Rational design of common transition metal-nitrogen-carbon catalysts for oxygen reduction reaction in fuel cells

Zheng, Yongping; Yang, Dae Soo; Kweun, Joshua Minwoo; Li, Chenzhe; Tan, Kui; Kong, Fantai; Liang, Chaoping; Chabal, Yves J.; Kim, Yoon Young; Cho, Maenghyo; Yu, Jong-Sung; Cho, Kyeongjae

doi:10.1016/j.nanoen.2016.10.037

Cited by 119 publications

(85 citation statements)

References 40 publications

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“…This Fe content is similar to other NPMCs that have been reported in literature. [11,[28][29][30] The DTG shows a peak around 450°C with a small shoulder indicating the combustion of the carbon and tpy, respectively. Through the various stages of modification, the combustion temperature of the material begins to shift to lower temperatures when compared to the unmodified carbon support.…”

Section: Physical Characterizationmentioning

confidence: 99%

“…NPMCs are typically prepared from a microporous carbon support, nitrogen precursor (nitrogen source), and a nonprecious metal such as Fe or Co. [5,6] The development of NPMCs is continually advancing, however, the exact nature of the active site(s) remain ambiguous. Furthermore, many reported catalysts were prepared via methods that have very limited control over the final active site geometry, yielding catalysts with randomly distributed nitrogen-enriched domains with unknown/mixed geometry and as a result diverse activity in the ORR.…”

Section: Introductionmentioning

confidence: 99%

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Fe−N₃/C Active Catalytic Sites for the Oxygen Reduction Reaction Prepared with Molecular‐Level Geometry Control through the Covalent Immobilization of an Iron−Terpyridine Motif onto Carbon

et al. 2019

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A model for a non-precious metal catalyst for the oxygen reduction reaction (ORR) in aqueous media has been prepared by functionalizing a commercial Vulcan XC-72 carbon support with a terpyridine-based nitrogenous ligand. The terpyridine ligand geometry allows the formation of active catalytic sites by selectively embedding a N 3 /C structural motif into the carbon support confirmed by using thermogravimetric analysis (TGA) and X-ray photoelectron spectroscopy (XPS) measurements. Room-temperature metal-ligand coordination results in the desired FeÀ N 3 /C moieties on the surface. This model system was used to demonstrate the catalytic activity of the surfaces containing mainly FeÀ N 3 sites for the ORR in acidic and basic media. Importantly, we demonstrate that the system could be prepared under mild reaction conditions, does not require hightemperature treatments, and shows catalytic activity for the ORR. Interestingly, when the system was pyrolyzed in an N 2 atmosphere at 700°C the resulting activity declined. The nonheat-treated FeÀ N 3 /C surface demonstrates comparable activity in acidic electrolyte medium when compared to most literature catalysts that are typically heat treated to produce four nitrogen atoms coordinated to one iron center (FeÀ N 2 + 2 /C). Interestingly, despite the fact that many systems reported so far in the literature exhibit enhanced activity after heat treatment, our system showed an increase in activity when the material was not pyrolyzed.

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Section: Physical Characterizationmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Fe−N₃/C Active Catalytic Sites for the Oxygen Reduction Reaction Prepared with Molecular‐Level Geometry Control through the Covalent Immobilization of an Iron−Terpyridine Motif onto Carbon

et al. 2019

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“…[11] Among the different M-N-C catalysts, Fe-N-Cc atalysts have been studied extensively because of their excellent catalytic activity. [12] Both theoreticalc alculations [13] and experiments [14] have revealed that nitrogen incorporation and Fe-coordinated carbon speciesa re responsible for great improvements in the ORR activity.N evertheless, to date, most Fe-N-C catalysts still suffer from unsatisfactory stability or durability in harsh electrolyte solutionso wing to the instability of iron. [15] More importantly, complicated fabrication processes and expensive chemical reagents also restrict scalablep roduction.…”

Section: Introductionmentioning

confidence: 99%

Preparation of Iron‐ and Nitrogen‐Codoped Carbon Nanotubes from Waste Plastics Pyrolysis for the Oxygen Reduction Reaction

et al. 2020

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A novel method for the preparation of iron‐ and nitrogen‐codoped carbon nanotubes (Fe‐N‐CNTs) is proposed, based on the catalytic pyrolysis of waste plastics. First, carbon nanotubes are produced from pyrolysis of plastic waste over Fe‐Al2O3; then, Fe‐CNTs and melamine are heated together in an inert atmosphere. Different co‐pyrolysis temperatures are tested to optimize the electrocatalyst production. A high doping temperature improves the degree of graphite formation and promotes the conversion of nitrogen into a more stable form. Compared with commercial Pt/C, the electrocatalyst obtained from pyrolysis at 850 °C shows remarkable properties, with an onset potential of 0.943 V versus RHE and a half‐wave potential of 0.811 V versus RHE, and even better stability and anti‐poisoning properties. In addition, zinc–air battery tests are performed, and the optimized catalyst exhibits a high maximum power density.

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“…in M-N-C electrocatalysts. Additionally, several studies show a synergistic effect between Fe and Co, enhancing the activity for the ORR [14,[45][46][47]. This fact can be observed in Figure 4A, which shows higher activity and higher limiting current for FeCo-N-C when compared to pure Fe-N-C or Co-N-C. Additionally, as noted in Figure 4A, the obtained ORR activity for FeCo-N-C is close to that of Pt/C, which is an important advance for the development of cathodes for fuel cells that operate with alkaline electrolytes.…”

Section: Investigation Of the Electrocatalytic Activity For The Orrmentioning

confidence: 99%

Investigation of Earth-Abundant Oxygen Reduction Electrocatalysts for the Cathode of Passive Air-Breathing Direct Formate Fuel Cells

2018

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Abstract:The development of direct formate fuel cells encounters important obstacles related to the sluggish oxygen reduction reaction (ORR) and low tolerance to formate ions in Pt-based cathodes. In this study, electrocatalysts formed by earth-abundant elements were synthesized, and their activity and selectivity for the ORR were tested in alkaline electrolyte. The results showed that carbon-encapsulated iron-cobalt alloy nanoparticles and carbon-supported metal nitrides, characterized by transmission electron microscopy (TEM) and X-ray diffraction (XRD), do not present significant activity for the ORR, showing the same half-wave potential of Vulcan carbon. Contrarily, nitrogen-doped carbon, synthesized using imidazole as the nitrogen source, showed an increase in the half-wave potential, evidencing an influential role of nitrogen in the ORR electrocatalysis. The synthesis with the combination of Vulcan, imidazole, and iron or cobalt precursors resulted in the formation of nitrogen-coordinated iron (or cobalt) moieties, inserted in a carbon matrix, as revealed by X-ray absorption spectroscopy (XAS). Steady-state polarization curves for the ORR evidenced a synergistic effect between Fe and Co when these two metals were included in the synthesis (FeCo-N-C material), showing higher activity and higher limiting current density than the materials prepared only with Fe or Co. The FeCo-N-C material presented not only the highest activity for the ORR (approaching that of the state-of-the-art Pt/C) but also high tolerance to the presence of formate ions in the electrolyte. In addition, measurements with FeCo-N-C in the cathode of an passive air-breathing direct formate fuel cells, (natural diffusion of formate), showed peak power densities of 15.5 and 10.5 mW cm −2 using hydroxide and carbonate-based electrolytes, respectively, and high stability over 120 h of operation.

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Rational design of common transition metal-nitrogen-carbon catalysts for oxygen reduction reaction in fuel cells

Cited by 119 publications

References 40 publications

Fe−N₃/C Active Catalytic Sites for the Oxygen Reduction Reaction Prepared with Molecular‐Level Geometry Control through the Covalent Immobilization of an Iron−Terpyridine Motif onto Carbon

Fe−N₃/C Active Catalytic Sites for the Oxygen Reduction Reaction Prepared with Molecular‐Level Geometry Control through the Covalent Immobilization of an Iron−Terpyridine Motif onto Carbon

Preparation of Iron‐ and Nitrogen‐Codoped Carbon Nanotubes from Waste Plastics Pyrolysis for the Oxygen Reduction Reaction

Investigation of Earth-Abundant Oxygen Reduction Electrocatalysts for the Cathode of Passive Air-Breathing Direct Formate Fuel Cells

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Rational design of common transition metal-nitrogen-carbon catalysts for oxygen reduction reaction in fuel cells

Cited by 119 publications

References 40 publications

Fe−N3/C Active Catalytic Sites for the Oxygen Reduction Reaction Prepared with Molecular‐Level Geometry Control through the Covalent Immobilization of an Iron−Terpyridine Motif onto Carbon

Fe−N3/C Active Catalytic Sites for the Oxygen Reduction Reaction Prepared with Molecular‐Level Geometry Control through the Covalent Immobilization of an Iron−Terpyridine Motif onto Carbon

Preparation of Iron‐ and Nitrogen‐Codoped Carbon Nanotubes from Waste Plastics Pyrolysis for the Oxygen Reduction Reaction

Investigation of Earth-Abundant Oxygen Reduction Electrocatalysts for the Cathode of Passive Air-Breathing Direct Formate Fuel Cells

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Fe−N₃/C Active Catalytic Sites for the Oxygen Reduction Reaction Prepared with Molecular‐Level Geometry Control through the Covalent Immobilization of an Iron−Terpyridine Motif onto Carbon

Fe−N₃/C Active Catalytic Sites for the Oxygen Reduction Reaction Prepared with Molecular‐Level Geometry Control through the Covalent Immobilization of an Iron−Terpyridine Motif onto Carbon