Katalyseforschung auf dem Computer

Thiel, Walter

doi:10.1002/ange.201402118

Cited by 9 publications

(2 citation statements)

References 159 publications

(256 reference statements)

Supporting

Mentioning

Contrasting

Order By: Relevance

“…The computational analysis and elucidation of chemical reaction paths provide important mechanistic insights into organic and biochemical reactions [1] . These quantum chemical calculations could yield the geometries and/or energy relationships among reactants, intermediates, products, and transition states (TSs) [2–5] . Conventionally, the calculations are carried out for known chemical processes based on the experimental results or chemist's intuition.…”

Section: Introductionmentioning

confidence: 99%

Oxidation and Reduction Pathways in the Knowles Hydroamination via a Photoredox‐Catalyzed Radical Reaction**

et al. 2022

View full text Add to dashboard Cite

Systematic exploration of reaction paths based on quantum chemical calculations revealed the entire mechanism of Knowles's light-promoted catalytic intramolecular hydroamination via radical processes. Bond formation/cleavage competes with single electron transfer (SET) from the catalyst/substrate to substrate/catalyst. All these processes were theoretically described by reactions through transition states in the same electronic state and non-radiative transitions through the seam of crossings (SX) between different electronic states. This study determined the energetically favorable reaction path by combining the reaction path searches and the SX geometry searches, and then discusses the entire reaction mechanism. Such a calculation was achieved by establishing a novel computational approach that represents SET as a non-adiabatic transition between substrate's PESs for different charge states adjusted based on the catalyst's redox potential. Finally, we uncovered the whole picture of the reaction process, in which N atom of the substrate is oxidized by photoredox catalyst via SET, the resulting aminium radical is added to alkene, and the hydroamination product is produced after SET process accompanying protonolysis with MeOH. The present calculations showed that the reduction and proton transfer proceed concertedly. Also, in the reduction process, there are SET paths leading to both the product and the reactant, and the redox potentials of the catalyst change the contribution of the SET path leading to the product.Computational details of the conformation search (PDF), and the list of MIN, TS and SX geometries (xyz files).

show abstract

Section: Introductionmentioning

confidence: 99%

Oxidation and Reduction Pathways in the Knowles Hydroamination via a Photoredox‐Catalyzed Radical Reaction**

et al. 2022

View full text Add to dashboard Cite

show abstract

“…Quantum chemical calculation has grown to a useful tool to estimate Gibbs energy barriers. There have been numerous studies that discussed reactivity and selectivity utilizing quantum chemical calculations [11–19] . Quantum chemical calculations have also been conducted for predicting reactivity and selectivity [20–23] .…”

Section: Introductionmentioning

confidence: 99%

A Dataset of Computational Reaction Barriers for the Claisen Rearrangement: Chemical and Numerical Analysis

Okada

Maeda

2021

Molecular Informatics

View full text Add to dashboard Cite

Theoretical reaction screening based on Gibbs energy barriers would be promising to accelerate chemical reactions mining. The number of quantum chemical calculations can be reduced by using an optimization algorithm such as genetic algorithm (GA) and Bayesian optimization (BO). The focus of this study is to generate a dataset of reaction barriers of size ~100000. Such a dataset would be useful to quickly evaluate various implementations of an optimization algorithm such as GA and BO. The dataset includes Gibbs energy barriers of the Claisen rearrangement for ~100000 molecules computed on the basis of a semiempirical theory PM7. After evaluating its chemical and numerical features, it is found that the dataset well reflects chemical trends of various substitutions and is useful in testing various implementations of an optimization algorithm. The dataset is available in the supplementary material of this paper.

show abstract

100 Jahre Max‐Planck‐Institut für Kohlenforschung

Reetz

2014

Angewandte Chemie

View full text Add to dashboard Cite

Dieser Essay beschreibt die institutionelle und wissenschaftliche Entwicklung des Max‐Planck‐Instituts für Kohlenforschung in Mülheim an der Ruhr, des Nachfolge‐Instituts des 1914 gegründeten Kaiser‐Wilhelm‐Instituts für Kohlenforschung. Die vier Hauptteile des Essays entsprechen den vier historischen Perioden, die mit den jeweiligen Direktoren zusammenhängen: 1) Franz Fischer; 2) Karl Ziegler; 3) Günther Wilke; 4) die von Manfred T. Reetz initiierte Umstrukturierung, in deren Folge ein Direktorium bestehend aus fünf gleichberechtigten Direktoren mit jeweils einer Abteilung etabliert wurde. Zusätzlich zu den rein historischen und politischen Entwicklungen werden auch Höhepunkte der Forschung aus den vier Perioden beschrieben.

show abstract

Katalyseforschung auf dem Computer

Abstract: Die exponentiell zunehmende Zahl an Zitationen verdeutlicht das explosive Wachstum der „Computational Catalysis“ in den beiden letzten Jahrzehnten. Der Essay skizziert die historische Entwicklung, den jetzigen Stand der Forschung und die zukünftigen Perspektiven auf diesem Gebiet.

Cited by 9 publications

References 159 publications

Oxidation and Reduction Pathways in the Knowles Hydroamination via a Photoredox‐Catalyzed Radical Reaction**

Oxidation and Reduction Pathways in the Knowles Hydroamination via a Photoredox‐Catalyzed Radical Reaction**

A Dataset of Computational Reaction Barriers for the Claisen Rearrangement: Chemical and Numerical Analysis

100 Jahre Max‐Planck‐Institut für Kohlenforschung

Contact Info

Product

Resources

About