A DFT study of oxygen reduction reaction mechanism over O-doped graphene-supported Pt4, Pt3Fe and Pt3V alloy catalysts

Jin, Nian; Han, Jinyu; Wang, Hua; Zhu, Xinli; Ge, Qingfeng

doi:10.1016/j.ijhydene.2015.02.101

Cited by 37 publications

(19 citation statements)

References 85 publications

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“…These include monometallic nanoparticles [4][5][6][7], alloy nanoparticles [8][9][10], metal oxides nanoparticles [11][12][13][14][15], and transition metal chalcogenide nanoparticles [16] that are supported on diverse substrates including metal structures [17], metal oxides [18], or carbon-based materials such as carbon black, standard carbon fibers [19], single-or multi-walled carbon nanotubes [20], and graphene sheets [21][22][23][24]. As summarized in several recent reviews [25][26][27], these supporting materials play important roles in, for instance, preventing nanoparticle aggregation and increasing the corresponding surface areas; manipulating electronic energy of the metal nanoparticles and hence interactions with O 2 molecules via intimate electronic interactions with the supporting substrates; enhancing electronic conductivity and serving as current collectors; as well as improving structural stability of the catalysts in extreme acidic or basic environments.…”

Section: Introductionmentioning

confidence: 99%

Oxygen reduction catalyzed by nanocomposites based on graphene quantum dots-supported copper nanoparticles

Liu

Yang

Chen

2016

International Journal of Hydrogen Energy

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Nanocomposites based on graphene quantum dots (GQDs)-supported copper nanoparticles were prepared by thermal refluxing of copper salts in 1,2-propanediol at 140 °C in the presence of GQDs. Transmission electron microscopic measurements showed that the resulting Cu/GQD nanoparticles increased from 5 to 15 nm in average diameter with increasing metal loadings. Raman spectroscopic measurements showed that all nanocomposites exhibited well-defined D and G vibrational bands. X-ray photoelectron spectroscopic studies indicated the formation of Cu 2 O and CuO in the nanocomposite particles, along with various defect concentrations within the GQD graphitic skeletons. Electrochemical studies showed that the nanocomposites exhibited apparent electrocatalytic activity in oxygen reduction in alkaline media, and the sample with a Cu/C atomic ratio of 2.88% exhibited the best ORR activity among the series, within the context of onset potential, number of electron transfer and kinetic current density. The performance was further improved by deliberate hydrothermal treatments of the sample, and 160 °C was identified as the optimal temperature, which was ascribed to manipulation of the electronic interactions between copper nanoparticles and oxygen intermediates by the GQD structural defects.

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Section: Introductionmentioning

confidence: 99%

Oxygen reduction catalyzed by nanocomposites based on graphene quantum dots-supported copper nanoparticles

Liu

Yang

Chen

2016

International Journal of Hydrogen Energy

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“…It can convert the chemical energy from a fuel into electricity via a chemical reaction in the presence of oxygen or other oxidizing agents. Interestingly, Pt nanoparticles supported on the various 2D nanomaterials, such as defective graphene, [14][15][16][17][18] graphene oxide, 19 functionalized graphene, 20,21 BN sheet 22,23 etc. 1 In fact, the sluggish kinetics of ORR accounts for the major portion of the voltage drop.…”

Section: Introductionmentioning

confidence: 99%

Size-selective electrocatalytic activity of (Pt)_n/MoS₂ for oxygen reduction reaction

Bothra

Pandey

Pati

2016

Catal. Sci. Technol.

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In the present work, we have investigated the electrocatalytic activity of the oxygen reduction reaction (ORR), O 2 + 4 H + + 4 e − → 2H 2 O, for (Pt) n clusters (n = 1, 2, 3, 5, 7, 10 and 12) adsorbed on semiconducting (2H) and metallic (1T) MoS 2 monolayers using first principles density functional theory. We have considered four elementary reactions involved in ORR within a unified electrochemical thermodynamic framework and the corresponding Gibbs adsorption free energies of the key intermediates ( * OOH, * O, * OH) associated with each step have been calculated. The results indicate that the reduction of adsorbed hydroxyl ( * OH) to water, ( * OH + H + + e − → H 2 O) is the bottleneck step in the ORR process. The adsorption free energy of * OH (∆ G * OH ) is found to be the thermodynamic descriptor for the present systems. Eventually, the ORR activity has been described as a function of ∆ G * OH and that establishes a volcano plot predicting (Pt) 7 /2H-MoS 2 as the best ORR catalyst amongst (Pt) n /MoS 2 heterosystems with overpotential value of 0.33 V. Our finding propose a new promising electrocatalyst towards better activity for ORR with very less amount of Pt loading.

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“…Our previous study showed that the O-doping site is the anchoring site for the tetrahedral Pt 4 cluster [36]. The OG-supported Pt 3 M clusters (OG-Pt 3 M) were constructed by replacing one Pt atom of the supported Pt 4 cluster with M at either the interfacial or the top of tetrahedron.…”

Section: Optimized Pt 3 M Structures On O-doped Graphenementioning

confidence: 99%

“…Our previous study on the ORR process over Pt 4 , Pt 3 V, and Pt 3 Fe supported on O-doped graphene showed that V and Fe change the ORR mechanism and activity on the Pt-based catalysts differently [36]. Other studies also reported that early and late 3d transition metals could affect the adsorption of O 2 and the ORR activity in a different way [13,37].…”

Section: Introductionmentioning

confidence: 97%

Oxygen Reduction Reaction Catalyzed by Pt3M (M = 3d Transition Metals) Supported on O-doped Graphene

et al. 2020

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Pt3M (M = 3d transition metals) supported on oxygen-doped graphene as an electrocatalyst for oxygen reduction was investigated using the periodic density functional theory-based computational method. The results show that oxygen prefers to adsorb on supported Pt3M in a bridging di-oxygen configuration. Upon reduction, the O–O bond breaks spontaneously and the oxygen adatom next to the metal–graphene interface is hydrogenated, resulting in co-adsorbed O* and OH* species. Water formation was found to be the potential-limiting step on all catalysts. The activity for the oxygen reduction reaction was evaluated against the difference of the oxygen adsorption energy on the Pt site and the M site of Pt3M and the results indicate that the oxygen adsorption energy difference offers an improved prediction of the oxygen reduction activity on these catalysts. Based on the analysis, Pt3Ni supported on oxygen-doped graphene exhibits an enhanced catalytic performance for oxygen reduction over Pt4.

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A DFT study of oxygen reduction reaction mechanism over O-doped graphene-supported Pt4, Pt3Fe and Pt3V alloy catalysts

Cited by 37 publications

References 85 publications

Oxygen reduction catalyzed by nanocomposites based on graphene quantum dots-supported copper nanoparticles

Oxygen reduction catalyzed by nanocomposites based on graphene quantum dots-supported copper nanoparticles

Size-selective electrocatalytic activity of (Pt)_n/MoS₂ for oxygen reduction reaction

Oxygen Reduction Reaction Catalyzed by Pt3M (M = 3d Transition Metals) Supported on O-doped Graphene

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A DFT study of oxygen reduction reaction mechanism over O-doped graphene-supported Pt4, Pt3Fe and Pt3V alloy catalysts

Cited by 37 publications

References 85 publications

Oxygen reduction catalyzed by nanocomposites based on graphene quantum dots-supported copper nanoparticles

Oxygen reduction catalyzed by nanocomposites based on graphene quantum dots-supported copper nanoparticles

Size-selective electrocatalytic activity of (Pt)n/MoS2 for oxygen reduction reaction

Oxygen Reduction Reaction Catalyzed by Pt3M (M = 3d Transition Metals) Supported on O-doped Graphene

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Size-selective electrocatalytic activity of (Pt)_n/MoS₂ for oxygen reduction reaction