Exploring the active sites of nitrogen-doped graphene as catalysts for the oxygen reduction reaction

Ouyang, Wenpeng; Zeng, Dongrong; Yu, Xiang; Xie, Fangyan; Zhang, Weihong; Chen, Jian; Yan, Jing; Xie, Fangjing; Wang, Lei; Meng, Hui; Yuan, Dingsheng

doi:10.1016/j.ijhydene.2014.01.045

Cited by 102 publications

(47 citation statements)

References 45 publications

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“…47,48 Some experimental results support the modeling conclusion. 25,49 In many studies, the graphitic-N in the basal planes and in the valley sites are not distinguishable and are classified into graphite-N which plays an important role for the ORR activity. 50 51-53 The relative electro-negativity of graphitic-N atoms reduces the electron density on the adjacent C nuclei, which helps electrons transfer from the adjacent C to N atoms, and N back donates electrons to adjacent carbon p z orbitals.…”

Section: Resultsmentioning

confidence: 99%

Carbon Nitrogen Nanotubes as Efficient Bifunctional Electrocatalysts for Oxygen Reduction and Evolution Reactions

Yadav

Raji

et al. 2015

ACS Appl. Mater. Interfaces

118

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Oxygen reduction and evolution reactions are essential for broad range of renewable energy technologies such as fuel cells, metal-air batteries and hydrogen production through water splitting, therefore, tremendous effort has been taken to develop excellent catalysts for these reactions. However, the development of cost-effective and efficient bifunctional catalysts for both reactions still remained a grand challenge. Herein, we report the electrocatalytic investigations of bamboo-shaped carbon nitrogen nanotubes (CNNTs) having different diameter distribution synthesized by liquid chemical vapor deposition technique using different nitrogen containing precursors. These CNNTs are found to be efficient bifunctional electrocatalyst for oxygen reduction and evolution reactions. The electrocatalytic activity strongly depends on the nanotube diameter as well as nitrogen functionality type. The higher diameter CNNTs are more favorable for these reactions. The increase in nanotube diameter itself enhances the catalytic activity by lowering the oxygen adsorption energy, better conductivity, and further facilitates the reaction by increasing the percentage of catalytically active nitrogen moieties in CNNTs.

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Section: Resultsmentioning

confidence: 99%

Carbon Nitrogen Nanotubes as Efficient Bifunctional Electrocatalysts for Oxygen Reduction and Evolution Reactions

Yadav

Raji

et al. 2015

ACS Appl. Mater. Interfaces

118

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“…15, 35 The deconvolution of N1s XPS peak reveals three different N configurations at 398.45, 400.06, and 401.20 eV, assigned to the pyridinic-N (N1), pyrrolic-N (N2), graphitic-Ncenter (N3), respectively(Figure 2a and c) 10,15. The graphitic-Nvalley in the valley sites (N4) with binding energy > 402 eV is not found in our NGs 10,11. The total surface N content as calculated from N/(N+C) atomic ratio is higher at lower doping temperature, e.g.…”

mentioning

confidence: 80%

“…[3][4][5][6][7] The N incorporates into the carbon network with bonding configurations of N atom in sixmember ring (pyridinic-N), five-member ring (pyrrolic-N), graphene basal plane (graphitic/quaternary-Ncenter), graphene zigzag edge or valley sites (graphitic-Nvalley) and bonding to O atoms (oxidized nitrogen species). [8][9][10][11] However, the role of different N functional groups in the electrocatalysis of ORR is still under debate in results from theoretical calculation and experimental measurement since the first exploration of nitrogen doped carbon nanotubes (N-CNTs) as active ORR catalysts. 3,4,10 Most of the previous work did not distinguish between graphitic-Ncenter and graphitic-Nvalley and just proclaimed the graphitic N was of paramount importance for the ORR activity.…”

Section: Introductionmentioning

confidence: 99%

Nitrogen-Doped Graphene with Pyridinic Dominance as a Highly Active and Stable Electrocatalyst for Oxygen Reduction

Yadav

et al. 2015

ACS Appl. Mater. Interfaces

250

147

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The nitrogen-doped graphene (NG) with dominance of the pyridinic-N configuration is synthesized via a straightforward process including chemical vapor deposition (CVD) growth of graphene and postdoping with a solid nitrogen precursor of graphitic C3N4 at elevated temperature. The NG fabricated from CVD-grown graphene contains a high N content up to 6.5 at. % when postdoped at 800 °C but maintains high crystalline quality of graphene. The obtained NG exhibits high activity, long-standing stability, and outstanding crossover resistance for electrocatalysis of oxygen reduction reaction (ORR) in alkaline medium. The NG treated at 800 °C shows the best ORR performance. Further study of the dependence of ORR activity on different N functional groups in these metal-free NG electrodes provides deeper insights into the origin of ORR activity. Our results reveal that the pyridinic-N tends to be the most active N functional group to facilitate ORR at low overpotential via a four-electron pathway.

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“…Usually the following nitrogen functionalities can be identified: pyridinic-N, pyrrolic-N, graphitic-N and valley-N. Pyridinic-N and/or graphitic-N are believed to be active sites in ORR [12]. There is still dispute on whether the total nitrogen content is directly related with the activity of the oxygen reduction reaction [13,14].…”

Section: Introductionmentioning

confidence: 99%

Exploring the active sites of nitrogen-doped graphene as catalysts for the oxygen reduction reaction

Cited by 102 publications

References 45 publications

Carbon Nitrogen Nanotubes as Efficient Bifunctional Electrocatalysts for Oxygen Reduction and Evolution Reactions

Carbon Nitrogen Nanotubes as Efficient Bifunctional Electrocatalysts for Oxygen Reduction and Evolution Reactions

Nitrogen-Doped Graphene with Pyridinic Dominance as a Highly Active and Stable Electrocatalyst for Oxygen Reduction

Nitrogen doped graphitic carbon ribbons from cellulose as non noble metal catalyst for oxygen reduction reaction

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