Catalytic NO activation and NO–H 2 reaction pathways

Hibbitts, David; Jiménez, Romel; Yoshimura, Masayuki; Weiss, Brian M.; Iglesia, Enrique

doi:10.1016/j.jcat.2014.07.012

Cited by 39 publications

(80 citation statements)

References 48 publications

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“…Molecular hydrogen (H 2 ) is a common reagent in metal‐catalyzed reactions, such as the hydrogenation of unsaturated C = C bonds and the reduction of CO, NO, or N 2 ; it is also used to cleave C–C bonds in alkane hydrogenolysis, C–O bonds in hydrodeoxygenation, and C–S bonds in hydrodesulfurization . H 2 readily dissociates on most noble metal catalysts, including Pt and Ir, at ambient or near‐ambient conditions.…”

Section: Introductionmentioning

confidence: 99%

Supra‐monolayer coverages on small metal clusters and their effects on H₂ chemisorption particle size estimates

Almithn

Hibbitts

2018

AIChE Journal

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H 2 chemisorption measurements are used to estimate the size of supported metal particles, often using a hydrogen-tosurface-metal stoichiometry of unity. This technique is most useful for small particles whose sizes are difficult to estimate through electron microscopy or X-ray diffraction. Undercoordinated metal atoms at the edges and corners of particles, however, make up large fractions of small metal clusters, and can accommodate multiple hydrogen atoms leading to coverages which exceed 1 ML (supra-monolayer). Density functional theory was used to calculate hydrogen adsorption energies on Pt and Ir particles (38-586 atoms, 0.8-2.4 nm) at high coverages (3.63 ML). Calculated differential binding energies confirm that Pt and Ir (111) single-crystal surfaces saturate at 1 ML; however, Pt and Ir clusters saturate at supra-monolayer coverages as large as 2.9 ML. Correlations between particle size and saturation coverage are provided that improve particle size estimates from H 2 chemisorption for Pt-group metals.

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Section: Introductionmentioning

confidence: 99%

Supra‐monolayer coverages on small metal clusters and their effects on H₂ chemisorption particle size estimates

Almithn

Hibbitts

2018

AIChE Journal

Self Cite

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“…7 for examples) to close-packed surfaces with add_adsorbate ( Table 3 shows adsorbates which can currently be added using this command). These have been used to examine the binding energies of CO* on Ru(0001) surfaces, 16 H* on Pt and Ir(111), 17,18 and NO* on Pt(111). 17 Cubo-octahedral FCC metal particles can be generated with build_particle with user-specified shape and size (users specify the size of (111) and (100) crystal facets and thus can build a wide variety of particle models -see Section S3 in the SI for examples).…”

Section: Structure Generation and Manipulationmentioning

confidence: 99%

“…These have been used to examine the binding energies of CO* on Ru(0001) surfaces, 16 H* on Pt and Ir(111), 17,18 and NO* on Pt(111). 17 Cubo-octahedral FCC metal particles can be generated with build_particle with user-specified shape and size (users specify the size of (111) and (100) crystal facets and thus can build a wide variety of particle models -see Section S3 in the SI for examples). Tools also exist to add adsorbates to metal particles based on binding site ensembles (i.e., adding a H* atop to all corner atoms on a 538-atom cluster).…”

Section: Structure Generation and Manipulationmentioning

confidence: 99%

A New Computational Interface for Catalysis

Kravchenko

Plaisance²,

Hibbitts³

2019

Preprint

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“…7 for examples) to close-packed surfaces with add_adsorbate ( Table 3 shows adsorbates which can currently be added using this command). These have been used to examine the binding energies of CO* on Ru(0001) surfaces, 4 H* on Pt and Ir(111), 5,6 and NO* on Pt(111). 5 Cubo-octahedral FCC metal particles can be generated with build_particle with user-specified shape and size (users specify the size of (111) and (100) crystal facets and thus can build a wide variety of particle models (see Section S3 in the SI for examples).…”

Section: Structure Generation and Manipulationmentioning

confidence: 99%

“…These have been used to examine the binding energies of CO* on Ru(0001) surfaces, 4 H* on Pt and Ir(111), 5,6 and NO* on Pt(111). 5 Cubo-octahedral FCC metal particles can be generated with build_particle with user-specified shape and size (users specify the size of (111) and (100) crystal facets and thus can build a wide variety of particle models (see Section S3 in the SI for examples). Tools also exist to add adsorbates to metal particles based on binding site ensembles (i.e., adding a H* atop to all corner atoms on a 538atom cluster).…”

Section: Structure Generation and Manipulationmentioning

confidence: 99%

A New Computational Interface for Catalysis

Kravchenko

Plaisance²,

Hibbitts³

2019

Preprint

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Here we present a new interface for conducting DFT simulations-the computational catalysis interface (CCI). CCI focuses on simplifying DFT studies and enabling multi-step and high-throughput studies with varying degrees of automation. CCI sets up calculations using descriptive language, allowing users with a wide range of backgrounds to rapidly begin studies. Multi-step calculations gradually increase accuracy, resulting in gains in cpu-efficiency by up to an order of magnitude over single-step calculations. CCI is designed to operate from a centralized data server connected to all compute servers you have access to with automated file management between machines. Structure manipulation tools allow one to add/remove adsorbates from catalysts, modify chemical fragments, catalyst composition, and the location of reactions on catalyst surfaces. Specific tools have been made for modeling metal surfaces and clusters as well as a suite of tools for tackling the configurational complexity of reactions occurring within zeolite micropores. These structure manipulation tools allow one to generate structures from previously converged calculations by programmatically altering the catalyst, reactant, and/or environment (i.e., adding solvent or altering adsorbate coverages). Calculations are monitored, with emails sent when they begin to diverge, fail, or finish. Emails are customized, contain relevant information, and link to a web-based GUI that provides 3-D visualization of structures and movies for convergence trajectories, reaction pathways, and vibrational modes. This web-GUI also allows users to directly start calculations using contextspecific commands. This web-GUI facilitates dissemination and interfaces with the POV-Ray utility to generate high-resolution publication and presentation-quality visualizations. These tools are described here, at a high level, to describe how CCI interacts with VASP to enable computational catalysis studies on a range of reactions and catalysts.

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Catalytic NO activation and NO–H 2 reaction pathways

Cited by 39 publications

References 48 publications

Supra‐monolayer coverages on small metal clusters and their effects on H₂ chemisorption particle size estimates

Supra‐monolayer coverages on small metal clusters and their effects on H₂ chemisorption particle size estimates

A New Computational Interface for Catalysis

A New Computational Interface for Catalysis

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Catalytic NO activation and NO–H 2 reaction pathways

Cited by 39 publications

References 48 publications

Supra‐monolayer coverages on small metal clusters and their effects on H2 chemisorption particle size estimates

Supra‐monolayer coverages on small metal clusters and their effects on H2 chemisorption particle size estimates

A New Computational Interface for Catalysis

A New Computational Interface for Catalysis

Contact Info

Product

Resources

About

Supra‐monolayer coverages on small metal clusters and their effects on H₂ chemisorption particle size estimates

Supra‐monolayer coverages on small metal clusters and their effects on H₂ chemisorption particle size estimates