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Augmenting zero-Kelvin quantum mechanics with machine learning for the prediction of chemical reactions at high temperatures.

ABSTRACT: The prediction of temperature effects from first principles is computationally demanding and typically too approximate for the engineering of high-temperature processes. Here, we introduce a hybrid approach combining zero-Kelvin first-principles calculations with a Gaussian process regression model trained on temperature-dependent reaction free energies. We apply this physics-based machine-learning model to the prediction of metal oxide reduction temperatures in high-temperature smelting processes that are commonly used for the extraction of metals from their ores and from electronics waste and have a significant impact on the global energy economy and greenhouse gas emissions. The hybrid model predicts accurate reduction temperatures of unseen oxides, is computationally efficient, and surpasses in accuracy computationally much more demanding first-principles simulations that explicitly include temperature effects. The approach provides a general paradigm for capturing the temperature dependence of reaction free energies and derived thermodynamic properties when limited experimental reference data is available.

SUBMITTER: Garrido Torres JA

PROVIDER: S-EPMC8636515 | biostudies-literature | 2021 Dec

REPOSITORIES: biostudies-literature

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Augmenting zero-Kelvin quantum mechanics with machine learning for the prediction of chemical reactions at high temperatures.

Garrido Torres Jose Antonio JA Gharakhanyan Vahe V Artrith Nongnuch N Eegholm Tobias Hoffmann TH Urban Alexander A

Nature communications 20211201 1

The prediction of temperature effects from first principles is computationally demanding and typically too approximate for the engineering of high-temperature processes. Here, we introduce a hybrid approach combining zero-Kelvin first-principles calculations with a Gaussian process regression model trained on temperature-dependent reaction free energies. We apply this physics-based machine-learning model to the prediction of metal oxide reduction temperatures in high-temperature smelting process ...[more]

PMID: 34853301

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Augmenting zero-Kelvin quantum mechanics with machine learning for the prediction of chemical reactions at high temperatures.

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Augmenting zero-Kelvin quantum mechanics with machine learning for the prediction of chemical reactions at high temperatures.

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