Dynamics in hydrated inorganic nanotubes studied by neutron scattering: towards nanoreactors in water

Caër, Sophie Le; Pignié, Marie-Claire; Berrod, Quentin; Grzimek, Veronika; Russina, Margarita; Carteret, Cédric; Thill, Antoine; Zanotti, Jean-Marc; Teixeira, J.

doi:10.1039/d0na00765j

Cited by 7 publications

(8 citation statements)

References 54 publications

(91 reference statements)

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“…Adding salts, such as NaCl that fully dissociates and does not affect bulk solution pH, can drive a pH change in an aqueous suspension of oxide particles. This is typically explained to be a consequence of ion driven deprotonation above the point of zero charge of surface hydroxyl groups that leaves behind negatively charged surface groups that complex with salt cations, driving changes in interfacial water structure. , …”

Section: Methodsmentioning

confidence: 99%

“…This is typically explained to be a consequence of ion driven deprotonation above the point of zero charge of surface hydroxyl groups that leaves behind negatively charged surface groups that complex with salt cations, 241 driving changes in interfacial water structure. 338,339 2.3.2.5. Spatial and Structural Heterogeneities of Surfaces and Interfaces.…”

Section: H-bondmentioning

confidence: 99%

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Oxide– and Silicate–Water Interfaces and Their Roles in Technology and the Environment

et al. 2023

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Interfacial reactions drive all elemental cycling on Earth and play pivotal roles in human activities such as agriculture, water purification, energy production and storage, environmental contaminant remediation, and nuclear waste repository management. The onset of the 21st century marked the beginning of a more detailed understanding of mineral aqueous interfaces enabled by advances in techniques that use tunable high-flux focused ultrafast laser and X-ray sources to provide near-atomic measurement resolution, as well as by nanofabrication approaches that enable transmission electron microscopy in a liquid cell. This leap into atomic-and nanometer-scale measurements has uncovered scale-dependent phenomena whose reaction thermodynamics, kinetics, and pathways deviate from previous observations made on larger systems. A second key advance is new experimental evidence for what scientists hypothesized but could not test previously, namely, interfacial chemical reactions are frequently driven by "anomalies" or "non-idealities" such as defects, nanoconfinement, and other nontypical chemical structures. Third, progress in computational chemistry has yielded new insights that allow a move beyond simple schematics, leading to a molecular model of these complex interfaces. In combination with surfacesensitive measurements, we have gained knowledge of the interfacial structure and dynamics, including the underlying solid surface and the immediately adjacent water and aqueous ions, enabling a better definition of what constitutes the oxide− and silicate−water interfaces. This critical review discusses how science progresses from understanding ideal solid−water interfaces to more realistic systems, focusing on accomplishments in the last 20 years and identifying challenges and future opportunities for the community to address. We anticipate that the next 20 years will focus on understanding and predicting dynamic transient and reactive structures over greater spatial and temporal ranges as well as systems of greater structural and chemical complexity. Closer collaborations of theoretical and experimental experts across disciplines will continue to be critical to achieving this great aspiration.

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Section: Methodsmentioning

confidence: 99%

Section: H-bondmentioning

confidence: 99%

Oxide– and Silicate–Water Interfaces and Their Roles in Technology and the Environment

et al. 2023

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“…The morphology of Imo-CH3 nanotubes is well characterized by various techniques such as FT-IR, SAXS and TEM, as extensively discussed in previous publications from our group. [47][48][49]67 CH3 (e-g). The DBAN loading concentrations are: 9 x 10 -6 mol.g -1 (e), 3.1 x 10 -5 mol.g -1 (f) and 8.1 x 10 -4 mol.g -1 (g).…”

Section: Resultsmentioning

confidence: 99%

Inorganic nanotubes with permanent wall polarization as dual photo-reactors for wastewater treatment with simultaneous fuel production

Patra

Schaming

Picot

et al. 2021

Environ. Sci.: Nano

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“…DFT simulation of different hydroxylated and methylated INTs indicates that the dipole density across the wall, and associated electrostatic potential steps (Figure 2 ), is effective in tuning not only the adsorption geometry and energies of interacting molecules such as H 2 O but also the energy alignment of the molecules’ electron acceptor and donor levels. [ 86 ] Combined with the demonstrated effects of the nanotubes structure and electrostatic environment in altering the molecular motions at the nanotube–H 2 O interfaces, [ 87 , 88 ] these findings prompt for additional research in the potential of INTs and associated radial polarization for the design and control of electron transfer kinetics at H 2 O interfaces as necessary for improved, up‐scalable photocatalytic strategies to hydrogen generation.…”

Section: Main Features and Physical‐chemical Propertiesmentioning

confidence: 99%

Imogolite Nanotubes and Their Permanently Polarized Bifunctional Surfaces for Photocatalytic Hydrogen Production

Paineau,

Teobaldi,

Jiménez‐Calvo

2023

Global Challenges

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To date, imogolite nanotubes (INTs) have been primarily used for environmental applications such as dye and pollutant degradation. However, imogolite's well‐defined porous structure and distinctive electro‐optical properties have prompted interest in the system's potential for energy‐relevant chemical reactions. The imogolite structure leads to a permanent intrawall polarization arising from the presence of bifunctional surfaces at the inner and outer tube walls. Density functional theory simulations suggest such bifunctionality to encompass also spatially separated band edges. Altogether, these elements make INTs appealing candidates for facilitating chemical conversion reactions. Despite their potential, the exploitation of imogolite's features for photocatalysis is at its infancy, thence relatively unexplored. This perspective overviews the basic physical‐chemical and optoelectronical properties of imogolite nanotubes, emphasizing their role as wide bandgap insulator. Imogolite nanotubes have multifaceted properties that could lead to beneficial outcomes in energy‐related applications. This work illustrates two case studies demonstrating a step‐forward on photocatalytic hydrogen production achieved through atomic doping or metal co‐catalyst. INTs exhibit potential in energy conversion and storage, due to their ability to accommodate functions such as enhancing charge separation and influencing the chemical potentials of interacting species. Yet, tapping into potential for energy‐relevant application needs further experimental research, computational, and theoretical analysis.

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Dynamics in hydrated inorganic nanotubes studied by neutron scattering: towards nanoreactors in water

Abstract: The interior of hydrophobic inorganic nanotubes is a favorable place for nanoconfined chemical reactions, contrary to water-filled hydrophilic nanotubes.

Cited by 7 publications

References 54 publications

Oxide– and Silicate–Water Interfaces and Their Roles in Technology and the Environment

Oxide– and Silicate–Water Interfaces and Their Roles in Technology and the Environment

Inorganic nanotubes with permanent wall polarization as dual photo-reactors for wastewater treatment with simultaneous fuel production

Imogolite Nanotubes and Their Permanently Polarized Bifunctional Surfaces for Photocatalytic Hydrogen Production

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