A hybrid MC/MD reaction method with rare event-driving mechanism: Atomistic realization of 2-chlorobutane racemization process in DMF solution

Nagaoka, Masataka; Suzuki, Yuichi; Okamoto, Takuya; Takenaka, Norio

doi:10.1016/j.cplett.2013.08.017

Cited by 48 publications

(92 citation statements)

References 21 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…To investigate microscopically the polymerization process in the CP system, we employed the RM methodology, which is constructed by alternately using the MD and the Monte Carlo (MC) methods. The former describes the dynamics of molecules in the short‐time scale, while the latter does the reactions which accompany the bond breaking and formation in the long‐time scale.…”

Section: Theoretical Treatmentsmentioning

confidence: 99%

“…It is, therefore, considered extremely difficult to simulate the CP process as a whole. As one of the solutions, Nagaoka et al have been developing the Red Moon (RM) methodology that can simulate a so‐called “chemical reaction” as a succession of elementary reaction processes. So far, they succeeded in clarifying microscopic mechanism of not only the interfacial polycondensation but also the solid electrolyte interphase film formation .…”

Section: Introductionmentioning

confidence: 99%

See 1 more Smart Citation

Atomistic chemical computation of Olefin polymerization reaction catalyzed by (pyridylamido)hafnium(IV) complex: Application of Red Moon simulation

et al. 2018

Self Cite

View full text Add to dashboard Cite

We have realized the microscopic simulation of olefin polymerization, that is, the simulation of the catalytic polymerization (CP) reaction system composed of (pyridylamido)hafnium (IV) complex as the catalyst. For this purpose, we adopted Red Moon (RM) method, a novel molecular simulation method to simulate the complex reaction system. First, according to the previous research, with the help of the QM calculation, we proposed a model system and elementary processes and explained the theoretical treatment of the simulation by the RM method (the RM simulation). In addition, we also proposed a macroscopic simulation based on chemical kinetics simulation. Then, we performed two simulations and compared them in terms of the effective time evolution of the three macroscopic physical quantities, the number-average molecular weight M n , the massaverage molecular weight M w , and the molar-mass dispersity Đ M . The comparison showed that the two simulations are in quantitative or partially qualitative agreement with each other. Therefore, it is concluded that the RM simulation could not only simulate the CP reaction process microscopically, but also it is connected essentially to reproduce the time evolution of the macroscopic physical quantities on the basis of its microscopic simulation data.

show abstract

Section: Theoretical Treatmentsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Atomistic chemical computation of Olefin polymerization reaction catalyzed by (pyridylamido)hafnium(IV) complex: Application of Red Moon simulation

et al. 2018

Self Cite

View full text Add to dashboard Cite

show abstract

“…1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60 Under the circumstances, we have recently proposed a new atomistic reaction simulation method, which is a hybrid Monte Carlo (MC)/molecular dynamics (MD) reaction method (or Red Moon method), in order to deal with the long-term characteristics of the sub-micro scale structure produced by successive complex chemical reaction processes. [29][30][31] It must be worth noting a characteristic contrast between first principles methods and the hybrid MC/MD reaction method. The AIMD method has been mainly applied to investigate the initial stage of SEI film formation, focusing a few reduction reactions of electrolyte solvents and lithium salts on the anode surface.…”

Section: Introductionmentioning

confidence: 99%

A Computational Chemical Insight into Microscopic Additive Effect on Solid Electrolyte Interphase Film Formation in Sodium-Ion Batteries: Suppression of Unstable Film Growth by Intact Fluoroethylene Carbonate

et al. 2015

Self Cite

View full text Add to dashboard Cite

Sodium (Na)-ion batteries (NIB) have recently attracted special attention as a substitute for Li-ion batteries (LIB) due to the increase in the cost of Li. The performance of NIB with liquid electrolytes, e.g., propylene carbonate (PC), is strongly dependent on a stable solid electrolyte interphase (SEI) film on the anode surface. According to a recent experiment, fluoroethylene carbonate (FEC) can be an efficient electrolyte additive to improve the SEI film formation in NIB. However, the molecular mechanism of such additive effect remains unknown. To investigate this mechanism, atomistic reaction simulations in PC-based electrolyte with and without FEC additives were performed using the hybrid Monte Carlo (MC)/molecular dynamics (MD) reaction method and, successfully reproduced experimental observations such as the smaller irreversible capacity and the smoother SEI film in FEC-added electrolyte. Further, this study showed for the first time that intact FEC molecules can improve SEI film formation so as to enhance the network formation of organic species owing to the large electronegativity of their fluorine atoms. This new microscopic insight may provide an important guiding principle for use in designing the most suitable electrolytes for developing high-performance NIB. KEYWORDS:・Na-ion battery ・Irreversible capacity ・SEI film ・FEC ・Hybrid MC/MD reaction method

show abstract

“…The RM method repeats a combined cycle consisting of a set of MC and MD treatments, which is hereafter called the “MC/MD cycle” . The former treatment manages such a rare event stochastically as a chemical reaction, while the latter simply performs a common dynamical process in the stable phase space to naturally search for candidate molecular configurations for reaction occurrences.…”

Section: Methodsmentioning

confidence: 99%

“…Under the circumstances, we have recently developed a new atomistic reaction simulation method, i. e., the Red Moon (RM) method (a hybrid Monte Carlo (MC)/molecular dynamics (MD) reaction method), in order to investigate the long‐term characteristics of the sub‐micro scale structure produced by successive complex chemical reaction processes …”

Section: Introductionmentioning

confidence: 99%

Microscopic Elucidation of Solid‐Electrolyte Interphase (SEI) Film Formation via Atomistic Reaction Simulations: Importance of Functional Groups of Electrolyte and Intact Additive Molecules

Takenaka

Nagaoka

2019

The Chemical Record

Self Cite

View full text Add to dashboard Cite

Secondary batteries such as Li‐ion battery are expected to be utilized as not only ubiquitous electric power sources such as mobile phones but also large‐scale electricity storage devices. Therefore, it is urgent to develop the higher performance secondary batteries. Their lifetime and stability are found to be strongly dependent on the nature of passivation film called solid electrolyte interphase (SEI) film formed on the anode surface in the initial charge‐discharge cycle. However, since it is difficult to directly observe the film formation processes in experiment, its microscopic mechanism is still not found. On the other hand, although the theoretical methods are useful complement to the experiment, some new methodologies are necessary to understand the long‐term processes of SEI film, which is produced as a result of that a lot of chemical reactions proceed simultaneously. Under the circumstances, we have developed Red Moon method that can simulate such complex chemical reaction systems, and were able to analyze for the first time the SEI film formation processes on the anode surface at the atomistic level. Then, we clarified theoretically the microscopic mechanism of the additive effect which is essential to improve the Na‐ion battery performance so as to enhance the SEI film formation. This new microscopic insight must provide an important guiding principle for use in designing the most suitable electrolytes for developing high‐performance secondary batteries.

show abstract

A hybrid MC/MD reaction method with rare event-driving mechanism: Atomistic realization of 2-chlorobutane racemization process in DMF solution

Cited by 48 publications

References 21 publications

Atomistic chemical computation of Olefin polymerization reaction catalyzed by (pyridylamido)hafnium(IV) complex: Application of Red Moon simulation

Atomistic chemical computation of Olefin polymerization reaction catalyzed by (pyridylamido)hafnium(IV) complex: Application of Red Moon simulation

A Computational Chemical Insight into Microscopic Additive Effect on Solid Electrolyte Interphase Film Formation in Sodium-Ion Batteries: Suppression of Unstable Film Growth by Intact Fluoroethylene Carbonate

Microscopic Elucidation of Solid‐Electrolyte Interphase (SEI) Film Formation via Atomistic Reaction Simulations: Importance of Functional Groups of Electrolyte and Intact Additive Molecules

Contact Info

Product

Resources

About