Artificial Force-Induced Reaction Method for Systematic Elucidation of Mechanism and Selectivity in Organometallic Reactions

Hatanaka, Miho; Yoshimura, Takayoshi; Maeda, Satoshi

doi:10.1007/3418_2020_51

Cited by 11 publications

(14 citation statements)

References 90 publications

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“…This showed that the entire reaction path network was essential in explaining the enantioselectivity of that reaction. These results are discussed in more detail in our very recent review article specifically focusing on organometallic catalysis 61 …”

Section: Application Examplesmentioning

confidence: 88%

“…In particular, it succeeded in clarifying the entire catalytic cycle of an organometallic catalytic reaction without using any assumption on its reaction mechanism 60 . To date, the reaction mechanisms of many organocatalytic and organometallic catalytic reactions have been elucidated by the AFIR method 4,61 . AFIR would also be the most versatile automated path search method.…”

Section: Introductionmentioning

confidence: 99%

“…60 To date, the reaction mechanisms of many organocatalytic and organometallic catalytic reactions have been elucidated by the AFIR method. 4,61 AFIR would also be the most versatile automated path search method. It has been successfully applied to chemical transformations of various kinds such as photoreaction, [62][63][64][65][66] enzyme reaction, [67][68][69] crystal phase transition, [70][71][72][73] surface reaction, 74,75 and carbon material synthesis reaction.…”

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confidence: 99%

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Exploring paths of chemical transformations in molecular and periodic systems: An approach utilizing force

Maeda

Harabuchi

2021

WIREs Comput Mol Sci

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This article provides an overview on an automated reaction path search method called artificial force induced reaction (AFIR). The AFIR method induces various chemical transformations by applying force between pairs of fragments in a system. By pushing fragments from their various mutual orientations or by applying force between various fragment pairs using the AFIR method, many reaction paths can be explored systematically. In this article, the basic ideas and several different implementations are introduced first. Then, its thoroughness in the automated reaction path search is discussed with its applications to two small molecules. In the later part, its versatility is shown with discussing some previous application examples to organic reaction, organometallic catalysis, photoreaction, surface reaction, phase transition, and enzyme reaction. In addition, an attempt of predicting an idea of new synthesis method from scratch on the basis of the concept quantum chemistry‐aided retrosynthetic analysis (QCaRA) is presented, where the AFIR method was used as a reaction path search engine in QCaRA. Finally, future outlook and a comment on the GRRM program in which the AFIR method is available are given. This article is categorized under: Structure and Mechanism > Reaction Mechanisms and Catalysis Theoretical and Physical Chemistry > Reaction Dynamics and Kinetics

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Section: Application Examplesmentioning

confidence: 88%

Section: Introductionmentioning

confidence: 99%

mentioning

confidence: 99%

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Exploring paths of chemical transformations in molecular and periodic systems: An approach utilizing force

Maeda

Harabuchi

2021

WIREs Comput Mol Sci

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“…The emergence, in the last years, of the automated reaction path methods, promises to revolutionize the way of exploring the PES. With these methods, which have been successfully applied to organometallic reactions, [48][49][50] an unbiased exploration of the full PES can be performed. They do not only allow exploration of multiple reaction paths accounting for product selectivity in connection with microkinetic models but also pave the way for the discovery of unexpected reactions in the full potential energy surface of the system.…”

Section: Designing Catalysts and Discovering New Reactionsmentioning

confidence: 99%

Computational Organometallic Catalysis: Where We Are, Where We Are Going

Lledós

2021

Eur J Inorg Chem

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Dedicated to Professor Joan Bertran, who opened the doors to the quantum world for me, on the occasion of his 90th birthday This essay gives my personal perspective of the current stage of computational methods applied to modeling organometallic catalysis, as well as the new directions the field is taking. The first part of the essay deals with what I consider the state-ofthe-art to build up energy profiles, regarding both chemical and computational models. With a proper choice of the chemical model and computational methods, quantum mechanical calculations are nowadays able to provide accurate energy profiles of organometallic reactions in solution involving closed-shell species. However, in most cases they are still used to "predict the past", providing after-the-fact explanations and missing out the full potential of contemporary simulation techniques. Simulations are mature enough to be incorporated at the design stage and to guide the experimental exploration. The new directions the field is taking, incorporating automated exploration methods and combined with extensive data analysis and machine learning algorithms, approach the holy grail of catalyst discovering.

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“…Recently, several automated reaction path search methods that do not require the initial structure of TS have been developed� 9 -11 The methods enable systematic analysis of reaction mechanisms without relying on the computators' experience or intuition. In addition, the automated reaction path search methods are opening the way to ab initio prediction of new chemical reactions passing through unknown reaction paths� This article outlines the artificial force induced reaction (AFIR) method, which has been developed by the authors� [12][13][14][15] Further, by applying the rate constant matrix contraction (RCMC) method, a kinetic analysis method developed by the authors, to the reaction path network obtained by the AFIR method, the products and their formation paths can be elucidated� 16,17 Combined usage of the AFIR and RCMC methods also facilitates on-thefly kinetic simulation to explore elementary reaction processes while solving the chemical kinetics� 18 Finally, this article introduces quantum chemistry aided retrosynthetic analysis (QCaRA), which searches reaction paths backward from a product to possible reactants, and its application to chemical reaction discovery� 19…”

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confidence: 99%

Reactivity prediction through quantum chemical calculations

Maeda¹,

Harabuchi²,

Hasegawa³

et al. 2021

ACM

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The main challenge in chemistry is understanding and controlling the movement of atoms, which play a leading role in chemical reactions. In principle, one could predict the movement of atoms by solving the Schrödinger equation, however, which for many-particle systems is too complicated to solve with high accuracy. Thanks to advances in quantum chemical calculation methods, the Schrödinger equation for the motion of electrons is solvable with reasonable accuracy under various approximations.1 Among the approximation algorithms, the density functional theory (DFT) based on the Kohn-Sham equation is routinely used in calculations of the potential energy surface (PES) for a system of several hundred atoms.

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Artificial Force-Induced Reaction Method for Systematic Elucidation of Mechanism and Selectivity in Organometallic Reactions

Cited by 11 publications

References 90 publications

Exploring paths of chemical transformations in molecular and periodic systems: An approach utilizing force

Exploring paths of chemical transformations in molecular and periodic systems: An approach utilizing force

Computational Organometallic Catalysis: Where We Are, Where We Are Going

Reactivity prediction through quantum chemical calculations

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