Dataset Information

Predicting the influence of particle size on the glass transition temperature and viscosity of secondary organic material.

ABSTRACT: Atmospheric aerosols can assume liquid, amorphous semi-solid or glassy, and crystalline phase states. Particle phase state plays a critical role in understanding and predicting aerosol impacts on human health, visibility, cloud formation, and climate. Melting point depression increases with decreasing particle diameter and is predicted by the Gibbs-Thompson relationship. This work reviews existing data on the melting point depression to constrain a simple parameterization of the process. The parameter [Formula: see text] describes the degree to which particle size lowers the melting point and is found to vary between 300 and 1800 K nm for a wide range of particle compositions. The parameterization is used together with existing frameworks for modeling the temperature and RH dependence of viscosity to predict the influence of particle size on the glass transition temperature and viscosity of secondary organic aerosol formed from the oxidation of [Formula: see text]-pinene. Literature data are broadly consistent with the predictions. The model predicts a sharp decrease in viscosity for particles less than 100 nm in diameter. It is computationally efficient and suitable for inclusion in models to evaluate the potential influence of the phase change on atmospheric processes. New experimental data of the size-dependence of particle viscosity for atmospheric aerosol mimics are needed to thoroughly validate the predictions.

SUBMITTER: Petters M

PROVIDER: S-EPMC7495436 | biostudies-literature | 2020 Sep

REPOSITORIES: biostudies-literature

ACCESS DATA

Publications

Predicting the influence of particle size on the glass transition temperature and viscosity of secondary organic material.

Petters Markus M Kasparoglu Sabin S

Scientific reports 20200916 1

Atmospheric aerosols can assume liquid, amorphous semi-solid or glassy, and crystalline phase states. Particle phase state plays a critical role in understanding and predicting aerosol impacts on human health, visibility, cloud formation, and climate. Melting point depression increases with decreasing particle diameter and is predicted by the Gibbs-Thompson relationship. This work reviews existing data on the melting point depression to constrain a simple parameterization of the process. The par ...[more]

PMID: 32938963

Similar Datasets

Project description:Knowledge of the glass transition temperature of molecular compounds that occur in atmospheric aerosol particles is important for estimating their viscosity, as it directly influences the kinetics of chemical reactions and particle phase state. While there is a great diversity of organic compounds present in aerosol particles, for only a minor fraction of them experimental glass transition temperatures are known. Therefore, we have developed a machine learning model designed to predict the glass transition temperature of organic molecular compounds based on molecule-derived input variables. The extremely randomized trees (extra trees) procedure was chosen for this purpose. Two approaches using different sets of input variables were followed. The first one uses the number of selected functional groups present in the compound, while the second one generates descriptors from a SMILES (Simplified Molecular Input Line Entry System) string. Organic compounds containing carbon, hydrogen, oxygen, nitrogen, and halogen atoms are included. For improved results, both approaches can be combined with the melting temperature of the compound as an additional input variable. The results show that the predictions of both approaches show a similar mean absolute error of about 12-13 K, with the SMILES-based predictions performing slightly better. In general, the model shows good predictive power considering the diversity of the experimental input data. Furthermore, we also show that its performance exceeds that of previous parameterizations developed for this purpose and also performs better than existing machine learning models. In order to provide user-friendly versions of the model for applications, we have developed a web site where the model can be run by interested scientists via a web-based interface without prior technical knowledge. We also provide Python code of the model. Additionally, all experimental input data are provided in form of the Bielefeld Molecular Organic Glasses (BIMOG) database. We believe that this model is a powerful tool for many applications in atmospheric aerosol science and material science.

Project description:In the present work, we address the problem of utilizing machine learning (ML) methods to predict the thermal properties of polymers by establishing "structure-property" relationships. Having focused on a particular class of heterocyclic polymers, namely polyimides (PIs), we developed a graph convolutional neural network (GCNN), being one of the most promising tools for working with big data, to predict the PI glass transition temperature T g as an example of the fundamental property of polymers. To train the GCNN, we propose an original methodology based on using a "transfer learning" approach with an enormous "synthetic" data set for pretraining and a small experimental data set for its fine-tuning. The "synthetic" data set contains more than 6 million combinatorically generated repeating units of PIs and theoretical values of their T g values calculated using the well-established Askadskii's quantitative structure-property relationship (QSPR) computational scheme. Additionally, an experimental data set for 214 PIs was also collected from the literature for training, fine-tuning, and validation of the GCNN. Both "synthetic" and experimental data sets are included into a PolyAskInG database (Polymer Askadskii's Intelligent Gateway). By using the PolyAskInG database, we developed GCNN which allows estimation of T g of PI with a mean absolute error (MAE) of about 20 K, which is 1.5 times lower than in the case of Askadskii QSPR analysis (33 K). To prove the efficiency and usability of the proposed GCNN architecture and training methodology for predicting polymer properties, we also employed "transfer learning" to develop alternative GCNN pretrained on proxy-characteristics taken from the popular quantum-chemical QM9 database for small compounds and fine-tuned on an experimental T g values data set from PolyAskInG database. The obtained results indicate that pretraining of GCNN on the "synthetic" polymer data set provides MAE which is almost twice as low as that in the case of using the QM9 data set in the pretraining stage (∼41 K). Furthermore, we address the questions associated with the influence of the differences in the size of the experimental and "synthetic" data sets (so-called "reality gap" problem), as well as their chemical composition on the training quality. Our results state the overall priority of using polymer data sets for developing deep neural networks, and GCNN in particular, for efficient prediction of polymer properties. Moreover, our work opens up a challenge for the theoretically supported generation of large "synthetic" data sets of polymer properties for the training of the complex ML models. The proposed methodology is rather versatile and may be generalized for predicting other properties of different polymers and copolymers synthesized through the polycondensation reaction.

Dataset Information

Predicting the influence of particle size on the glass transition temperature and viscosity of secondary organic material.

Publications

Predicting the influence of particle size on the glass transition temperature and viscosity of secondary organic material.

Similar Datasets

OmicsDI is part of the ELIXIR infrastructure

Tweets