Mes travaux de thèse s'inscrivent dans le cadre de l'étude de l'adsorption de systèmes moléculaires confinés dans des matériaux nanoporeux. Le confinement d'un fluide a des effets importants sur ses propriétés thermodynamiques car la compétition entre les effets de la taille des pores et les effets d'interface engendre des comportements nouveaux très spécifiques, comme de nouvelles phases et de nouvelles transitions de phase. Ces phénomènes interviennent communément dans de nombreux processus et procédés industriels : échange ionique, séparations sélectives, catalyse hétérogène... En particulier, j'ai étudié par simulation moléculaire les propriétés d'adsorption de molécules polaires d'intérêt industriel (CO2 et H2O) dans une nouvelle classe de matériaux poreux cristallins hybrides organiques-inorganiques dénommés MOFs (Metal-Organic Frameworks). Il s'agit de systèmes avec des propriétés d'adsorption remarquables déterminées par leur variété topologique et versatilité dues à la richesse de la chimie organique et de coordination et au fait qu'ils peuvent être fonctionnalisés avant comme après synthèse. Dans un premier temps je me suis intéressée à l'adsorption du CO2 dans une famille de systèmes ayant tous la même topologie mais des volumes poreux différents, les IRMOFs. J'ai pu ainsi caractériser l'effet du confinement sur leur capacité d'adsorption et un comportement universel a été mis en évidence : la température critique diminue lorsque le confinement augmente. Ensuite, j'ai étudié une nouvelle MOF cationique dénommée Zn2(CBTACN). Après avoir réussi à localiser les anions halogénure extra-charpente (ce qui n'était pas possible expérimentalement), j'ai caractérisé l'adsorption du CO2 dans ce matériau, d'abord comme corps pur et ensuite dans des mélanges. Enfin, je me suis intéressée à la stabilité hydrothermique de ces matériaux, qui est une thématique cruciale pour les applications. En particulier, j'ai observé le mécanisme d'hydratation d'un analogue de la MOF-5 qui se fait en deux étapes. Des effets collaboratifs, qui n'avaient pas été soulignés jusqu'à présent dans la littérature, ont été également mis en évidence.

Cloud computing is emerging as a promising platform for compute and data intensive scientific applications. Thanks to the on-demand elastic provisioning capabilities, cloud computing has instigated curiosity among researchers from a wide range of disciplines. However, even though many vendors have rolled out their commercial cloud infrastructures, the service offerings are usually only best-effort based without any performance guarantees. Utilization of these resources will be questionable if it can not meet the performance expectations of deployed applications. Additionally, the lack of the familiar development tools hamper the productivity of eScience developers to write robust scientific high performance computing (HPC) applications. There are no standard frameworks that are currently supported by any large set of vendors offering cloud computing services. Consequently, the application portability among different cloud platforms for scientific applications is hard. Among all clouds, the emerging Azure cloud from Microsoft in particular remains a challenge for HPC program development both due to lack of its support for traditional parallel programming support such as Message Passing Interface (MPI) and map-reduce and due to its evolving application programming interfaces (APIs). We have designed newer frameworks and runtime environments to help HPC application developers by providing them with easy to use tools similar to those known from traditional parallel and distributed computing environment set- ting, such as MPI, for scientific application development on the Azure cloud platform. It is challenging to create an efficient framework for any cloud platform, including the Windows Azure platform, as they are mostly offered to users as a black-box with a set of application programming interfaces (APIs) to access various service components. The primary contributions of this Ph.D. thesis are (i) creating a generic framework for bag-of-tasks HPC applications to serve as the basic building block for application development on the Azure cloud platform, (ii) creating a set of APIs for HPC application development over the Azure cloud platform, which is similar to message passing interface (MPI) from traditional parallel and distributed setting, and (iii) implementing Crayons using the proposed APIs as the first end-to-end parallel scientific application to parallelize the fundamental GIS operations.

Metal-organic frameworks (MOFs) are porous networks of metal-centers connect by organic ligands, which have potential for an array of applications including gas separations and storage, drug delivery, and molecular sensing. A multitude of structures are reported with specific pore geometries and functionalities, but MOFs are not currently implemented in consumer or industrial applications. Two major setbacks have hindered their transition to the applied level. 1) Many MOFs are not stable in the presence of ambient moisture. 2) Most syntheses are costly and take place under batch-style solvothermal conditions. This thesis addresses both of these setbacks and examines the performance potential of water-stable MOFs for selective gas adsorption. A representative set of MOFs are exposed to water, and structural effects are monitored from a before and after comparison to identify properties of water-stable MOFs. A novel continuous-flow MOF synthesis process is reported along with preliminary optimization experiments, which yield direct suggestions for future process improvements. Batch-style scale-up experiments are also conducted for three other MOFs, which provide insight into synthesis phenomena. Application specific results are reported for toxic chemical filtration and carbon dioxide removal from flue gas using MOFs. The thesis concludes by summarizing the experimental findings, discussing the application potential of specific MOFs, and recommending topics for future research projects. Pitfalls observed during this research are also directly discussed along with potential solutions.

Ideas about water use and ethics have been linked for many thousands of years. In this millennium, water resources remain a primary area of concern throughout the world, including such issues as shortages, supply, flooding, quality, restoration, allocation and regulation. Today, electronic environmental news and specialty websites contain a breadth of information on current water resources conflicts and issues throughout the world. In many parts of the world, water quantity is decreasing and water quality is worsening, lack of access to improved water supplies is decreasing, as is access to basic sanitation. Water challenges relating to water quantity and water quality are increasingly common in Canada and the United States due to water resources being under increasing pressure from population growth, economic activity and intensifying competition for the water among users. Faced with these challenges, humans are confronted with momentous decisions. Before making more decisions that will have an influence over water resources, and in response to repeated calls for a water ethic, this research takes the perspective that it is necessary to explore the ethical intentions of decision-makers with respect to water resources legislation and policy in Canada. The ultimate goal is to define a set of principles for a proposed water ethic that could and should be implemented at the municipal level of government in Canada. A review of academic and professional literature and a mixed methods research approach comparing two case study areas was used to gain a baseline understanding of the potential influences of underlying ethical frameworks on policy makers in Calgary, Alberta and Guelph, Ontario. A proposed water ethic, containing a set of principles compiled from ethical considerations for water use in academic and professional literature, was also developed and presented to case study participants. Participants provided feedback on their strength of agreement with each principle, thoughts on modifications, improvements and/or deletions of any principle, and implementation considerations of the proposed water ethic at the municipal level of government. The results indicate that case study participants in both areas apply a variety of ethical frameworks when making professional decisions about water resources management, and when preparing water legislation and policy. A review of relevant legislation, policies, documents and strategies in the case study areas supports this conclusion. In particular, components of the Consequentialist ethical framework (a perspective that can be associated with sustainable development and sustainability) are most often acknowledged in the statements of intent of the participants and water resource legislation and policies. Respondents also indicated that value positions associated with the Intrinsic Value ethical framework influenced policy preparation and decision-making; however, the ethical considerations associated with this framework are not as obvious in the language and intent of relevant legislation, plans, documents, and strategies. The case study participants in both areas supported all six proposed principles of the proposed water ethic and offered only minor modifications to the presented wording and intent. The endorsed principles of the proposed water ethic are: (1) allocate sufficient water to maintain and enhance ecosystem integrity; (2) establish conservation and efficiency measures as a priority over new supply initiatives in water resources planning; (3) meet basic human needs and enhance equity; (4)establish open and participative decision-making processes; (5) identify and seek to obtain multiple sustainability benefits from water-centered initiatives; and, (6) explicitly acknowledge system complexity and emphasize precaution. The feedback from the participants about the proposed water ethic, in association with the results of the ethical frameworks, informed the eight implementation recommendations, including: (1) entrench a water ethic vision in Provincial and municipal legislation; (2) work from within existing governance structures and institutional arrangements; (3) use an incremental model of decision-making; (4) provide specific policy examples for each principle within a water ethic; (5) include realistic and measurable targets within the policies; (6) accept that all six water ethic principles are unlikely to be accepted at once; (7) ensure the overall vision of the water ethic, principles, associated examples, and measureable targets, are defensible; and, (8)acknowledge the importance of strategy. The recommendations acknowledge that while the proposed water ethic is presented as a package and each principle is valuable, conflict and trade-offs may occur during the implementation process. The recommendations are therefore pragmatic and take into account the current governance structures and institutional arrangements. There is a growing recognition that understanding the underlying ethical perspectives that influence decision-makers may contribute to more effective water resources management legislation and policy. This research adds to this body of knowledge by showing that it is possible to identify ethical frameworks, extract the defining characteristics associated with each framework, and use case studies to suggest which ethical frameworks assert varying degrees of influence. This link between theory and practice may help organizations recognize what ethical considerations influence decision-making and identify the strengths and limitations of these ethical approaches to managing water resources. In addition, prior to this study, research had only been conducted into the identification of principles for the ethical use of water and not into the potential for implementation of a realistic and desirable water ethic that reflects sustainability and lasting well-being at the municipal level of government in Canada. Several opportunities exist to build on this research. They include (1) investigate if the ethical intent of legislation and policy related to water resources management is put into practice, (2) identify other ethical frameworks that may apply to decision-making, (3) focus on political decision-makers and their claims and intentions about water use, (4) test the implementation of the water ethic proposed in this study, and (5) investigate how to integrate ethical considerations about water into checklists and protocols related to land use development, professional codes of conduct and standards, institutional and organizational training programs, performance measures for official plans, and as standard components for municipal council reports and ministerial presentations. This exploratory research concludes that policy makers are willing to become more aware of their underlying ethical underpinnings and to learn how ethical considerations embedded in legislation and policy have the potential to exert significant influence over the behaviour of current and future water users.

Fault diagnosis in discrete event systems is studied using a state-based framework. Faults can be either intermittent or permanent. For intermittent faults, system may recover from faulty behaviour through reset. To diagnose such intermittent faults, fault counters are introduced. Fault counters record the number of intermittent faults which must have occurred according to the output observations. This provides the main diagnosis. They also record the number of possible intermittent faults which may have occurred but cannot be confirmed. This provides auxiliary diagnostic information. Fault diagnosability is then studied. Since faults may be intermittent, they may occur repeatedly. Three different notions are studied: 1-diagnosability, 1,k-diagnosability, and 1,infty-diagnosability, and criteria for each of these notions are obtained. The criteria are expressed in terms of fault counters and extend the diagnosability criteria for permanent faults. The concept of a resonant path is introduced, which plays an important role in studying diagnosability.

Fault diagnosis in discrete event systems is studied using a state-based framework. Faults can be either intermittent or permanent. For intermittent faults, system may recover from faulty behaviour through reset. To diagnose such intermittent faults, fault counters are introduced. Fault counters record the number of intermittent faults which must have occurred according to the output observations. This provides the main diagnosis. They also record the number of possible intermittent faults which may have occurred but cannot be confirmed. This provides auxiliary diagnostic information. Fault diagnosability is then studied. Since faults may be intermittent, they may occur repeatedly. Three different notions are studied: 1-diagnosability, 1,k-diagnosability, and 1,infty-diagnosability, and criteria for each of these notions are obtained. The criteria are expressed in terms of fault counters and extend the diagnosability criteria for permanent faults. The concept of a resonant path is introduced, which plays an important role in studying diagnosability.

Les MOFs résultent de l'organisation de polyèdres métalliques reliés par des molécules organiques chélatantes pour former un réseau poreux. La construction de solides hybrides organiques/inorganiques permet d'imaginer un très grand nombre de matériaux aux propriétés structurales et physico-chimiques variées. Le confinement du substrat dans une structure rigide, associé à des propriétés particulières des clusters métalliques ainsi qu'à des parois pouvant être fonctionnalisées, fournissent un environnement catalytique unique, plaçant les MOF à la frontière entre les espèces types zéolites et les enzymes. Cependant, il existe aujourd'hui très peu de MOFs possédant plus d'une fonction catalytique. Néanmoins, les propriétés catalytiques des MOFs peuvent être améliorées de façons non négligeables grâce aux méthodes de post-fonctionalisation. Dans ce travail, nous reportons le développement d'une méthode de post-fonctionnalisation originale des amino-MOFs. La première étape consiste à convertir la fonction amine en fonction azoture. Puis, sans isolation ni purification, le MOF fonctionnalisé est obtenu par " Click Chemistry " en ajoutant l'alcyne correspondant. Cette méthode peut être appliquée à tous les types d'amino-MOFs et à quasi toutes les fonctions chimiques que l'on souhaite greffer. Une large librairie de nouveaux matériaux a ainsi été obtenue et complètement caractérisée. Cette méthode a aussi été utilisée pour créer des MOFs catalytiques à façon pour une réaction de transesterification, ainsi que pour l'investigation de nouvelles applications plus fines (niches industrielle)

The very large number of distinct structures that are known for metal-organic frameworks (MOFs) and zeolites presents both an opportunity and a challenge for identifying materials with useful properties for targeted separations. In this thesis we propose a three-stage computational methodology for addressing this issue and comprehensively screening all available nanoporous materials. We introduce efficient pore size calculations as a way of discarding large number of materials, which are unsuitable for a specific separation. Materials identified as having desired geometric characteristics can be further analyzed for their infinite dilution adsorption and diffusion properties by calculating the Henry's constants and activation energy barriers for diffusion. This enables us to calculate membrane selectivity in an unprecedented scale and use these values to generate a small set of materials for which the membrane selectivity can be calculated in detail and at finite loading using well-established computational tools. We display the results of using these methods for >500 MOFs and >160 silica zeolites for spherical adsorbates at first and for small linear molecules such as CO₂ later on. In addition we also demonstrate the size of the group of materials this procedure can be applied to, by performing these calculations, for simple adsorbate molecules, for an existing library of >250,000 hypothetical silica zeolites. Finally, efficient methods are introduced for assessing the role of framework flexibility on molecular diffusion in MOFs that do not require defining a classical forcefield for the MOF. These methods combine ab initio MD of the MOF with classical transition state theory and molecular dynamics simulations of the diffusing molecules. The effects of flexibility are shown to be large for CH₄, but not for CO₂ and other small spherical adsorbates, in ZIF-8.

Internationalization is an important strategic issue for survival for most business schools of today. Following this, various international accreditation bodies have in recent years been very succes­s­ful in promoting accreditation as a means of gaining status and prove high quality. These business school accreditation schemes clearly state their targets against top quality international schools and programs. Internationalization of the business school opera­tions can thus be stated to be of vital impor­tance for schools aiming for one or more of these accreditations. The intention of this study is to turn the issue around and explore to which extent, and with what kind of impact, the accreditation processes in turn have on the area of interna­tiona­li­­­zation within the business school organization.   The theoretical framework consists of three main areas: ’The Business School Environment’, ‘Strategy as Practice’ and ‘Institutional Theory’. The first part aims to reach an understanding for the environment and situation that business schools of today are facing. It also highlights major challenges for the future. In the second part, Strategy as Practice research theories are used to gain understanding for strategy behaviour and strategy creation within plu­ra­listic organi­zations, such as the higher education insti­tution. The third part deals with issues on Quality Frameworks with the aim to reach understanding for the im­pact such processes can have on the organization. Sensemaking Theory is further used to illustrate the rational behind decision making of busi­ness school leaders and the concluding part connects theories on quality frameworks to Identity Creation, linking together identity with culture and image.   The research approach for this qualitative study is the abductive one and the empirical data is collected through a number of semi-structured interviews with business school repre­sen­tatives at various levels working in the area of international relations.   Main findings are presented within the framework of a time structured (past, present, future) model connected to the study’s five objectives: The development of internationali­zation within the school; the view on internationalization among organizational members; the charac­teristics of decision making and implementation processes; the main impact factors of accreditation and the expectations of major future challenges.   The results indicate that although accreditation has shown to have had a substantial impact on the success of business school operations in an international perspective, it is to a much lesser extent a concrete tool for change and improvement within the area of internatio­nali­zation as such. Accreditation has shown to be strongly connected to previous develop­ment and view on internationalization within the organizations. Also, a strong belief in, and commit­ment to, internationalization among influential organizational members has proved to be vital for the accreditation processes. Furthermore, a number of unique charac­teristics connected to the identities’ of the organiza­tions studied, showed to have notable impact on the success of the schools’ international opera­tions, so also the accreditation processes. This includes organiza­tional culture and tradition; working methods; dissemi­nation of information; strong social connections; knowledge, dedication and commitment by individuals and management’s ability to provide organizational members with trust, respect, autonomy and encouragement.

This paper examines the informal economy’s greenhouse-gas (GHG) emissions and whether it poses a problem to the effectiveness of international frameworks designed to reduce GHG emissions. With the results of a literature review conducted on the relation between the informal economy and regulations and results on 160 nations’ theoretical informal-economy emissions over time, this paper finds that the informal economy does hinder the ability of governments to manage GHG emissions. This paper then discusses how this aspect of the world’s economy limits the efficacy of international frameworks to reduce GHG emissions. Suggestions are made on how to incorporate this sector into the proposed frameworks. The paper concludes with summarizing the main findings and proposals for further research.