Bridging model and real catalysts: general discussion

Campbell, Charles H.; Bowker, Michael; Stamatakis, Michail; Hutchings, Graham J.; Davies, P.L.; Earley, James H.; Howard, Mark J.; Garrett, Bruce C.; Oloye, Femi Francis; Gross, Elad; Kotarba, Andrzej; Landau, Miron V.; Panas, Itai; Anderson, James D.; Weckhuysen, Bert M.; Dononelli, Wilke; Iqbal, Sarwat; Temel, Burcin; Nowicka, Ewa; Bruix, Albert; Reece, Christian; Moulijn, Jacob A.; Gates, Bruce C.; Catlow, C. Richard A.; Tušar, Nataša Novak; Willock, David J.; Wotton, Daniel; Barceló, Francisco Ivars; Palmer, Richard E.; Madix, Robert J.; Friend, Cynthia M.; Corma, Avelino; Freund, Hans‐Joachim; Whiting, Gareth T.; Sauer, Joachim

doi:10.1039/c6fd90017h

Cited by 3 publications

(2 citation statements)

References 1 publication

(9 reference statements)

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“…The traditional investigation of adsorption behaviors by DFT calculation was generally carried out by placing reactant molecules on the typical facets, , which cannot represent the practical facts of nanoparticle catalysts because the true adsorption was generally contributed by all exposed facets of the nanoparticle under the working condition. ,,− To approach the experimental facts, the equilibrium Wulff morphology of the χ-Fe 5 C 2 nanoparticle was established to represent the nanoparticle catalyst by calculating the surface free energies of 14 different facets under the practical FTS pretreatment (600 K, 1 atm, H 2 /CO = 2.5) . Based on the area proportion of the Wulff morphology, nine facets which are up to 85% of the area for χ-Fe 5 C 2 nanoparticles were selected for the further DFT calculation of CO adsorption.…”

Section: Resultsmentioning

confidence: 99%

Unraveling the Detailed Interactions between the Surface Species and Nanoparticle Catalyst by a Temperature-Programed Desorption Spectrum at the Molecular Level via a Multi-Scale Simulation and Modeling Experiment

Wang

Liu³

et al. 2023

J. Phys. Chem. C

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Exploring the binding information of surface species with the active sites of a catalyst plays a key role in reaction mechanism study. The temperature-programed desorption (TPD) spectrum is a powerful approach to probe the interactions between surface species and a catalyst. However, it is hard to unravel their detailed interactions at the molecular level because TPD peaks are the statistical information derived from all surfaces of the nanoparticle catalyst. How to unravel these bonding details at the molecular level remains a substantial challenge in TPD spectrum analysis. To solve this difficult problem, a new strategy combining a density functional theory calculation, kinetic Monte Carlo simulation, and modeling experiment was proposed using CO TPD on χ-Fe5C2 nanoparticles as a demonstration. The good agreement between the simulated and experimental TPD spectra indicates the reasonability and feasibility of our strategy. It is anticipated to be a general method to unravel the interactions between surface species and catalysts at the molecular level.

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Section: Resultsmentioning

confidence: 99%

Unraveling the Detailed Interactions between the Surface Species and Nanoparticle Catalyst by a Temperature-Programed Desorption Spectrum at the Molecular Level via a Multi-Scale Simulation and Modeling Experiment

Wang

Liu³

et al. 2023

J. Phys. Chem. C

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“…Computational modeling techniques have advanced the atomistic understanding of heterogeneous catalysis, correlating electronic structure to surface reactivity, 310,311 interpreting microscopic and spectroscopic observations, 312 and predicting kinetics of reaction networks. 18,313,314 Methods based on the explicit quantum mechanical treatment of electronic structures, such as DFT calculations, are critically important since they can accurately describe the forming and breaking of bonds in catalytic reactions. However, modeling dilute alloy catalysts is still an untrivial task due to the complexity of these systems.…”

Section: Machine Learning Accelerated Molecular Dynamicsmentioning

confidence: 99%

Dilute Alloys Based on Au, Ag, or Cu for Efficient Catalysis: From Synthesis to Active Sites

et al. 2022

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The development of new catalyst materials for energy-efficient chemical synthesis is critical as over 80% of industrial processes rely on catalysts, with many of the most energy-intensive processes specifically using heterogeneous catalysis. Catalytic performance is a complex interplay of phenomena involving temperature, pressure, gas composition, surface composition, and structure over multiple length and time scales. In response to this complexity, the integrated approach to heterogeneous dilute alloy catalysis reviewed here brings together materials synthesis, mechanistic surface chemistry, reaction kinetics, in situ and operando characterization, and theoretical calculations in a coordinated effort to develop design principles to predict and improve catalytic selectivity. Dilute alloy catalystsin which isolated atoms or small ensembles of the minority metal on the host metal lead to enhanced reactivity while retaining selectivityare particularly promising as selective catalysts. Several dilute alloy materials using Au, Ag, and Cu as the majority host element, including more recently introduced support-free nanoporous metals and oxide-supported nanoparticle “raspberry colloid templated (RCT)” materials, are reviewed for selective oxidation and hydrogenation reactions. Progress in understanding how such dilute alloy catalysts can be used to enhance selectivity of key synthetic reactions is reviewed, including quantitative scaling from model studies to catalytic conditions. The dynamic evolution of catalyst structure and composition studied in surface science and catalytic conditions and their relationship to catalytic function are also discussed, followed by advanced characterization and theoretical modeling that have been developed to determine the distribution of minority metal atoms at or near the surface. The integrated approach demonstrates the success of bridging the divide between fundamental knowledge and design of catalytic processes in complex catalytic systems, which can accelerate the development of new and efficient catalytic processes.

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On Compton scattering as a source of background in coherent diffraction imaging experiments

Bikondoa¹,

Carbone²

2021

J Synchrotron Radiat

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Compton scattering is generally neglected in diffraction experiments because the incoherent radiation it generates does not give rise to interference effects and therefore is negligible at Bragg peaks. However, as the scattering volume is reduced, the difference between the Rayleigh (coherent) and Compton (incoherent) contributions at Bragg peaks diminishes and the incoherent part may become substantial. The consequences can be significant for coherent diffraction imaging at high scattering angles: the incoherent radiation produces background that smears out the secondary interference fringes, affecting thus the achievable resolution of the technique. Here, a criterion that relates the object shape and the resolution is introduced. The Compton contribution for several object shapes is quantified, and it is shown that the maximum achievable resolution along different directions has a strong dependence on the crystal shape and size.

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Bridging model and real catalysts: general discussion

Cited by 3 publications

References 1 publication

Unraveling the Detailed Interactions between the Surface Species and Nanoparticle Catalyst by a Temperature-Programed Desorption Spectrum at the Molecular Level via a Multi-Scale Simulation and Modeling Experiment

Unraveling the Detailed Interactions between the Surface Species and Nanoparticle Catalyst by a Temperature-Programed Desorption Spectrum at the Molecular Level via a Multi-Scale Simulation and Modeling Experiment

Dilute Alloys Based on Au, Ag, or Cu for Efficient Catalysis: From Synthesis to Active Sites

On Compton scattering as a source of background in coherent diffraction imaging experiments

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