<i>In situ</i> electrochemistry inside a TEM with controlled mass transport

Sun, Hongyu; Lemang, Mathilde; Omme, J. Tijn van; Spruit, Ronald G.; Bremmer, Marien; Basak, Shibabrata; Garza, Héctor Hugo Pérez

doi:10.1039/d0nr04961a

Cited by 33 publications

(26 citation statements)

References 27 publications

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“…The advent of in situ liquid phase TEM (LP-TEM) and SEM (LP-SEM) in microfabricated silicon/silicon nitride cells and sandwiched graphene films has enabled direct observation of mineral particles in solution, including their nucleation, growth, interaction dynamics, aggregation, and fusion. ,− Commercial microfabricated TEM cells can include capabilities for fluid flow, ,− mixing of reagents, heating to near 100 °C, , and the application of electric fields. − In situ LP-TEM and -SEM have led to numerous important discoveries about the behavior of mineral systems in aqueous electrolytes. For example, a recent study by Zhu et al provided an explanation for the formation of self-similar hematite mesocrystals from ferrihydrite suspensions, which has significant consequences for understanding the structural and chemical heterogeneity at mineral–water interfaces.…”

Section: Future Directionsmentioning

confidence: 99%

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: Future Directionsmentioning

confidence: 99%

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

et al. 2023

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“…The system allows to control the liquid thickness well below the beam broadening threshold, enabling resolutions that can go even down to 2.15 Å [1], as it has been reported before for a 100nm liquid thickness. Such control of the liquid thickness enables elemental mapping, allowing users to distinguish the spatial distribution of different elements in liquid.…”

mentioning

confidence: 78%

Advanced In-situ Liquid Phase Transmission Electron Microscopy: A Powerful Tool for Pharmaceutical Studies and Life Science Applications

Sun

Mathisen

Bladt

et al. 2022

Microscopy and Microanalysis

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We introduce our technology for in-situ liquid phase studies inside the Transmission Electron Microscope. The system relies on a Micro Electro-Mechanical System (MEMS)-based device as a smart sample carrier, which contains an integrated set of biasing electrodes (i.e. to perform liquid biasing, or bio-electrochemical studies) or an integrated microheater (i.e. to perform liquid heating experiments). These capabilities enable in-situ pharmaceutical and life science studies.

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“…Various experimental LP-TEM setups supporting flow of the liquid in the imaging area are available nowadays [17,18,33,35,36]. All setups are based on microchips being allocated in the tip of a microfluidic TEM sample holder and can be categorised in two classes based on the way how the flow is directed.…”

Section: Strategies To Account For Radiolysismentioning

confidence: 99%

The effect of flow on radiolysis in liquid phase-TEM flow cells

Merkens

Salvo

2022

Nano Ex.

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Applying a continuous flow to rinse radiolytic species from the irradiated volume is a widely proposed strategy to reduce beam-related artefacts in Liquid-Phase Transmission Electron Microscopy (LP-TEM). However, this has not been verified experimentally nor theoretically to date. Here we explore an extended numerical model implementing radiolytic chemistry, diffusion and liquid convection to study the peculiarities of beam-induced chemistry in the presence of a flowing liquid within a heterogenously irradiated nanoconfined channel corresponding to a LP-TEM flow cell. Intruigingly, the concentration of some principal chemical species, predominantly hydrogen radicals and hydrated electrons, is found to grow significantly rather than to decrease in respect to zero-flow when moderate flow conditions are applied. This counterintuitive behaviour is discussed in terms of reactants’ lifetimes, spatial separation of the reaction network and self-scavenging by secondary radiolitic species. In the presence of a flow the consumption of highly reactive species is suppressed due to removal of the self-scavengers, and as a result their concentration in irradiated area increases. A proof of concept for the scavengers supply by the flow is demonstrated. Unravelling the effect of flow on radiolysis spawns direct implications for LP-TEM flow experiments providing yet one more control parameter for adjusting the chemistry in the irradiated/imaging area, in particular for mitigation strategies by continuous supply of scavengers.

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In situ electrochemistry inside a TEM with controlled mass transport

Abstract: The field of electrochemistry promises solutions for the future energy crisis and environmental deterioration by developing optimized batteries, fuel-cells and catalysts. Combined with in situ Transmission Electron Microscope (TEM), it...

Cited by 33 publications

References 27 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

Advanced In-situ Liquid Phase Transmission Electron Microscopy: A Powerful Tool for Pharmaceutical Studies and Life Science Applications

The effect of flow on radiolysis in liquid phase-TEM flow cells

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