Aluminium oxide

Summary

Aluminium oxide (or Aluminium(III) oxide) is a chemical compound of aluminium and oxygen with the chemical formula . It is the most commonly occurring of several aluminium oxides, and specifically identified as aluminium oxide. It is commonly called alumina and may also be called aloxide, aloxite, or alundum in various forms and applications. It occurs naturally in its crystalline polymorphic phase α-Al2O3 as the mineral corundum, varieties of which form the precious gemstones ruby and sapphire. Al2O3 is significant in its use to produce aluminium metal, as an abrasive owing to its hardness, and as a refractory material owing to its high melting point. Corundum is the most common naturally occurring crystalline form of aluminium oxide. Rubies and sapphires are gem-quality forms of corundum, which owe their characteristic colours to trace impurities. Rubies are given their characteristic deep red colour and their laser qualities by traces of chromium. Sapphires come in different colours given by various other impurities, such as iron and titanium. An extremely rare δ form occurs as the mineral deltalumite. Al2O3 is an electrical insulator but has a relatively high thermal conductivity (30 Wm−1K−1) for a ceramic material. Aluminium oxide is insoluble in water. In its most commonly occurring crystalline form, called corundum or α-aluminium oxide, its hardness makes it suitable for use as an abrasive and as a component in cutting tools. Aluminium oxide is responsible for the resistance of metallic aluminium to weathering. Metallic aluminium is very reactive with atmospheric oxygen, and a thin passivation layer of aluminium oxide (4 nm thickness) forms on any exposed aluminium surface in a matter of hundreds of picoseconds. This layer protects the metal from further oxidation. The thickness and properties of this oxide layer can be enhanced using a process called anodising. A number of alloys, such as aluminium bronzes, exploit this property by including a proportion of aluminium in the alloy to enhance corrosion resistance.

Official source

https://en.wikipedia.org/wiki/Aluminium_oxide

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Aluminium is a metal sought in the industry because of its various physical properties. It is produced by an electrolysis reduction process in large cells. In these cells, a large electric current goes through the electrolytic bath and the liquid aluminium. This electric current generates electromagnetic forces that set the bath and the aluminium into motion. Moreover, large quantities of carbon dioxide gas are produced through chemical reactions in the electrolytic bath: the presence of these gases alleviates the density of the liquid bath and changes the dynamics of the flow. Accurate knowledge of this fluid flow is essential to improve the efficiency of the whole process.The purpose of this thesis is to study and approximate the interaction of carbon dioxide with the fluid flow in the aluminium electrolysis process.In the first chapter of this work, a mixture-averaged model is developed for mixtures of gas and liquid. The model is based on the conservation of mass and momentum equations of the two phases, liquid and gas. By combining these equations, a system is established that takes into account the velocity of the liquid-gas mixture, the pressure, the gas velocity and the local gas concentration as unknowns.In the second chapter, a simplified problem is studied theoretically. It is shown that under the assumption that the gas concentration is small, the problem is well-posed. Moreover, we prove a priori error estimates of a finite element approximation of this problem.In the third chapter, we compare this liquid-gas model with a water column reactor experiment. Finally, the last chapter shows that the fluid flow is changed in aluminium electrolysis cells when we take into account the density of the bath reduced by carbon dioxide. These changes are quantified as being of the order of 30% and explain partially the differences between previous models and observations from Rio Tinto Aluminium engineers.

EPFL2022

Atomic doping & coating for Electrocatalysis & Li-ion batteries

Albert Claude Jean-Pierre Daubry

molybdenum atomic-doping on bio-waste derived nitrogen-doped conductive carbon electrocatalyst was synthesized and investigated for the dinitrogen reduction to ammonia in alkaline media. The assessment of the catalytic activity was found to be non-trivial as nearly any external source can be the cause of ammonia contamination. In a closed-cell set-up using isotopically labelled 15N2 as feed gas for 48h chronoamperometry at -0.1 V vs RHE that the current density was correlated to the availability of the gas. Non-precious metals were incorporated in an oxidized carbon black conductive matrix and investigated for their activity towards oxygen evolution reaction in 0.1 M H2SO4, 0.5 M H2SO4 and 0.1 M HClO4. The stability of the deposited catalyst was insufficient and their deterioration was attributed to the oxidation of the carbon support as well as the dissolution of the metal ions upon high anodic potentials.The same metal-incorporated oxidized conductive carbon black agents were investigated for the enhancement of the performance of Si/C anodes in lithium-ion batteries. It was found that cobalt incorporation in the oxidized matrix displayed a significant influence in the electrochemical kinetics and consequent rate performances. With 0.8% cobalt ions by mass incorporated in oxidized KetJen Black the average capacity of the Si/C anode was increased by 180% at 1.5 A.g-1. This metal incorporation approach was extended to other ionic species (copper, iron and nickel) and other carbon conductive agents (SuperP). The electrolyte affinity, the desolvation process and the improved electronic conductivity synergistically improved the rate performance without compromising the gravimetric capacity of the electrode.The deposition of ultra-thin aluminium oxide by atomic layered deposition on the surface of LiNi0.5Co0.2Mn0.3O2 cathode material in lithium-ion batteries for the improvement of cyclic performances at high voltages (4.3-4.6 V) was investigated. One source of the failure mechanisms of the battery comes from unwanted side reactions between surface species and the electrolyte. The aluminium oxide layers of 1.42 nm and 2,36 nm were found to be beneficial at current densities exceeding 1.0 C (1 C = 170 mAh.g-1), and especially at 5.0 C with an increase of about 20 mAh.g-1 and 35 mAh.g-1 compared to uncoated NCM523, respectively. The capacity retention was found to be improved for all coated samples compared to pristine upon 140 cycles at 1.0 C. Mitigating side reactions and increasing the specific capacity at higher C-rates by atomically controlled layered deposition of inexpensive metal oxides is desirable for the implementation next-generation of safer and stable fast-charging high-voltage lithium-ion batteries.

EPFL2022

Effect of alkali, aluminium and equilibration time on calcium-silicate-hydrates

Yu Yan

Calcium silicate hydrate (C-S-H) is the main hydration product in Portland and blended cements, and greatly affects durability and mechanical properties of the hydrated cement. In the presence of Al-rich supplementary cementitious materials (SCMs), C-(A-)S-H can contain more Al than C-S-H in plain Portland cements. The use of SCMs in cementitious system not only lowers CO2 emission, but may also enhance the mechanical properties in the long term, its durability and can help to suppress alkali silica reaction. However, important questions regarding the effect of Al, alkali and equilibration time on C-A-S-H structure and solubility are still not fully understood. This thesis focuses on the interplay between aluminium, alkali hydroxides in solution, the structure of C-A-S-H and aluminium, alkali uptake by C-A-S-H and kinetics of C-A-S-H formation. For aluminium free C-S-H, KOH and NaOH have a similar effect, they increase pH values and silicon concentrations, and decrease calcium concentrations. At higher alkali hydroxide concentrations, more portlandite precipitates, while amorphous silica dissolves. This increases the Ca/SiC-S-H at low Ca/Sitarget but lowers the maximum Ca/SiC-S-H from 1.5 to 1.2 in 1 M KOH/NaOH. The amount of alkalis bound in C-S-H increases with increasing alkali hydroxide concentrations and is higher at low Ca/SiC-S-H. KOH/NaOH lead to a structural rearrangement in C-S-H, increasing the interlayer distance, number of layers stacked in c direction and shortening the silica chains. Comparison with the independently developed CASH+ thermodynamic model showed a good agreement between the observed and modelled changes, including the shortening of the MCL.For C-A-S-H with Ca/Si=1, the presence of Al led to higher amounts of secondary phases, larger interlayer distance, longer silicate chain, higher dissolved Al and Si, and lower Ca concentrations. The amount of secondary phases is reduced at higher pH; strätlingite and Al(OH)3 dominate at lower pH, and katoite at higher pH values. High pH is also associated with shortened silicate chain length, increased Al and Si concentrations, maximum Al/SiC-S-H and lower Ca concentrations. The Al uptake in C-A-S-H increased with aluminum concentration in solution, indicating the predominance of a common Al sorption mechanism independent of dissolved Al concentration or pH values. XANES data showed the presence of both Al(IV) and Al(VI) with different chemical environments in C-S-H.The effect of equilibration time on C-A-S-H was investigated from 6 hours to 3 years. Rapid changes within the first day were observed in both the solid phase and the aqueous phase. Portlandite was formed in all samples with different Ca/Si and its amount decreased rapidly within the first day and remained stable after more than 7 days. Gismondine-P1 precipitated between 1 and 3 years and destabilized the C-A-S-H phases at target Ca/Si 0.6. In the solid phase, the Al migration from secondary phases to C-A-S-H and an increasing fraction of Al(V) and Al(VI) in C-S-H were observed with longer equilibration time. The Ca/Si ratio of C-S-H played an important role on the extent of changes in aqueous concentration: an increasing of Al concentrations with time was observed in C-A-S-H with Ca/Sitarget=0.6, while a decrease was observed for C-A-S-H with Ca/Sitarget=1.0. The uptake of Al and Na in C-A-S-H was observed to decrease after 4 days and 1 day separately, which indicates a rearrangement of C-A-S-H with time.

EPFL2022