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Quantum Chemical Study on Two-State Reactivity of Small Molecules Activated by Transition Metal

Author: WangQingYun
Tutor: WangYongCheng
School: Northwest Normal University
Course: Physical and chemical
Keywords: Two-state reaction Reaction Mechanism Potential energy surfaces crossing MECP SOC
CLC: O643.1
Type: Master's thesis
Year: 2009
Downloads: 110
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Abstract


In recent years, people found in the study transition metal vapor phase reaction the reactant (or intermediate) of the ground state and the product of the ground state has a different spin states. That does not comply with the spin conservation law. Such a reaction process involving two or more energy surface, the reaction is always maintained at a low energy of the potential energy surface, such reactions are usually referred to as \However, due to the restrictions of the experimental conditions and the impact of the law of conservation of spin, the spin-flip caused by changes in spin state of the phenomenon in the reaction is often overlooked. Until 1994, with the development of high-tech experimental means, during the reaction people monitored the class reaction indeed contrary to the spin conservation law, potential energy surface of the cross is a two-state reaction of the statement of the fundamental mechanisms was only people slowly to accept. In this paper, based on the principle of two-state reaction (TSR), refer to the B (o | ¨) the hme Schwarz and Schr (o | ¨) der et al of the experimental observations, using density functional theory (density functional theory, DFT) calculations cation of some transition metal ions and transition metal oxides CO keys and the reaction mechanism of CH bond activation of small molecules NO key depth theoretical study. The text is divided into four chapters. The first chapter gives an overview of the ab initio theoretical basis, applications, limitations, and error correction method and the two-state reaction theory of progress and research status. The second chapter briefly describes the basic theory, including the potential energy surface intersects with disjoint rules, transition state theory, spin - orbit coupling theory. The first two chapters are mainly summarizes the theoretical background and theoretical basis of this work, our study provides a reliable quantum chemical methods. Chapter III, Chapter IV, we were selected after the sixth cycle of transition metal ions Pt catalytic N 2 O and CO reaction, the reaction system and the fourth cycle early transition metal dioxide cations CrO 2 C 2 H 6 reaction system as the research object, focuses wins the oxygen capacity of the post-transition metal ions on the activation of the NO bond and metal ions in different spin states, as well as transition metal dioxide cations CH bond activation of the two-state reactivity (TSR) conducted in-depth research. In the course of the study, first, we primarily use charge-transfer, the natural bond orbital (NBO) analysis and molecular orbital theory in combination with other analytical methods discussed initial reaction complexes as well as the formation of the transition state, nature. And reaction path to do a simple description of the microscopic mechanism of the reaction at a glance. Next, on the basis of the obtained reaction path, first with Hammond assumptions push the approximate location of the potential energy surfaces crossing, i.e. in a spin states in the further use of the vertical excitation Yoshizaw et al intrinsic reaction coordinate single point method of IRC reaction coordinate corresponding point on the configuration, the configuration is calculated single-point energy in the other spin states, spin potential energy surface of the potential energy curves of the IRC reaction coordinate projection surface in another spin momentum cross point (CP) to find the approximate energy spin states IRC curve can surface intersects with another spin momentum and continue to be used to find the intersection Harvery et al mathematical algorithm in two different electronic trend surface cross sewn on to find the minimum energy reaction hypersurface crossing point (MECP), and discuss its impact for the entire reaction efficiency. Finally, we chose this intersection of representatives to discuss the spin-flip behavior, the study of the frontier molecular orbital and spin - orbit coupling (SOC) Crossing points to analyze \optimum reaction channel.

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CLC: > Mathematical sciences and chemical > Chemistry > Physical Chemistry ( theoretical chemistry ),chemical physics > Chemical kinetics,catalysis > Chemical kinetics
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