Unraveling the Nature of Sites Active toward Hydrogen Peroxide Reduction in Fe‐N‐C Catalysts

Choi, Chang Hyuck; Choi, Won Seok; Kasian, Olga; Mechler, Anna K.; Sougrati, Moulay Tahar; Brüller, Sebastian; Strickland, Kara; Jia, Qingying; Mukerjee, Sanjeev; Mayrhofer, Karl Johann Jakob; Jaouen, Frédéric

doi:10.1002/anie.201704356

Cited by 192 publications

(155 citation statements)

References 38 publications

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“…Metal impurities can influence the ORR even when present at very low concentrations, causing controversy on the nature of certain carbon-based catalysts [29]. Numerous reports show that the presence of transition metals, such as Fe [39,40] and Co [9,41] plays a strong role. Even concentrations in the range of hundreds or even tens of ppm can influence their electrocatalytic properties [42,43].…”

Section: A C C E P T E D Accepted Manuscriptmentioning

confidence: 99%

Carbon catalysts for electrochemical hydrogen peroxide production in acidic media

Čolić

Yang

Révay

et al. 2018

Electrochimica Acta

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Section: A C C E P T E D Accepted Manuscriptmentioning

confidence: 99%

Carbon catalysts for electrochemical hydrogen peroxide production in acidic media

Čolić

Yang

Révay

et al. 2018

Electrochimica Acta

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“…Planar M−N 4 type transition metal complexes, such as iron–porphyrins, are well known homogeneous catalysts for ORR which could be used as viable and cheaper alternatives to platinum . These catalysts are however dispersed in the homogeneous reaction mixture and therefore it could be challenging to couple them effectively to the electrode surface.…”

Section: Introductionmentioning

confidence: 99%

Exploring the Effect of Gold Support on the Oxygen Reduction Reaction Activity of Metal Porphycenes

Siahrostami

Nørskov

2018

ChemCatChem

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It has been a long‐standing goal to find alternative, cost effective catalysts for oxygen reduction reaction (ORR) in fuel cells. Molecular complexes capable of efficiently catalyzing ORR, when supported on a conducting solid surface could provide interesting hybrid materials combining the best of homogeneous and heterogeneous catalysis. We use density functional theory to study the ORR activity of molecular (unsupported) and gold supported 3d metal (II)‐porphycenes (MPc). All the 3d metal‐porphycenes adsorb strongly on the Au(111) support with negative free energy of formation ranging from 1.0–3.0 eV while solvation lowers the energy of molecular MPc by only 0.5 eV compared to the gas phase. These indicate that the 3d MPc are stable and anchored firmly to the gold surface under ORR conditions. Based on our analysis, the gold support enhances the ORR activity in some of the examined MPc systems. We find that the molecular MnPc and FePc are the best ORR electrocatalysts with theoretical overpotentials of 0.44 V and 0.36 V. This work highlights the important role of the support in preserving/increasing the activity of molecular catalyst.

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“…[1][2][3] Adv. These active moieties for catalysis reactions can be commonly exposed by increasing the specific areas of the materials or by tailoring the densities of metal-nitrogen moieties in composites.…”

Section: Metallic Porous Single Crystalsmentioning

confidence: 99%

“…[1][2][3] www.advmat.de www.advancedsciencenews.com metal nitride single crystals with high density of active metalnitrogen moieties have long-range ordering and interconnected open frameworks, which could provide long-range electronic connectivity, and thus reduce energy losses at grain boundaries and maintain high stability and activity. These active moieties for catalysis reactions can be commonly exposed by increasing the specific areas of the materials or by tailoring the densities of metal-nitrogen moieties in composites.…”

Section: Metallic Porous Single Crystalsmentioning

confidence: 99%

“…[4][5][6] These results indeed give an in-depth insight at the atomic level into structural dependence of catalytic activity of metal nitride nanoparticles by closely correlating the average structural information with catalytic performances. [1][2][3] Adv. The state-of-the-art pyrolysis technique of specific precursors is commonly used to construct metal-nitrogen moieties.…”

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confidence: 99%

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Metallic Porous Iron Nitride and Tantalum Nitride Single Crystals with Enhanced Electrocatalysis Performance

Zhang

Lin

et al. 2018

Advanced Materials

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Previous studies show that the metalnitrogen moieties with unsaturated nitrogen coordination numbers possess higher catalytic activities and the reported smallest nitrogen coordination number is confirmed to be ≈2 for Co-N 2 and Fe-N 2 moieties using extended X-ray absorption fine structure spectra analysis. [4][5][6] These results indeed give an in-depth insight at the atomic level into structural dependence of catalytic activity of metal nitride nanoparticles by closely correlating the average structural information with catalytic performances. However, the active metalnitrogen moieties confined at the surface layer of materials that host catalysis reactions still remain unclear.Building metal-nitrogen moieties with unsaturated nitrogen coordination numbers to enhance material's catalytic activity remains a fundamental challenge. The state-of-the-art pyrolysis technique of specific precursors is commonly used to construct metal-nitrogen moieties. However, the simultaneous presence of multiple metal species in most composite catalysts makes it highly complex to understand the nature of metal-nitrogen moieties. [7][8][9][10] The short length scale of nanostructured catalysts makes it extremely challenging to quantify metal-nitrogen moiety structure and distributions and to correspondingly elucidate the electronic structure features and unusual activity. The metal-nitrogen moieties are indeed a kind of active clusters at atomic level, which are strictly confined at lattice in local structures in crystalline composites. The polycrystalline or amorphous states of composites make it highly uncertain to construct resolved metal-nitrogen moieties and to accordingly expose these active centers on material's surfaces to host catalysis reactions. Another consideration should be given to the resolved structural feature and chemical composition of moieties that tailor electronic structures to facilitate catalysis functionalities.Single crystals with porosity, combining the advantages of long-range structural coherence of bulk crystals and large surface areas of porous materials, could provide opportunities to host the metal-nitrogen moieties with unsaturated nitrogen coordination on surface. The long-range structural coherence in single crystals offers the possibility to stabilize the metalnitrogen moieties in lattice of local structures on crystalline surfaces especially on the condition that the surface moieties have similar chemical compositions to bulk crystals. Porous Altering a material's catalytic properties would require identifying structural features that deliver electrochemically active surfaces. Single-crystalline porous materials, combining the advantages of long-range ordering of bulk crystals and large surface areas of porous materials, would create sufficient active surfaces by stabilizing 2D active moieties confined in lattice and may provide an alternative way to create high-energy surfaces for electrocatalysis that are kinetically trapped. Here, a radical concept of building active metalnitrogen moieties ...

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Unraveling the Nature of Sites Active toward Hydrogen Peroxide Reduction in Fe‐N‐C Catalysts

Cited by 192 publications

References 38 publications

Carbon catalysts for electrochemical hydrogen peroxide production in acidic media

Carbon catalysts for electrochemical hydrogen peroxide production in acidic media

Exploring the Effect of Gold Support on the Oxygen Reduction Reaction Activity of Metal Porphycenes

Metallic Porous Iron Nitride and Tantalum Nitride Single Crystals with Enhanced Electrocatalysis Performance

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