arXiv subjects

Julie Villanova

Publications and source records attributed to Julie Villanova.

4 recordsLinked to original sources

arXiv2025

The crystalline properties of silica biomorphs vary within and between morphologies

Silica-witherite biomorphs are a class of emergent materials, i.e. composite microstructures made of nanometric barium carbonate surrounded by amorphous silica. They form via co-precipitation of barium carbonate and siliceous species, and self-organize into a multitude of shapes with a distinct long-range order of the carbonate nanocrystals. However, the internal structural organization within and across different morphologies remains insufficiently resolved. Here, we use X-ray texture and diffraction tomography to create three-dimensional, spatially resolved maps of crystallographic orientation and structural parameters in silica-witherite biomorphs. At the sub-micron voxel level, all morphologies exhibit a crystallographic order consistent with a fiber texture around the c-axis. At larger length scales, however, the orientation field as well as crystallite size, crystallite shape anisotropy and the unit cell volume show systematic spatial variations. Leaf-like and helical morphologies contain defined directions along which structural parameters change systematically. Furthermore, we find recurring structural regimes with strong similarities between these morphologies. Conversely, coral-like morphologies are overall less textured and outside of the nucleation region we do not find clear structural regimes in the crystalline properties. These results provide a three-dimensional description of the internal organization of crystallites in silica-witherite biomorphs and establish a basis for systematically relating crystallographic organization to morphology.

cond-mat.mtrl-sci↗

arXiv2025

4D operando X-ray nano-holo-tomography reveals multiscale chemomechanics in Silicon-Graphite anode

Linking electrode microstructure to electrochemical performance is essential for optimizing Li-ion batteries. However, this requires mechanistic 4D observations at ultimate spatio-temporal scales, which remains elusive. Here we demonstrate the use of operando synchrotron X-ray nano-holo-tomography combined with Digital Volume Correlation to track chemomechanical dynamics at both particle (local) and electrode (averaged) scales. Quantitative scale-bridging image analysis is applied to a high-capacity silicon-graphite anode during its formation cycle. Our findings reveal that local diffusion properties, graphite particle morphology and position in the electrode, distance to silicon clusters, surface contact with electrolyte and mechanical deformations, all have a direct impact on the local electrochemical activity and irreversibility - but these parameters are not equally important. Particularly, we identify fast diffusion channels that play a key role and counterbalance intrinsic depth-dependent reaction heterogeneities due to ionic/electronic diffusion limitations. The various structural factors that determine Gr-Si battery performance beyond ensemble properties are classified using a scale of influence, providing a practical framework for the optimization of materials and electrode manufacturing.

physics.app-ph↗

arXiv2023

Binder-free CNT cathodes for Li-O$_2$ batteries with more than one life

Li-O$_2$ batteries (LOB) performance degradation ultimately occurs through the accumulation of discharge products and irreversible clogging of the porous electrode during the cycling. Electrode binder degradation in the presence of reduced oxygen species can result in additional coating of the conductive surface, exacerbating capacity fading. Herein, we establish a facile method to fabricate free-standing, binder-free electrodes for LOBs in which multi-wall carbon nanotubes (MWCNT) form cross-linked networks exhibiting high porosity, conductivity, and flexibility. These electrodes demonstrate high reproducibility upon cycling in LOBs. After cell death, efficient and inexpensive methods to wash away the accumulated discharge products are demonstrated, as reconditioning method. The second life usage of these electrodes is validated, without noticeable loss of performance. These findings aim to assist in the development of greener high energy density batteries while reducing manufacturing and recycling costs.

cond-mat.mtrl-sci↗

arXiv2020

Boosting spatial resolution by incorporating periodic boundary conditions into single-distance hard-x-ray phase retrieval

A simple coherent-imaging method due to Paganin et al. is widely employed for phase-amplitude reconstruction of samples using a single paraxial x-ray propagation-based phase-contrast image. The method assumes that the sample-to-detector distance is sufficiently small for the associated Fresnel number to be large compared to unity. The algorithm is particularly effective when employed in a tomographic setting, using a single propagation-based phase-contrast image for each projection. Here we develop a simple extension of the method, which improves the reconstructed contrast of very fine sample features. This provides first-principles motivation for boosting fine spatial detail associated with high Fourier frequencies, relative to the original method, and was inspired by several recent works employing empirically-obtained Fourier filters to a similar end.

eess.IV↗