Recent Advances in Understanding CO Oxidation on Gold Nanoparticles Using Density Functional Theory

Chen, Y.; Crawford, Paul; Hu, P.

doi:10.1007/s10562-007-9200-z

Cited by 68 publications

(36 citation statements)

References 83 publications

(109 reference statements)

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“…Recent studies on oxide supported Au and Pt catalysts for the WGS reaction indicate that the role of the dispersed metallic phase is not restricted to providing sites for CO adsorption, but that it furthermore affects the reducibility of the support, thereby creating new active sites for the WGS reaction. 71,76 We have investigated this hypothesis by calculating the oxygen vacancy formation energies ͑E vf ͒ in the presence and absence of metal clusters. We used the following equation to calculate E vf in the presence of metal clusters:…”

Section: Reducibility Of the Tio 2 Surfacementioning

confidence: 99%

Modeling the noble metal/TiO2 (110) interface with hybrid DFT functionals: A periodic electrostatic embedded cluster model study

Ammal

Heyden

2010

The Journal of Chemical Physics

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Articles you may be interested inEmbedded cluster density functional and second-order Møller-Plesset perturbation theory study on the adsorption of N2 on the rutile (110) This article is copyrighted as indicated in the article. Reuse of AIP content is subject to the terms at: http://scitation. The interaction of Au n and Pt n ͑n=2,3͒ clusters with the stoichiometric and partially reduced rutile TiO 2 ͑110͒ surfaces has been investigated using periodic slab and periodic electrostatic embedded cluster models. Compared to Au clusters, Pt clusters interact strongly with both stoichiometric and reduced TiO 2 ͑110͒ surfaces and are able to enhance the reducibility of the TiO 2 ͑110͒ surface, i.e., reduce the oxygen vacancy formation energy. The focus of this study is the effect of Hartree-Fock exchange on the description of the strength of chemical bonds at the interface of Au/Pt clusters and the TiO 2 ͑110͒ surface. Hartree-Fock exchange helps describing the changes in the electronic structures due to metal cluster adsorption as well as their effect on the reducibility of the TiO 2 surface. Finally, the performance of periodic embedded cluster models has been assessed by calculating the Pt adsorption and oxygen vacancy formation energies. Cluster models, together with hybrid PBE0 functional, are able to efficiently compute reasonable electronic structures of the reduced TiO 2 surface and predict charge localization at surface oxygen vacancies, in agreement with the experimental data, that significantly affect computed adsorption and reaction energies.

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Section: Reducibility Of the Tio 2 Surfacementioning

confidence: 99%

Modeling the noble metal/TiO2 (110) interface with hybrid DFT functionals: A periodic electrostatic embedded cluster model study

Ammal

Heyden

2010

The Journal of Chemical Physics

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“…Unfortunately, modeling complex, disordered systems presents a major challenge for theoretical treatment because a specific starting structure must be assumed. Indeed, previous theoretical studies of CO oxidation on Au surfaces have used static, zero-temperature DFT calculations [56,89,[141][142][143][144][145][146][147][148][149][150][151][152][153][154][155]. A popular theoretical technique used for modeling dynamic events on surfaces is kinetic Monte Carlo (kMC) [156], but it presumes prior complete knowledge of events important to the dynamics of the system.…”

Section: Impact Of Gold Release On Reactivity: Aimd Simulations Of O mentioning

confidence: 99%

Insights from Theory on the Relationship Between Surface Reactivity and Gold Atom Release

2010

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Density functional theory, informed by experimental studies, is used to investigate the interplay of surface morphology, the adsorption site of reactants, the nature of the interaction between adsorbates and the surface, the potential energy landscape for adsorbates on the surface, adsorbate coverage, temperature, and the dynamic evolution of these factors during adsorption and reaction. We summarize our current understanding of Au atom release on the (111) surface and the corresponding effects on adsorption and reactivity. Gold was selected for these investigations because of the recent intense interest in the activity of gold nanoparticles for several important catalytic reactions. Fundamental experimental studies on Au single-crystal surfaces have established that atomic O is extremely active for oxidation of CO and olefins, that the local bonding of O is an important factor in determining the reactivity and selectivity for oxidation, and that Au atom release is induced by electronegative adsorbates, such as O, Cl, and S. These experimental results guided our theoretical studies. Density functional theory is an extremely useful tool since it evaluates the energetics associated with the incorporation of gold into the adsorbate layer, while providing fundamental physical insight into the underlying cause of gold incorporation. We use our results from static DFT calculations along with ab initio molecular dynamics simulations to understand the effect of surface morphology on the activity of gold for CO oxidation. Our investigation of Au atom release and incorporation induced by electronegative atoms clearly illustrates the importance of using experiments in combination with theory to establish the importance of and the underlying reasons for metal atom release and the affect on bonding and reactivity.

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“…These results are in agreement with previous investigations, which have shown that metal particles can stabilize the adsorption of the molecule on the surface. [43][44][45][46] For example, Carrasco et al [47] showed that CO prefers to bind to the Ni 1 /CeO 2 (111) surface, rather than on the pristine CeO 2 (111) surface, in a similar configuration as the one presented in Figure 3.…”

Section: Accepted Manuscriptmentioning

confidence: 81%

Density functional theory study of the interaction of H2O, CO2 and CO with the ZrO2 (111), Ni/ZrO2 (111), YSZ (111) and Ni/YSZ (111) surfaces

2016

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Density functional theory study of the interaction of H 2 O, CO 2 and CO with the ZrO 2 (111), Ni/ZrO 2 (111), YSZ (111) and Ni/YSZ (111) surfaces AbstractThe triple phase boundary (TPB), where the gas phase, Ni particles and the yttria-stabilised zirconia (YSZ) surface meet, plays a significant role in the performance of solid oxide fuel cells (SOFC). Indeed, the key reactions take place at the TPB, where molecules such as H 2 O, CO 2 and CO interact and react. We have systematically studied the interaction of H 2 O, CO 2 and CO with the dominant surfaces of four materials that are relevant to SOFC, i.e. ZrO 2 (111), Ni/ZrO 2 (111), YSZ(111) and Ni/YSZ(111) of cubic ZrO 2 stabilized with 9% of yttria (Y 2 O 3 ). The study employed spin polarized density functional theory (DFT), taking into account the long-range dispersion forces. We have investigated up to five initial adsorption sites for the three molecules and have identified the geometries and electronic structures of the most stable adsorption configurations. We have also analysed the vibrational modes of the three molecules in the gas phase and compared them with the adsorbed molecules. A decrease of the wavenumbers of the vibrational modes for the three adsorbed molecules was observed, confirming the influence of the surface on the molecules' intra-molecular bonds. These results are in line with the important role of Ni in this system, in particular for the CO adsorption and activation.

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Recent Advances in Understanding CO Oxidation on Gold Nanoparticles Using Density Functional Theory

Cited by 68 publications

References 83 publications

Modeling the noble metal/TiO2 (110) interface with hybrid DFT functionals: A periodic electrostatic embedded cluster model study

Modeling the noble metal/TiO2 (110) interface with hybrid DFT functionals: A periodic electrostatic embedded cluster model study

Insights from Theory on the Relationship Between Surface Reactivity and Gold Atom Release

Density functional theory study of the interaction of H2O, CO2 and CO with the ZrO2 (111), Ni/ZrO2 (111), YSZ (111) and Ni/YSZ (111) surfaces

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