Theoretical Approaches to Excited-State-Related Phenomena in Oxide Surfaces

Sousa, Carmen; Tosoni, Sergio; Illas, Francesc

doi:10.1021/cr300228z

Cited by 86 publications

(100 citation statements)

References 621 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…U methods. The PBE results yields similar free energy diagrams and ORR activities for LaMnO 3 and LaFeO 3 , while the PBE ? U data suggest that LaCrO 3 has the lowest ORR overpotential.…”

Section: The Thermochemistry Problemmentioning

confidence: 68%

“…The modeling and theoretical description of processes occurring at the surface of a solid catalyst are expected to increase in importance also due to the increasing computational power. To this end, new methods and approaches are continuously being developed and applied to problems related to heterogeneous catalysis by oxide surfaces [3,4]. While theoretical chemists have developed over the past 50 years a wide set of computational approaches to study with extremely high accuracy molecular reactions (from configuration interaction [5] to coupled cluster [6] methods and quantum Monte Carlo [7] ), when one deals with reactions occurring at solid surfaces the method of choice becomes density functional theory (DFT).…”

Section: Introductionmentioning

confidence: 99%

See 1 more Smart Citation

First Principles Calculations on Oxide-Based Heterogeneous Catalysts and Photocatalysts: Problems and Advances

Pacchioni

2014

Catal Lett

View full text Add to dashboard Cite

Density functional theory (DFT) has become an essential complement of experiments to interpret, rationalize, and understand structures, spectroscopic data, microscopy analyses, etc. of relevance in heterogeneous catalysis and photocatalysis. However, one of the major goals of theory in catalysis remains the prediction of reaction enthalpies and entropies, of transition state structures, and the identification of reaction mechanisms. While accurate theoretical methods are currently available to study the thermochemistry of molecular systems, this is much less so when reactions involve solid surfaces and in particular oxide materials. The problem stems from the approximate nature of the exchange-correlation functionals used in all DFT approaches. Attempts to improve the accuracy of reaction energies is at the core of the efforts made in the past 30 years to generate new functionals. In this review we will discuss some recent advances in the theoretical description of oxides and their surfaces in heterogeneous catalysis and photocatalysis. In particular, we will focus on two problems: (1) the determination of an oxide band gap and the proper alignment of the occupied and unoccupied levels with respect to the vacuum level, an aspect relevant for the red-ox properties of the material, and (2) the calculation of reaction energies at oxide surfaces. To this end, we will discuss and comment on the performance of current implementations of exchange-correlation functionals (standard GGA, GGA?U, hybrid functionals, meta-GGA, etc.) or alternative approaches (like the quasiparticle GW method), in predicting band alignment and chemical reactivity at oxide surfaces. The role of dispersion forces will be also briefly discussed.

show abstract

“…U methods. The PBE results yields similar free energy diagrams and ORR activities for LaMnO 3 and LaFeO 3 , while the PBE ? U data suggest that LaCrO 3 has the lowest ORR overpotential.…”

Section: The Thermochemistry Problemmentioning

confidence: 68%

Section: Introductionmentioning

confidence: 99%

First Principles Calculations on Oxide-Based Heterogeneous Catalysts and Photocatalysts: Problems and Advances

Pacchioni

2014

Catal Lett

View full text Add to dashboard Cite

show abstract

“…The description of chemical catalytic reactions occurring at the surface of a solid catalyst has led to many studies by chemists and physicists all over the world since the 1960s, favoured by the huge increase of computational power [28][29][30]. A wide set of theoretical approaches has been developed from configuration interactions [31] to coupled cluster methods [32] and quantum chemistry Monte Carlo [33].…”

Section: Theoretical Approach and Calculations On Metal Oxide-based Hmentioning

confidence: 99%

Heterogeneous Catalysis on Metal Oxides

2017

View full text Add to dashboard Cite

This review article contains a reminder of the fundamentals of heterogeneous catalysis and a description of the main domains of heterogeneous catalysis and main families of metal oxide catalysts, which cover acid-base reactions, selective partial oxidation reactions, total oxidation reactions, depollution, biomass conversion, green chemistry and photocatalysis. Metal oxide catalysts are essential components in most refining and petrochemical processes. These catalysts are also critical to improving environmental quality. This paper attempts to review the major current industrial applications of supported and unsupported metal oxide catalysts. Viewpoints for understanding the catalysts' action are given, while applications and several case studies from academia and industry are given. Emphases are on catalyst description from synthesis to reaction conditions, on main industrial applications in the different domains and on views for the future, mainly regulated by environmental issues. Following a review of the major types of metal oxide catalysts and the processes that use these catalysts, this paper considers current and prospective major applications, where recent advances in the science of metal oxide catalysts have major economic and environmental impacts.

show abstract

“…A typical DSSC consists of the wide band gap TiO 2 semiconductor, the dye is employed to absorb light radiation, and the photo-excited electrons are subsequently transferred to the TiO 2 [8]. The fast interfacial electron transfer between the dye and TiO 2 could, in principle, minimize the loss of the utilized photon energy as heat through the electron-phonon relaxation pathway.…”

Section: The Electronic Band Structure Of Titanium Dioxidementioning

confidence: 99%

Theoretical Studies of Titanium Dioxide for Dye-Sensitized Solar Cell and Photocatalytic Reaction

Bai¹,

Li²,

Zhang³

2017

Titanium Dioxide

View full text Add to dashboard Cite

This chapter aims to provide researchers in the field of photovoltaics with the valuable information and knowledge needed to understand the physics and modeling of titanium dioxide for dye-sensitized solar cell and photocatalytic reaction. The electronic band structure of titanium dioxide, the treatment of the excited state of titanium dioxide, the molecular dynamics and ultrafast quantum dynamics simulations, and several promising photocatalytic schemes and important considerations for theoretical study are addressed and reviewed. The advanced computational strategies and methods and optimized models to achieve exact simulation are described and discussed, including first principle calculations, nonadiabatic molecular and quantum dynamics, wave function propagation methods, and surface construction of titanium dioxide. These advanced theoretical investigations have become highly active areas of photovoltaics research and powerful tools for the supplement and prediction of related experimental efforts.

show abstract

Theoretical Approaches to Excited-State-Related Phenomena in Oxide Surfaces

Cited by 86 publications

References 621 publications

First Principles Calculations on Oxide-Based Heterogeneous Catalysts and Photocatalysts: Problems and Advances

First Principles Calculations on Oxide-Based Heterogeneous Catalysts and Photocatalysts: Problems and Advances

Heterogeneous Catalysis on Metal Oxides

Theoretical Studies of Titanium Dioxide for Dye-Sensitized Solar Cell and Photocatalytic Reaction

Contact Info

Product

Resources

About