دانلود کتاب Direct Hydroxylation of Methane: Interplay Between Theory and Experiment

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Contents
Orbital Concept for Methane Activation
1 Introduction
2 C–H Bond Activation of Methane
2.1 Molecular Orbitals of Methane
2.2 Orbital Concept for Methane Activation Based on Second-Order Perturbation
2.3 Methane Activation by sMMO Model
3 Reaction Mechanism for the Direct Hydroxylation of Methane
3.1 Methane Hydroxylation by the FeO+ Species
3.2 Methane Hydroxylation Mechanisms by sMMO
3.3 Methane Hydroxylation Mechanisms by pMMO
4 Conclusions
References
Theoretical Study of the Direct Conversion of Methane by First-Row Transition-Metal Oxide Cations in the Gas Phase
1 Introduction
2 Electronic Structures of MO+ Ions
3 Potential-Energy Diagrams for the Methane-To-Methanol Conversion
3.1 Conversion of Methane to Methanol by ScO+, TiO+, and VO+
3.2 Conversion of Methane to Methanol by CrO+ and MnO+
3.3 Conversion of Methane to Methanol by FeO+, CoO+, and NiO+
3.4 Conversion of Methane to Methanol by CuO+
4 Surface Crossing and Spin–Orbit Coupling
4.1 Crossing Seams of Potential-Energy Surfaces
4.2 Spin–Orbit Coupling of Methane Conversion
5 Summary
References and Notes
Enzymatic Methane Hydroxylation: sMMO and pMMO
1 Experimental Background
2 History of Computational Approach
3 Key Factors in Determining Reactivity of MMOHQ Toward Methane
4 Proposed Mechanisms for the Methane to Methanol Conversion by MMOHQ
5 Details in Mechanisms for the Methane Hydroxylation by MMOHQ
5.1 Nonradical Mechanism
5.2 Radical Rebound Mechanism
5.3 Nonsynchronous Concerted Mechanism
6 Mechanism for Methane Hydroxylation on pMMO
7 Conclusions, Emerging Issues, and Challenges
References and Notes
Mechanistic Understanding of Methane Hydroxylation by Cu-Exchanged Zeolites
1 Introduction
2 Methane Hydroxylation by [Cu2(μ-O)]2+ and [Cu3(μ-O)3]2+ in Zeolites
2.1 Mechanism of C–H Activation
2.2 Mechanism of CH3OH Formation
3 Conclusion
References
Oxidative Activation of Metal-Exchanged Zeolite Catalysts for Methane Hydroxylation
1 Introduction
2 Oxidative Activation of Fe-Exchanged Zeolites
2.1 N2O Decomposition on FeII-ZSM-5
2.2 H2O2 Decomposition on [FeIII–(μO)2–FeIII]-ZSM-5
3 Oxidative Activation of Cu-Exchanged Zeolites
3.1 N2O Decomposition on 2CuI-ZSM-5
3.2 O2 Activation on 2[CuI2]-MOR and [CuIII2CuI(ΜO)]-MOR
4 Conclusion
References
Dynamics and Energetics of Methane on the Surfaces of Transition Metal Oxides
1 Introduction
2 Kinetics of Methane on Surface
2.1 Langmuir Model
2.2 Two Mechanisms: Direct Mechanism and Trapping-Mediated Mechanism
3 Energetics of Methane on Surface
3.1 How Strongly Methane Can be Adsorbed on the Surface?
3.2 PdO, IrO2, and RuO2
3.3 Adsorption of Methane on a Metal Oxide
3.4 C–H Bond Dissociation of Methane on a Metal Oxide Surface
4 Conclusions and Outlook
Appendix
References
Machine Learning Predictions of Adsorption Energies of CH4-Related Species
1 Introduction
2 Machine Learning Prediction of Adsorption Energies
2.1 DFT Calculations of Adsorption Energies
2.2 ML Methods
2.3 ML Prediction of Adsorption Energies
2.4 ML Prediction of ECH3–ECH2 Values for Methane Utilization
3 Conclusion
References
Theoretical Approach to Homogeneous Catalyst of Methane Hydroxylation: Collaboration with Computation and Experiment
1 Introduction
2 Computational Methods
3 Organometallic Approaches
4 Biomimetic Approaches
5 Theoretical Predictions for a Methane Hydroxylation Catalyst
6 Summary and Outlook
References