<i>Ab initio</i>lattice dynamics and thermodynamics of<mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" display="inline"><mml:mrow><mml:msub><mml:mrow><mml:mtext>RuO</mml:mtext></mml:mrow><mml:mn>2</mml:mn></mml:msub><mml:mrow><mml:mo>(</mml:mo><mml:mrow><mml:mn>110</mml:mn></mml:mrow><mml:mo>)</mml:mo></mml:mrow></mml:mrow></mml:math>surfaces

Bohnen, K.‐P.; Heid, R.; Peña-Seaman, O. De la

doi:10.1103/physrevb.81.081405

Cited by 4 publications

(3 citation statements)

References 18 publications

(20 reference statements)

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“…The DFT calculated surface energies of the stoichiometric RuO 2 (110) surface is 71–90 meV/Å 2 . ,,, The other Ru–O bond lengths are between 1.90 Å and 2.03 Å. The structural parameters obtained by LEED and DFT agree quantitatively and the atomic geometry has been corroborated by several recent ab initio studies. ,, When removing the bridging O atoms, 2-fold under-coordinated Ru atoms (2f-cus Ru) are exposed (cf. Figure B).…”

Section: Atomic Scale Chemistry and Properties Of Single-crystalline ...supporting

confidence: 59%

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Surface Chemistry of Ruthenium Dioxide in Heterogeneous Catalysis and Electrocatalysis: From Fundamental to Applied Research

Over¹

2012

Chem. Rev.

616

643

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CONTENTS 1. Introduction 3357 2. Physicochemical Properties of Ruthenium Oxides 3358 3. Synthesis of RuO 2 3360 3.1. RuO 2 Single Crystals 3360 3.2. Polycrystalline RuO 2 3361 3.3. RuO 2 Thin Film Preparation 3361 3.4. Supported RuO 2 Nanoparticles 3362 3.5. Nanoscale RuO 2 in Diverse Forms 3362 3.6. Hydrous RuO 2 •xH 2 O 3363 3.7. RuO 2 -Based Electrode Coatings 3364 4. Complex Surface-Redox-Chemistry of Ruthenium 3364 4.1. Gas Phase Oxidation of Single Crystalline Ruthenium Surfaces 3364 4.1.1. Ru(0001) 3364 4.1.2. Ru(101̅ 0) 3368 4.2. Electro-oxidation of Ru(0001) 3369 4.3. Reduction of RuO 2 (110) 3369 4.3.1. Reduction by Hydrogen 3370 4.3.2. Reduction by CO 3370 4.3.3. Reduction by Methanol 3370 4.4. Reduction and Oxidation Behavior of Structurally More Complex Ru-Based Materials 3370 4.4.1. Polycrystalline Powder and Supported Nanoparticles of Ru and RuO 2 3370 4.4.2. Polycrystalline Ru Films 3370 4.5. Redox Surface Chemistry of other Platinum Group Metal Single Crystals 3371 4.5.1. Rhodium 3371 4.5.2. Palladium 3372 4.5.3. Platinum 3373 4.5.4. Iridium 3373 5. Atomic Scale Chemistry and Properties of Single-Crystalline RuO 2 Surfaces 3373 5.1. RuO 2 (110) Surface 3374 5.1.1. General (Atomic Scale) Properties of the Stoichiometric RuO 2 (110) Surfaces 3374 5.1.2. Chemical Properties of the RuO 2 (110) Surface: General Adsorption and Reaction Behavior 3376 5.1.3. Interaction of Oxygen with the RuO 2 (110) Surface 3378 5.1.4. Interaction of CO with the RuO 2 (110) Surface 3378 5.1.5. Interaction of H 2 with the RuO 2 (110) Surface 3379 5.1.6. Interaction of Water with RuO 2 (110) Surface 3379 5.1.7. Chemical Reduction of the RuO 2 (110) Surface 3380 5.2. RuO 2 (100) Surface 3380 5.2.1. General Properties of RuO 2 (100) 5.2.2. Adsorption Properties of RuO 2 (100) 5.3. Comparison with Rutile TiO 2 Single Crystals 6. Case Study: CO Oxidation over RuO 2 6.1. Scientific Background 6.2. CO Oxidation over RuO 2 (110): Reaction Mechanism 6.2.1. Experimental Evidence 6.2.2. Theoretical Modeling 6.3. CO Oxidation over RuO 2 Powder and Supported RuO 2 Catalysts: Bridging the Materials Gap 6.4. Deactivation and Poisoning of RuO 2 -Based Catalysts 6.4.1. Structural Deactivation 6.4.2. Poisoning of the Catalyst 6.5. Comparison with the Electrochemical Oxidation of CO at RuO 2 (100) Model Electrodes 6.6. CO Oxidation over RuO 2 : Concluding Remarks and Open Questions 7. Application of RuO 2 in Heterogeneous Catalysis 7.1. Low Temperature CO Oxidation 7.2. Water Production 7.3. Methanol Oxidation 7.4. Ammonia Oxidation and Related Reactions 7.5. HCl Oxidation: Deacon Process 8. Application of RuO 2 in Electrocatalysis 8.1. General Electrochemical Properties of RuO 2 8.2. Hydrogen Evolution Reaction (HER) 8.3. Chlor-Alkali Electrolysis: Dimensionally Stable Anode (DSA) 8.4. Oxygen Evolution Reaction (OER): Electrolysis of Water 8.5. Oxygen Reduction Reaction (ORR) 9. Energy-Related Applications of RuO 2 9.1. Super Capacitors 9.2. Fuel Cells 9.3. Rechargeable Li-Ion Batteries 9.4. Photocatalysis 10. Applications of RuO 2 in Ele...

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Section: Atomic Scale Chemistry and Properties Of Single-crystalline ...supporting

confidence: 59%

“…The structural parameters obtained by LEED and DFT agree quantitatively 236 and the atomic geometry has been corroborated by several recent ab initio studies. 51,375,376 When removing the bridging O atoms, 2-fold under-coordinated Ru atoms (2f-cus Ru) are exposed (cf. Figure 24B).…”

Section: Ruo 2 (110) Surfacementioning

confidence: 99%

Surface Chemistry of Ruthenium Dioxide in Heterogeneous Catalysis and Electrocatalysis: From Fundamental to Applied Research

Over¹

2012

Chem. Rev.

616

643

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“…These contributions would be needed to resolve, as a function of the temperature, an inversion of stability between two terminations separated by a few tens of meV. [52][53][54] The surface energies found in this work are well separated by a few hundreds of meV and these contributions can be safely neglected in a first approximation. Doing that, the surface grand potential has no more explicit temperature dependence but keeps an implicit one via the oxygen chemical potential.…”

Section: Ab Initio Atomistic Thermodynamicsmentioning

confidence: 85%

Thermodynamic stability of PuO2surfaces: Influence of electronic correlations

Jomard

Bottin

2011

Phys. Rev. B

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In this article, we performed accurate ab initio calculations in order to address the influence of electronic correlations on the surface stability of PuO 2 . Various terminations of the (100), (110), and (111) orientations were considered, among which some are polar. Standard density-functional theory (DFT), which is known to provide a poor description of the electronic structure of plutonium oxides, predicts an unexpected stabilization of the polar uncompensated terminations O 2 -(111) and Pu-(111). We show that this shortcoming is no longer observed when the more relevant PBE + U framework is used. The so-obtained better description of the strong electronic correlations leads to a destabilization of these two terminations, leaving only one stable surface, the O-(111) stoichiometric one. Beyond the surface stability, we show that the electronic structure is strongly affected since the PBE + U approach is able to render only a proper insulating behavior. This should have a strong effect on the surface reactivity of these systems and prevent the use of standard DFT.

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Alloys in catalysis: phase separation and surface segregation phenomena in response to the reactive environment

Zafeiratos

Piccinin

Teschner

2012

Catal. Sci. Technol.

213

182

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Alloys play a crucial role in several heterogeneous catalytic processes, and their applications are expected to rise rapidly. This is essentially related to the vast number of configurations and type of surface sites that multi-component materials can afford. It is well established that the chemical composition at the surface of an alloy usually differs from that in the bulk. This phenomenon, referred to as surface segregation, is largely controlled by the surface free energy. However, surface energy alone cannot safely predict the active surface state of a solid catalyst, since the contribution of other parameters such as size and support effects, as well as influence of the adsorbates, play a major role. This can lead to numerous surface configurations as for example over the length of a catalytic reactor, as the chemical potential of the gas phase changes continuously over the catalyst bed and hence different reactions may prevail at different catalyst bed segments. Thanks to the rapid improvement of the analytical surface science characterization techniques and theoretical methodologies, the potential effects induced by alloyed catalysts are better understood. For catalysis, the relevance of measurements performed on well-defined surfaces under idealized ultrahigh vacuum conditions has been questioned and studies in environments that closely resemble conditions of working alloy catalysts are needed. In this review we focus on experimental and theoretical studies related to in situ (operando) observations of surface segregation and phase separation phenomena taking place on the outermost surface layers of alloy catalysts. The combination of first principles theoretical treatment and in situ observation opens up new perspectives of designing alloy catalysts with tailored properties

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Ab initiolattice dynamics and thermodynamics ofRuO2(110)surfaces

Cited by 4 publications

References 18 publications

Surface Chemistry of Ruthenium Dioxide in Heterogeneous Catalysis and Electrocatalysis: From Fundamental to Applied Research

Surface Chemistry of Ruthenium Dioxide in Heterogeneous Catalysis and Electrocatalysis: From Fundamental to Applied Research

Thermodynamic stability of PuO2surfaces: Influence of electronic correlations

Alloys in catalysis: phase separation and surface segregation phenomena in response to the reactive environment

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