Interpretable machine learning‐assisted high‐throughput screening of highly active nitrogen fixation dual‐atom catalysts

AIChE Journal, Journal Year: 2025, Volume and Issue: unknown

Published: April 22, 2025

Abstract Machine learning (ML) has addressed the traditional challenges of large data processing in density functional theory (DFT) calculations. However, understanding relationship between fundamental descriptors and catalytic performance identifying key drivers activity remain challenging. Here, we present a cost‐effective, high‐throughput, interpretable ML method to accurately identify nitrogen reduction reaction (NRR) determinants. Initially, 378 M 1 2 @TiO catalysts are screened, yielding 33 promising candidates through high‐throughput techniques. Subsequently, models (primarily XGBoost) predict free energy changes NRR intermediates. Shapley Additive Explanations (SHAP) analysis identifies two critical features: NN bond angle (M NN) N length. Four exhibiting below 0.3 eV potential‐determining step identified as candidates. Combined SHAP electronic structure calculations confirm inherent catalysts, highlighting importance properties modulating active sites for superior performance.

Language: Английский

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NiO Matrix Decorated by Ru Single Atoms: Electron-Rich Ru-Induced High Activity and Selectivity toward Electrochemical N₂ Reduction

The Journal of Physical Chemistry Letters, Journal Year: 2023, Volume and Issue: 14(16), P. 3785 - 3793

Published: April 13, 2023

Developing a single-atom catalyst with electron-rich active sites is promising strategy for catalyzing the electrochemical N2 reduction reaction (NRR). Herein, we choose NiO(001) as model template and deposit series of single transition metal (TM) atoms higher formal charges to create centers. Our first-principles calculations show that low-valent Ru (+2) on can significantly activate N2, its oxidation states varying from +2 +4 throughout catalytic cycle. The Ru/NiO(001) exhibits best activity relatively low limiting potential −0.49 V. Furthermore, under NRR operating conditions, site primarily occupied by *N2 rather than *H, indicating overwhelms hydrogen evolution thus excellent selectivity. work highlights designing catalysts NRR.

Language: Английский

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Boosting Nitrogen Reduction Activity by Defect Engineering in 2D Iron Monochalcogenides FeX (X=S, Se)

Small Structures, Journal Year: 2022, Volume and Issue: 3(11)

Published: Aug. 13, 2022

Large‐scale ammonia synthesis under ambient environment is a highly demanding technology which promising to replace the energy‐consuming Haber–Bosch process. Motivated by crucial iron–sulfur interaction in nitrogenase, performance of 2D iron monochalcogenides (FeX, X=S, or Se) toward electrochemical nitrogen reduction reaction (e‐N2RR) means density functional theory calculations explored. It confirmed that pristine FeX inert for even N 2 adsorption while defective with single‐anion‐point vacancy ( V X ) demonstrates considerable activity NRR. The enhancement attributed between defect‐induced states and p ‐orbitals nitrogen, greatly alters behavior molecule. Meanwhile, relation free energy theoretical limiting potential U L agrees well previous report. Moreover, nature provides flexible sites both proton, alleviating competition e‐N2RR hydrogen evolution reaction. As existence S Se tetragonal has been validified experiments, facile strategy designing practical economical NRR electrocatalysts provided might be extended study other species defects catalysis.

Language: Английский

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First-principles, machine learning and symbolic regression modelling for organic molecule adsorption on two-dimensional CaO surface

Journal of Molecular Graphics and Modelling, Journal Year: 2023, Volume and Issue: 124, P. 108530 - 108530

Published: June 3, 2023

Language: Английский

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Density Functional Theory Investigation on the Nitrogen Reduction Mechanism in Two-Dimensional Transition-Metal Boride with Ordered Metal Vacancies

Langmuir, Journal Year: 2024, Volume and Issue: 40(28), P. 14355 - 14367

Published: July 4, 2024

The creation of ordered collective vacancies in experiment proves challenging within a two-dimensional lattice, resulting limited understanding their impact on catalyst performance. Motivated by the successful experimental synthesis monolayer molybdenum borides with precisely metal [Zhou et al.

Language: Английский

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