DFT study on dry reforming of methane over Ni2Fe overlayer of Ni(1 1 1) surface

Xu, Liqiang; Wen, Hao; Jin, Xin; Bing, Qiming; Liu, Jing-Yao

doi:10.1016/j.apsusc.2018.02.268

Cited by 50 publications

(33 citation statements)

References 44 publications

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“…This result agrees with Heil and [31], who used both fast ion beam and fast molecular beam techniques to study CO2 dissociation, and found no chemisorbed CO2 on Ni (111). Moreover, it agrees with the computational studies performed on Ni (111) and on Ni2Fe (111) surfaces [19,32]. CO molecules prefer to adsorb at the B 2Ni site with an Eads of −1.52 eV.…”

Section: Ch 4 + Cosupporting

confidence: 89%

“…In contrast, CH dehydrogenation has a relatively higher E a,f of 1.40 eV, while the reverse reaction is energetically favorable with E a,r of 0.71 eV. Thus, coke formation due to CH decomposition is less desirable for Ni 2 Cu (111) compared to pure Ni (111) and Ni 2 Fe (111) surfaces with energy barriers of 1.33 eV [19] and 1.36 eV [28], respectively. Moreover, only CH* and C* are the most stable major intermediates remaining on the surface than the kinetically unstable CH 3 * and CH 2 * intermediates, as discussed in Table 1.…”

Section: Oxidation Of C and Chmentioning

confidence: 99%

“…In the case of CO, the adsorption is preferable on the Top Ni site with Eads of −1.52 eV, while the O atom is favorably bound to the FCC site with an Eads of −6.34 eV. It indicates that the Cu dopant in Ni (111) network improved atomic O adsorption while reducing CO adsorption compared to both pure Ni (111) and Ni2Fe (111) surfaces, respectively [19]. As a descriptor of coke resistance, the adsorption energy of the C atom indicates that the more strongly the carbon is adsorbed on a specific surface, the lower the coke resistance.…”

Section: Ch 4 + Comentioning

confidence: 99%

“…Consequently, the energy barriers for CHx (x = 1-4) dissociation increase in order of CH 2 < CH 3 < CH 4 < CH [36], which is in line with CH 4 decomposition on pure Ni (111) and Ni 2 Fe (111) systems. In addition, the energy barriers of those subsequent steps are much higher in the case of Ni 2 Cu (111) than Ni (111) and Ni 2 Fe (111) systems, which reduce carbon deposition from CH radical dehydrogenation [19,28,37].…”

Section: Chx Dissociation (X = 1-4)mentioning

confidence: 99%

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Mechanistic Insights for Dry Reforming of Methane on Cu/Ni Bimetallic Catalysts: DFT-Assisted Microkinetic Analysis for Coke Resistance

et al. 2020

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Density functional theory (DFT) calculations have been utilized to evaluate the complete reaction mechanism of methane dry reforming (DRM) over Ni2Cu (111) bimetallic catalyst. The detailed catalytic cycle on Ni2Cu (111) catalyst demonstrated superior coke resistance compared to pure Ni (111) and Ni2Fe (111) reported in the literature. Doping Cu in the Ni–Ni network enhanced the competitive CH oxidation by both atomic O and OH species with the latter having only 0.02 eV higher than the 1.06 eV energy barrier required for CH oxidation by atomic O. Among the C/CH oxidation pathways, C* + O* → CO (g) was the most favorable with an energy barrier of 0.72 eV. This was almost half of the energy barrier required for the rate-limiting step of CH decomposition (1.40 eV) and indicated enhanced coke deposition removal. Finally, we investigated the effect of temperature (800~1000 K) on the carbon deposition and elimination mechanism over Ni2Cu (111) catalyst. Under those realistic DRM conditions, the calculations showed a periodic cycle of simultaneous carbon deposition and elimination resulting in improved catalyst stability.

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Section: Ch 4 + Cosupporting

confidence: 89%

Section: Oxidation Of C and Chmentioning

confidence: 99%

Section: Ch 4 + Comentioning

confidence: 99%

Section: Chx Dissociation (X = 1-4)mentioning

confidence: 99%

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Mechanistic Insights for Dry Reforming of Methane on Cu/Ni Bimetallic Catalysts: DFT-Assisted Microkinetic Analysis for Coke Resistance

et al. 2020

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“…The combination of two metals as the active phase has shown an increased catalyst performance by density functional theory (DFT) studies [65], since it may promote the WGS reaction (Eq. (2)), while increasing metal dispersion and coke resistance.…”

Section: Figurementioning

confidence: 99%

Coke formation and deactivation during catalytic reforming of biomass and waste pyrolysis products: A review

Ochoa

Bilbao

Gayubo

et al. 2020

Renewable and Sustainable Energy Reviews

326

158

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Comparative density functional theory study of carbon formation and removal mechanism on Rh modified Ni‐based catalyst in theCH₄/CO₂reforming

et al. 2021

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Summary Rh catalyst shows promising performance for coke resistance in the CH4/CO2 reforming reaction. In this study, a single atom Rh was added to the surface of Ni(111) by doping and adsorbing ways, and the performance of these surfaces was compared with the pure Ni(111) through density functional theory (DFT) calculation. The reactions related to the carbon formation were studied to obtain the favored adsorption site and dominant reaction paths on three surfaces. A good linear relationship between the charge difference and the reaction barrier was proposed. On the Ni(111) surface, the highest energy barrier of CH* oxidation and decomposition is 1.24 and 1.30 eV, respectively, thus these two reaction paths are dominant. The most favorable pathway for the Rh/Ni(111) is CH* + O* → CHO* → CO* + H*, with the highest energy barrier of 1.34 eV. However, C* is more likely to be converted into C‐C (C2) than oxidized on all three catalyst surfaces. As a result, Rh/Ni(111) surface shows better catalytic activity thermodynamically and more superior carbon deposition resistance. In general, compared with pure Ni catalyst, the modification of Rh could manipulate the reaction path of CH* consumption, which could inhibit the direct decomposition of CH*, and finally suppress the carbon deposition.

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DFT study on dry reforming of methane over Ni2Fe overlayer of Ni(1 1 1) surface

Cited by 50 publications

References 44 publications

Mechanistic Insights for Dry Reforming of Methane on Cu/Ni Bimetallic Catalysts: DFT-Assisted Microkinetic Analysis for Coke Resistance

Mechanistic Insights for Dry Reforming of Methane on Cu/Ni Bimetallic Catalysts: DFT-Assisted Microkinetic Analysis for Coke Resistance

Coke formation and deactivation during catalytic reforming of biomass and waste pyrolysis products: A review

Comparative density functional theory study of carbon formation and removal mechanism on Rh modified Ni‐based catalyst in theCH₄/CO₂reforming

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DFT study on dry reforming of methane over Ni2Fe overlayer of Ni(1 1 1) surface

Cited by 50 publications

References 44 publications

Mechanistic Insights for Dry Reforming of Methane on Cu/Ni Bimetallic Catalysts: DFT-Assisted Microkinetic Analysis for Coke Resistance

Mechanistic Insights for Dry Reforming of Methane on Cu/Ni Bimetallic Catalysts: DFT-Assisted Microkinetic Analysis for Coke Resistance

Coke formation and deactivation during catalytic reforming of biomass and waste pyrolysis products: A review

Comparative density functional theory study of carbon formation and removal mechanism on Rh modified Ni‐based catalyst in theCH4/CO2reforming

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Product

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DFT study on dry reforming of methane over Ni2Fe overlayer of Ni(1 1 1) surface

Comparative density functional theory study of carbon formation and removal mechanism on Rh modified Ni‐based catalyst in theCH₄/CO₂reforming