Atomic-level characterization of liquid/solid interface

Hong, Jiani; Jiang, Ying

doi:10.1088/1674-1056/aba9d0

Cited by 4 publications

(3 citation statements)

References 271 publications

(299 reference statements)

Supporting

Mentioning

Contrasting

Order By: Relevance

“…Although a direct experimental comparison to our results at the atomistic/molecular scale would be desirable, it is not fully available yet to the best of our knowledge. We expect, however, that the rapid development of liquid-phase scanning probe microscopy (SPM) along with spectroscopic techniques will lead in the next few years to atomic-resolution measurements under ambient conditions applicable to NPs in solution. ,− Within the context of SPM, scanning tunneling microscope (STM), electrochemical STM, and two-dimensional and three-dimensional noncontact atomic force microscopy (AFM) are imaging techniques tailored to understand solid–liquid interfaces from an atomistic perspective that, along with spectroscopic techniques, would be ideal for validating the results that we present in this work.…”

Section: Extended Discussionmentioning

confidence: 97%

Highly Heterogeneous Polarization and Solvation of Gold Nanoparticles in Aqueous Electrolytes

Ruiz

Kanduč

et al. 2021

ACS Nano

View full text Add to dashboard Cite

The performance of gold nanoparticles (NPs) in applications depends critically on the structure of the NP−solvent interface, at which the electrostatic surface polarization is one of the key characteristics that affects hydration, ionic adsorption, and electrochemical reactions. Here, we demonstrate significant effects of explicit metal polarizability on the solvation and electrostatic properties of bare gold NPs in aqueous electrolyte solutions of sodium salts of various anions (Cl − , BF 4 − , PF 6 − , nitrophenolate, and 3-and 4-valent hexacyanoferrate), using classical molecular dynamics simulations with a polarizable core−shell model for the gold atoms. We find considerable spatial heterogeneity of the polarization and electrostatic potentials on the NP surface, mediated by a highly facet-dependent structuring of the interfacial water molecules. Moreover, ion-specific, facet-dependent ion adsorption leads to considerable alterations of the interfacial polarization. Compared to nonpolarizable NPs, surface polarization modifies water local dipole densities only slightly but has substantial effects on the electrostatic surface potentials and leads to significant lateral redistributions of ions on the NP surface. Besides, interfacial polarization effects cancel out in the far field for monovalent ions but not for polyvalent ions, as anticipated from continuum "image-charge" concepts. Far-field effective Debye−Huckel surface potentials change accordingly in a valence-specific fashion. Hence, the explicit charge response of metal NPs is crucial for the accurate description and interpretation of interfacial electrostatics (e.g., for charge transfer and interfacial polarization in catalysis and electrochemistry).

show abstract

Section: Extended Discussionmentioning

confidence: 97%

Highly Heterogeneous Polarization and Solvation of Gold Nanoparticles in Aqueous Electrolytes

Ruiz

Kanduč

et al. 2021

ACS Nano

View full text Add to dashboard Cite

show abstract

“…It can be verified from macroscopic experimental phenomena that a larger degree of supercooling can be obtained when supercooled water is cooled with a temperature difference. [34,37] In order to eliminate discrepancies caused by model simplification and assumptions, more accurate temperature distribution within the cluster and on the interface between the water and ice embryo needs to be studied in depth, and the corresponding strict experiments need to be designed with the help of the relevant numerical simulation and advanced experimental techniques [59][60][61] in future work. Our analysis and results will help us to understand ice nucleation under nonequilibrium conditions in fundamental researches, and to better control the stability of supercooled water by using a temperature gradient in practical applications.…”

Section: Discussionmentioning

confidence: 99%

Suppression of ice nucleation in supercooled water under temperature gradients

et al. 2021

View full text Add to dashboard Cite

Understanding the behaviours of ice nucleation in non-isothermal conditions is of great importance for the preparation and retention of supercooled water. Here ice nucleation in supercooled water under temperature gradients is analyzed thermodynamically based on classical nucleation theory (CNT). Given that the free energy barrier for nucleation is dependent on temperature, different from a uniform temperature usually used in CNT, an assumption of linear temperature distribution in the ice nucleus was made and taken into consideration in analysis. The critical radius of the ice nucleus for nucleation and the corresponding nucleation model in the presence of a temperature gradient were obtained. It is observed that the critical radius is determined not only by the degree of supercooling, the only dependence in CNT, but also by the temperature gradient and even the Young’s contact angle. Effects of temperature gradient on the change in free energy, critical radius, nucleation barrier and nucleation rate with different contact angles and degrees of supercooling are illustrated successively. The results show that a temperature gradient will increase the nucleation barrier and decrease the nucleation rate, particularly in the cases of large contact angle and low degree of supercooling. In addition, there is a critical temperature gradient for a given degree of supercooling and contact angle, at the higher of which the nucleation can be suppressed completely.

show abstract

“…at solid surfaces or under confinement in order to understand the electric double layers (EDLs) at electrochemical interfaces , and the water/ion transport in nanofluidic systems . Emerging techniques, such as nitrogen-vacancy center technology and tip-enhanced Raman spectroscopy based on SPM, need to be developed and utilized to achieve the atomic-scale characterization of liquid–solid interfaces and confined water at various interfaces. − Finally, the role of NQEs in water-mediated heterogeneous catalysis, such as water splitting, the formation of hydroxyl/hydronium, water-promoted proton transfer, and solvation effects at interfaces, also deserves in-depth exploration.…”

Section: Conclusion and Perspectivementioning

confidence: 99%

Submolecular Insights into Interfacial Water by Hydrogen-Sensitive Scanning Probe Microscopy

Guo

Jiang

2022

Acc. Chem. Res.

Self Cite

View full text Add to dashboard Cite

Conspectus Water–solid interfaces have attracted extensive attention because of their crucial roles in a wide range of chemical and physical processes, such as ice nucleation and growth, dissolution, corrosion, heterogeneous catalysis, and electrochemistry. To understand these processes, enormous efforts have been made to obtain a molecular-level understanding of the structure and dynamics of water on various solid surfaces. By the use of scanning probe microscopy (SPM), many remarkable structures of H-bonding networks have been directly visualized, significantly advancing our understanding of the delicate competition between water–water and water–solid interactions. Moreover, the detailed dynamics of water molecules, such as diffusion, clustering, dissociation, and intermolecular and intramolecular proton transfer, have been investigated in a well-controlled manner by tip manipulation. However, resolving the submolecular structure of surface water has remained a great challenge for a long time because of the small size and light mass of protons. Discerning the position of hydrogen in water is not only crucial for the accurate determination of the structure of H-bonding networks but also indispensable in probing the proton transfer dynamics and the quantum nature of protons. In this Account, we focus on the recent advances in the H-sensitive SPM technique and its applications in probing the structures, dynamics, and nuclear quantum effects (NQEs) of surface water and ion hydrates at the submolecular level. First, we introduce the development of high-resolution scanning tunneling microscopy/spectroscopy (STM/S) and qPlus-based atomic force microscopy (qPlus-AFM), which allow access to the degrees of freedom of protons in both real and energy space. qPlus-AFM even allows imaging of interfacial water in a weakly perturbative manner by measuring the high-order electrostatic force between the CO-terminated tip and the polar water molecule, which enables the subtle difference of OH directionality to be discerned. Next we showcase the applications of H-sensitive STM/AFM in addressing several key issues related to water–solid interfaces. The surface wetting behavior and the H-bonding structure of low-dimensional ice on various hydrophilic and hydrophobic solid surfaces are characterized at the atomic scale. Then we discuss the quantitative assessment of NQEs of surface water, including proton tunneling and quantum delocalization. Moreover, the weakly perturbative and H-sensitive SPM technique can be also extended to investigations of water–ion interactions on solid surfaces, revealing the effect of hydration structure on the interfacial ion transport. Finally, we provide an outlook on the further directions and challenges for SPM studies of water–solid interfaces.

show abstract

Atomic-level characterization of liquid/solid interface

Cited by 4 publications

References 271 publications

Highly Heterogeneous Polarization and Solvation of Gold Nanoparticles in Aqueous Electrolytes

Highly Heterogeneous Polarization and Solvation of Gold Nanoparticles in Aqueous Electrolytes

Suppression of ice nucleation in supercooled water under temperature gradients

Submolecular Insights into Interfacial Water by Hydrogen-Sensitive Scanning Probe Microscopy

Contact Info

Product

Resources

About