Physical Chemistry Chemical Physics, Journal Year: 2024, Volume and Issue: unknown
Published: Dec. 10, 2024
The theoretical B3LYP+D2 spectrum of a single adsorbed ethanol molecule at H-ZSM-5 described using the Fermi resonance model allows us to assign all vibrational bands in experimentally measured spectrum.
Language: Английский
Nature Communications, Journal Year: 2025, Volume and Issue: 16(1)
Published: March 12, 2025
The modern view of industrial heterogeneous catalysis is evolving from the traditional static paradigm where catalyst merely provides active sites, to that a functional material in which dynamics plays crucial role. Using machine learning-driven molecular simulations, we confirm this picture for ammonia synthesis catalysed by BaH2. Recent experiments show system acts as highly efficient catalyst, but only when exposed first N2 and then H2 chemical looping process. Our simulations reveal N2, BaH2 undergoes profound change, transforming into superionic mixed compound, BaH2−2x(NH)x, characterized high mobility both hydrides imides. This transformation not limited surface involves entire catalyst. When compound second step process, readily formed released, process greatly facilitated ionic mobility. Once all nitrogen are hydrogenated, reverts its initial state, ready next cycle. microscopic analysis underlines dynamic nature does serve platform reactions, rather it entity evolves under reaction conditions. shifting paradigm. Here, authors reactions during synthesis,
Language: Английский
Citations
2
Physical Chemistry Chemical Physics, Journal Year: 2024, Volume and Issue: 26(36), P. 23588 - 23599
Published: Jan. 1, 2024
Accurate predictions of the heat water adsorption and protonation state requires passing from density functional theory (PBE+D) to wavefunction methods (MP2).
Language: Английский
Citations
4
The Journal of Physical Chemistry A, Journal Year: 2025, Volume and Issue: unknown
Published: Jan. 4, 2025
Microkinetic modeling of heterogeneous catalysis serves as an efficient tool bridging atom-scale first-principles calculations and macroscale industrial reactor simulations. Fundamental understanding the microkinetic mechanism relies on a combination experimental theoretical studies. This Perspective presents overview latest progress approaches applied to gas-solid catalytic kinetics. Then, opportunities challenges are presented based recent research in combustion chemistry. For approaches, importance ideal reactors, structured catalysts, precise elementary rate measurements is emphasized. Additionally, integrating spatiotemporally resolved
Language: Английский
Citations
0
ACS Catalysis, Journal Year: 2025, Volume and Issue: 15(3), P. 1616 - 1634
Published: Jan. 15, 2025
The production of many bulk chemicals relies on heterogeneous catalysis. rational design or improvement the required catalysts critically depends insights into underlying mechanisms atomic scale. In recent years, substantial progress has been made in applying advanced experimental techniques to complex catalytic reactions operando, but order achieve a comprehensive understanding, additional information from computer simulations is indispensable cases. particular, ab initio molecular dynamics (AIMD) become an important tool explicitly address atomistic level structure, dynamics, and reactivity interfacial systems, high computational costs limit applications systems consisting at most few hundred atoms for simulation times up tens picoseconds. Rapid advances development modern machine learning potentials (MLP) now offer promising approach bridge this gap, enabling with accuracy small fraction costs. Perspective, we provide overview current state art MLPs relevant catalysis along discussion prospects use science years come.
Language: Английский
Citations
0
Nature Chemical Engineering, Journal Year: 2025, Volume and Issue: unknown
Published: Feb. 17, 2025
Language: Английский
Citations
0
Communications Chemistry, Journal Year: 2025, Volume and Issue: 8(1)
Published: March 13, 2025
Semiconductor nanocrystals, including their superstructures and hybridized systems, have opened up a new realm to design next-generation functional materials creatively. Their great success unlimited potential should be largely attributed surface-adsorbed ligands. However, due lack of means probe understand roles in experiments, only handful effective ligands been identified through trial-and-error processes. Alternatively, computational theoretical methods are ideal for providing physical insights further guidance. Still, applications ligand-coated semiconductor nanocrystals relatively scarce compared those other such as biological chemistry. In this perspective, we first highlight the ab initio modeling ligand adsorption. Then, discuss opportunities molecular dynamics theory accommodating complex colloidal nature, where unfold challenges therein. Finally, emphasize need high-quality force fields resolve these look forward simulation-guided inverse design. Surface-adsorbed paramount applicability but experimental investigation is challenging. Here, authors successes dedicated modeling, advancing nanocrystalline materials.
Language: Английский
Citations
0
The Journal of Physical Chemistry C, Journal Year: 2025, Volume and Issue: 129(16), P. 7751 - 7761
Published: April 13, 2025
Microkinetic models (MKMs) are widely used within the computational heterogeneous catalysis community to investigate complex reaction mechanisms, rationalize experimental trends, and accelerate rational design of novel catalysts. However, constructing these requires computationally expensive manually tedious density functional theory (DFT) calculations for identifying transition states each elementary MKM. To address challenges, we demonstrate a protocol that uses open-source kinetics workflow tool Pynta automate iterative training reactive machine learning potential (rMLP). Specifically, using silver-catalyzed partial oxidation methanol as prototypical example, first our by an rMLP parallel calculation DFT-quality all 53 reactions, achieving 7× speedup compared DFT-only strategy. Detailed analysis curriculum reveals shortcomings adaptive sampling scheme with single model describe reactions MKM simultaneously. We show limitations can be overcome balanced "reaction class" approach multiple models, describing class similar states. Finally, Pynta-based is also compatible large pretrained foundational models. For fine-tuning top-performing graph neural network trained on OC20 dataset, observe impressive 20× 89% success rate in This work highlights synergistic integrating automated tools advance research.
Language: Английский
Citations
0
The Journal of Physical Chemistry Letters, Journal Year: 2024, Volume and Issue: 15(39), P. 9852 - 9862
Published: Sept. 19, 2024
A combination of machine learned interatomic potentials (MLIPs) and enhanced sampling simulations is used to investigate the activation methane on a Ni(111) surface. The work entails development iterative refinement MLIPs, initially trained data set constructed via ab initio molecular dynamics simulations, supplemented by adaptive biasing forces, enrich catalytically relevant configurations. Our results reveal that upon incorporation collective variables capture behavior reactant molecule, as well additional frames describe dynamic response catalytic surface, it possible enhance considerably accuracy predicted energies forces. By employing schemes in MLIP, we systematically explore potential energy leading refined MLIP capable predicting density functional theory-level forces replicating key geometric characteristics system. resulting free landscapes at several temperatures provide detailed view thermodynamics activation. Specifically, approaches dissociates process involves interplay CH4 Ni catalyst includes both enthalpic entropic contributions. progression toward transition state moiety increasingly restrained its ability rotate or translate, while stage following characterized notable rise atom interacts with cleaved C-H bond. This leads an increase mobility adsorbed species, feature becomes more pronounced higher temperatures.
Language: Английский
Citations
3
The Journal of Physical Chemistry C, Journal Year: 2024, Volume and Issue: 128(37), P. 15367 - 15379
Published: Sept. 3, 2024
Lewis acid sites (LAS) at the CHA(001) and CHA(101) surfaces are investigated regarding their activity for MeOH-mediated hydrogen transfer reactions from MeOH to alkenes, yielding alkanes formaldehyde. Direct decomposition formaldehyde is also investigated. Furthermore, coupling of produced olefins with dienes H2O via Prins reaction studied. The reactivity LAS these compared that bulk Brønsted (BAS) surface BAS. Periodic density functional theory (DFT) used in connection DLPNO-CCSD(T) calculations on cluster models. Hydrogen found be often more favorable LAS, while both BAS have similar reactions.
Language: Английский
Citations
2
Advanced Energy Materials, Journal Year: 2024, Volume and Issue: unknown
Published: Sept. 17, 2024
Abstract Photocatalysis and electrocatalysis have emerged as promising technologies for addressing the energy crisis environmental issues. However, widespread application of these is hampered by challenge scaling up production photo/electrocatalysts that are not only highly active stable but also cost‐effective environmentally benign. This review delves into latest advancements in large‐scale synthesis photo/electrocatalysts. The factors to be considered catalysts discussed first. methods batch preparation then comprehensively introduced, with a thorough discussion their respective advantages limitations. Moreover, data analysis via machine learning techniques, which accelerates identification refinement potential new offers insights enhancing high‐throughput catalysts, introduced detail. Then representative examples presented illustrate applications field industrial‐level photo/electrocatalysis. Finally, challenges prospects development discussed. By bridging gap between laboratory research industrial application, this aims provide reference future sustainable conversion beyond.
Language: Английский
Citations
2