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Within the framework of this thesis, three innovative electrochemical devices have been studied. A part of the work is devoted to an already existing device, laminates which are debonded by the application of a voltage. This type of material can potentially be used in a wide range of applications, including adhesive joints in vehicles to both reduce the total weight and to simplify the disassembly after end-of-life, enabling an inexpensive recycling process. Although already a functioning device, the development and tailoring of this process was slowed by a lack of knowledge concerning the actual electrochemical processes responsible for the debonding. The laminate studied consisted of an epoxy adhesive, mixed with an ionic liquid, bonding two aluminium foils. The results showed that the electrochemical reaction taking place at the releasing anode interface caused a very large increase in potential during galvanostatic polarization. Scanning electron microscopy images showed reaction products growing out from the electrode surface into the adhesive. These reaction products were believed to cause the debonding through swelling of the anodic interface so rupturing the adhesive bond. The other part of the work in this thesis was aimed at innovative lithium ion (Li‑ion) battery concepts. Commercial Li-ion batteries are two-dimensional thin film constructions utilized in most often mechanically rigid products. Two routes were followed in this thesis. In the first, the aim was flexible batteries that could be used in applications such as bendable reading devices. For this purpose, nano-fibrillated cellulose was used as binder material to make flexible battery components. This was achieved through a water-based filtration process, creating flexible and strong papers. These paper-based battery components showed good mechanical properties as well as good rate capabilities during cycling. The drawback using this method was relatively low coulombic efficiencies believed to originate from side-reactions caused by water remnants in the cellulose structure. The second Li-ion battery route comprised an electrochemical process to coat carbon fibers, shown to perform well as negative electrode in Li-ion batteries, from a monomer solution. The resulting polymer coatings were ~500 nm thick and contained lithium ions. This process could be controlled by mainly salt content in the monomer solution and polarization time, yielding thin and apparently pin-hole free coatings. By utilizing the carbon fiber/polymer composite as integrated electrode and electrolyte, a variety of battery designs could possibly be created, such as three-dimensional batteries and structural batteries. / <p>QC 20130403</p>

<p>Paper-based flexible devices represent a new frontier in electronics technology. The research has focused on the fabrication of the lightweight, and flexible paper-based lithium ion batteries. A lithium ion battery relies on the interplay of multiple components. These components themselves, as well as the processes used to create them, need to be adjusted and modified in order to achieve a fully flexible lithium ion battery. These components include the electrode current collector, active material, and electrolyte. By modifying these components to be fully flexible and resistant to damages caused by deformation, a fully flexible battery can be achieved.</p> <p> </p> <p>Herein, the paper-based platform utilized is key to provide flexibility for the battery components. The goal of this work not only focused on the creation of a paper-based flexible battery to be used as an integrable energy storage system for flexible devices, but also on developing methodologies and processes that can advance the emerging area of paper-based electronics, where different functional units must be fabricated within a single paper substrate. The key to make effective paper-based batteries, is to achieve a highly conductive paper structure as the base. In this work, conductive nanomaterials including carbon nanotubes (CNT) and graphene were used to fabricate conductive paper, where wood microfibers were coated with layers of these nanomaterials via layer-by-layer nanoassembly. These fibers were then combined into paper sheets. The resulting paper offers a conductive and porous base for electronic devices that utilized only small quantities of CNT or reduced graphene oxide (rGO) to provide length resistances of 468 Ω/cm and 74.6 Ω/cm, respectively for each fabricated conductive paper. </p> <p> </p> <p>Flexible lithium ion batteries were then made by using CNT paper-based electrodes and a solid polymer gel electrolyte. The electrodes were made by deposition of lithium active materials over the conductive paper and where shown to be flexible, durable, and light weight. With respect to the electrolyte, a new type of gel electrolyte based on PVDF-HFP was fabricated to overcome problems related to the use of liquid electrolytes in flexible batteries. This gel, which provides a high electrolyte uptake (450% by weight), was made by infusing both liquid and ceramic electrolytes inside a polymer gel structure and demonstrated conductivity up to 10^-4 S/cm. The paper-based battery developed with these new materials has a comparable capacity to commercial batteries and represents a flexible and light weight alternative. The use of ultra-high capacity lithium compounds as cathode materials, such as vanadium pentoxide (with theoretical capacities of 440 mAh/g) in conjunction with rGO-paper as a stand-alone electrode (with a reversible capacity 546 mAh/g) were also explored and results will be discussed. </p> <p> </p> <p>This research has led to the development of a novel method of making a fully flexible lithium ion batteries, using paper-based current collectors, leak proof polymer gel electrolytes and ultra-high capacity lithium ion active materials. Thus, flexible high conductive paper-based current collectors, polymer-gel electrolytes, vanadium based ultra-high capacity cathode electrodes, and graphene-based stand-alone paper-based anodes have been developed and tested.</p> <p> </p>

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Le travail présenté dans ce mémoire concerne la réalisation des batteries souples lithium-ion. Il a comme objectif le développement de nouveaux procédés comme l'impression par sérigraphie pour la fabrication de batteries et le remplacement des polymères issus de la chimie de synthèse par des matériaux bio-sourcés utilisables en milieu aqueux. Les résultats obtenus ont montré qu'il est possible de formuler des encres aqueuses à base des matériaux actifs classiquement utilisés pour l'élaboration d'électrodes (anode et cathode) de batterie Li-ion mais avec des liants dérivés de cellulose en substitution du PVDF qui intègre les formulations standards. Cette encre, dont les propriétés rhéologiques sont compatibles avec le procédé d'impression sérigraphique, permet l'obtention d'électrodes présentant des propriétés spécifiques aux bons fonctionnements de la batterie. Les résultats obtenus ont montré que cette technique d'impression du séparateur pouvait être utilisée pour remplacer la technique de déposition classique des matières actives sur les collecteurs de courant, basée sur un procédé d'enduction à lame (blade coating). Enfin, une batterie lithium-ion imprimée a pu être élaborée en utilisant la stratégie d'impression recto/verso du séparateur avec l'intégration des collecteurs de courant pendant la phase d'impression, validant ainsi cette nouvelle technique d'assemblage. / The work presented in this manuscript describes the manufacturing of lithium-ion batteries on papers substrates by printing technique. Its aim is the development of new up scalable and large area techniques as screen printing for the fabrication of lithium-ion batteries and the replacement of conventional toxic components by bio-sourced one and water based solvent. First results shows how it is possible to formulate cellulose based ink tailored for screen printing technology with suitable properties for lithium-ion batteries requirements. Electrodes were manufactured and tested from a physical and electrochemical point of view and two strategies were proposed to enhance performances. Finally, by considering results obtained for the electrodes, a full cell was manufactured with a new assembling strategy based on: front / reverse printing approach and the embedding of the current collectors during printing stage. As a final point cells were characterized and compared with others obtained by conventional assembling strategies.

A prototype 3-dimensional (3D) anode, based on multiwall carbon nanotubes (MWCNTs), for Li-ion batteries (LIBs), with potential use in Electric Vehicles (EVs) was investigated. The unique 3D design of the anode allowed much higher areal mass density of MWCNTs as active materials, resulting in more amount of Li+ ion intake, compared to that of a conventional 2D counterpart. Furthermore, 3D amorphous Si/MWCNTs hybrid structure offered enhancement in electrochemical response (specific capacity 549 mAhg-1). Also, an anode stack was fabricated to further increase the areal or volumetric mass density of MWCNTs. An areal mass density of the anode stack 34.9 mg/cm2 was attained, which is 1,342% higher than the value for a single layer 2.6 mg/cm2. Furthermore, the binder-assisted and hot-pressed anode stack yielded the average reversible, stable gravimetric and volumetric specific capacities of 213 mAhg-1 and 265 mAh/cm3, respectively (at 0.5C). Moreover, a large-scale patterned novel flexible 3D MWCNTs-graphene-polyethylene terephthalate (PET) anode structure was prepared. It generated a reversible specific capacity of 153 mAhg-1 at 0.17C and cycling stability of 130 mAhg-1 up to 50 cycles at 1.7C.