Improving the Accuracy of Atomistic Simulations of the Electrochemical Interface

Chemical Reviews, Год журнала: 2022, Номер 122(12), С. 10651 - 10674

Опубликована: Май 6, 2022

Atomistic simulation of the electrochemical double layer is an ambitious undertaking, requiring quantum mechanical description electrons, phase space sampling liquid electrolytes, and equilibration electrolytes over nanosecond time scales. All models electrochemistry make different trade-offs in approximation electrons atomic configurations, from extremes classical molecular dynamics a complete interface with point-charge atoms to correlated electronic structure methods single electrode configuration no or electrolyte. Here, we review spectrum techniques suitable for electrochemistry, focusing on key approximations accuracy considerations each technique. We discuss promising approaches, such as enhanced configurations computationally efficient beyond density functional theory (DFT) methods, that will push simulations present frontier.

Язык: Английский

---

Dynamic Copper Site Redispersion through Atom Trapping in Zeolite Defects

Journal of the American Chemical Society, Год журнала: 2024, Номер 146(12), С. 8280 - 8297

Опубликована: Март 11, 2024

Single-site copper-based catalysts have shown remarkable activity and selectivity for a variety of reactions. However, deactivation by sintering in high-temperature reducing environments remains challenge often limits their use due to irreversible structural changes the catalyst. Here, we report zeolite-based copper which oxide agglomerates formed after reaction can be repeatedly redispersed back single sites using an oxidative treatment air at 550 °C. Under different environments, single-site Cu–Zn–Y/deAlBeta undergoes dynamic structure oxidation state that tuned promote formation key active while minimizing through Cu sintering. For example, Cu2+ reduces Cu1+ catalyst pretreatment (270 °C, 101 kPa H2) further Cu0 nanoparticles under conditions (270–350 7 EtOH, 94 or accelerated aging (400–450 H2). After regeneration °C air, agglomerated CuO was dispersed presence absence Zn Y, verified imaging, situ spectroscopy, catalytic rate measurements. Ab initio molecular dynamics simulations show solvation monomers water facilitates transport zeolite pore, condensation monomer with fully protonated silanol nest entraps reforms structure. The capability nests trap stabilize oxidizing could extend wider reactions allows simple strategy catalysts.

Язык: Английский

---

Theoretical insights into the surface physics and chemistry of redox-active oxides

Nature Reviews Materials, Год журнала: 2020, Номер 5(6), С. 460 - 475

Опубликована: Май 27, 2020

Язык: Английский

---

Potential Application of Machine-Learning-Based Quantum Chemical Methods in Environmental Chemistry

Environmental Science & Technology, Год журнала: 2022, Номер 56(4), С. 2115 - 2123

Опубликована: Янв. 27, 2022

It is an important topic in environmental sciences to understand the behavior and toxicology of chemical pollutants. Quantum methodologies have served as useful tools for probing pollutants recent decades. In years, machine learning (ML) techniques brought revolutionary developments field quantum chemistry, which may be beneficial investigating However, ML-based methods (ML-QCMs) only scarcely been used studies so far. To promote applications promising methods, this Perspective summarizes progress ML-QCMs focuses on their potential that could hardly achieved by conventional methods. Potential challenges predicting degradation networks pollutants, searching global minima atmospheric nanoclusters, discovering heterogeneous or photochemical transformation pathways well environmentally relevant end points with wave functions descriptors are introduced discussed.

Язык: Английский

---

The application of machine learning to air pollution research: A bibliometric analysis

Ecotoxicology and Environmental Safety, Год журнала: 2023, Номер 257, С. 114911 - 114911

Опубликована: Апрель 15, 2023

Machine learning (ML) is an advanced computer algorithm that simulates the human process to solve problems. With explosion of monitoring data and increasing demand for fast accurate prediction, ML models have been rapidly developed applied in air pollution research. In order explore status applications research, a bibliometric analysis was made based on 2962 articles published from 1990 2021. The number publications increased sharply after 2017, comprising approximately 75% total. Institutions China United States contributed half all with most research being conducted by individual groups rather than global collaborations. Cluster revealed four main topics application ML: chemical characterization pollutants, short-term forecasting, detection improvement optimizing emission control. rapid development algorithms has capability characteristics multiple analyze reactions their driving factors, simulate scenarios. Combined multi-field data, are powerful tool analyzing atmospheric processes evaluating management quality deserve greater attention future.

Язык: Английский

---

Structural behaviors, optical properties and electronic structures of rare earth samarium doped germanium anion nanocluster SmGe− (n = 4–20): A density functional theory investigation

Materials Science and Engineering B, Год журнала: 2025, Номер 315, С. 118095 - 118095

Опубликована: Фев. 10, 2025

Язык: Английский

---

Structural, Electronic, and Nonlinear Optical Characteristics of Europium-Doped Germanium Anion Nanocluster EuGen− (n = 7–20): A Theoretical Investigation

Molecules, Год журнала: 2025, Номер 30(6), С. 1377 - 1377

Опубликована: Март 19, 2025

Doping rare-earth metals into semiconductor germanium clusters can significantly enhance the stability of these while introducing novel and noteworthy optical properties. Herein, a series EuGen− (n = 7–20) their structural nonlinear properties are investigated via ABCluster global search technique combined with double-hybrid density functional theory mPW2PLYP. The structure growth pattern be divided two stages: an adsorption linked (when n 7–10 11–20, respectively). In addition to simulating photoelectron spectra clusters, various properties, including (hyper)polarizability, magnetism, charge transfer, relative stability, energy gap, identified. According our examination, EuGe13− cluster exhibits significant response βtot value 7.47 × 105 a.u., is thus considered promising candidate for outstanding nanomaterials.

Язык: Английский

---

Global optimization of chemical cluster structures: Methods, applications, and challenges

International Journal of Quantum Chemistry, Год журнала: 2020, Номер 121(7)

Опубликована: Ноя. 21, 2020

Abstract Chemical clusters are relevant to many applications in catalysis, separations, materials, and energy sciences. Experimentally, the structure of is difficult determine, but it very important understanding their chemistry properties. Computational methods can be used examine cluster structure, however finding most stable not simple, particularly as size increases. Global optimization techniques have long been tackle problem such approaches would look for a global minimum, while sampling local minima over whole potential surface well. In this review, state‐of‐the‐art theory summarized. First, definition, significance, relation experiments, brief history presented. We then discuss, more detail, three versatile methods: basin hopping, artificial bee colony algorithm, genetic algorithm. close with some representative application examples since 2016 challenges, open questions opportunities field.

Язык: Английский

---

Dynamics of Heterogeneous Catalytic Processes at Operando Conditions

JACS Au, Год журнала: 2021, Номер 1(12), С. 2100 - 2120

Опубликована: Ноя. 4, 2021

The rational design of high-performance catalysts is hindered by the lack knowledge structures active sites and reaction pathways under conditions, which can be ideally addressed an in situ/operando characterization. Besides experimental insights, a theoretical investigation that simulates conditions─so-called operando modeling─is necessary for plausible understanding working catalyst system at atomic scale. However, there still huge gap between current widely used computational model concept modeling, should achieved through multiscale modeling. This Perspective describes various modeling approaches machine learning techniques step toward followed selected examples present thermo- electrocatalytic processes. At last, remaining challenges this area are outlined.

Язык: Английский

---

Atmospheric clusters to nanoparticles: Recent progress and challenges in closing the gap in chemical composition

Journal of Aerosol Science, Год журнала: 2020, Номер 153, С. 105733 - 105733

Опубликована: Дек. 11, 2020

Язык: Английский

---