Practical principles of density functional theory for catalytic reaction simulations on metal surfaces – from theory to applications

Shan, Nannan; Zhou, Mingxia; Hanchett, Mary K.; Chen, Josephine; Liu, Bin

doi:10.1080/08927022.2017.1303687

Cited by 25 publications

(23 citation statements)

References 278 publications

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“…The supremacy of PdAg-catalysts over other compositions of the active metal phase has widely been demonstrated from experimental investigations but also by theoretical studies. As for many other reactions [99][100][101][102], density functional theory (DFT) calculations have been used to study the decomposition of FA. Huang et al reported a DFT study for the decomposition of FA over noble metals (Pt, Au, Pd, etc.)…”

Section: Theoretical Investigationsmentioning

confidence: 99%

Hydrogen Production from Formic Acid Attained by Bimetallic Heterogeneous PdAg Catalytic Systems

2019

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The production of H 2 from the so-called Liquid Organic Hydrogen Carriers (LOHC) has recently received great focus as an auspicious option to conventional hydrogen storage technologies. Among them, formic acid, the simplest carboxylic acid, has recently emerged as one of the most promising candidates. Catalysts based on Pd nanoparticles are the most fruitfully investigated, and, more specifically, excellent results have been achieved with bimetallic PdAg-based catalytic systems. The enhancement displayed by PdAg catalysts as compared to the monometallic counterpart is ascribed to several effects, such as the formation of electron-rich Pd species or the increased resistance against CO-poisoning. Aside from the features of the metal active phases, the properties of the selected support also play an important role in determining the final catalytic performance. Among them, the use of carbon materials has resulted in great interest by virtue of their outstanding properties and versatility. In the present review, some of the most representative investigations dealing with the design of high-performance PdAg bimetallic heterogeneous catalysts are summarised, paying attention to the impact of the features of the support in the final ability of the catalysts towards the production of H 2 from formic acid.Energies 2019, 12, 4027 2 of 27 fact, it is challenging not only for developed countries in which the living standard requires large energy supplies, but also for those developing countries that experience a high population growth.Among greenhouse gases, carbon dioxide (CO 2 ) is considered the most important because, even though its global warming potential (GWP) is much lower than that of other gases, the emissions of CO 2 are far more abundant. GWP parameter was developed to compare the global warming impacts of different gases and it is a measure of how much energy the emissions of 1 ton of a gas will absorb over a given period, relative to the emissions of 1 ton of CO 2 , which is used as the reference. Then, CO 2 has a GWP of 1 regardless of the time used, while GWP is 28-36 and 265-298 times that of CO 2 for methane (CH 4 ) and nitrous oxide (N 2 O), respectively [1]. Such considerations, that are nowadays central scientific and social concerns, have a long historical background within the research community. Arrhenius was among the first to hypothesise about the impact of CO 2 on the Earth's climate [2], but his hypothesis was overlooked until the 1950s [3]. Now, after more than half a century, there is not yet a chemical process able to efficiently clean the growing volumes of CO 2 in the atmosphere. Some interesting actions taken so far are related to the production of hydrocarbon fuels by recycling H 2 O and CO 2 with renewable energy sources or the CO 2 capture and sequestration (CCS) technology [4][5][6][7].In such energy and environmental context, the search for alternative carbon emission-free energy sources is required to avoid further disastrous consequences. Hydrogen (H 2 ), a carbon-free fuel, is consi...

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Section: Theoretical Investigationsmentioning

confidence: 99%

Hydrogen Production from Formic Acid Attained by Bimetallic Heterogeneous PdAg Catalytic Systems

2019

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“…The free energy change (

Δ G

), Equation (4), was calculated with the inclusion of the zero‐point energy (

Δ Z P E

) correction, and the entropic term (

T Δ S

) estimated from respective translational, rotational, and vibrational contributions . Vibrational frequencies were computed by assuming simple harmonic vibrations.…”

Section: Methodsmentioning

confidence: 99%

Manipulating the Geometric and Electronic Structures of Manganese Nitrides for Ammonia Synthesis

et al. 2020

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Manganese (Mn) nitrides are important nitrogen (N) carriers for small-scale intermittent ammonia (NH 3 ) synthesis. However, only 3~8 % of lattice N are converted into NH 3 . In this study, the geometric and electronic structures of well-defined Mn 4 N and Mn 2 N lattices were altered using transition metal heteroatoms (Cr, Fe, Co, Ni, Mo) to understand the driving force behind lattice N diffusion and extraction. Density Functional Theory (DFT) revealed that the binding of early hydrogenation product (NH) follows a linear relationship with lattice N over a wide range of close-packed surfaces. But, the binding of NH 2 and NH 3 are more sensitive to the geometric and electronic structures. Further, the chemical bonding can be quantitatively characterized with the covalency derived from Crystal Orbital Hamiltonian Population (COHP). In the Eley Rideal-Mars van Krevelan pathway, the overall NH 3 formation free energy ( DG NH 3 ) and lattice N diffusion barrier (E a ) are the respective thermodynamic and kinetic determining factors. Aided by a rate-determining step (RDS) model, Mn 4 N modified with Fe, Co, Ni single-atom dopants all show enhanced rates for NH 3 formation.[a] Dr.

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“…This work successfully aligns with the literature to conclude that the hydrogenation of CO is the limiting energy barrier for CO 2 electroreduction into CH 4 . Shan et al mention that it is contested whether this step involves the formation of HCO or COH [30]. The range of metals in this study cov- (Figure 23, top), the first six reactions are observed to be unfavorable for surfaces with weaker adsorption energies.…”

Section: Table 4 | Selected Ch 4 Oxidation Pathways For Sofc Anodesmentioning

confidence: 59%

“…This script discovers BEP correlations for the reactions in the model empirically. Necessary data were taken from several sources: [1,[6][7][8][9]13,18,23,24,30,42,43,45,55,58,60,65,[67][68][69][70][71][72][73][74][75][76]78,85].…”

Section: Cantera Solid Oxide Fuel Cell Modelingmentioning

confidence: 99%

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Development of RMG-Electrocat for electrochemical kinetic analysis of solid oxide fuel cells

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Practical principles of density functional theory for catalytic reaction simulations on metal surfaces – from theory to applications

Cited by 25 publications

References 278 publications

Hydrogen Production from Formic Acid Attained by Bimetallic Heterogeneous PdAg Catalytic Systems

Hydrogen Production from Formic Acid Attained by Bimetallic Heterogeneous PdAg Catalytic Systems

Manipulating the Geometric and Electronic Structures of Manganese Nitrides for Ammonia Synthesis

Development of RMG-Electrocat for electrochemical kinetic analysis of solid oxide fuel cells

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