Possibility of designing catalysts beyond the traditional volcano curve: a theoretical framework for multi-phase surfaces

Phys. Chem. Chem. Phys.

2017

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The relation between surface structure and adsorption energy of adsorbate is of great importance in heterogeneous catalysis. Based on density functional theory calculations, we propose an explicit equation with three chemically meaningful terms, namely the bonding contribution equation, to quantitatively account the surface structures and the adsorption energies. Successful predictions of oxygen adsorption energies on complex alloy surfaces containing up to 4 components are demonstrated, and the generality of this equation is also tested using different surface sizes and other adsorbates. This work not only may offer a powerful tool to understand the structureadsorption relation, but also may be used to inversely design novel catalysts.

Section: Resultsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Formulating the bonding contribution equation in heterogeneous catalysis: a quantitative description between the surface structure and adsorption energy

Phys. Chem. Chem. Phys.

2017

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“…For the modelling of platinum on tin oxide, we used a global optimization method, namely the particle swarm optimization (PSO), to obtain the most stable structures of cluster-oxide structures. Comparing to some previous modelling of bi-component systems, [43,44] this global optimization algorithm can provide a much more realistic and accurate illustration of cluster and interface structures, which may be of great importance in the selective hydrogenation of benzoic acid. In this work, the PSO were carried out using the CALYPSO code, [45][46][47] which is a power tool to get the stable structures at given external conditions.…”

Section: Hydrogenation Reactionsmentioning

confidence: 99%

Hydrogenation of benzoic acid to benzyl alcohol over Pt/SnO2

Chen

Applied Catalysis A: General

Daly

et al. 2020

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This is a PDF file of an article that has undergone enhancements after acceptance, such as the addition of a cover page and metadata, and formatting for readability, but it is not yet the definitive version of record. This version will undergo additional copyediting, typesetting and review before it is published in its final form, but we are providing this version to give early visibility of the article. Please note that, during the production process, errors may be discovered which could affect the content, and all legal disclaimers that apply to the journal pertain.

“…33 They showed that with multiphase catalysts, traditional constraints of the reaction rate would be broken, which provides a new idea for designing catalysts with high efficiency. The concepts of microkinetics and the volcano curve will be discussed in detail in the following sections (Figure (a)-(d) is reprinted from Refs 16,26,30,32 with permission from the American Association for the Advancement of Science, Nature Publishing Group, Springer, and the Royal Society of Chemistry, respectively).…”

Section: Box 1 Advances and Latest Computational Techniques For The Rmentioning

confidence: 99%

Theory and applications of surface micro‐kinetics in the rational design of catalysts using density functional theory calculations

Mao

2017

WIREs Comput Mol Sci

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Rational design of catalysts has long been an important and challenging goal in heterogeneous catalysis. To achieve this target, density functional theory (DFT) calculations and micro‐kinetics are two of the cornerstones. The DFT calculations make it possible to obtain microscopic properties of catalytic systems by computational simulations, and the micro‐kinetic modeling of surface reactions provides a tool to link quantum‐chemical data with macroscopic behaviors of the systems. In this review, we focus on the basic concepts and latest theoretical progresses of strategies for the catalysts design, including Brønsted−Evans−Polanyi relation, the volcano curve, and the activity window. Among the progresses, the theory of chemical potential kinetics in heterogeneous catalysis and its implications on catalysts design, which was developed by our group, are described in detail with extensive derivations. Furthermore, the applications of this method on screening low‐cost counter electrodes for dye‐sensitized solar cells are presented with experimental evidences. WIREs Comput Mol Sci 2017, 7:e1321. doi: 10.1002/wcms.1321 This article is categorized under: Structure and Mechanism > Reaction Mechanisms and Catalysis Theoretical and Physical Chemistry > Reaction Dynamics and Kinetics