Oxygen reduction reaction mechanism on nitrogen-doped graphene: A density functional theory study

Yu, Liang; Pan, Xiulian; Cao, Xiaoming; Hu, P.; Bao, Xinhe

doi:10.1016/j.jcat.2011.06.015

Cited by 560 publications

(408 citation statements)

References 57 publications

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“…For this purpose, we utilized the constrained optimization method [47][48][49][50]. In this technique, the Z variable of the transferring atomic nucleus is constrained in defined steps, between values corresponding to the fully optimized initial and final states.…”

Section: Resultsmentioning

confidence: 99%

Atomistic Mechanism of Pt Extraction at Oxidized Surfaces: Insights from DFT

Eslamibidgoli

Eikerling

2016

Electrocatalysis

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In this article, we propose a novel mechanism for the atomic-level processes that lead to oxide formation and eventually Pt dissolution at an oxidized Pt(111) surface. The mechanism involves a Pt extraction step followed by the substitution of chemisorbed oxygen to the subsurface. The energy diagrams of these processes have been generated using density functional theory and were analyzed to determine the critical coverages of chemisorbed oxygen for the Pt extraction and O ads substitution steps. The Pt extraction process depends on two essential conditions: (1) the local coordination of a Pt surface atom by three chemisorbed oxygen atoms at nearestneighboring fcc adsorption sites; (2) the interaction of the buckled Pt atom with surface water molecules. Results are discussed in terms of surface charging effects caused by oxygen coverage, surface strain effects, as well the contribution from electronic interaction effects. The utility of the proposed mechanism for the understanding of Pt stability at bimetallic surfaces will be demonstrated by evaluating the energy diagram of a Cu ML /Pt(111) near-surface alloy.

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Section: Resultsmentioning

confidence: 99%

Atomistic Mechanism of Pt Extraction at Oxidized Surfaces: Insights from DFT

Eslamibidgoli

Eikerling

2016

Electrocatalysis

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“…Whether the reaction takes a dissociative or an associative pathway mainly depends on the initial O 2 dissociating energy barrier on a provided surface [42]. Previous first-principle calculations have shown that the adsorbed oxygen species including OOH*, OH* and HOOH* might be involved during the ORR process [43].…”

Section: The General Orr Mechanismmentioning

confidence: 99%

Oxygen Reduction Reaction Catalyzed by Noble Metal Clusters

Tang

Wang

2018

Catalysts

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Highly-efficient catalysts for the oxygen reduction reaction (ORR) have been extensively investigated for the development of proton exchange membrane fuel cells (PEMFCs). The state-ofthe-art Pt/C catalysts suffer from high price, limited accessibility of Pt, sluggish reaction kinetics, as well as undesirable long-term durability. Engineering ultra-small noble metal clusters with high surface-to-volume ratios and robust stabilities for ORR represents a new avenue. After a simple introduction regarding the significance of ORR and the recent development of noble metal clusters, the general ORR mechanism in both acidic and basic media is firstly discussed. Subsequently, we will summarize the recent efforts employing Pt, Au, Ag, Pd and Ru clusters, as well as the alloyed bi-metallic clusters for acquiring highly efficient catalysts to enhance both the activity and stability of ORR. Molecular noble metal clusters with definitive composition to reveal the relevant ORR mechanism will be particularly highlighted. Finally, the current challenges, the future outlook, as well as the perspectives in this booming field will be proposed, featuring the great opportunities and potentials to engineering noble metal clusters as highly-efficient and durable cathodic catalysts for fuel cell applications.

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“…The calculated data indicate that the catalytic activity for oxygen reduction of Au n clusters could be improved by supporting them on N-graphene through increasing the interaction between the adsorbate and adsorbent. Actually, N-graphene itself has a good oxygen reduction activity both in acid and base solution [44,45]. Therefore, when Au clusters are supported on graphene, there may be a synergistic effect between them.…”

Section: Pure Au N Clusters On N-graphenementioning

confidence: 99%

The Interactions of Oxygen with Small Gold Clusters on Nitrogen-Doped Graphene

Chen

Sun

et al. 2013

Molecules

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By means of density functional theory, the adsorption properties of O 2 molecule on both isolated and N-graphene supported gold clusters have been studied. The N-graphene is modeled by a C 65 NH 22 cluster of finite size. The results indicate that the catalytic activity and the O 2 adsorption energies of odd-numbered Au clusters are larger than those of adjacent even-numbered ones. The O 2 molecule is in favor of bonding to the bridge sites of odd-numbered Au clusters, whereas for odd-numbered ones, the end-on adsorption mode is favored. The perpendicular adsorption orientation on N-graphene is preferred than the parallel one for Au 2 , Au 3 and Au 4 clusters, while for Au 5 , Au 6 and Au 7 , the parallel ones are favored. When O 2 is adsorbed on N-graphene supported Au clusters, the adsorption energies are largely increased compared with those on gas-phase ones. The increased adsorption energies would significantly facilitate the electron transfer from Au d-orbital to π* orbital of O 2 , which would further weakening the O-O bond and therefore enhancing the catalytic activity. The carbon atoms on N-graphene could anchor the clusters, which could make them more difficult to structural distortion, therefore enhance their stability.

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Oxygen reduction reaction mechanism on nitrogen-doped graphene: A density functional theory study

Cited by 560 publications

References 57 publications

Atomistic Mechanism of Pt Extraction at Oxidized Surfaces: Insights from DFT

Atomistic Mechanism of Pt Extraction at Oxidized Surfaces: Insights from DFT

Oxygen Reduction Reaction Catalyzed by Noble Metal Clusters

The Interactions of Oxygen with Small Gold Clusters on Nitrogen-Doped Graphene

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