A5039136448- Calcium Carbonate Crystallization and Inhibition
- Advanced X-ray Imaging Techniques
- Advanced Battery Materials and Technologies
- Advancements in Battery Materials
- X-ray Diffraction in Crystallography
- Bone Tissue Engineering Materials
- Paleontology and Stratigraphy of Fossils
- Advanced Battery Technologies Research
- Advanced Electron Microscopy Techniques and Applications
- Catalytic Processes in Materials Science
- Force Microscopy Techniques and Applications
- Nuclear Physics and Applications
- Hydrocarbon exploration and reservoir analysis
- High-pressure geophysics and materials
- Mesoporous Materials and Catalysis
- Advanced X-ray and CT Imaging
- Building materials and conservation
- Zeolite Catalysis and Synthesis
- Chemical Synthesis and Characterization
- Mineral Processing and Grinding
- Enhanced Oil Recovery Techniques
- Fuel Cells and Related Materials
- Diatoms and Algae Research
- Crystallization and Solubility Studies
- Clay minerals and soil interactions
Paul Scherrer Institute
2017-2024
University of Oxford
2019-2024
Swiss Light Source
2018-2021
University of Leeds
2012-2019
Trier University of Applied Sciences
2014
Abstract The mechanisms by which amorphous intermediates transform into crystalline materials are poorly understood. Currently, attracting enormous interest is the crystallization of calcium carbonate, a key intermediary in synthetic, biological and environmental systems. Here we attempt to unify many contrasting apparently contradictory studies investigating this process detail. We show that carbonate can dehydrate before crystallizing, both solution air, while thermal analyses solid-state...
Abstract The term mesocrystal has been widely used to describe crystals that form by oriented assembly, and exhibit nanoparticle substructures. Using calcite co-precipitated with polymers as a suitable test case, this article looks critically at the concept of mesocrystals. Here we demonstrate data commonly assign structure may be frequently misinterpreted, these calcite/polymer do not have Although morphologies suggest presence nanoparticles, are only present on crystal surface. High...
Abstract Aggregation‐based crystal growth often gives rise to crystals with complex morphologies which cannot be generated via classical processes. Despite this, understanding of the mechanism is rather poor, particularly when organic additives or amorphous precursor phases are present. In this work, advantage taken observation that aggregation‐based calcium carbonate, and indeed many other minerals, most observed using diffusion‐based synthetic methods. By fully characterizing widely used...
Abstract Amorphous calcium carbonate (ACC) is an important intermediate in the formation of crystalline CaCO 3 biominerals, where its crystallization controlled using soluble additives. However, although this transformation often occurs solid state, experiments mainly focus on effect additives ACC solution. This paper addresses issue and compares crystallization, solution precipitated presence a range Surprisingly, these results show that some exhibit Janus behavior, they retard solution,...
Abstract Since its commercial introduction three-quarters of a century ago, fluid catalytic cracking has been one the most important conversion processes in petroleum industry. In this process, porous composites composed zeolite and clay crack heavy fractions crude oil into transportation fuel petrochemical feedstocks. Yet, over time activity these composite particles decreases. Here, we report on ptychographic tomography, diffraction, fluorescence as well electron microscopy measurements,...
Knowledge of electrolyte transport and thermodynamic properties in Li-ion beyond technologies is vital for their continued development success. Here, we present a method fully characterising systems. By measuring the concentration gradient over time via operando Raman microspectroscopy, tandem with potentiostatic electrochemical impedance spectroscopy, Fickian "apparent" diffusion coefficient, transference number, factor, ionic conductivity resistance charge-transfer were quantified within...
Understanding and characterizing the transport thermodynamic properties of electrolytes are critical for optimizing battery performance. In this study, we employ operando Raman gradient analysis (ORGA) to characterize concentration-dependent diffusion coefficient, transference number, ionic conductivity, factor potassium bis(fluorosulfonyl)imide (KFSI) in triethyl phosphate (TEP), an ideal model system one most promising K-ion electrolytes. ORGA demonstrates results consistent with...
A facile one-pot method is described for the formation of novel heterostructures in which inorganic nanoparticles are homogeneously distributed throughout an single crystal matrix. Our strategy uses functionalised with a poly(sodium 4-styrenesulphonate)-poly(methacrylic acid) [PNaStS-PMAA] diblock copolymer as soluble growth additive. This plays number essential roles. The PMAA anchor block physically adsorbed onto nanoparticles, while PNaStS acts electrosteric stabiliser and ensures that...
A simple synthetic method is presented for the precipitation of high purity, dry amorphous calcium carbonate (ACC) based on freeze-drying saturated, counter ion free CaCO3 solutions, where ACC produced shows an extended atmospheric stability. Translation methodology to phosphate demonstrates generality approach.
X-ray absorption near-edge structure (XANES) spectroscopy and spectromicroscopy have been extensively used to characterize biominerals. Using either Ca or C spectra, unique information has obtained regarding amorphous biominerals nanocrystal orientations. Building on these results, we demonstrate that recording XANES spectra of calcium carbonate at the oxygen K-edge enables polarization-dependent imaging contrast (PIC) mapping with unprecedented contrast, signal-to-noise ratio,...
Inspired by the observation that crystalline calcium carbonate and phosphate biominerals frequently form via amorphous precursors, a wide range of studies have been performed which demonstrate many inorganic crystals can precipitate from solution phases. This article considers crystallization mechanism oxalate, is significant biomineral in plants primary constituent kidney stones vertebrates, shows this also an precursor phase aqueous solution. A approaches were employed to study oxalate...
To a large extent, the performance of imaging systems is determined by their objectives, which affect properties as varied collection efficiency, resolving power, and image distortions. Such limitations can be addressed so-called aperture synthesis, technique used, for instance, in radar, astronomy, and, increasingly, microscopy. Here, we apply such techniques to x-ray demonstrate how Fourier ptychography used at transmission microscopes increase resolution, provide quantitative absorption...
Abstract Most of our knowledge dislocation-mediated stress relaxation during epitaxial crystal growth comes from the study inorganic heterostructures. Here we use Bragg coherent diffraction imaging to investigate a contrasting system, calcite (CaCO 3 ) crystals on organic self-assembled monolayers, where these are widely used as model for biomineralization processes. The imaged simultaneously visualize morphology and internal strain fields. Our data reveal that each possesses single...
Single-crystals of vaterite, the least-stable anhydrous polymorph CaCO3, are rare in biogenic and synthetic systems. We here describe synthesis high aspect ratio single crystal vaterite rods under additive-free conditions by precipitating CaCO3 within cylindrical pores track-etch membranes.
Abstract From biomineralization to synthesis, organic additives provide an effective means of controlling crystallization processes. There is growing evidence that these are often occluded within the crystal lattice. This promises elegant creating nanocomposites and tuning physical properties. Here we use incorporation sulfonated fluorescent dyes gain new understanding additive occlusion in calcite (CaCO 3 ), link morphological changes mechanisms. We demonstrate incorporated specific zones,...
A "crystal hotel" microfluidic device that allows crystal growth in confined volumes to be studied situ is used produce large calcite single crystals with predefined crystallographic orientation, microstructure, and shape by control of the detailed physical environment, flow, surface chemistry. This general approach can extended form technologically important, nanopatterned crystals. Control over crystallization yield particles defined sizes, morphologies, polymorphs, orientations a subject...
Biomineralisation processes invariably occur in the presence of multiple organic additives, which act combination to give exceptional control over structures and properties. However, few synthetic studies have investigated cooperative effects soluble additives. This work addresses this challenge focuses on combined amino acids coloured dye molecules. The experiments demonstrate that strongly calcite crystals only form Brilliant Blue R (BBR) four seventeen acids, as compared with almost...
Fluid catalytic cracking is a chemical conversion process of industrial scale. This process, utilizing porous catalysts composed clay and zeolite, converts heavy crude-oil fractions into transportation fuel petrochemical feedstocks. Among other factors iron-rich reactor feedstream impurities cause these catalyst particles to permanently deactivate. Herein, we report tomographic X-ray absorption spectroscopy measurements that reveal the presence dissimilar iron specific localization within...
Bragg coherent diffraction imaging to visualize the effects of lysine and magnesium on internal structures calcite crystals.
Highlights•Correlative ptychographic tomography with 35 nm resolution and diffraction tomography•3D micro-cracks in secondary Li-rich NMC particles correlated crystal lattice•Radial secondary-particle-size-dependent material degradation•Intriguing core-shell structure observed 3D crystalline mapsSummaryThe search for higher performance, improved safety, lifetime of lithium-ion batteries relies on the understanding degradation mechanisms. Complementary to methods studies primary or bulk...
We developed a spectro-nanotomography method that enables fast chemical characterization of functional materials.
Abstract The introduction of structural defects in metal–organic frameworks (MOFs), often achieved through the fractional use defective linkers, is emerging as a means to refine properties existing MOFs. These missing coordination fragments, create unsaturated framework nodes that may alter MOF. A property‐targeted utilization this approach demands an understanding structure defect‐engineered We demonstrate full‐field X‐ray absorption near‐edge computed tomography can help improve our...
The high-voltage (4.7 V vs Li+/Li) spinel lithium nickel manganese oxide (LiNi0.5Mn1.5O4, LNMO) is a promising candidate for the next generation of lithium-ion batteries due to its high energy density, low cost, and environmental impact. However, poor cycling performance at cutoff potentials limits commercialization. Herein, hollow-structured LNMO synergistically paired with an ionic liquid electrolyte, 1 M bis(fluorosulfonyl)imide (LiFSI) in N-propyl-N-methylpyrrolidinium (Pyr1,3FSI),...