Nanocellulose has gained lots of attentions in recent years due to the development of nanotechnology. Thousands of publications have been reported about the fabrication, characterization and application of nanocellulose, among which most of the nanocelluloses were fabricated from the microcrystalline cellulose (MCC) or pulp, and only two methods about the nanocellulose fabrication have been reported, i.e. sulphuric acid hydrolysis and mechanical treatment. The sulphuric acid method can only obtain low yield of nanocellulose and the mechanical treatment can not fabricate nanocellulose with high crystallinity index (CI) and well separation. These problems limit the scale up of nanocellulose to industrial area. Moreover, none of works has reported the application of nanocellulose for the modification of natural fibres and only a few works reported the reinforcement of epoxy with nanocellulose. In this this research, we fabricated nanocellulose directly from hemp fibres by employing oxidation/sonication method with the aim to solve the main problems of nanocellulose fabrication with sulphuric acid hydrolysis or mechanical. By using this method the yield of nanocellulose could up to 54.11 % and the crystallinity of nanocellulose was 86.59 %. In order to expand the application of nanocellulose, we investigated the modification of natural fibres (hemp) with nanocellulose and the fabrication of nanocomposite. Two-step modification, i.e. dodecyltrimethylammonium bromide (DTAB) pretreatment and nanocellulose modification, was used to modify hemp fibres. In this process, we systematically investigated the deformation of hemp fibres, revealed the mechanism of deformation on the mechanical property of single fibre by using Fourier transform infrared spectroscopy (FTIR) and investigated the effect of deformation on the hemp fibre modification with nanocellulose by using energy dispersive X-ray (EDX). The two-step modification increased the mechanical properties of hemp fibres significantly. Compared with raw hemp fibres, the modulus, tensile stress and tensile strain of the two-step nanocellulose modified hemp fibres increase by 36.13 %, 72.80 % and 67.89 %, respectively. Moreover, two-step modification facilitated the improvement of interfacial property of fibres. This novel natural fibre modification provides new clue to exploit nanocellulose as a green chemical agent for natural fibres modification. We modified nanocellulose by using curing agent of epoxy---diethylenetriamine (DETA). This modification could increase the dispersity of nanocellulose in epoxy and reinforce epoxy. Compared with epoxy, the modulus, tensile stress and tensile strain of the modified nanocellulose/epoxy nanocomposite increased 1.42 %, 15.44 % and 27.47 %, respectively.

Face à la nécessité de trouver des alternatives aux ressources d’origine fossile et de limiter les impacts environnementaux de l’activité humaine, un important effort de recherche est actuellement en cours pour favoriser et accroître l’utilisation de produits issus de ressources renouvelables, comme les fibres végétales, dans la conception de pièces industrielles. Toutefois, de nombreux verrous scientifiques et technologiques restent encore à lever avant de pouvoir valoriser de façon fiable et durable ces fibres dans un contexte technique exigeant tel que celui du secteur l’automobile. Ainsi, l’amélioration de la qualité de l’interface fibres végétales / matrice polymère est un enjeu de taille car elle constitue une condition permettant de satisfaire les performances mécaniques requises telles que la rigidité, la résistance ou la tenue au choc. Dans ce contexte, l’objectif de la thèse a été le développement de fibres courtes de chanvre à propriétés de surface maitrisées et ciblées. Des solutions de fonctionnalisation de surface applicables par des procédés industrialisables ont été développées dans le but d’incorporer ces fibres dans une matrice polypropylène (PP). Les fibres de chanvre ont ainsi été traitées selon différentes stratégies de fonctionnalisation incluant l’utilisant du polypropylène greffé anhydride maléique (PP-g-MA), d’organosilanes, d’un acide aminé, d’isocyanates et d’un polyuréthane. Deux procédés de traitement à faible impact environnemental ont été comparés : le sprayage direct des fibres par les molécules de fonctionnalisation et l’incorporation de ces molécules par extrusion réactive. Les traitements en extrusion réactive se sont montrés plus efficaces que ceux réalisés par sprayage dans le cas du PP-g-MA. Trois voies de fonctionnalisation se sont avérées pertinentes au regard des propriétés mécaniques visées  : i) l’utilisation de PP-g-MA seul en extrusion réactive ; ii) la fonctionnalisation par sprayage d’un aminosilane ou d’un acide aminé couplée à l’incorporation du PP-g-MA en extrusion réactive. S’appuyant sur le développement de moyens expérimentaux et d’analyses spécifiques, l’étude du comportement au choc des biocomposites a montré que les composites renforcés fibres de chanvre permettent d’absorber d’avantage d’énergie que les composites PP / verre (à taux volumique de renfort identique) pour une longueur de fissuration similaire. Une modélisation par éléments finis du comportement au choc des composites étudiés est également proposée. / Due to the necessity to find alternatives to fossil resources and to reduce the environmental impacts of human activity, a major research effort is currently ongoing in order to develop and increase the use of biobased products from renewable resources, such as natural fibers, in the design of industrial parts. However, many scientific and technological hurdles have yet to be removed so as to promote these products before we can reliably and durably use these fibers in a demanding technical context as in automotive sector. Thus, improving the quality of the interface between natural fibers and polymer matrix is a major challenge, since it constitutes a condition for satisfying the required mechanical performances, such as stiffness, tensile or impact strengths. In this context, the thesis objective was to develop short hemp fibers with controlled and targeted surface properties. Surface-functionalization solutions have been developed, to be used by industrial processes, with the aim of incorporating these fibers in a polypropylene (PP) matrix. Therefore, hemp fibers have been treated according to various functionalization strategies including the use of grafted polypropylene maleic anhydride (PP-g-MA), organosilanes, an amino acid, isocyanates and a polyurethane. Two treatments processes, with low environmental impact, were compared: the direct spraying of functionalization molecules on fibers and reactive extrusion incorporation of these molecules. Reactive extrusion treatments were more efficient than those performed by spraying in the case of PP-g-MA. Three functionalization lanes have been found to be relevant regarding the mechanical properties targeted: i) using PP-g-MA alone in reactive extrusion; ii) spraying-functionalization of an aminosilane or of an amino acid coupled with the incorporation of PP-g-MA into the reactive extrusion. Based on the development of experimental means and specific analyzes, the study of the impact behavior of biocomposites has shown that hemp fiber reinforced composites allow to absorb more energy than PP / glass composites (at identical reinforcing volume rate) for a similar crack length. Also, a finite element modeling of the impact behavior of the studied composites is propounded.

There is an increasing demand for natural fibres in the textile industry as a consequence of the negative impact of the industry on the environment. Svensk Hampaindustri (SHI) is currently growing hemp in Sweden for its seeds. This leaves residue in the form of hemp stems that could be processed for textile products. Today this residue material is not used for anything, however there is a desire that it could be used for added value. This study investigates the possibility of extracting fibres from the hemp residue mechanically and using them in applications. Hemp, a variety of Cannabis sativa L., is a multipurpose low-input crop cultivated for its seeds, fibres and hurds. Hemp fibre is a bast fibre, derived from the plant’s outer stem tissues. To extract hemp fibres from hemp stems, the first step is to separate the fibre bundles from the other, non-fibrous parts of the stem. This process is done using various mechanical methods. In order to ease the separation, hemp stems are retted. Retting is a biological process that uses enzymatic activities to degrade the pectins and thus making the separation easier. Retting is one of the most considerable challenges towards a wider use of hemp fibres. Water retting offers high fibre-quality but consumes high amounts of water and causes effluents in the wastewater. Dew retting offers a high fibre yield and low labour costs but will result in a lower fibre-quality. Alternative methods that can contribute with a more consistent fibre yield and quality are available, but with an economic uncertainty for the farmers that limits the competitiveness of the hemp fibre. The hemp material provided by SHI was unretted and needed to be broken down by means of mechanical processing in order to extract the fibres. This was done using a domestic blender. The crushed material was then carded using a hand carding machine to achieve oriented and clean fibres. The obtained fibres were then evaluated for their length and fineness. Three different types of nonwoven were made using the hemp fibres: NW1, NW2 and NW3. NW1 consists of 100% hemp, whereas NW2 and NW3 are 80/20 blends of hemp and PLA. NW1 was needle punched, NW2 was thermally bonded and NW3 was manufactured by both thermal bonding and needle punching. The produced nonwovens were evaluated by their air permeability, thermal conductivity, sound absorption, drapability and tensile strength. The results from the study showed that it is possible to extract unretted fibres using mechanical methods. The fibres are quite coarse and therefore more suitable for industrial applications. The different production methods for the nonwovens gave different results which supports the diversity of hemp applications. This study suggests that the residue should be used rather than be disposed of.

More sustainable and efficient degumming methods are required to extract finner bast fibres, especially from agro-industrial waste streams such as stalks from hemp for food purposes. For this reason, in this study, two urea-based treatments were evaluated as degumming alternatives for unretted hemp fibres from residual streams, one at cold and alkaline conditions (CUA) and the other in combination with microwave radiation (MWU). Both approaches reduced fiber bundles diameter, decreasing 61% at -7°C 5 minutes, 12%Urea-5%NaOH, and 44% for microwave-30%urea for 30 minutes. Although both methods resulted in considerable fibre bundle diameter reduction, they resulted in a lower reduction than the 74% obtained for a traditional alkali (TA) degumming. Shorter fibres were obtained after the treatments. CUA and TA treatments obtained similar fibre lengths, while MWU resulted in longer than the other treatments. The chemical and thermal analysis showed that the highest removal of no cellulosic components was achieved by the TA treatment, followed by CUA and MWU. The treatments were applied to nonwovens produced by needle punching, showing no significant differences in tenacity and flexural rigidity compared to non-treated nonwovens. An increase of mass per unit area was identified for the CUA-treated fabrics, attributed to crimp generated in the treatment. Both urea-based treatments showed potential as more sustainable alternatives for degumming unretted hemp fibre bundles extracted from agro-waste.

Ce travail de thèse, s'inscrit dans un accord co-tutelle entre l’École Polytechnique de Thiès du Sénégal, et de l'Université de Franche-Comté. Il a été réalisé au Département de Mécanique Appliquée de l'institut FEMO-ST à Besançon (France). [...]L'objectif de cette thèse est de contribuer à la caractérisation du comportement thermo-hygro-mécaniques des fibres libériennes élémentaires issues du chanvre. Les fibres élémentaires testées dans ce travail ont des diamètres extérieurs moyens d'environ 20µm et des longueurs utiles de l'ordre de 10mm. Des essais couplant des chargements mécaniques, hygroscopiques et thermiques sont réalisés afin d'apporter des éléments de compréhension sur le comportement des fibres et de collecter une base de données sur leurs performances mécaniques.Trois types de comportement sont identifiés sur les fibres en traction quasi statique en fluage pour les différents niveaux hygro-thermique testés. Une rigidification de la fibre est révélée sous chargements cycliques progressifs dans des conditions environnementales constantes. Une chute du module d' Young initial de la fibre est remarquée quand l'humidité relative augmente. Une accélération de la vitesse de déformation différée de la fibre est obtenue en fluage lorsque des cycles d'humidité relative sont appliqués. Une baisse des propriétés mécaniques des fibres sous l'effet de la température est également observée. Elle dépend directement du niveau de la durée de l'exposition à la température. / The thesis work joins in the framework in joint supervision between the Polytechnic school in Thies (Sénégal) and the University of Franche-Comté (France)[...]The aim of this thesis is to contribute to the characterization of thermo-hygro-mechanical behaviour of elementary hemp fibres. These fibres used in this work have an average diameter approximately 20µm and useful length of only 10 mm. The méchanical, hygroscopic and thermal coupling testing are realized to provide some understanding of the behaviour of the hemp fibres and to collect details from a database on their mechanical performance.From the uniaxial quasi static tensile tests and creep tests, three categories of behaviours are measured and observed. How ever subject to constant environmental conditions, a fibre hardening is observed under cyclic tensile loading. It was also found that a drop of the initial Young 's modulus of the hemp fibres when the relative humidity gradually increases. Thus, the strain rates measured on the fibres during creep exhibited a speeding up relative humidity cycles are imposed . We found also that the mechanical properties of the fibres decrease under temperature effects. It depends directly on the level and exposure time to temperature

Les réelles opportunités de croissance dont bénéficient les marchés liés à l'utilisation de fibres végétales en tant que renfort dans les matériaux composites sont intimement liées aux performances concurrentielles de ces fibres par rapport à celles de fibres de verre en particulier l’allégement, l’amortissement et l’isolation thermique. Dans l'industrie de la fibre de chanvre, le rouissage est le premier traitement appliqué aux plantes afin de faciliter la séparation des fibres de la partie ligneuse centrale de la tige. Ce traitement est actuellement réalisé de manière empirique en champ conduisant à l’obtention de fibres de qualité variable (couleur, morphologie, microstructure, composition biochimique, propriétés thermiques et mécaniques) ce qui constitue un frein à leur utilisation plus large dans des composites hautes performances. Par conséquent, la maîtrise du rouissage est primordiale. L’objectif de ce travail de thèse est de développer une approche globale de cette étape-clé de la production des fibres de chanvre en combinant à la fois l’étude du mécanisme biologique du rouissage, celle des caractéristiques intrinsèques des fibres et celle des émissions gazeuses et des odeurs associées à l’étape de rouissage. Différents items ont été particulièrement examinés :- L’influence de la durée du rouissage et de la période de récolte sur les caractéristiques intrinsèques des fibres de chanvre (couleur, morphologie, composition biochimique, microstructure, propriétés mécaniques, propriétés thermiques).- L’évolution des émissions de composés organiques volatils (COV) et de l'odeur lors du rouissage en champ.- La dynamique temporelle des densités de population des communautés bactériennes et fongiques pendant le rouissage- L'impact du rouissage en champ (climat méditerranéen) et du rouissage accéléré (conditions contrôlées en laboratoire) sur les propriétés microstructurales, thermiques et mécaniques d’un biocomposite polypropylène/fibre de chanvre / The natural fibres are increasingly used as reinforcements in polymer composites due to their challenging performances compared to conventional fibres in term of good specific mechanical properties, damping and thermal insulation. In the hemp industry, the retting is an upstream processing applied to the plants in order to facilitate the separation of fibres from the central woody part of the stem. This treatment is currently carried out in an empirical way in the fields that leads to a large variability in the hemp fibres instrinsic characteristics (color, morphology, biochemical composition, microstructure, thermal and mechanical properties) which limit their large use in high-performance composites. Therefore, controlling retting treatment is a crucial step. The aim of this thesis is to develop a global approach to this key step in the production of hemp fibers by combining the study of the biological mechanism of retting, the intrinsic characteristics of fibers and that of emissions volatile organic compounds and odors associated with the retting step. Different items were particularly examined:- The influence of retting duration and harvest period on the intrinsic characteristics of hemp fibers (color, morphology, biochemical composition, microstructure, mechanical and thermal properties).- The evolution of Volatile Organic Compounds (VOCs) and odors of hemp stems during field retting- Temporal dynamics of population densities of bacterial and fungal communities during retting- The impact of field retting (Mediterranean climate) and accelerated retting (controlled conditions in the laboratory) on the microstructural, thermal and mechanical properties of a polypropylene / hemp fibers biocomposite

Ces travaux de thèse constituent une contribution au développement de composites chanvre/époxy 100% bio-sourcés. Les enjeux environnementaux actuels favorisent l'émergence de matériaux issus de ressources renouvelables telles que les fibres végétales mais conduisant aussi à une large gamme de synthons bio-sourcés, notamment à l'origine de prépolymères époxydiques. Une étude approfondie des deux constituants (fibres de chanvre et matrices polyépoxydiques) est réalisée avant l'étape d'élaboration des composites. Un traitement au CO2 supercritique est appliqué sur les fibres de chanvre utilisées comme renfort dans les matériaux composites. Le résultat de ce traitement mène à une meilleure individualisation ainsi qu'à une baisse du pouvoir hygroscopique des fibres. Ces aspects, décisifs pour garantir de bonnes propriétés pour le composite final, sont néanmoins nuancés par une baisse des propriétés ultimes en traction à l'échelle des fibres mais également à l'échelle du composite. De la même façon, la diminution du pouvoir hygroscopique des fibres après traitement se répercute à l'échelle du composite, permettant ainsi d'améliorer la durabilité du composite. La synthèse des résines époxydiques utilisées dans cette étude est réalisée à partir de ressources renouvelables et abondantes telles que la lignine. Les polyépoxydes thermodurcissables ainsi préparés présentent de bonnes performances, compatibles avec le cahier des charges pour des applications composites à renfort végétal. Au regard des résultats obtenus, les composites 100% bio-sourcés sont des matériaux d'avenir. Leur développement nécessite néanmoins une étude approfondie de leur durabilité. / This thesis contributes to the development of 100% bio-based hemp/epoxy composites. Current environmental issues favor the emergence of materials derived from renewable resources such as plant fibres and a wide range of bio-based building-blocks, source of epoxy prepolymers in particular. An intensive investigation of the two constituents (hemp fibres and polyepoxidic matrix) is carried out before the composites manufacturing. Supercritical CO2 treatment is applied to hemp fibres used as reinforcement in composite materials. This treatment, not optimized, leads to better individualization as well as a decrease in the hygroscopic power of the fibres. These aspects, which are essential in order to guarantee good properties for the final composite, are nevertheless qualified by a loss of mechanical properties at the fibre scale but also at the composite scale. In the same way, the decrease in the hygroscopic power of the hemp fibres after treatment is reflected at the composite scale, thus improving the durability of the crosslinked material. The synthesis of the epoxy resins used in this study is made from abundant resources such as lignin. The thermosetting polyepoxides prepared in this study have good performance, compatible with the specification for composite applications with plant fibres reinforcement. In view of the results obtained, 100% bio-based composites are materials with a high future potential. Nevertheless, their development requires a comprehensive sustainability study.