Nonclassical nucleation towards separation and recycling science: Iron and aluminium (Oxy)(hydr)oxides

Lukić, Miodrag J.; Gebauer, Denis; Rose, Arthur W.

doi:10.1016/j.cocis.2020.03.010

Cited by 13 publications

(16 citation statements)

References 79 publications

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Section: Theme 3: Dissolution Nucleation and Growthmentioning

confidence: 99%

“…Specifically, for metal oxides, Figure 56 illustrates both classical and nonclassical nucleation theoretic views of the formation of Fe-and Al-oxides (FeO x /AlO x ). 995 Based on classical nucleation theory, ferrihydrite can form directly (top), via unstable and metastable crystalline nuclei. In nonclassical nucleation (blue box), there are multiple overlapping pathways for forming stable associated states.…”

Section: Mineral Precipitationmentioning

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: Theme 3: Dissolution Nucleation and Growthmentioning

confidence: 99%

Section: Mineral Precipitationmentioning

confidence: 99%

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

et al. 2023

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“…In the case of the PNC pathway, the event of phase separation then does not rely on overcoming a certain critical size (nucleation barrier, or level of supersaturation) as in CNT (Figure 1, top), but rather on a distinct decrease in their structural and/or configurational dynamics upon coordination or chemical changes occurring within the clusters. [17,[19][20][21][22] Hereby, phase separation does not occur spontaneously from PNCs due to significant barriers associated with further dehydration. [23] This provides an answer to the above question: Stable solute clusters (PNCs) can participate in phase separation when they undergo subtle changes in structure, slowing down the cluster dynamics.…”

Section: G Rtmentioning

confidence: 99%

“…[32,33] Sommerdijk and co-workers [34] recently introduced a novel, quantitative, kinetic model for non-classical crystallization. While the claimed initial occurrence of very small ferrihydrite nanoparticles has been challenged elsewhere, [21] due to the highly ambiguous interpretation of experimental data, this model considers the balance of colloidal forces between nanocrystals as previously proposed by Cölfen and Figure 2. Flow scheme for the assignment of theories (circles) based on distinct experimental observations for crystallization from solution.…”

Section: Recent Progress In Nucleation and Crystallization Theoriesmentioning

confidence: 99%

Crystal Nucleation and Growth of Inorganic Ionic Materials from Aqueous Solution: Selected Recent Developments, and Implications

Gebauer

Gale

Cölfen

2022

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In this review article, selected, latest theoretical, and experimental developments in the field of nucleation and crystal growth of inorganic materials from aqueous solution are highlighted, with a focus on literature after 2015 and on non‐classical pathways. A key point is to emphasize the so far underappreciated role of water and solvent entropy in crystallization at all stages from solution speciation through to the final crystal. While drawing on examples from current inorganic materials where non‐classical behavior has been proposed, the potential of these approaches to be adapted to a wide‐range of systems is also discussed, while considering the broader implications of the current re‐assessment of pathways for crystallization. Various techniques that are suitable for the exploration of crystallization pathways in aqueous solution, from nucleation to crystal growth are summarized, and a flow chart for the assignment of specific theories based on experimental observations is proposed.

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“…In aqueous solution, Fe 3+ exists as hexacoordinated aquo complexes (Fe(H 2 O) 6 3+ ), which deprotonate and form monomeric complexes Fe(OH) n (H 2 O) 6– n (3– n )+ at elevated temperature or pH . Continuously, these monomers condense into dimers, trimers, and higher nuclearity species through the elimination of water, known as the olation and oxolation process. − A similar process occurs for Fe 2+ , except for beginning with the condensation of ferrous monomers [Fe(OH) n (H 2 O) 6– n ] (2– n )+ . For iron oxides, thermodynamically stable solute nanometric species are widely observed at this stage and are recognized as PNCs, − including the Fe 13 Keggin clusters with radius of ∼0.45 nm − and olation polymers [Fe(OH) 2+ ] cluster up to a few nanometers in size .…”

Section: Crystallization Pathway Of Magnetitementioning

confidence: 99%

Recent Advances in Magnetite Crystallization: Pathway, Modulation, and Characterization

Shi

Feng

et al. 2023

Crystal Growth & Design

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Magnetite has wide applications in the fields of environment, biomedicine, and energy storage. Understanding the crystallization process of magnetite will improve the design and control of its properties. However, the challenge lies in determining the crystallization pathway of magnetite due to its nanosized and unstable intermediates. Recent developments in the in situ characterization techniques have shed light on this process, which has rarely been elucidated systematically. This review builds the correlation between the typical synthesis methods and the corresponding properties of magnetite. It also outlines a general multistage crystallization pathway involving a series of intermediates and explains how various strategies (e.g., pH and additives) modulate magnetite properties by influencing its intermediates during crystallization. To better illustrate published observations and reconcile conflicting perspectives, classical and state-of-the-art crystallization theories will be incorporated into each aspect. Moreover, this review highlights the importance of in situ characterization techniques, which enables the precise observation of crystallization processes. The goal of this review is to provide a fundamental understanding of magnetite crystallization and to guide the bottom-up design of magnetic materials for diverse applications.

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Nonclassical nucleation towards separation and recycling science: Iron and aluminium (Oxy)(hydr)oxides

Cited by 13 publications

References 79 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

Crystal Nucleation and Growth of Inorganic Ionic Materials from Aqueous Solution: Selected Recent Developments, and Implications

Recent Advances in Magnetite Crystallization: Pathway, Modulation, and Characterization

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