The first-principles-based microkinetic simulation of the dry reforming of methane over Ru(0001)
02 Mar 2021-Catalysis Science & Technology (The Royal Society of Chemistry)-Vol. 11, Iss: 4, pp 1395-1406
TL;DR: In this paper, a density functional theory was used to study dry reforming and its related processes on the Ru(0001) surface, and the results showed that CO2 dissociation occurred mainly by direct dissociation and O* produced by CO 2 dissociation was the main oxidant of intermediates on the surface of Ru (0001).
About: This article is published in Catalysis Science & Technology.The article was published on 2021-03-02. It has received 18 citations till now. The article focuses on the topics: Carbon dioxide reforming & Steam reforming.
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TL;DR: In this paper, the progress in the development of non-precious catalytic materials has been discussed from a theoretical point of view, such as the interaction of reaction intermediates with particular crystal facets (typically active sites in the reaction), combined with electronic structure insights, directly influencing the kinetic behaviour of the catalyst system.
Abstract: It is worthwhile to invest in the development of CO2 reforming of methane, as it presents a promising alternative for transforming two global warming gases into a very versatile product such as syngas. A syngas rich feed gas presents extensive prospects for existing downstream industrial processes for producing valuable fuels and chemicals. The commercialization of the DRM process greatly depends upon the development of low cost, non-precious transition metal-based catalysts, to provide a desirable balance between catalytic activity and stability. In this review, the progress in the advancements of non-precious catalytic materials have been discussed from a theoretical point of view. A theoretical perspective gives an opportunity to gain fundamental information at the atomic level, such as the interaction of reaction intermediates with particular crystal facets (typically active sites in the reaction), combined with electronic structure insights, directly influencing the kinetic behaviour of the catalyst system. Theoretical insights into the DRM reaction mechanisms on non-precious Ni-based bimetallic and transition metal phosphide catalysts are extensively discussed, together with the mitigation mechanisms to avoid carbon deposition and catalyst deactivation under DRM reaction conditions. Prospects of future development of DRM are also provided, highlighting the importance of computational chemistry studies in the development of the next-generation advanced DRM catalysts.
24 citations
TL;DR: In this article, a review of the advances in the experimental and theoretical approaches for CO2 activation and conversion to C1 products via heterogeneous catalytic routes is presented, which can significantly pave the way to sustainably produce chemicals and fuels and mitigate the additional CO2 load.
12 citations
TL;DR: In this article, the authors performed density functional theory (DFT) calculation and micro-kinetic modeling to study the methanol synthesis from CO2 hydrogenation on indium-terminated In2O3(100), defective In2 O3(110), and In2 o3(111) surfaces.
9 citations
TL;DR: In this paper , the effect of the Ru particles' micro-morphology on the CO2 methanation was studied theoretically, and it was shown that the Ru nanoparticles with more fractions of five-coordinated Ru-Ru configurations would be beneficial for CO2 meta-hanation.
7 citations
References
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TL;DR: A simple derivation of a simple GGA is presented, in which all parameters (other than those in LSD) are fundamental constants, and only general features of the detailed construction underlying the Perdew-Wang 1991 (PW91) GGA are invoked.
Abstract: Generalized gradient approximations (GGA’s) for the exchange-correlation energy improve upon the local spin density (LSD) description of atoms, molecules, and solids. We present a simple derivation of a simple GGA, in which all parameters (other than those in LSD) are fundamental constants. Only general features of the detailed construction underlying the Perdew-Wang 1991 (PW91) GGA are invoked. Improvements over PW91 include an accurate description of the linear response of the uniform electron gas, correct behavior under uniform scaling, and a smoother potential. [S0031-9007(96)01479-2] PACS numbers: 71.15.Mb, 71.45.Gm Kohn-Sham density functional theory [1,2] is widely used for self-consistent-field electronic structure calculations of the ground-state properties of atoms, molecules, and solids. In this theory, only the exchange-correlation energy EXC › EX 1 EC as a functional of the electron spin densities n"srd and n#srd must be approximated. The most popular functionals have a form appropriate for slowly varying densities: the local spin density (LSD) approximation Z d 3 rn e unif
146,533 citations
IBM1
TL;DR: An approach for electronic structure calculations is described that generalizes both the pseudopotential method and the linear augmented-plane-wave (LAPW) method in a natural way and can be used to treat first-row and transition-metal elements with affordable effort and provides access to the full wave function.
Abstract: An approach for electronic structure calculations is described that generalizes both the pseudopotential method and the linear augmented-plane-wave (LAPW) method in a natural way. The method allows high-quality first-principles molecular-dynamics calculations to be performed using the original fictitious Lagrangian approach of Car and Parrinello. Like the LAPW method it can be used to treat first-row and transition-metal elements with affordable effort and provides access to the full wave function. The augmentation procedure is generalized in that partial-wave expansions are not determined by the value and the derivative of the envelope function at some muffin-tin radius, but rather by the overlap with localized projector functions. The pseudopotential approach based on generalized separable pseudopotentials can be regained by a simple approximation.
61,450 citations
TL;DR: In this paper, the formal relationship between US Vanderbilt-type pseudopotentials and Blochl's projector augmented wave (PAW) method is derived and the Hamilton operator, the forces, and the stress tensor are derived for this modified PAW functional.
Abstract: The formal relationship between ultrasoft (US) Vanderbilt-type pseudopotentials and Bl\"ochl's projector augmented wave (PAW) method is derived. It is shown that the total energy functional for US pseudopotentials can be obtained by linearization of two terms in a slightly modified PAW total energy functional. The Hamilton operator, the forces, and the stress tensor are derived for this modified PAW functional. A simple way to implement the PAW method in existing plane-wave codes supporting US pseudopotentials is pointed out. In addition, critical tests are presented to compare the accuracy and efficiency of the PAW and the US pseudopotential method with relaxed core all electron methods. These tests include small molecules $({\mathrm{H}}_{2}{,\mathrm{}\mathrm{H}}_{2}{\mathrm{O},\mathrm{}\mathrm{Li}}_{2}{,\mathrm{}\mathrm{N}}_{2}{,\mathrm{}\mathrm{F}}_{2}{,\mathrm{}\mathrm{BF}}_{3}{,\mathrm{}\mathrm{SiF}}_{4})$ and several bulk systems (diamond, Si, V, Li, Ca, ${\mathrm{CaF}}_{2},$ Fe, Co, Ni). Particular attention is paid to the bulk properties and magnetic energies of Fe, Co, and Ni.
57,691 citations
TL;DR: In this article, a method for generating sets of special points in the Brillouin zone which provides an efficient means of integrating periodic functions of the wave vector is given, where the integration can be over the entire zone or over specified portions thereof.
Abstract: A method is given for generating sets of special points in the Brillouin zone which provides an efficient means of integrating periodic functions of the wave vector. The integration can be over the entire Brillouin zone or over specified portions thereof. This method also has applications in spectral and density-of-state calculations. The relationships to the Chadi-Cohen and Gilat-Raubenheimer methods are indicated.
51,059 citations
TL;DR: A detailed description and comparison of algorithms for performing ab-initio quantum-mechanical calculations using pseudopotentials and a plane-wave basis set is presented in this article. But this is not a comparison of our algorithm with the one presented in this paper.
47,666 citations