Effect of Ni(111) surface alloying by Pt on partial oxidation of methane to syngas: A DFT study

Zhang, Minhua; Yang, Kuiwei; Zhang, Xiaohang; Yu, Yingzhe

doi:10.1016/j.susc.2014.08.023

Cited by 46 publications

(20 citation statements)

References 68 publications

(91 reference statements)

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“…The most stable adsorption configuration for CH adsorption on Pt 3 M is at hollow site (both hollow sites have similar adsorption energy) with molecular axis of CH normal to the surface and C atom bonded to an atom on the surface in agreement with other theoretical studies [94][95][96]. It is noted in Figure 6, a trend similar to CO adsorption, adsorption on sites with only Pt in the alloy is weaker than pure Pt, whereas the sites with metal atoms have higher or similar adsorption energy than pure Pt with the exception of Pt 3 Sn, which is significantly lower.…”

Section: Calculation Of Reactivity Descriptorssupporting

confidence: 88%

Modeling with DFT and Chemical Descriptors Approach for the Development of Catalytic Alloys for PEMFCs

Pérez¹,

Paz²

2019

Density Functional Theory

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Material properties and process modeling with density functional theory (DFT) is an accurate method to facilitate the study and the design of materials computationally for the development of different electrochemical technologies such as fuel cells, solar cells, and batteries, among others, mainly to achieve alternative ways for energy conversion and storage. Considering the relevance of DFT in the development of these alternative technologies for energy generation and storage, in this chapter, the application of DFT to study catalytic alloys and their reactivity processes to develop polymer membrane fuel cells (PEMFCs) is presented. In this sense, firstly, a brief review of the application of DFT to develop catalysts for PEMFCs and the relation with the concept of chemical descriptors is presented. Secondly, the main chemical descriptors for this task are presented and discussed. Finally, a summary of the main findings of the modeling with DFT and chemical descriptors approach of catalytic alloys for PEMFCs is presented and analyzed.

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Section: Calculation Of Reactivity Descriptorssupporting

confidence: 88%

Modeling with DFT and Chemical Descriptors Approach for the Development of Catalytic Alloys for PEMFCs

Pérez¹,

Paz²

2019

Density Functional Theory

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“…The oxidation of CH 4 to CO involves the oxidation process of CH and C. In order to investigate the effect of oxygen atoms on the formation of CO on a Pd catalyst, three possible reaction pathways of Catalysts 2019, 9, 666 9 of 14 CO formation on Pd 2 and Pd 2 O were studied using DFT calculation [45,46]. The processes were: (1) CH→C + H, C + O→CO; (2) CH + O→CHO→CO + H; and (3) CH + O→COH→CO + H.…”

Section: Carbon Monoxide Formationmentioning

confidence: 99%

Oxygen Atom Function: The Case of Methane Oxidation Mechanism to Synthesis Gas over a Pd Cluster

et al. 2019

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A dimer model Pd 2 was established to study the adsorption of CH x (x = 1-4) and CH 4 dehydrogenation, as well as syngas formation using density functional theory (DFT) at the atomic level. Meanwhile, insight into understanding the role of the oxygen atom on the partial oxidation of methane (POM) was also calculated based on a trimer model of Pd 2 O. For the adsorption of CH x , results showed that the presence of an oxygen atom was a disadvantage to the adsorption of CH x (x = 1-3) species. For CH 4 dissociation, the process of CH 2 →CH + H was found to be the rate-limiting step (RSD) on both Pd 2 and Pd 2 O. H 2 was formed by the reaction of CH 2 + 2H→CH 2 + H 2 . For CO formation, it was primarily formed in the process of CH + O→CHO→CO + H on both the Pd 2 and the Pd 2 O catalyst. Thermodynamic and kinetic calculations revealed that formation and maintainance of the oxygen atom on the Pd surface could promote a POM reaction to achieve high H 2 and CO yield and selectivity. Our study provides a helpful understanding of the effect of an adsorbed oxygen atom on a POM reaction with a Pd catalyst.

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“…Based on the above results and our previous work [32], we explored the reactivity of CH x (x = 1-3) species on Ni(111) in order to screen feasible routes toward CO and identify the effect of adsorbed O on CH x transformation. Figure 6a presents the barrier heights of direct, O-assisted one-step, and O-assisted two-step dehydrogenation routes from CH 3 .…”

Section: Analysis Of Ch X (X = 1-3) Transformation To Comentioning

confidence: 99%

“…This can give us insight into the factors controlling carbon deposition and assist in designing the optimal catalyst. In our preliminary work in the laboratory [32], we studied the adsorption and dissociation of methane as well as syngas formation over Ni(111) and NiPt(111) to understand the effect of Ni(111) surface alloying on POM. The results showed that Pt-doped Ni(111) surface is beneficial to the adsorption of CH x and H species and unfavorable to the desorption of H 2 .…”

Section: Introductionmentioning

confidence: 99%

Mechanisms of Transforming CHx to CO on Ni(111) Surface by Density Functional Theory

Lei

Wang

et al. 2019

Trans. Tianjin Univ.

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To elucidate feasible routes of producing CO from CH 3 and unravel the effect of adsorbed O on CH x transformation, the reactivity of CH x (x = 1-3) with and without the assistance of adsorbed atomic O on Ni(111) was explored using density functional theory calculations. The adsorption energies of CH x (x = 0-3) were found to be significantly reduced on an O-preadsorbed Ni(111) surface compared to a pure surface. Furthermore, O-assisted one-step dehydrogenation of CH x (x = 1-3) features energy barriers and thus is difficult to proceed. In terms of energy, the direct dissociation of CH 3 is favorable, except for the last CH dehydrogenation, which is energy intensive. Interestingly, in O-assisted two-step CH transformation to CO via CHO intermediate, the barrier is dramatically lowered. The successive dehydrogenations of CH x O (x = 1-3) were also found to be a route for CO formation. Finally, two possible pathways from CH 3 to CO are proposed: (a) CH 3 → CH 2 → CH → CHO → CO;

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Effect of Ni(111) surface alloying by Pt on partial oxidation of methane to syngas: A DFT study

Cited by 46 publications

References 68 publications

Modeling with DFT and Chemical Descriptors Approach for the Development of Catalytic Alloys for PEMFCs

Modeling with DFT and Chemical Descriptors Approach for the Development of Catalytic Alloys for PEMFCs

Oxygen Atom Function: The Case of Methane Oxidation Mechanism to Synthesis Gas over a Pd Cluster

Mechanisms of Transforming CHx to CO on Ni(111) Surface by Density Functional Theory

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