Minimal crystallographic descriptors of sorption properties in hypothetical MOFs and role in sequential learning optimization

Trezza, Giovanni; Bergamasco, Luca; Fasano, Matteo; Chiavazzo, Eliodoro

doi:10.1038/s41524-022-00806-7

Cited by 20 publications

(12 citation statements)

References 84 publications

(103 reference statements)

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“…On the other hand, the rapid development of machine learning-based (MLFF) and neural network-based force fields 97 – 101 (NNFF) may provide alternative and accurate approaches to the ReaxFF. The database constructed using the proposed protocol (or even further automatized by algorithmic orchestration 102 ) could be used for training these new force fields, which may provide superior performance, possibly at the cost of compromising on the physical insight into the parameters obtained from the training. With their flexibility and high interpolation capabilities, these newly developed force fields 101 , 103 , 104 offer promising solutions to the challenges identified in this work and with the ReaxFF.…”

Section: Discussionmentioning

confidence: 99%

Enhancing ReaxFF for molecular dynamics simulations of lithium-ion batteries: an interactive reparameterization protocol

De Angelis,

Cappabianca,

Fasano

et al. 2024

Sci Rep

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Lithium-ion batteries (LIBs) have become an essential technology for the green economy transition, as they are widely used in portable electronics, electric vehicles, and renewable energy systems. The solid-electrolyte interphase (SEI) is a key component for the correct operation, performance, and safety of LIBs. The SEI arises from the initial thermal metastability of the anode-electrolyte interface, and the resulting electrolyte reduction products stabilize the interface by forming an electrochemical buffer window. This article aims to make a first—but important—step towards enhancing the parametrization of a widely-used reactive force field (ReaxFF) for accurate molecular dynamics (MD) simulations of SEI components in LIBs. To this end, we focus on Lithium Fluoride (LiF), an inorganic salt of great interest due to its beneficial properties in the passivation layer. The protocol relies heavily on various Python libraries designed to work with atomistic simulations allowing robust automation of all the reparameterization steps. The proposed set of configurations, and the resulting dataset, allow the new ReaxFF to recover the solid nature of the inorganic salt and improve the mass transport properties prediction from MD simulation. The optimized ReaxFF surpasses the previously available force field by accurately adjusting the diffusivity of lithium in the solid lattice, resulting in a two-order-of-magnitude improvement in its prediction at room temperature. However, our comprehensive investigation of the simulation shows the strong sensitivity of the ReaxFF to the training set, making its ability to interpolate the potential energy surface challenging. Consequently, the current formulation of ReaxFF can be effectively employed to model specific and well-defined phenomena by utilizing the proposed interactive reparameterization protocol to construct the dataset. Overall, this work represents a significant initial step towards refining ReaxFF for precise reactive MD simulations, shedding light on the challenges and limitations of ReaxFF force field parametrization. The demonstrated limitations emphasize the potential for developing more versatile and advanced force fields to upscale ab initio simulation through our interactive reparameterization protocol, enabling more accurate and comprehensive MD simulations in the future.

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Section: Discussionmentioning

confidence: 99%

Enhancing ReaxFF for molecular dynamics simulations of lithium-ion batteries: an interactive reparameterization protocol

De Angelis,

Cappabianca,

Fasano

et al. 2024

Sci Rep

Self Cite

View full text Add to dashboard Cite

show abstract

“…On the other hand, the rapid development of neural network-based force fields [96][97][98][99] (NNFF) may provide alternative and accurate approaches to the ReaxFF. The database constructed using the proposed protocol (or even further automatized by algorithmic orchestration [100]) could be used for training these new force fields, which may provide superior performance possibly at the cost of compromising on the physical insight into the parameters obtained from the training. In summary, the proposed methodology can be extended to the parameterization of other potentials, and by increasing the number of initial configurations, it may also be possible to proceed with the parameterization of neural network potentials.…”

Section: Discussionmentioning

confidence: 99%

Enhancing ReaxFF for Molecular Dynamics Simulations of Lithium-Ion Batteries: An interactive reparameterization protocol

Chiavazzo

Angelis

Cappabianca

et al. 2023

Preprint

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Lithium-ion batteries (LIBs) have become an essential technology for the green economy transition, as they are widely used in portable electronics, electric vehicles, and renewable energy systems. The solid-electrolyte interphase (SEI) is a key component for the correct operation, performance, and safety of LIBs. The SEI arises from the initial thermal metastability of the anode-electrolyte interface, and the resulting electrolyte reduction products stabilize the interface by forming an electrochemical buffer window. This article aims to make a first -- but important -- step towards enhancing the parametrization of a widely-used reactive force field (ReaxFF) for accurate molecular dynamics (MD) simulations of SEI components in LIBs. To this end, we focus on Lithium Fluoride (LiF), an inorganic salt of great interest due to its beneficial properties in the passivation layer. The protocol relies heavily on various Python libraries designed to work with atomistic simulations allowing robust automation of all the reparameterization steps. The proposed set of configurations, and the resulting dataset, allow the new ReaxFF to recover the solid nature of the inorganic salt and improve the mass transport properties prediction from MD simulation. The optimized ReaxFF surpasses the previously available force field by accurately adjusting the diffusivity of lithium in the solid lattice, resulting in a two-order-of-magnitude improvement in its prediction at room temperature. However, our comprehensive investigation of the simulation shows the strong sensitivity of the ReaxFF to the training set, making its ability to interpolate the potential energy surface challenging. Consequently, the current formulation of ReaxFF can be effectively employed to model specific and well-defined phenomena by utilizing the proposed interactive reparameterization protocol to construct the dataset. Overall, this work represents a significant initial step towards refining ReaxFF for precise reactive MD simulations, shedding light on the challenges and limitations of ReaxFF force field parametrization. The demonstrated limitations emphasize the potential for developing more versatile and advanced force fields to upscale ab initio simulation through our interactive reparameterization protocol, enabling more accurate and comprehensive MD simulations in the future.

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“…To predict the performance of the regression models, the n predicted results ( y i ) were compared to the original ones ( y i ) using the following metrics: 65 .…”

Section: Ratio Between D and G Peaks (I D /I G [-])mentioning

confidence: 99%

The impact of physicochemical features of carbon electrodes on the capacitive performance of supercapacitors: a machine learning approach

Mishra

Srivastava

Muhammad

et al. 2023

Sci Rep

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Hybrid electric vehicles and portable electronic systems use supercapacitors for energy storage owing to their fast charging/discharging rates, long life cycle, and low maintenance. Specific capacitance is regarded as one of the most important performance-related characteristics of a supercapacitor’s electrode. In the current study, Machine Learning (ML) algorithms were used to determine the impact of various physicochemical properties of carbon-based materials on the capacitive performance of electric double-layer capacitors. Published experimental datasets from 147 references (4899 data entries) were extracted and then used to train and test the ML models, to determine the relative importance of electrode material features on specific capacitance. These features include current density, pore volume, pore size, presence of defects, potential window, specific surface area, oxygen, and nitrogen content of the carbon-based electrode material. Additionally, categorical variables as the testing method, electrolyte, and carbon structure of the electrodes are considered as well. Among five applied regression models, an extreme gradient boosting model was found to best correlate those features with the capacitive performance, highlighting that the specific surface area, the presence of nitrogen doping, and the potential window are the most significant descriptors for the specific capacitance. These findings are summarized in a modular and open-source application for estimating the capacitance of supercapacitors given, as only inputs, the features of their carbon-based electrodes, the electrolyte and testing method. In perspective, this work introduces a new wide dataset of carbon electrodes for supercapacitors extracted from the experimental literature, also giving an instance of how electrochemical technology can benefit from ML models.

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Minimal crystallographic descriptors of sorption properties in hypothetical MOFs and role in sequential learning optimization

Cited by 20 publications

References 84 publications

Enhancing ReaxFF for molecular dynamics simulations of lithium-ion batteries: an interactive reparameterization protocol

Enhancing ReaxFF for molecular dynamics simulations of lithium-ion batteries: an interactive reparameterization protocol

Enhancing ReaxFF for Molecular Dynamics Simulations of Lithium-Ion Batteries: An interactive reparameterization protocol

The impact of physicochemical features of carbon electrodes on the capacitive performance of supercapacitors: a machine learning approach

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