Surface immobilization of probe molecules in surface based assays is a key area of research in the continued development of immunoassay microarrays. Interest continues to grow in microarray based immunoassays given their potential as a high throughput technique for immunodiagnostics. Therefore, it is important to thoroughly study and understand the implications of interfacial chemistry and immobilization conditions on the performance of the assay. This thesis presents a body of work that examines the impact of probe density, interfacial chemistry, and enhancement factors for arrays read with surface plasmon resonance (SPR) imaging. An array of structurally similar Salmonella disaccharides was immobilized at varying densities and the interface formed was thoroughly investigated to determine the properties of the interface. The arrays were then used with SPR imaging to evaluate the binding of an antibody specific for one disaccharide of the three stereoisomers on the array. A dilute disaccharide surface was found to provide optimal antibody binding. Higher densities result in steric hindrance of antibody binding by not allowing the disaccharide to insert into the antibody binding pocket. The role of interfacial chemistry in antibody attachment was studied to determine optimum conditions. The study examined physical adsorption, covalent attachment, and affinity capture. It was found that covalent attachment provided the most stable attachment and resulted in the lowest levels of antigen detection. Both the physical adsorption and affinity capture provided larger antigen binding capacity and therefore more sensitive antigen detection. The covalent attachment was chosen to evaluate an enhanced assay with the incorporation of gold nanoparticles. These particles provided detection limits that were an order of magnitude improved over those excluding the nanoparticles. A novel surface chemistry for antibody immobilization in SPR imaging studies was evaluated. This involved the electrochemical driven formation of mono- to multilayers of diazonium benzoic acid films. The studies showed the ability to control the thickness of the films formed and also the ability of the antibody chips to capture antigen from solution.

L'electroquímica ha experimentat un salt significatiu en els darrers anys, donada la possibilitat de control dels sistemes experimentals mitjançant les innovacions tecnològiques. Malgrat això, el caire heterogeni dels processos electroquímics no permet el tractament teòric d'aquests sistemes, tant des d'un punt de vista macroscòpic, ja que un estudi així requeriria l'ús de la termodinàmica de processos irreversibles, la qual és inaplicable donat que a la regió interfacial no es verifica la hipòtesi d'equilibri local, peça clau d'aquesta teoria, com des d'un punt de vista microscòpic, ja que l'estructura ds la regió interfacial és d'una gran complexitat i encara no hi ha models microscòpics que ens descriguin les interfases d'una forma bastant general a menys que es simplifiqui molt el model. Això fa que existeixin formalismes aproximats que permeten estudiar els processos electròdics des d'un punt de vista cinètic on la interfase juga un paper secundari o té una definició purament geomètrica de separació de fases.Cal esmentar que recenment s'ha desenvolupat una teoria general de sistemes (Kalman, Falb i Arbib - 1969; von Bertalanffy et al. - 1972, Aracil - 1978, Epelboin, Gabrielli i Keddam - 1984, entre d'altres) en el cas de no disposar d'una teoria concreta que descrigui el comportament del sistema i la seva evolució devant de pertorbacions externes.La realització d'una experiència que permeti d'un cantó la regulació i llavors l'anàlisi de processos electròdics i per una altra banda, l'elaboració de models, els quals s'han de comparar amb les dades experimentals, requereix una descripció acurada de les lleis que governen el comportament elèctric i cinètic de la interfase.Dins d'aquesta línia, el present treball es troba orientat a l'obtenció de funcions resposta de sistemes electroquímics tot utilitzant el mètode matemàtic de les transformades integrals. Si bé aquest mètode ha estat utilitzat en la resolució de determinats sistemes simples, la forma de tractar el problema, havia deixat pas a mètodes de linearització o de simulació numèrica per a resoldre problemes més complexes.El mètode, que consisteix en transformar el conjunt d'equacions diferencials que descriuen l'evolució de les variables d'estat en un conjunt d'equacions integrals més fàcils de resoldre, s'ha generalitzat per a sistemes en què imposem unes poques hipótesis de caràcter físic. La funció resposta s'obté de forma exacta i permet garantir la bondat de possibles mètodes aproximats a propasar a partir de les equacions integrals. En efecte, en utilitzar el mètode de les aproximacions succesives, s'obtenen solucions analítiques per a aquestes equacions, o sinò sistemes d'equacions funcionals implícites més senzilles que el sistema, d'equacions integrals, tot retrobant les aproximarà ons possibles donades a la bibliografia per a estudiar els mateixos sistemes, la qual cosa ens dóna un marc general i unificat per a deduir de les equacions generals les solucions aproximades.En el capítol II, s'ha fet un petit resum de l'estat actual de les teories físiques que ens descriuen les interfases electrificades, en particular les electròdiques. Això ens permet escollir quines són les variables d'estat que ens caracteritzaran la interfase.El capítol III es centra en l'establiment de les equacions diferencials que ens descriuen l'evolució de les variables que ens caracteritza l'estat del sistema, així com de les condicions inicials i de contorn associades amb les característiques del procés i amb els lligams del sistema (variables de control).Dins dels mètodes matemàtics més emprats per a resoldre aquest tipus d'equacions que trobem en el capítol III, en el capítol IV esmentem els més importants, i d'entre ells destaquem el mètode de les transformades integrals que es el que desenvolupem en els capítols V i VI, dedicats l'un a trobar les variables d' estat i l'altra a trobar les funcions resposta, en especial la intensitat i la càrrega total,d'un procés elemental de transferènciade càrrega, bescanviada a la interfase electròdica. Els sistemes estudiats, centrant-nos en llur geometria i règim hidrodinàmic, són l'elèctrode pla estacionari, l'elèctrode esfèric estacionari, l'elèctrode de gotes de mercuri, tant dins del model de pla en expansió com d'esfera, en expansió i l'elèctrod&ae disc rotatori.En el capítol VII, es fa l'aplicació d'aquest formalisme a un exemple concret, el de la polarografia, que ha estat molt estudiat en casos sense complicacions degudes a l'adsorció a la interfase electròdica. En aquest cas s'han resol les equacions plantejades per a descriure el procés, amb les hipòtesis fetes en els darrers capítols, i quan l'adsorció dels components de la reacció segueixen una isoterma de Langmuir o de Frurnkin. Això ens permetrà valorar l'exactitud de les altres tècniques matemàtiques emprades per a resoldre aquest problema, generalment de forma aproximada, algunes de les quals es dedueixen de les equacions generals plantejades al aplicar el mètode d'aproximacions succesives per a resoldre les equacions integrals que surten. A més a més es veu l'aplicabilitat del mètode per a resoldre casos en què les tècniques convencionals no ho aconsegueixen o porten a equacions d'un grau molt elevat de complexitat per a dur-ho a la pràctica.Aquest estudi es troba restringit als processos electròdics convencionals, puix que pot extendre's a la caracterització d'altres tipus de processos en què s'escaiguin hipòtesis similars. En particular, i a títol d'exemple, cal destacar l'ús d'aquest mètode en el futur esclariment de certs processos biològics, com ara el transport d'informació al cervell (González - 1984, Ghizmadzhev i Pastushenko - 1985) mitjançant el sistema nerviós.

Theoretical models for the electrokinetics of weakly permeable porous colloidal particles are absent from the literature. The understanding of this topic will be advanced through a systematic analysis of the standard electrokinetic equations, resulting in a theory for the electrophoretic mobility of weakly permeable porous colloidal particles. / The standard electrokinetic equations are employed to model the flux of solvent and ions outside the porous particle. To be consistent with this approach, the flux of solvent and ions in the pores must also be governed by the standard electrokinetic equations. However, in practice, only transport phenomena on the particle scale are observed and it is sufficient for information regarding pore-scale behaviour to be retained purely in the form of averaged quantities. To complete the theoretical description, the standard electrokinetic equations outside the particle must be coupled to particle-scale transport equations inside the particle via boundary conditions at the porous/free-fluid interface. / It has been shown experimentally and theoretically for coupled Stokes and Darcy flows, that the correct interfacial boundary condition for the tangential external flow is given by the Beavers-Joseph-Saffman (BJS) condition. The effect of the BJS boundary condition on the hydrodynamic drag on an oscillating porous particle is investigated. It is found that the particle may be regarded as impermeable with a slip length independent of frequency, and the resulting drag is significantly reduced in comparison with an equivalent impermeable particle that does not exhibit a slip length. / The transport of a general electrolyte solution through a rigid porous body subjected to a static (d.c.) electric field is studied. The pore-scale description is given by the standard electrokinetic equations, including the effects of ion diffusion, electromigration and convection. Homogenization theory is used to derive transport equations that capture the particle-scale behaviour. It is proven that the transport coefficient tensors obey Onsager’s reciprocal relations and the diagonal coefficient tensors are positive definite. / New interfacial boundary conditions are derived using conservation arguments supplemented by Stern-layer theory. When combined with the particle-scale transport equations, these boundary conditions incorporate four principal effects into the standard electrokinetic model: solvent slip and Stern-layer ionic conduction at the interface, and macroscopic ionic conduction together with the electroosmotic flow of solvent through the particle. / The method of matched asymptotic expansions is then used to construct an approximate solution to the aforementioned system, in the thin double-layer limit. An expression for the electrophoretic mobility of a weakly permeable colloidal sphere is produced that consists of a generalization of Smoluchowski’s formula to encompass porous particles, and a next order correction. For the first time, the effects of solvent slip and Stern-layer ionic conduction within the porous/free-fluid interface, in conjunction with macroscopic ionic conduction and electroosmosis through the particle, are exhibited. It is shown that solvent slip at the porous interface is overwhelmingly the dominant effect on the mobility of weakly permeable porous colloidal particles.

Soldering results from the interfacial interactions between the die and the casting alloy during high pressure die casting and is one of the major die failure modes. To prevent this occurring, lubricant layers and surface coatings are used to act as a barrier between the die and the casting alloy. The microstructures of a series of soldered layers on H13 tool steel core pins were examined after conducting high pressure die casting experiments with a specially designed die using removable core pins and Al-11Si-3Cu casting alloy. This showed that first, a casting alloy build-up layer formed, and then intermetallic phases nucleated at the die steel interface and grew to cover the entire surface in subsequent casting cycles. The structures of intermetallic layers formed during immersion of H13 tool steel into an Al-11Si-3Cu casting alloy melt were studied by X-ray diffraction and energy dispersive spectroscopy (EDS). A thick composite layer away from the H13 steel substrate consisted of irregular intermetallic phases and solidified casting alloy. A thin intermetallic layer was present between the composite layer and an inner compact layer next to the steel substrate. The irregular intermetallic phase in the thick composite layer away from the H13 steel substrate was identified to have a body centre cubic (bcc) structure, abcc-( FeSiAlCrMnCu). The thin and continuous intermetallic layer between the composite layer and the inner compact layer was found to be structurally isomorphous with aH-Fe2SiAl8. The compositional differences observed between aH and abcc phases indicated that the latter consisted of a higher amount of chromium, manganese, copper, and a lower amount of iron. It was likely that the presence of chromium, manganese and copper in the H13 tool steel caused the transformation of aH®abcc. The inner compact layer next to the steel substrate was identified to be orthorhombic h-Fe2Al5 containing silicon and chromium. An examination of lubricants to prevent soldering in high pressure die casting in conjunction with Nissan Casting Australia Pty Ltd. found that soldering was reduced by using a suitable lubricant. The chemistry of the lubricant, spray parameters, and die surface temperature were important factors in producing a protective lubricant layer. It was found that lubricant containing polypropylene waxes prevented soldering significantly better than lubricant containing polyethylene waxes. It was also found that the lubricant containing polypropylene waxes had lower surface tension. An examination of the use of iron oxide layers to prevent soldering in high pressure die casting was performed. H13 tool steel was oxidised in air and produced porous iron oxide with a mixture of haematite (Fe2O3) and magnetite (Fe3O4). These porous iron oxides did not completely prevent the H13 steel from soldering in immersion tests as intermetallic cones formed at the surface of the steel. Commercial steam tempering of H13 steel produced more compact iron oxide layers with magnetite (Fe3O4) and haematite (Fe2O3) structures. It was found that these compact iron oxide layers offered better protection against soldering than the porous layers created in air. Pure iron oxidised in a CO2/H2 gas mixture at a ratio of 95:5 at 550°C produced structurally pure, compact magnetite (Fe3O4) layers. H13 steel oxidised in a CO2/H2 gas mixture at a ratio of 95:5 at 550°C produced compact iron oxide layers that showed only magnetite (Fe3O4) structure. The magnetite (Fe3O4) layer containing chromium, manganese, silicon and vanadium formed next to the H13 substrate was found to be a very adherent layer and protected H13 steel from soldering in high pressure die casting experiments with a specially designed die using removable core pins and Al-11Si-3Cu casting alloy. An examination of aluminium oxide layers to prevent soldering in high pressure die casting was performed. Incoloy MA956 containing 4.5 wt.% aluminium, oxidised in air at 1100°C, produced a single, compact, adherent oxide layer with a-alumina (Al2O3) structure, that prevented the formation of intermetallic phases between aluminium alloy and Incoloy MA956 during high pressure die casting. However, non-reactive casting alloy build-up formed on the oxide coatings, similarly to physical vapour deposition (PVD) and vanadium carbide coatings. It was found that the thickness of the non-reactive casting alloy build-up was reduced by decreasing the roughness of the oxide coatings by lightly grinding of the surface of the coatings. The industrial application of these findings are discussed and directions for further research are presented.

Στην εργασία αυτή μελετάται η ηλεκτρική απόκριση νανοσύνθετων υλικών πολυαιθυλενοξειδίου (poly(ethylene oxide)) – τροποποιημένων νανοσωλήνων άνθρακα πολλαπλού τοιχίου (MWCNT), ως συνάρτηση της περιεκτικότητας σε νανοσωλήνες άνθρακα. Συγκεκριμένα εξετάζεται η διηλεκτρική απόκριση και η ειδική αγωγιμότητα των νανοσύνθετων με παραμέτρους την περιεκτικότητα σε MWCNT, τη θερμοκρασία και τη συχνότητα του εφαρμοζόμενου ηλεκτρικού πεδίου. Από τη διηλεκτρική απόκριση εξάγονται πληροφορίες σχετικά με την μοριακή κινητικότητα του συστήματος και διεπιφανειακά φαινόμενα. Η εξάρτηση της ειδικής αγωγιμότητας από την περιεκτικότητα σε MWCNT δίνει τη δυνατότητα προσδιορισμού του κατωφλιού μετάβασης από τη μονωτική στην αγώγιμη συμπεριφορά, ενώ η εξάρτηση της ειδικής αγωγιμότητας από τη θερμοκρασία και τη συχνότητα προσφέρει τη δυνατότητα μελέτης των μηχανισμών μεταφοράς ηλεκτρικού φορτίου. Για τον καλύτερο προσδιορισμό των μηχανισμών ηλεκτρικής αγωγής εξετάζεται η δυνατότητα περιγραφής των πειραματικών αποτελεσμάτων μέσω των θεωρητικών προσεγγίσεων Variable Range Hopping model και Symmetric Hopping model. Για λόγους αναφοράς εξετάζεται και η ηλεκτρική απόκριση του καθαρού πολυμερούς και νανοσύνθετων, της ίδιας πολυμερικής μήτρας, που περιλαμβάνουν μη τροποποιημένους νανοσωλήνες άνθρακα. Τέλος, το σύνολο των αποτελεσμάτων γίνεται αντικείμενο εκτεταμένης συζήτησης. / In the present work the electric response of nanocomposites material consisted of poly (ethylene oxide) as matrix and modified multiwall carbon nanotubes (MWCNT) as reinforcing phase, is studied. Specifically, the dielectric response and the conductivity of nanocomposites is examined with parameters the content in MWCNT, the temperature and the frequency of the applied electric field. From the dielectric response valuable information concerning the molecular mobility of the systems and the interfacial phenomena can be extracted. The dependence of conductivity on the MWCNT content allows the determination of percolation threshold or critical concentration, which governs the transition from the insulating to the conductive behaviour. Moreover, the dependence of conductivity on temperature and frequency offers the possibility of studying the occurring charge transport mechanisms. Aiming to study further the type of the conduction mechanisms, the applicability of Variable Range Hopping model and Symmetric Hopping model is tested. For reasons of reference the electric response of pure polymer matrix and nanocomposites incorporating unmodified MWCNT is also examined. Finally, results become the object of an extensive discussion.

Les interfaces entre deux fluides sont le siège de nombreuses instabilités de forme de l’interface si un champ électrique intense est appliqué : génération de gouttelettes, jets micrométriques, etc. Le contrôle de telles instabilités est indispensable pour une fabrication optimale de microsphères ou microfibres : taille, propriétés physico-chimiques, dispersion et structuration spatiale macroscopique d’un agrégat de tels objets. Cette diversité provient de la compétition entre la tension de surface et la gravité avec l’électrodynamique des fluides sous champ électrique induite par les charges électriques, les charges de polarisation, les décharges électriques et/ou le vent ionique. La thèse expérimentale s’articule autour de deux thèmes. Le premier, une compréhension intime des phénomènes spatio-temporels observables lorsqu’un injecteur métallique à la haute tension placé au-dessus d’un bain. Une instabilité originale menant à la formation d’une cloche fluide macroscopique connectant les deux électrodes a été mise en évidence et caractérisée non linéairement. La bifurcation est sous-critique et imparfaite. Le second thème propose une méthode originale de fabrication de microfibres modifiées en une étape par électrofilage au mouillé. Le polymère électrofilé choisi est le PSMA et celui permettant la modification, le PEGDA. Cette étude a été réalisée dans un contexte d’applications de type catalyse. Pour cela les fibres ont été fonctionnalisées à l’aide de la peroxydase (HRP) comme protéine modèle. Les résultats montrent notamment une meilleure stabilité temporelle avec la possibilité de réutilisation du matériau en comparaison à la catalyse utilisant des méthodes standards. / Interfaces between two fluids can lead to various interfacial shape instabilities if an electrical field is applied. Leading, for instance, to micrometric droplets or jets formation. Controlling those instabilities is much-needed for an optimal fabrication of microspheres or microfibers : size, physicochemical properties, dispersion and macroscopic spatial structuring of aggregates of those kind of objects. This diversity is based in the competition between surface tension and gravity forces with gravity during the electrodynamics of fluids under electric field induced by electrical charges, polarization charges, electrical discharges and ionic wind. The experimental thesis deals with two main topics. The first one is a precise understanding of spatiotemporals phenomena occurring in a configuration made of a metallic injector raised to high voltage placed above a liquid bath. We present the formation of an original instability leading to a macroscopic bell-shaped link between both electrodes and its non linear characterization. The bifurcation is subcritical and imperfect. The second topic, based on the experience gained with the first one, is an original method of fabrication of microfibers modified in only one step by wet electrospinning. The chosen electrospun polymer is PSMA and the one used for modification is PEGDA. This study has been realized with a catalyze application context. To do so, fibers has been functionalized with peroxydase (HRP) as the model protein. The results especially show a better temporal stability and possible reuse compared to catalysis with standard methods.

In the mammalian embryo, between 3.5 and 4.5 days after fertilisation, the cells of the inner cell mass evolve from a uniform aggregate to an ordered structure with two distinct tissue layers - the primitive endoderm and epiblast. It was originally assumed that cells differentiated to form these layers in situ, but more recent evidence suggests that both cell types arise scattered throughout the inner cell mass, and it is thus proposed that the tissue layers self-organise by physical mechanisms after the specification of the two cell types. We have developed a computational model based on the subcellular element method to combine theoretical and experimental work and elucidate the mechanisms that drive this self-organisation. The subcellular element method models each cell as a cloud of infinitesimal points that interact with their nearest neighbours by local forces. Our method is built around the introduction of a tensile cortex in each cell by identifying boundary elements and using a Delaunay triangulation to define a network of forces that act within this boundary layer. Once the cortex has been established, we allow the tension in the network to vary locally at interfaces, modelling the exclusion of myosin at cell-cell interfaces and consequent reduction in tension. The model is validated by testing the simulated interfaces in cell doublets and comparing to experimental data and previous theoretical work. Furthermore, we introduce dynamic tension to model blebbing in primitive endoderm cells. We investigate the effects of cortical tension, differential interfacial tension, and blebbing on interfaces, rearrangement, and sorting. By establishing quantitative measurements of sorting we produce phase diagrams of sorting magnitude given system parameters and find that robust sorting in a 30 cell aggregate is best achieved by a combination of differential interfacial tension and blebbing.

[pt] Os processos de formação e de dissociação de hidratos são de grande interesse nas áreas ambiental e energética. Especificamente para a indústria de petróleo e gás, o hidrato aparece como um empecilho à garantia de escoamento, alavancando ainda mais a necessidade urgente de ampliar o conhecimento sobre seus fenômenos. Neste trabalho, uma nova abordagem para observar e compreender a cinética e as propriedades mecânicas de hidratos por meio da reologia interfacial é apresentada. O conhecido anel du Nouy é empregado com uma nova célula de latão projetada para permitir o necessário gerenciamento da temperatura de teste. Ciclopentano é utilizado como formador de hidrato. Com a nova geometria interfacial, diferentes temperaturas e protocolos de contato água/ciclopentano são explorados. A importância de primeiro provocar o contato do CP com cristais de gelo a fim de iniciar a formação de hidrato é de particular interesse. Assim, time sweeps são realizados em duas etapas: uma para a formação de gelo e outra para os formação de hidrato. Foi determinado que os hidratos de ciclopentano são detectados em temperaturas Tf menor ou igual a 6 graus Celsius. Uma interessante discussão a respeito do estado de metaestabilidade dos hidratos é, então, apresentada. Depois que os hidratos preenchem completamente a interface água/ciclopentano, strain sweeps são realizados para examinar a fragilidade dos filmes de hidrato, medindo os módulos interfaciais elástico e viscoso (G e G). As propriedades mecânicas desses filmes demonstraram uma forte dependência da temperatura (Tf ): o tempo de indução (tc), medido a partir do primeiro contato do ciclopentano com gelo, bem como o módulo elástico (G) e a deformação de escoamento (γy) aumentam conforme Tf é aumentada. / [en] Hydrate formation and dissociation processes are of major interest in environmental and energy fields. Specifically for the oil and gas industry, hydrate appears as an issue regarding flow assurance, pushing even more the urgent need for expanding the knowledge on hydrate phenomena. In the current work, a new approach to observe and understand the kinetics and mechanical properties of hydrates by interfacial rheology is presented. The standard du Nouy ring is employed with a novel brass cell designed to permit the necessary temperature management. Cyclopentane is used as hydrate former. With the new interfacial geometry, different temperature and water/cyclopentane contact protocols are explored. The importance of first contacting CP against ice crystals in order to initiate hydrate formation is of particular interest. Thus, time sweeps are performed in two stages: one for ice formation and another for hydrate formation. It was determined that cyclopentane hydrates only arise at temperatures Tf less than or equal to 6 celsius degree. A worthwhile discussion regarding the hydrate metastability state is then presented. After hydrates completely populate the water/cyclopentane interface, strain sweeps of the interfacial elastic and viscous moduli (G and G) are conducted to examine the fragility of the hydrate films. The mechanical properties of hydrate films demonstrated high dependence on temperature (Tf): the induction time (tc), measured from the moment when cyclopentane first contacts ice, as well as the elastic modulus (G) and the yield strain (γy) increase as Tf is increased.

This dissertation examines the motion of colloids in a temperature gradient, a non-equilibrium phenomenon also known as thermophoresis. Chapter 1 gives an introduction to the existing applications and basic concepts of thermophoresis and outlines some of the experimental and theoretical challenges that serve as a motivation for this PhD project. In Chapter 2, a general theoretical description for thermophoresis is formulated using the theory of non-equilibrium thermodynamics. The colloidal flux is split up into an interfacial single-colloid contribution and a bulk contribution, followed by a determination of transport coefficients based on Onsager’s reciprocal relations. It is further shown how the phenomenological expression of the thermophoretic flux can be recovered when the fluid is at steady-state. The results issuing from this description are then discussed and compared to other existing approaches, some of which are shown to neglect the hydrodynamic character of colloidal thermophoresis. Chapter 3 is dedicated to the validation of the introduced theoretical framework by means of computer simulations, using a simulation technique known as multi-particle collision dynamics. More specifically, the dependence of the thermophoretic force on different system parameters is examined and deviations from the theoretical prediction are explained by an advective distortion of interfacial fluid properties at the colloidal surface. Chapter 4 presents steady-state measurements of functionalised colloids in a temperature gradient, showing how the addition of molecular surface groups increases the experimental complexity of thermophoretic motion. The relaxation process behind this steady-state is also studied, to determine how the relaxation speed depends on the applied temperature gradient. In chapter 5, a general conclusion is drawn from the presented work and its implications are briefly discussed in relation to the current state of knowledge. Finally, the discussion is closed with an outlook on remaining challenges in understanding colloidal motion that could be the subject of future research.

The technology employed by human beings for the generation, storage and usage of energy is presently undergoing the fastest and most profound change since the industrial revolution. The changes in the generation and usage of energy necessitate the development of new methods of energy storage. In these systems, electrochemical energy storage will play a crucial role and to this end new electrolytes need to be explored to complement these changes. One such class of liquids is ionic liquids, a class of salts that are molten at room temperature. These liquids have a broad applicability to batteries and supercapacitors. This thesis details work where molecular dynamics simulations have been used to explore the nanostructure of ionic liquids and their mixtures with various molecular solvents at simplistic electrodes. The thesis has two broad sections. The first is covered in Chapter 3, and explores the nanostructure of ionic liquid propylene carbonate solutions, developing a framework through which these nanostructures can be understood. The section concludes that the increasing dilution of ionic liquids decreases the surface charge at which the characteristic ionic liquid oscillatory interfacial structure gives way to a different structure featuring monotonic charge decay. The behaviour of ionic liquids at interfaces is found to be correlated to ion size and type, as well as concentration. A wide divergence in the observed behaviour is shown at positive and negative electrodes due to the asymmetry of propylene carbonate. The second section, consisting of two chapters, explores the interfacial nanostructure of solvate ionic liquids using two different boundary conditions to model the electrode. This work is the first simulation of solvate ionic liquids at electrified interfaces. This section will explore the effect of electrode model on the behaviour of these ionic liquids at the electrode. Chapter 4 uses a fixed charge electrode, whereas Chapter 5 uses one with a fixed potential. The section concludes that regardless of electrode model, the idealised portrait of a solvate ionic liquid - one where the liquid behaves exactly as an aprotic ionic liquid - is not applicable. In Chapter 4's exploration of fixed charged electrodes, the formation of 2 glyme to lithium complexes contradicts the idealised portrait of the liquid. A different change is observed in Chapter 5's exploration of fixed potential electrodes, with both lithium glyme and lithium anion clusters forming at the interface. The key difference between the two studies is that lithium does not coordinate to the electrode in the fixed charge simulations, while in the fixed potential case it does. At the end of Chapter 5 the results are compared against experimental data, with the efficacy of the two models discussed. The aim of both studies is to look at the nanostructure of ionic liquids, when the symmetry between co-ion and cation repulsion - and related effects - is broken by the presence of a non ionic constituent in the liquid.