Heterogeneous catalysis: looking forward with molecular simulation

Andzelm, Jan; Alvarado-Swaisgood, Aileen E.; Axe, Frank U.; Doyle, Michael W.; Fitzgerald, George; Freeman, C. M.; Gorman, A. M.; Hill, Jörg‐Rüdiger; Kölmel, Christoph; Levine, S. M.; Saxe, Paul; Stark, K.; Subramanian, Lalitha; Daelen, M. A. van; Wimmer, E.; Newsam, J. M.

doi:10.1016/s0920-5861(98)00482-9

Cited by 23 publications

(7 citation statements)

References 158 publications

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“…EadsEasorbed system (Emetai cluster +Eadsorbed molecule) (1) where Emetai cluster, Eadsorbed molecule, and Eadsorbed system represent the binding energies of the metal cluster, free molecule, and the adsorbed system, respectively. The negative value of Eads means that the corresponding adsorption state is thermodynamically favorable.…”

Section: Combinatorial Methodology and Calculational Detailesmentioning

confidence: 99%

<title>Theoretical design of heterogenous catalysts by combinatorial computational chemistry approach: application to Fischer-Tropsch synthesis</title>

Belosludov

Kubota

Sakahara

et al. 2001

Combinatorial and Composition Spread Techniques in Materials and Device Development II

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The combinatorial computational chemistry approach was applied to design new types of Fe-based catalysts, which can be used for the production of ecologically high-quality transportation fuels by the Fischer-Tropsch (FT) synthesis. For this purpose, the density functional theory (DFT) was used to investigate the adsorption of 10 intermediate species for methylene formation on Fe-based multi-component catalysts. The energetic, electronic and structural properties of these species on the catalyst surfaces were calculated. The detailed analysis of possible reaction mechanisms was performed from the comprehensive set of binding energies and structures. It was found that Mn, Mo, and Zr could be used as additional elements in the Fe-based catalysts, since one cannot observe a degradation of the adsorption properties of the active sites as well as showing a high sulfur tolerance. The obtained results are in agreement with available experimental data, thus confirming the validity of combinatorial computational chemistry approach. This also illustrates the role in which combinatorial computational chemistry approach can be used to provide data for discovering and designing new catalysts.

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Section: Combinatorial Methodology and Calculational Detailesmentioning

confidence: 99%

<title>Theoretical design of heterogenous catalysts by combinatorial computational chemistry approach: application to Fischer-Tropsch synthesis</title>

Belosludov

Kubota

Sakahara

et al. 2001

Combinatorial and Composition Spread Techniques in Materials and Device Development II

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“…However, they can also serve as valuable tools for the discovery and optimization of new catalytic materials. That quantum chemistry as well as molecular simulation programs have already proven to be useful tools to complement experiments is most encouraging 78, 79. Some areas where computational methods could contribute to combinatorial catalysis include the building of structural models and pre‐screening of catalytic materials before undertaking experiments, the determination of structure–activity relationships from which the activities of new catalytic materials can be rapidly ascertained.…”

Section: Numerical Simulationsmentioning

confidence: 99%

Combinatorial Heterogeneous Catalysis—A New Path in an Old Field

Şenkan

2001

Angew. Chem. Int. Ed.

300

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Combinatorial catalysis is the systematic preparation, processing, and testing of large diversities of chemically and physically different materials libraries in a high‐throughput fashion. It also embodies microfabrication, robotics, automation, instrumentation, computational chemistry, and large‐scale information management (informatics), and as such carries the promise of a renaissance in catalytic reaction engineering. Significant progress has already been made in demonstrating the speed and economic advantage of combinatorial approaches by the discovery of superior catalytic materials in a matter of hours and days, as opposed to the months and years required using traditional methods. Combinatorial methods can also significantly contribute to our understanding of catalytic function by increasing our chances of discovering totally new and unexpected catalytic materials, and by expediting the recognition of trends and patterns of structure–activity relations, from which new catalytic materials can be designed more efficiently. Combinatorial catalysis undoubtedly will be the new paradigm of catalysis research as the industry faces increasing global competition and pressure for the development of environmentally friendly processes at a time when resources for research are diminishing.

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“…There are four possible types of simulation to describe the behavior of organic molecules in a microporous solid [11]. One of these, called Monte Carlo docking, is well suited for the detection of preferred adsorption sites [12].…”

Section: Introductionmentioning

confidence: 99%

“…These techniques can be divided into probabilistic and deterministic ones [11]. The probabilistic techniques include any variation of the Monte Carlo (MC) method in which the state of the system (atom positions) is generated randomly to be either accepted or rejected, according to the energetics involved.…”

Section: Introductionmentioning

confidence: 99%

Modeling benzene sorption and diffusion in a γAl2O3catalyst

Szyja

Szczygieł

2004

J Computer-Aided Mater Des

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The behavior of the benzene-Pt-Sn/γ -Al 2 O 3 catalytic system was simulated with the software Cerius 2 from Accelrys Inc. The Grand Canonical Monte Carlo (GCMC) method was used to assess the adsorption isotherms under conditions of constant pressure and an equilibrium number of benzene molecules. With the results of GCMC simulation it was possible to locate the adsorption centers on the micropore surface at low temperature and a homogeneous benzene monolayer surface at elevated temperature. The results obtained with the GCMC method were then used to simulate the molecular dynamics of the catalytic system and to assess the coefficients of benzene diffusion. Elevated temperature was found to limit molecular motion across the micropore to a large extent. From the temperature-dependence plots of the diffusion coefficients it can be inferred that if the number of molecules is constant, the diffusion in the micropore is a molecular one.

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Heterogeneous catalysis: looking forward with molecular simulation

Cited by 23 publications

References 158 publications

<title>Theoretical design of heterogenous catalysts by combinatorial computational chemistry approach: application to Fischer-Tropsch synthesis</title>

<title>Theoretical design of heterogenous catalysts by combinatorial computational chemistry approach: application to Fischer-Tropsch synthesis</title>

Combinatorial Heterogeneous Catalysis—A New Path in an Old Field

Modeling benzene sorption and diffusion in a γAl2O3catalyst

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