Applications of machine learning in surfaces and interfaces

Chemical Physics Reviews, Journal Year: 2025, Volume and Issue: 6(1)

Published: March 1, 2025

Surfaces and interfaces play key roles in chemical material science. Understanding physical processes at complex surfaces is a challenging task. Machine learning provides powerful tool to help analyze accelerate simulations. This comprehensive review affords an overview of the applications machine study systems materials. We categorize into following broad categories: solid–solid interface, solid–liquid liquid–liquid surface solid, liquid, three-phase interfaces. High-throughput screening, combined first-principles calculations, force field accelerated molecular dynamics simulations are used rational design such as all-solid-state batteries, solar cells, heterogeneous catalysis. detailed information on for

Language: Английский

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Probing the Role of Acid Site Distribution on the Water Structure in Aluminosilicate Zeolites: Insights from Molecular Dynamics

The Journal of Physical Chemistry C, Journal Year: 2024, Volume and Issue: 128(18), P. 7549 - 7559

Published: April 26, 2024

Water plays a pivotal role in numerous chemical processes, especially the production of fuels and fine chemicals derived from biobased feedstocks. Zeolites are porous catalysts used extensively due to their shape-selective adsorption confinement interactions; however, kinetics zeolite-catalyzed reactions significantly impacted by presence water, which may affect product selectivity intrinsic rate constants depending on transition-state polarity. In this study, we employed machine learning force fields (MLFFs) accelerate ab initio molecular dynamics (AIMD) simulations enhance phase space exploration water configurations mode Brønsted acid zeolite, H-AFI. We interrogated structure adsorbed based Si/Al ratio site distribution disentangle impact density matrix organization as function loading. integrated thermodynamics, vibrational spectroscopy simulations, local maps interrogate spatial orientation clusters degree hydrogen bonding. Our analysis unveiled intricate interplay between zeolite structure, location, where spatially disparate sites nucleate extended that span siliceous regions zeolite. found length scale ordered is directly related Al sites. These findings provide insights into molecular-level aluminosilicate micropores demonstrate how can be control activity, has applications heterogeneous catalysis adsorptive separations.

Language: Английский

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Harnessing air-water interface to generate interfacial ROS for ultrafast environmental remediation

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: Oct. 14, 2024

The air-water interface of microbubbles represents a crucial microenvironment that can dramatically accelerate reactive oxidative species (ROS) reactions. However, the dynamic nature presents challenges in probing ROS behaviors at interface, limiting comprehensive understanding their chemistry and application. Here we develop an approach to investigate interfacial via coupling with Fenton-like reaction. Amphiphilic single-Co-atom catalyst (Co@SCN) is employed efficiently transport oxidant peroxymonosulfate (PMS) from bulk solution microbubble interface. This triggers accelerated generation sulfate radicals (SO

Language: Английский

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Mechanism of Oh-Initiated Oxidation of Β-Diketone at the Acidic Droplet Interface

Published: Jan. 1, 2025

Language: Английский

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Prediction of Hydrolysis Pathways and Kinetics of Sulfamethoxazole: A Machine-Learning-Based Molecular Dynamics and Experimental Study

Journal of Hazardous Materials, Journal Year: 2025, Volume and Issue: 494, P. 138429 - 138429

Published: April 28, 2025

Language: Английский

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Mechanism of OH-initiated oxidation of β-diketone at the acidic droplet interface

Chemical Physics Letters, Journal Year: 2025, Volume and Issue: unknown, P. 142135 - 142135

Published: April 1, 2025

Language: Английский

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Comprehensive Understanding of the Electrocatalytic Mechanism for Co/Fe/Cu Doped Ni(OH)₂ on Urea Oxidation Reactions: Theory and Experiment

ACS Sustainable Chemistry & Engineering, Journal Year: 2024, Volume and Issue: 12(28), P. 10466 - 10474

Published: July 1, 2024

α-Ni(OH)2 is an efficient candidate for urea oxidation reaction (UOR) but its instability and high energy barriers restrict application. The introduction of transition metals a strategy to solve these problems, systematic investigations mechanisms are limited. Herein, range isoelectronic (ITMs) (M = Co, Fe, Cu) doped Ni(OH)2 catalysts on UOR studied simultaneously in theory experiment. By introducing Co Fe into the lattice Ni(OH)2, electronic structure transfer facilitated, resulting effective promotion absorption CO2 desorption, intrinsic activity can be increased. Among catalysts, Co–Ni(OH)2 with lowest barrier (1.76 eV) rate-determining steps might exhibit excellent activity. To verify theoretical prediction, samples synthesized via one-step hydrothermal method. ITMs incorporation stabilize α phase confirmed by chronopotentiometry X-ray diffraction results. Agreeing calculation, manifests superior properties than other providing smallest onset potential (1.304 V vs RHE) Tafel slope (24 mV dec–1). This study provide comprehensive understanding ITMs-Ni(OH)2 catalytic mechanism, which could instructive designing higher

Language: Английский

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Two-Step Noncatalyzed Hydrolysis Mechanism of Imines at the Air–Water Interface

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(42), P. 28866 - 28873

Published: Oct. 8, 2024

The hydrolysis of imines has long been assumed to be their main atmospheric fate, based on early studies in the field organic chemistry. However, mechanism and kinetics remain unclear. Here, an advanced Born-Oppenheimer molecular dynamics method was employed investigate noncatalyzed at air-water interface by selecting CH

Language: Английский

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Electrochemical Degradation of Pt₃Co Nanoparticles Investigated by Off-Lattice Kinetic Monte Carlo Simulations with Machine-Learned Potentials

ACS Catalysis, Journal Year: 2023, Volume and Issue: 13(24), P. 16078 - 16087

Published: Nov. 30, 2023

In fuel cell applications, the durability of catalysts is critical for large-scale industrial implementation. However, limited synthesis controllability and spectroscopic resolution impede a comprehensive understanding degradation mechanisms at atomic level. this study, we develop machine-learned potential (MLP) to simulate processes Pt3Co nanoparticles. The precision MLP determined be comparable that density functional theory calculations. Using off-lattice kinetic Monte Carlo simulations with MLP, successfully replicate established experimental trends offer logical ongoing debates regarding orderings. Based on simulation results, suggest design principles nanoparticles combine high activity durability. Finally, validate wide applicability our method by applying it Pt3Ni Pt3Co0.5Ni0.5 Our research serves as guideline developing MLPs alloy electrochemical lays foundation designing more durable active fuel-cell catalysts.

Language: Английский

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Probing the role of acid site distribution on water structure in aluminosilicate zeolites: insights from molecular dynamics

Published: Feb. 19, 2024

Water plays a pivotal role in numerous chemical processes, especially the production of fuels and fine chemicals de-rived from bio-based feedstocks. Zeolites are porous catalysts used extensively due to their shape-selective adsorption confinement interactions; However kinetics zeolite-catalyzed reactions significantly impacted by presence water, which may affect product selectivity intrinsic rate constants depending on transition state polarity. In this study, we employed machine learning force fields (MLFFs) accelerate ab initio molecular dynamics (AIMD) simulations enhance phase space exploration water configurations model Brønsted acid zeolite, H-AFI. We interrogated structure adsorbed based Si/Al ratio site distribution disentangle impact density matrix organization as function loading. integrated thermodynamics, vibrational spectroscopy simulations, local maps interrogate spatial orientation clusters degree hydrogen bonding. Our analysis unveiled intricate interplay between zeolite structure, location, where spatially disparate sites nucleate extended that span siliceous regions zeolite. found length scale ordered is directly related Al sites. These findings provide insights into molecular-level microporous aluminosilicate micropores demonstrate how can be control activity has applications heterogeneous catalysis adsorptive separations.

Language: Английский

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