in accordance with literature data [48] by which N5 and N6 are thermally unstable with respect to NQ. This latter NQ represents a class of compounds in which substitutional nitrogen in graphene layers is theoretically advocated [49,50] as active for ORR on metal-free catalysts.…”

Section: Electrochemical Measurementsmentioning

confidence: 99%

Iron and Copper Containing Oxygen Reduction Catalysts From Templated Glucose–Histidine

et al. 2010

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Nitrogen doped carbons loaded with non‐precious transition metals are currently investigated as substitutes of Pt‐based catalysts for oxygen reduction in polymer electrolyte fuel cells (PEMFCs). This paper reports the preparation of one kind of such catalysts using glucose/histidine mixtures added with Fe and Cu salts in the presence of silica gels as hard templating agent to increase carbon surface area. The resulting carbons contain nitrogen in amounts that depend on heating temperature (T = 600 and 900 °C) on the glucose/histidine molar ratio and, more weakly, on the relative Fe/Cu amount. Surface areas are a function of reactant concentration and heating temperature, whereas pore size and pore size distribution only depend on glucose/histidine molar ratio. Cyclic voltammetry results on oxygen reduction depend on Fe/Cu ratio, the best result both in terms of incipient oxygen reduction potentials and currents being observed on samples only containing Fe, with no Cu added.

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“…[2][3][4][5][6][7][8][9]11 Meanwhile, nitrogen doped carbon nanosystems were intensively studied in the last couple of years as possible alternative to metal-based catalysts. [12][13][14][15][16][17][18][19][20][21][22][23][24][25][26][27] Light weight, low cost and high efficiency makes these materials attractive for the further practical applications.…”

mentioning

confidence: 99%

Oxygen reduction reactions on pure and nitrogen-doped graphene: a first-principles modeling

2012

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Nitrogen-modified carbon-based catalysts for oxygen reduction reaction in polymer electrolyte membrane fuel cells

Cited by 449 publications

References 46 publications

Influence of the Synthesis Parameters in Carbon Nanotubes Doped with Nitrogen for Oxygen Electroreduction

Influence of the Synthesis Parameters in Carbon Nanotubes Doped with Nitrogen for Oxygen Electroreduction

Iron and Copper Containing Oxygen Reduction Catalysts From Templated Glucose–Histidine

Oxygen reduction reactions on pure and nitrogen-doped graphene: a first-principles modeling

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