A kinetic modeling approach to the design of catalysts: formulation of a catalyst design advisory program

Dumesic, James A.; Milligan, Brian; Greppi, L.A.; Balse, V.R.; Sarnowski, K.T.; Beall, Charles E.; Kataoka, Takuo; Rudd, Dale F.; Arellano-Treviño, Martha A.

doi:10.1021/ie00067a022

Cited by 53 publications

(26 citation statements)

References 4 publications

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“…One of the earliest works on theoretical catalyst design can be attributed to [2], who proposed a systematic catalyst design framework based on reaction mechanism analysis and quantum chemical calculation. The framework is modified and updated herein.…”

Section: First-principles Catalyst Designmentioning

confidence: 99%

Computational design of heterogeneous catalysts and gas separation materials for advanced chemical processing

Shi

Zhou

2020

Front. Chem. Sci. Eng.

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Functional materials are widely used in chemical industry in order to reduce the process cost while simultaneously increase the product quality. Considering their significant effects, systematic methods for the optimal selection and design of materials are essential. The conventional synthesis-and-test method for materials development is inefficient and costly. Additionally, the performance of the resulting materials is usually limited by the designer’s expertise. During the past few decades, computational methods have been significantly developed and they now become a very important tool for the optimal design of functional materials for various chemical processes. This article selectively focuses on two important process functional materials, namely heterogeneous catalyst and gas separation agent. Theoretical methods and representative works for computational screening and design of these materials are reviewed.

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Section: First-principles Catalyst Designmentioning

confidence: 99%

Computational design of heterogeneous catalysts and gas separation materials for advanced chemical processing

Shi

Zhou

2020

Front. Chem. Sci. Eng.

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“…9 and 13 have been removed. The reduced descriptions of (9) and (13) can then be combined, Eq. 17, and reorganized to solve for DS, Eq.…”

Section: R5diagðkþ3wmentioning

confidence: 99%

“…The mass balances are solved for a given set of conditions (T, P's) under the assumption that in a snapshot picture of the system, the concentration of adsorbate species are constant with respect to time; this is referred to as the pseudo steady-state approximation (PSSA). [11][12][13] Initial reactant and product concentrations are predefined at each condition for the calculation of instantaneous reaction rates at an exact location in a plug flow reactor operating at steady state, or the reaction rate at a given moment in an inherently transient batch reactor. Activation barriers, E a and frequency factors, A, associated with each elementary step are estimated via DFT calculations or through surface science approaches, such as microcalorimetry, thermal desorption spectroscopy, and vibrational spectroscopy.…”

Section: Introductionmentioning

confidence: 99%

A general and robust approach for defining and solving microkinetic catalytic systems

Gusmão

Christopher

2014

AIChE Journal

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Recent approaches for the rational design of heterogeneous catalysts have relied on first-principles-based microkinetic modeling to efficiently screen large phase spaces of catalytic materials for optimal activity and selectivity. Microkinetic modeling allows the calculation of catalytic rate and selectivity under a given set of conditions without a priori assumptions of rate or selectivity controlling steps by simultaneously solving nonlinear algebraic equations comprising species mass balances bound by the pseudo steady-state approximation. We introduce a general approach to define and solve microkinetic systems that relies solely on its stoichiometric matrix and kinetic parameters of considered reaction steps. Our approach relies on linearization of the microkinetic system, enabling analytical calculation of system derivatives for use in quasi-Newton solution schemes that exhibit excellent robustness and efficiency with minimal dependence on initial conditions.To develop a general approach for solving complex microkinetic systems, we start by defining all species in the system as S j 's rather than p j 's and h j 's. The rate equations Scheme 1. Three-step catalytic mechanism. Scheme 2. Reactions rate equations.

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“…This seems even more imperative as the field becomes more interdisciplinary, since specialists with different backgrounds working in catalysis must know more than that provided by the limits of their traditional training. Hybrid systems that use heuristics to describe those phenomena that cannot be modeled explicitly and rigorous numeric models for those phenomena that are deterministic may be particularly useful and important ( Dumesic et al, 1987;Banares-Alcantara et al, 1987;Kito et al, 1984). In other disciplines heuristics and deterministic models are combined quite satisfactorily to describe real problems that are too complex to handle ab initio.…”

Section: 416mentioning

confidence: 99%

“…The inputfrom surfacescience to micro-kineticshas made it meaningfulto solve the steady state rate equations, which is possible with modern computer techniques ( Dumesic et al, 1987;Stewart et al, 1993). Micro-kinetics analysis (Dumesic et al, 1993b) of various reaction sequences is a useful tool to cbmbine the kinetic data with information from related kinetic studies(TPD, tracer studies, etc.)…”

Section: T Nh3 + N Ni-i_ (1) Fast (6) No + Ni-i3-* Product + (2) Slowmentioning

confidence: 99%

Assessment of research needs for advanced heterogeneous catalysts for energy applications. Final report: Volume 2, Topic reports

Mills¹

1994

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This report assesses the direction, technical content, and priority of research needs judged to provide the best chance of yielding new and improved heterogeneous catalysts for energy related applications over a period of 5-20 years. It addresses issues of energy conservation, alternate fuels and feedstocks, and the economics and applications that could alleviate pollution from energy processes. Recommended goals are defined in three major, closely-linked research thrusts: I. CATALYTIC SCIENCE --Establish a scientific knowledge of essential catalyst structure/performance relationships and work toward developing the ability to predict the catalytic capabilities of novel materials. II. ENVIRONMENTAL PROTECTION BY CATALYSIS --Prevent pollution by developing economical processes that are free of pollutant formation. Diminish pollution by achieving higher selectivity in fuels and chemicals manufacture and by new and improved catalytic processes for the removal of pollutants. III. INDUSTRIAL CATALYTIC APPLICATIONS --Develop energy-saving, environmentally benign processes for manufacture of liquid fuels and commodity chemicals based on domestic natural gas, biomass, and coal. Emphasize research on synthesis gas (CO + H2) production and conversion, oxidation catalysis, new methods of hydrogen production, and the synthesis of novel materials for catalytic applications.This study was conducted by an eleven-member panel of experts from industry and academia, including one each from Japan and Europe. Discussions were held with a wide variety of authorities, supplementing an intensive review of technical literature. Panel conclusions were assisted by critical peer reviews.There is a high level of confidence that the research proposed can provide catalytic technology which will achieve major economic and environmental improvements in energy applications.Volume I provides a comprehensive Executive Summary, including Research Recommendations. Volume II first presents an in-depth overview of the role of catalysis in future energy technology in chapter 1. Then current catalytic research is critically reviewed and research recommended in eight topic chapters: 2.

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A kinetic modeling approach to the design of catalysts: formulation of a catalyst design advisory program

Abstract: There are five carbon atoms in this molecule, so Nc = 5. By use of eq 4, the upper flammability limit is estimated to be 11.4 vol %. Sax (1984) reported an experimental value of 9.0 vol %.

Cited by 53 publications

References 4 publications

Computational design of heterogeneous catalysts and gas separation materials for advanced chemical processing

Computational design of heterogeneous catalysts and gas separation materials for advanced chemical processing

A general and robust approach for defining and solving microkinetic catalytic systems

Assessment of research needs for advanced heterogeneous catalysts for energy applications. Final report: Volume 2, Topic reports

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