First-Principles Modeling of Direct versus Oxygen-Assisted Water Dissociation on Fe(100) Surfaces

Wang, Wenju; Wang, Guoping; Shao, Minhua

doi:10.3390/catal6020029

Cited by 14 publications

(12 citation statements)

References 72 publications

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“…In DFT calculations, the Generalized Gradient Approximation (GGA) in the form of the Perdew-Burke-Ernzerhof (PBE) method was used for the exchange-correlation function [13][14][15][16][17]. The spin value was set to be unrestricted, and the formal spin was expressed as the initial value [18].…”

Section: Theoretical Calculation Methodsmentioning

confidence: 99%

A DFT-Based Model on the Adsorption Behavior of H2O, H+, Cl−, and OH− on Clean and Cr-Doped Fe(110) Planes

Wang

et al. 2018

Coatings

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Abstract:The impact of four typical adsorbates, namely H 2 O, H + , Cl − , and OH − , on three different planes, namely, Fe(110), Cr(110) and Cr-doped Fe(110), was investigated by using a density functional theory (DFT)-based model. It is verified by the adsorption mechanism of the abovementioned four adsorbates that the Cr-doped Fe(110) plane is the most stable facet out of the three. As confirmed by the adsorption energy and electronic structure, Cr doping will greatly enhance the electron donor ability of neighboring Fe atoms, which in turn prompts the adsorption of the positively charged H + . Meanwhile, the affinity of Cr to negatively charged adsorbates (e.g., Cl − and O of H 2 O, OH − ) is improved due to the weakening of its electron donor ability. On the other hand, the strong bond between surface atoms and the adsorbates can also weaken the bond between metal atoms, which results in a structure deformation and charge redistribution among the native crystal structure. In this way, the crystal becomes more vulnerable to corrosion.

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Section: Theoretical Calculation Methodsmentioning

confidence: 99%

A DFT-Based Model on the Adsorption Behavior of H2O, H+, Cl−, and OH− on Clean and Cr-Doped Fe(110) Planes

Wang

et al. 2018

Coatings

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“…[47] For the surface structure, two atomic layers of Ni 3 ZnC 0.7 were cleaved at the 2D C 5 N 1 plane. The specific calculation details were given in ap revious report.…”

Section: Experimental Section Calculation Detailsmentioning

confidence: 99%

“…The specific calculation details were given in ap revious report. [47] For the surface structure, two atomic layers of Ni 3 ZnC 0.7 were cleaved at the 2D C 5 N 1 plane. In calculations of the adsorption energy, Ni 3 ZnC 0.7 /C 5 N 1 features are clarified.…”

Section: Experimental Section Calculation Detailsmentioning

confidence: 99%

Highly Dispersed Metal Carbide on ZIF‐Derived Pyridinic‐N‐Doped Carbon for CO₂ Enrichment and Selective Hydrogenation

Cai

Chen

et al. 2018

ChemSusChem

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Catalytic conversion of CO into chemicals is a critical issue for energy and environmental research. Among such reactions, converting CO into CO has been regarded as a significant foundation to generate a liquid fuels and chemicals on a large scale. In this work, zeolitic imidazolate framework-derived N-doped carbon-supported metal carbide catalysts (M/ZIF-8-C; M=Ni, Fe, Co and Cu) with highly dispersed metal carbide were prepared for selective CO hydrogenation. Under the same metal loadings, catalytic activity for CO hydrogenation to CO follows the order: Ni/ZIF-8-C≈Fe/ZIF-8-C>Co/ZIF-8-C>Cu/ZIF-8-C. These catalysts are composed of carbide or metal supported on pyridinic N sites within the N-doped carbon structure. ZIF-8-derived pyridinic nitrogen and carbide effect CO adsorption, whereas dispersed Ni or Fe carbide and metal species serve as an active site for CO hydrogenation. The supported Ni catalyst exhibits extraordinary catalytic performance, which results from high dispersion of the metal and exposure of the carbide. Based on high-sensitivity low-energy ion scattering (HS-LEIS) and line scan results, density functional theory (DFT) was used to understand reaction mechanism of selective CO hydrogenation over Ni/ZIF-8-C. The product CO is derived mainly from the direct cleavage of C-O bonds in CO * rather than decomposition of COOH*. The CO* desorption energy on Ni/ZIF-8-C is lower than that for further hydrogenation and dissociation. Comparison of Ni/ZIF-8-C with ZIF-8-C indicates that the combined effects of the highly dispersed metal or carbide and weak CO adsorption result in high CO selectivity for CO hydrogenation.

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“…In a similar manner, Wang W. et al [5] explored, by means of DFT calculations, the adsorption of H 2 O and its dissociation fragments (OH, H and O) on clean and O-pre-adsorbed Fe(100) surfaces. It was demonstrated that interactions between the different adsorbates and catalyst surface followed the order: H 2 O < OH < H < O.…”

Section: Contribution Highlightsmentioning

confidence: 99%

“…It consists of 14 high-quality papers, involving: a comprehensive review article on the surface analysis techniques that can be employed to elucidate the phenomenon of electrochemical promotion in catalysis [3]; two theoretical studies (Density Functional Theory, DFT) on H 2 O dissociation and its implications in catalysis [4,5]; two mechanistic studies by means of temperature-programmed desorption/surface reaction (TPD/TPSR) and/or operando spectroscopy on N 2 O formation over NO x storage-reduction (NSR) catalysts [6] and on methanol reforming over cobalt catalysts [7]; two articles on H 2 production by the steam reforming of ethanol [8] or diesel [9] over transition metal-based catalysts; two articles on the production of commercial fuels by Fisher-Tropsch synthesis [10,11]; two articles on Au-catalyzed CO oxidation [12] and preferential CO oxidation [13]; and three experimental investigations regarding the structure-activity correlation of NO oxidation to NO 2 over Mn-Co binary oxides [14], cyclohexene oxidation on TiZrCo mixed oxides [15] and alkene epoxidation on silica nanoparticles [16].…”

Section: This Special Issuementioning

confidence: 99%

Surface Chemistry and Catalysis

Konsolakis

2016

Catalysts

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BackgroundNowadays, heterogeneous catalysis plays a prominent role. The majority of industrial chemical processes, involving the manufacturing of commodity chemicals, pharmaceuticals, clean fuels, etc., as well as pollution abatement technologies, have a common catalytic origin. As catalysis proceeds at the surface, it is of paramount importance to gain insight into the fundamental understanding of local surface chemistry, which in turn governs the catalytic performance. The deep understanding at the atomic level of a catalyst surface could pave the way towards the design of novel catalytic systems for real-life energy and environmental applications.Thanks to surface science we can obtain profound insight into the structure of a surface, the chemical state of active sites, the interfacial reactivity, the way molecules bind and react, the role of surface defects and imperfections (e.g., surface oxygen vacancies), and the mode of action of various surface promoters/poisons. To elucidate the aforementioned surface phenomena, sophisticated techniques in combination with theoretical studies are necessary to reveal the composition and the structure/morphology of the surface as well as the chemical entity of adsorbed species. Moreover, time-resolved methods are required to investigate the dynamic phenomena occurring at the surface, such as adsorption/desorption, diffusion and chemical reactions. Under this perspective, it was clearly revealed, based on the recently published review articles by the Guest Editor, that the complete elucidation of a catalytic phenomenon (e.g., metal-support interactions [1]) or the fundamental understanding of a specific catalytic process (e.g., N 2 O decomposition [2]) requires a holistic approach involving the combination of advanced ex situ experimental and theoretical studies with in situ operando studies. This Special IssueIn light of the above aspects, the present themed issue aims to cover the recent advances in "surface chemistry and catalysis" that can be obtained by means of advanced characterization techniques, computational calculations and time-resolved methods, with particular emphasis on the structure-activity relationships (SARs). It consists of 14 high-quality papers, involving: a comprehensive review article on the surface analysis techniques that can be employed to elucidate the phenomenon of electrochemical promotion in catalysis [3]; two theoretical studies (Density Functional Theory, DFT) on H 2 O dissociation and its implications in catalysis [4,5]; two mechanistic studies by means of temperature-programmed desorption/surface reaction (TPD/TPSR) and/or operando spectroscopy on N 2 O formation over NO x storage-reduction (NSR) catalysts [6] and on methanol reforming over cobalt catalysts [7]; two articles on H 2 production by the steam reforming of ethanol [8] or diesel [9] over transition metal-based catalysts; two articles on the production of commercial fuels by Fisher-Tropsch synthesis [10,11]; two articles on Au-catalyzed CO oxidation [12] and preferential CO oxi...

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First-Principles Modeling of Direct versus Oxygen-Assisted Water Dissociation on Fe(100) Surfaces

Cited by 14 publications

References 72 publications

A DFT-Based Model on the Adsorption Behavior of H2O, H+, Cl−, and OH− on Clean and Cr-Doped Fe(110) Planes

A DFT-Based Model on the Adsorption Behavior of H2O, H+, Cl−, and OH− on Clean and Cr-Doped Fe(110) Planes

Highly Dispersed Metal Carbide on ZIF‐Derived Pyridinic‐N‐Doped Carbon for CO₂ Enrichment and Selective Hydrogenation

Surface Chemistry and Catalysis

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First-Principles Modeling of Direct versus Oxygen-Assisted Water Dissociation on Fe(100) Surfaces

Cited by 14 publications

References 72 publications

A DFT-Based Model on the Adsorption Behavior of H2O, H+, Cl−, and OH− on Clean and Cr-Doped Fe(110) Planes

A DFT-Based Model on the Adsorption Behavior of H2O, H+, Cl−, and OH− on Clean and Cr-Doped Fe(110) Planes

Highly Dispersed Metal Carbide on ZIF‐Derived Pyridinic‐N‐Doped Carbon for CO2 Enrichment and Selective Hydrogenation

Surface Chemistry and Catalysis

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Product

Resources

About

Highly Dispersed Metal Carbide on ZIF‐Derived Pyridinic‐N‐Doped Carbon for CO₂ Enrichment and Selective Hydrogenation