Tunable Surface Wettability via Terahertz Electrowave Controlled Vicinal Subnanoscale Water Layer

Nano Letters, Journal Year: 2024, Volume and Issue: 24(10), P. 3243 - 3248

Published: March 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.

Language: Английский

---

The Role of Interfaces and Charge for Chemical Reactivity in Microdroplets

Journal of the American Chemical Society, Journal Year: 2025, Volume and Issue: 147(8), P. 6299 - 6317

Published: Feb. 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.

Language: Английский

---

Development and Modus Operandi relating Surface Structure and Ion Complexation Modeling for Important Metal (Hydr)oxides

Reviews in Mineralogy and Geochemistry, Journal Year: 2025, Volume and Issue: 91A(1), P. 13 - 84

Published: March 28, 2025

Language: Английский

---

Molecular Controls on Complexation Reactions and Electrostatic Potential Development at Mineral Surfaces

Reviews in Mineralogy and Geochemistry, Journal Year: 2025, Volume and Issue: 91A(1), P. 105 - 147

Published: March 28, 2025

Language: Английский

---

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

Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: 145(49), P. 26711 - 26719

Published: Nov. 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.

Language: Английский

---

Mycotoxins in Food: Occurrence, Health Implications, and Control Strategies-A Comprehensive Review

Toxicon, Journal Year: 2024, Volume and Issue: 248, P. 108038 - 108038

Published: July 22, 2024

Language: Английский

---

Neural Network-Based Sum-Frequency Generation Spectra of Pure and Acidified Water Interfaces with Air

The Journal of Physical Chemistry Letters, Journal Year: 2024, Volume and Issue: 15(11), P. 3096 - 3102

Published: March 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.

Language: Английский

---

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

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: unknown

Published: May 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.

Language: Английский

---

Variable-Angle Surface Spectroscopy Reveals the Water Structure in the Stern Layer at Charged Aqueous Interfaces

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(17), P. 11756 - 11763

Published: April 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.

Language: Английский

---

Mechanism of Fe(II) Chemisorption on Hematite(001) Revealed by Reactive Neural Network Potential Molecular Dynamics

The Journal of Physical Chemistry Letters, Journal Year: 2025, Volume and Issue: unknown, P. 848 - 856

Published: Jan. 16, 2025

Atomic-scale understanding of important geochemical processes including sorption, dissolution, nucleation, and crystal growth is difficult to obtain from experimental measurements alone would benefit strong continuous progress in molecular simulation. To this end, we present a reactive neural network potential-based dynamics approach simulate the interaction aqueous ions on mineral surfaces contact with liquid water, taking Fe(II) hematite(001) as model system. We show that single potential predicts rate constants for water exchange exergonic chemisorption good agreement observations. The developed herein allows one converge free energy profiles transmission coefficients at density functional theory-level accuracy outperforming state-of-the-art classical force field potentials. This suggests machine learning should become method choice atomistic studies processes.

Language: Английский

---