Revealing the molecular structures of α-Al2O3(0001)–water interface by machine learning based computational vibrational spectroscopy DOI
Xianglong Du,

W. W. Shao,

Chenglong Bao

и другие.

The Journal of Chemical Physics, Год журнала: 2024, Номер 161(12)

Опубликована: Сен. 24, 2024

Solid–water interfaces are crucial to many physical and chemical processes extensively studied using surface-specific sum-frequency generation (SFG) spectroscopy. To establish clear correlations between specific spectral signatures distinct interfacial water structures, theoretical calculations molecular dynamics (MD) simulations required. These MD typically need relatively long trajectories (a few nanoseconds) achieve reliable SFG response function via the dipole moment–polarizability time correlation function. However, requirement for limits use of computationally expensive techniques, such as ab initio (AIMD) simulations, particularly complex solid–water interfaces. In this work, we present a pathway calculating vibrational spectra (IR, Raman, SFG) machine learning (ML)-accelerated methods. We employ both velocity–velocity approaches calculate spectra. Our results demonstrate successful acceleration AIMD calculation ML This advancement provides an opportunity complicated systems more rapidly at lower computational cost with aid ML.

Язык: Английский

Tunable Surface Wettability via Terahertz Electrowave Controlled Vicinal Subnanoscale Water Layer DOI
Zhi Zhu, Junquan Zhu,

Chao Chang

и другие.

Nano Letters, Год журнала: 2024, Номер 24(10), С. 3243 - 3248

Опубликована: Март 1, 2024

Achieving timely, reversible, and long-range remote tunability over surface wettability is highly demanded across diverse fields, including nanofluidic systems, drug delivery, heterogeneous catalysis. Herein, using molecular dynamic simulations, we show, for the first time, a theoretical design of electrowetting to achieve remotely controllable via terahertz wave. The key idea driving unique collective vibration identified in vicinal subnanoscale water layer, which absent bulk water, enabling efficient energy transfer from wave rotational motion layer. Consequently, frequency-specific alternating electric field near critical strength can significantly affect local hydrogen-bonding network contact layer on solid surface, thereby achieving tunable wettability.

Язык: Английский

Процитировано

51
The Role of Interfaces and Charge for Chemical Reactivity in Microdroplets DOI

R. Allen LaCour,

Joseph P. Heindel, Ruoqi Zhao

и другие.

Journal of the American Chemical Society, Год журнала: 2025, Номер 147(8), С. 6299 - 6317

Опубликована: Фев. 17, 2025

A wide variety of reactions are reported to be dramatically accelerated in aqueous microdroplets, making them a promising platform for environmentally clean chemical synthesis. However, fully utilize the microdroplets accelerating requires fundamental understanding how microdroplet chemistry differs from that homogeneous phase. Here we provide our perspective on recent progress this end, both experimentally and theoretically. We begin by reviewing many ways which can prepared, creating water/hydrophobic interfaces have been frequently implicated reactivity due preferential surface adsorption solutes, persistent electric fields, their acidity or basicity. These features interface interplay with specific mechanisms proposed reactivity, including partial solvation, possible gas phase channels, presence highly reactive intermediates. especially highlight role droplet charge associated appears key certain reactions, like formation hydrogen peroxide reduced transition metal complexes, thermodynamically microdroplets. Lastly, emphasize opportunities theoretical advances suggest experiments would greatly enhance fascinating subject.

Язык: Английский

Процитировано

9
Uncovering the Dominant Role of an Extended Asymmetric Four-Coordinated Water Network in the Hydrogen Evolution Reaction DOI

Shanshan Li,

Lie Wu, Qixin Liu

и другие.

Journal of the American Chemical Society, Год журнала: 2023, Номер 145(49), С. 26711 - 26719

Опубликована: Ноя. 30, 2023

In situ and accurate measurement of the structure dynamics interfacial water in hydrogen evolution reaction (HER) is a well-known challenge because coupling among varied structures its dual role as reactants solvents. Further, interference bulk intricate interactions always hinders probing water. Surface-enhanced infrared absorption spectroscopy extremely sensitive for water; herein, we develop nanoconfinement strategy by introducing nonaqueous ionic liquids to decouple tailor electric double layer further combined with molecular simulations, successfully gaining correlation between isolated water, clusters, network HER activity. Our results clearly disclosed that potential-dependent asymmetric four-coordinated network, whose connectivity could be regulated hydrophilic hydrophobic cations, was positively correlated activity, which provided pioneering guidance framework revealing function catalysis, energy, surface science.

Язык: Английский

Процитировано

37
Mycotoxins in Food: Occurrence, Health Implications, and Control Strategies-A Comprehensive Review DOI
Rahim Khan

Toxicon, Год журнала: 2024, Номер 248, С. 108038 - 108038

Опубликована: Июль 22, 2024

Язык: Английский

Процитировано

18
Neural Network-Based Sum-Frequency Generation Spectra of Pure and Acidified Water Interfaces with Air DOI
Miguel de la Puente, Axel Gomez, Damien Laage

и другие.

The Journal of Physical Chemistry Letters, Год журнала: 2024, Номер 15(11), С. 3096 - 3102

Опубликована: Март 12, 2024

The affinity of hydronium ions (H3O+) for the air–water interface is a crucial question in environmental chemistry. While sum-frequency generation (SFG) spectroscopy has been instrumental indicating preference H3O+ interface, key questions persist regarding molecular origin SFG spectral changes acidified water. Here we combine nanosecond long neural network (NN) reactive simulations pure and water slabs with NN predictions dipoles polarizabilities to calculate spectra trajectories including proton transfer events. Our show that cause two distinct phase-resolved spectra: first, low-frequency tail due vibrations its first hydration shell, analogous bulk continuum, second, an enhanced hydrogen-bonded band ion-induced static field polarizing molecules deeper layers. calculations confirm acidic solutions are caused by preferentially residing at interface.

Язык: Английский

Процитировано

15
All‐In‐One Self‐Floating Wood‐Based Solar‐Thermal Evaporators for Simultaneous Solar Steam Generation and Catalytic Degradation DOI

Tingting Zhang,

Jin Qu, Jing Wu

и другие.

Advanced Functional Materials, Год журнала: 2024, Номер unknown

Опубликована: Май 20, 2024

Abstract Solar‐driven steam generation has emerged as a sustainable technology for addressing freshwater scarcity. However, significant challenges still exist in developing high‐performance, multifunctional evaporators that are adept at both efficiently evaporating water and degrading pollutants, primarily because of the trade‐offs among functional designs. Here, self‐floating solar evaporator is reported by functionalizing balsa wood with solar‐thermal conversion material carbon nanotubes catalytic manganese dioxide (MnO 2 ) nanoflowers simultaneous evaporation pollutant degradation. MnO rich oxygen vacancies can effectively activate peroxymonosulfate to generate reactive species efficient organic A distinctive non‐wetted porous interior structure precisely targeted pathway spontaneously established evaporator, ensuring fast supply, thermal insulation, mass transfer, high buoyancy. The resulting successfully combine an impressive rate 2.74 kg m −2 h −1 , degradation efficiency (98.3% 100 mg L tetracycline 97.4% 200 Methyl orange), stable self‐standing capabilities ensure long‐term operation stability even complex real‐world environments. This work provides approach design evaporators, strong alignment practical requirements while expanding their potential application scenarios.

Язык: Английский

Процитировано

15
Quantifying Stern layer water alignment before and during the oxygen evolution reaction DOI Creative Commons
Raiden Speelman,

Ezra J. Marker,

Franz M. Geiger

и другие.

Science Advances, Год журнала: 2025, Номер 11(10)

Опубликована: Март 5, 2025

While water's oxygen is the electron source in industrially important evolution reaction, strong absorber problem clouds our view of how Stern layer water molecules orient themselves response to applied potentials. Here, we report nonlinear optical measurements on nickel electrodes held at pH 13 indicating a disorder-to-order transition before onset Faradaic current. A full monolayer (1.1 × 1015 centimeter-2) aligns with atoms pointing toward electrode +0.8 volt and associated work 80 kilojoule per mole. Our experiments identify flipping energetics as target for understanding overpotentials, advance molecular electrochemistry, provide benchmarks electrical double models, serve diagnostic tool electrocatalysis.

Язык: Английский

Процитировано

2
Development and Modus Operandi relating Surface Structure and Ion Complexation Modeling for Important Metal (Hydr)oxides DOI
Tjisse Hiemstra, Johannes Lützenkirchen

Reviews in Mineralogy and Geochemistry, Год журнала: 2025, Номер 91A(1), С. 13 - 84

Опубликована: Март 28, 2025

Язык: Английский

Процитировано

2
Molecular Controls on Complexation Reactions and Electrostatic Potential Development at Mineral Surfaces DOI
Jean‐François Boily

Reviews in Mineralogy and Geochemistry, Год журнала: 2025, Номер 91A(1), С. 105 - 147

Опубликована: Март 28, 2025

Язык: Английский

Процитировано

2
Variable-Angle Surface Spectroscopy Reveals the Water Structure in the Stern Layer at Charged Aqueous Interfaces DOI
Md. Mosfeq Uddin, Md. Shafiul Azam, Dennis K. Hore

и другие.

Journal of the American Chemical Society, Год журнала: 2024, Номер 146(17), С. 11756 - 11763

Опубликована: Апрель 11, 2024

At charged aqueous interfaces, the second-order nonlinear optical response originates from water molecules within diffuse part of electrical double layer, which are ordered by surface field and that additionally experiences chemical physical interactions with in Stern layer. These two environments can either reinforce or diminish overall signal be disentangled varying coherence length their interaction external laser fields. Here, we demonstrate a method angle incidence is varied to afford significant change length. When this technique was applied silica–water interface, it observed layers direct hydrogen atoms toward mineral at low ionic strength neutral pH. A decrease increasing attributed hydrated cation adsorption competes free for deprotonated silanol sites.

Язык: Английский

Процитировано

9