Electrocatalytic CO2 reduction has been developed as a promising and attractive strategy to achieve carbon neutrality for sustainable chemical production. Among various reduction products, multi-carbon (C2+) compounds with higher energy...

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Electrochemical Reduction of Carbon Dioxide to Multicarbon (C2+) Products: Challenges and Perspectives

Metal-organic frameworks (MOFs) are crystalline nanoporous materials with great potential for a wide range of industrial applications. Understanding the nucleation and early growth stages of these materials from a solution is critical for their design and synthesis. Despite their importance, the pathways through which MOFs nucleate are largely unknown. Using a combination of in situ liquid-phase and cryogenic transmission electron microscopy, we show that zeolitic imidazolate framework-8 MOF nanocrystals nucleate from precursor solution via three distinct steps: 1) liquid-liquid phase separation into solute-rich and solute-poor regions, followed by 2) direct condensation of the solute-rich region into an amorphous aggregate and 3) crystallization of the aggregate into a MOF. The three-step pathway for MOF nucleation shown here cannot be accounted for by conventional nucleation models and provides direct evidence for the nonclassical nucleation pathways in open-framework materials, suggesting that a solute-rich phase is a common precursor for crystallization from a solution.

https://www.pnas.org/content/pnas/118/10/e2008880118.full.pdf

Three-step nucleation of metal-organic framework nanocrystals.

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 surface-sensitive 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.

Oxide- and Silicate-Water Interfaces and Their Roles in Technology and the Environment.

Graphene liquid cell electron microscopy (GLC-EM), a cutting-edge liquid-phase EM technique, has become a powerful tool to directly visualize wet biological samples and the microstructural dynamics...

Graphene Liquid Cell Electron Microscopy: Progress, Applications, and Perspectives

Electron tomography (ET) has become a well-established technique to visualize nanomaterials in three dimensions. A vast richness in information can be gained by ET, but the conventional acquisition...

Fast Electron Tomography for Nanomaterials

Liquid phase transmission electron microscopy has become a powerful tool for imaging the structure and dynamics of materials in solution Direct observation of material formation, modification and operation has provided unique insights into the chemistry that governs the structure–property relationships of materials with myriad applications including optical, magnetic and electronic materials However, full control over the reaction environment inside the microscope, especially the solution temperature and concentration of reactants, remains challenging and has limited the application of this high-resolution methodology Here we present the ‘Stream Liquid Heating Holder’, a complete system for liquid phase experiments at elevated temperature inside the transmission electron microscope This system features a unique on-chip flow channel combined with a microheater The channel enables direct flow over the imaging area and rapid replenishment of the solution inside the Nano-cell with simultaneous heating to more than 100 °C The capabilities of the system are demonstrated by studying the liquid flow dynamics and comparing the temperature dependent etching kinetics of silica nanoparticles by in situ liquid phase electron microscopy to in-flask experiments

Liquid phase transmission electron microscopy with flow and temperature control

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 microscopy (TEM), it can reveal functional and structural changes. A drawback of this relatively young field is lack of reproducibility in controlling the liquid environment while retaining the imaging and analytical capabilities. Here, a platform for in situ electrochemical studies inside a TEM with a pressure-driven flow is presented, with the capability to control the flow direction and to ensure the liquid will always pass through the region of interest. As a result, the system offers the opportunity to define the mass transport and control the electric potential, giving access to the full kinetics of the redox reaction. In order to show the benefits of the system, copper dendrites are electrodeposited and show reliable electric potential control. Next, their morphology is changed by tuning the mass transport conditions. Finally, at a liquid thickness of approximately 100 nm, the diffraction pattern revealed the 〈1,1,1〉 planes of the copper crystals, indicating an atomic resolution down to 2.15 A. Such control of the liquid thickness enabled elemental mapping, allowing us to distinguish the spatial distribution of different elements in liquid.

In situ electrochemistry inside a TEM with controlled mass transport.

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Liquid phase transmission electron microscopy with flow and temperature control

In situ electrochemistry inside a TEM with controlled mass transport.