Evaluation of the compositional changes during flooding of reactive fluids using scanning electron microscopy, nano-secondary ion mass spectrometry, x-ray diffraction, and whole-rock geochemistry

Outcrop chalk of late Campanian age (Gulpen Formation) from Liège (Belgium) was flooded with MgCl2 in a triaxial cell for 516 days under reservoir conditions to understand how the non-equilibrium nature of the fluids altered the chalks. The study is motivated by enhanced oil recovery (EOR) processes because dissolution and precipitation change the way in which oils are trapped in chalk reservoirs. Relative to initial composition, the first centimeter of the flooded chalk sample shows an increase in MgO by approximately 100, from a weight percent of 0.33% to 33.03% and a corresponding depletion of CaO by more than 70% from 52.22 to 14.43 wt.%. Except for Sr, other major or trace elements do not show a significant change in concentration. Magnesite was identified as the major newly grown mineral phase. At the same time, porosity was reduced by approximately 20%. The amount of Cl− in the effluent brine remained unchanged, whereas Mg2+ was depleted and Ca2+ enriched. The loss of Ca2+ and gain in Mg2+ are attributed to precipitation of new minerals and leaching the tested core by approximately 20%, respectively. Dramatic mineralogical and geochemical changes are observed with scanning electron microscopy–energy-dispersive x-ray spectroscopy, nano secondary ion mass spectrometry, x-ray diffraction, and whole-rock geochemistry techniques. The understanding of how fluids interact with rocks is important to, for example, EOR, because textural changes in the pore space affect how water will imbibe and expel oil from the rock. The mechanisms of dissolution and mineralization of fine-grained chalk can be described and quantified and, when understood, offer numerous possibilities in the engineering of carbonate reservoirs.acceptedVersio

CASPワークショップ参加記

The nanostructure of the active layer in polymer/fullerene bulk heterojunction solar cells is known to have a strong impact on the device performances. Controlling the polymer/fullerene blend morphology is therefore particularly important. In this work, a rod-coil block copolymer, based on a regioregular poly(3-hexylthiophene) electron-donor rod block and a C-60-grafted coil block, is used as compatibilizer and its influences on the thin film morphology as well as the photovoltaic performances are investigated. It is shown that a small fraction of compatibilizer can enhance the device performances in an otherwise non-optimized process. At higher fractions or long annealing times however, the fullerene-grafted copolymer is found to behave as a nucleation center and triggers the formation of fullerene crystals

High-Resolution Topographic and Chemical Surface Imaging of Chalk for Oil Recovery Improvement Applications

Chalk is a very fine-grained carbonate and can accommodate high porosity which is a key characteristic for high-quality hydrocarbon reservoirs. A standard procedure within Improved Oil Recovery (IOR) is seawater-injection which repressurizes the reservoir pore pressure. Long-term seawater-injection will influence mineralogical processes as dissolution and precipitation of secondary minerals. These secondary minerals (<1 micrometer) precipitate during flooding experiments mimicking reservoir conditions. Due to their small sizes, analysis from traditional scanning electron microscopy combined with energy dispersive X-ray spectroscopy is not conclusive because of insufficient spatial resolution and detection limit. Therefore, chalk was analyzed with high-resolution imaging by helium ion microscopy (HIM) combined with secondary ion mass spectrometry (SIMS) for the first time. Our aim was to identify mineral phases at sub-micrometer scale and identify locations of brine–rock interactions. In addition, we wanted to test if current understanding of these alteration processes can be improved with the combination of complementary imaging techniques and give new insights to IOR. The HIM-SIMS imaging revealed well-defined crystal boundaries and provided images of excellent lateral resolution, allowing for identification of specific mineral phases. Using this new methodology, we developed chemical identification of clay minerals and could define their exact location on micron-sized coccolith grains. This shows that it is essential to study mineralogical processes at nanometer scale in general, specifically in the research field of applied petroleum geology within IOR.publishedVersio

Understanding and decoupling the role of wavelength and defects in light-induced degradation of metal-halide perovskites

peer reviewedLight-induced degradation in metal halide perovskites is a major concern that can potentially hamper the commercialization of perovskite optoelectronic devices. The phenomena viz. ion migration, phase segregation, and defect intolerance are believed to be the factors behind the degradation. However, a detailed mechanistic understanding of how and why light reduces the long-term stability of perovskites is still lacking. Here, by combining multiscale characterization techniques and computational studies, we uncover the role of white light in the surface degradation of state-of-the-art FAPbI3-rich perovskite absorbers (reaching up to 22% PCE in solar cells). We unravel the degradation kinetics and found that white light triggers the chemical degradation of perovskite into secondary phases with higher work function and metallic I-V characteristics. Furthermore, we demonstrate that perovskite degradation is triggered by a combined mechanism involving both light and the presence of defects. We employ surface passivation to understand the role of defect intolerance in the degradation process. Moreover, by using filtered light we uncover the wavelength dependency of the light-induced perovskite degradation. Based on our findings, we infer some strategies for material engineering and device design that can expedite the path toward stable perovskite optoelectronic devices

Computing with bacterial constituents, cells and populations: from bioputing to bactoputing

The relevance of biological materials and processes to computing—aliasbioputing—has been explored for decades. These materials include DNA, RNA and proteins, while the processes include transcription, translation, signal transduction and regulation. Recently, the use of bacteria themselves as living computers has been explored but this use generally falls within the classical paradigm of computing. Computer scientists, however, have a variety of problems to which they seek solutions, while microbiologists are having new insights into the problems bacteria are solving and how they are solving them. Here, we envisage that bacteria might be used for new sorts of computing. These could be based on the capacity of bacteria to grow, move and adapt to a myriad different fickle environments both as individuals and as populations of bacteria plus bacteriophage. New principles might be based on the way that bacteria explore phenotype space via hyperstructure dynamics and the fundamental nature of the cell cycle. This computing might even extend to developing a high level language appropriate to using populations of bacteria and bacteriophage. Here, we offer a speculative tour of what we term bactoputing, namely the use of the natural behaviour of bacteria for calculating

On new mixed conducting oxides for fuel cell cathodes SOFC

L'augmentation du pouvoir électrocatalytique d'une pile à combustible fonctionnant à haute température (SOFC, Solid Oxide Fuel Cell) passe notamment par l'amélioration des performances de la cathode. A cet effet, notre objectif a été de créer puis mesurer une conductivité mixte (électronique ou ionique) au sein de nouveaux oxydes de structure perovskite ABO3-d. Une étude fondamentale a été menée sur des composés choisis en fonction de l'état de valence et de la taille du cation B et du taux de lacunes d. La caractérisation des propriétés de transport (électronique et ionique) a été réalisée à l'aide de techniques nouvelles au laboratoire (meusure de la diffusion de 18O). Par la suite une corrélation entre les deux types de conductivité et les propriétés physico-chimiques des matériaux (paramètres de maille, polarisabilité des ions, ...) a été proposée.With the aim to increase the electrocatalytic power of the high temperature fuel cells (SOFC, Solid Oxide Fuel Cell), an interesting way is to developp new oxides usable as cathodes. For this purpose, we tried to create, then to measure, a mixed conductivity (electronic and ionic) in the host structure of perovskite-type ABO3-d. Fundamental studies were carried out on new chemical compositions, concerning especially the valence state or the atomic radius of the B cation, and also the oxygen vacancy rate d. The characterization of transport properties (electronic and ionic) has been realized with the help of new method in the lab, such as measurement of the 18O diffusion. Finally, a correlation between the properties (lattice parameter, ion polarizability, ...) has been proposed

Sur de nouveaux oxydes conducteurs mixtes pour cathodes de piles à combustible SOFC

With the aim to increase the electrocatalytic power of the high temperature fuel cells (SOFC, Solid Oxide Fuel Cell), an interesting way is to developp new oxides usable as cathodes. For this purpose, we tried to create, then to measure, a mixed conductivity (electronic and ionic) in the host structure of perovskite-type ABO3-d. Fundamental studies were carried out on new chemical compositions, concerning especially the valence state or the atomic radius of the B cation, and also the oxygen vacancy rate d. The characterization of transport properties (electronic and ionic) has been realized with the help of new method in the lab, such as measurement of the 18O diffusion. Finally, a correlation between the properties (lattice parameter, ion polarizability, ...) has been proposed.L'augmentation du pouvoir électrocatalytique d'une pile à combustible fonctionnant à haute température (SOFC, Solid Oxide Fuel Cell) passe notamment par l'amélioration des performances de la cathode. A cet effet, notre objectif a été de créer puis mesurer une conductivité mixte (électronique ou ionique) au sein de nouveaux oxydes de structure perovskite ABO3-d. Une étude fondamentale a été menée sur des composés choisis en fonction de l'état de valence et de la taille du cation B et du taux de lacunes d. La caractérisation des propriétés de transport (électronique et ionique) a été réalisée à l'aide de techniques nouvelles au laboratoire (meusure de la diffusion de 18O). Par la suite une corrélation entre les deux types de conductivité et les propriétés physico-chimiques des matériaux (paramètres de maille, polarisabilité des ions, ...) a été proposée

On new mixed conducting oxides for fuel cell cathodes SOFC

L'augmentation du pouvoir électrocatalytique d'une pile à combustible fonctionnant à haute température (SOFC, Solid Oxide Fuel Cell) passe notamment par l'amélioration des performances de la cathode. A cet effet, notre objectif a été de créer puis mesurer une conductivité mixte (électronique ou ionique) au sein de nouveaux oxydes de structure perovskite ABO3-d. Une étude fondamentale a été menée sur des composés choisis en fonction de l'état de valence et de la taille du cation B et du taux de lacunes d. La caractérisation des propriétés de transport (électronique et ionique) a été réalisée à l'aide de techniques nouvelles au laboratoire (meusure de la diffusion de 18O). Par la suite une corrélation entre les deux types de conductivité et les propriétés physico-chimiques des matériaux (paramètres de maille, polarisabilité des ions, ...) a été proposée.With the aim to increase the electrocatalytic power of the high temperature fuel cells (SOFC, Solid Oxide Fuel Cell), an interesting way is to developp new oxides usable as cathodes. For this purpose, we tried to create, then to measure, a mixed conductivity (electronic and ionic) in the host structure of perovskite-type ABO3-d. Fundamental studies were carried out on new chemical compositions, concerning especially the valence state or the atomic radius of the B cation, and also the oxygen vacancy rate d. The characterization of transport properties (electronic and ionic) has been realized with the help of new method in the lab, such as measurement of the 18O diffusion. Finally, a correlation between the properties (lattice parameter, ion polarizability, ...) has been proposed