Dissertations / Theses on the topic 'Réduction du dioxyde de carbone'
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Gomes, Christophe. "Une approche diagonale pour la transformation catalytique du dioxyde de carbone." Phd thesis, Université Paris Sud - Paris XI, 2013. http://tel.archives-ouvertes.fr/tel-00954408.
Full textSahin, Nihat Ege. "Réduction électrochimique du dioxyde de carbone sur des électrocatalyseurs à base de cuivre." Thesis, Poitiers, 2016. http://www.theses.fr/2016POIT2313/document.
Full textThe anthropogenic emissions of carbon dioxide (CO2) are the major cause of global warming. The selective CO2 reduction reaction (CO2RR) of has been proposed as a promising, convenient and efficient method for sustainable energy conversion systems. The reduction of CO2 to energetically valuable products requires the use of an appropriate electrode material. This study focuses on the preparation of Cu-based electrocatalysts supported on different types of carbon materials such as Vulcan XC-72R, mesoporous carbon CMK-3, mesoporous carbon FDU-15 and tannin based mesoporous carbon IS2M for the CO2RR under mild conditions. Besides, Vulcan XC-72R carbon supported bimetallic copper/palladium alloy materials were prepared for increasing the Faradaic yield. These copper-based catalysts were electrochemically characterized and preparative electrolyses set at constant potential were carried out in order to investigate the reduction products distribution and Faradaic yields as a function of the applied potential and catalyst loading. Chemicals such as HCOOH, CO and H2 issued from the CO2RR, were determined with in-situ and ex-situ complementary (electro)analytical and spectroscopic techniques. The significant difference in the product distribution is probably due to the ensemble (geometry and ligand) effects in the bimetallic CuPd materials, and textural structure of the supporting substrates. Selective CO2 to-HCOOH conversion has been successfully undertaken on Cu50Pd50/C with 62 % Faradaic efficiency
Frogneux, Xavier. "Transformations réductrices du CO2 pour la formation de liaisons C-N et C-C." Thesis, Paris 11, 2015. http://www.theses.fr/2015PA112136/document.
Full textIn the current world, carbon dioxide (CO2) is the major waste of the massive utilization of fossil resources but only few applications have been developed using this compound. In order to take advantage of its abundancy, the development of novel chemical transformation of CO2 to produce fine chemicals is of high interest in the scientific community. In particular, the formation of C-N bond(s) from CO2 and amine compounds unlocks a new way to access high energy and value-added. A second type of highly desirable transformation is the formation of C-C bonds with CO2 so as to synthesize carboxylic acid derivatives. The utilization of hydrosilanes as mild reductants allows the reactions to proceed under 1 bar of CO2 with abundant and cheap metal-based catalysts (iron, zinc) or with organocatalysts. The synthesis of formamides, methylamines and aminals from CO2 are described herein. Ultimately, the catalytic carboxylation of carbosilanes has been achieved for the first time using copper-based complexes. In the specific case of 2-pyridylsilanes, the use of pentavalent fluoride salts allowed us to perform the reaction without catalyst
Christophe, Jennifer. "Etude de l'électroactivité du cuivre pour la réduction du dioxyde de carbone et pour la réduction de l'ion nitrate." Doctoral thesis, Universite Libre de Bruxelles, 2007. http://hdl.handle.net/2013/ULB-DIPOT:oai:dipot.ulb.ac.be:2013/210680.
Full textDans la première partie du travail, nous avons comparé, à l’aide de la voltampérométrie, d’électrolyses à potentiel contrôlé et d’analyses chromatographiques, l'activité d'électrodes polycristalline et monocristallines de Cu et d'alliages AuxCuy de différentes orientations cristallines pour l'électroréduction de CO2.
Nous avons pu établir une étroite corrélation entre l'activité de l'électrode de Cu et l'arrangement atomique de sa surface. L'activité et la sélectivité pour CH4 de Cu décroissent selon la séquence :Cu (111) > Cu (100) > Cu (poly). La réduction du CO2 et la formation de CH4 sont favorisées sur les surfaces lisses et denses à l'échelle atomique.
La sélectivité des alliages AuxCuy est considérablement orientée vers CO quand la fraction superficielle de Au augmente. L'alliage de composition 50-50 conduit à la formation exclusive de CO.
La seconde partie de la thèse est consacrée à l'étude de l'activité d'électrodes massives de Cu polycristallin et monocristallin d’orientation (111) et de dispersions de Cu pour la réduction électrochimique de NO3-.
Nous avons mis en évidence l'importance des conditions de pH pour le déroulement des processus à l'électrode de cuivre. En milieu acide, NO3- est directement réduit en NH4+ alors qu’en milieu neutre, les réactions de réduction de NO3- en NO2- et de NO2- en NH4+ s’observent successivement en fonction du potentiel.
L'activité des dispersions de Cu dans un film de polyaniline dépend fortement des conditions de dépôt. Le cuivre incorporé au film sous sa forme réduite est plus actif que le cuivre incorporé au film initialement oxydé. Par ailleurs, nous avons montré que la concentration de H+ dans le polymère est limitée. En conséquence, le processus de réduction de NO3- sur le cuivre dispersé dans un film de polyaniline est modifié en milieu acide.
L’utilisation d’un film de poly-3,4-éthylènedioxythiophène déposé sur une surface de Pt s'est quant à elle révélée inadéquate comme support pour l'incorporation de Cu dans le cadre de l'étude de la réduction de NO3- en milieu acide.
Doctorat en Sciences
info:eu-repo/semantics/nonPublished
Stanbury, Matthew. "Réduction photo et électro-assistée sélective du dioxyde de carbone sur des catalyseurs moléculaires." Thesis, Université Grenoble Alpes (ComUE), 2016. http://www.theses.fr/2016GREAV094/document.
Full textThe general context of this thesis is on CO2 valorisation, and recounts fundamental research aimed at finding new molecular catalysts in order to achieve CO2 conversion. The results obtained provide additional knowledge in view of developing an efficient and selective catalytic CO2 reduction process. The first chapter begins with the general picture of CO2 utilisation and contains a bibliographical overview on the use of molecular catalysts for CO2 photo- and electroreduction. This short review demonstrates the wide variety of transition metal complexes used as catalysts, in particularly those based on rhenium. An analysis on the current state of CO2 reduction research using molecular catalyst complexes of the manganese carbonyl type is then reported. In Chapter II, the discussion begins with a brief overview of the research developed during this thesis relating to new complexes of the general formula: [Mn(L)(CO)3(X)] (X = Br, n = 0 ou CH3CN, n = 1; L = terpyridine derivatives). The interest in these complexes is twofold, as their physico-chemical properties give them potential catalytic CO2 reduction applications, as well as applications in the field relating to controlled CO release molecules. Developing new complexes based on ligands derived from terpy is one of the main routes that were chosen for catalyst performance optimisation and improvement. In this context, Mn complexes were synthesised, their photo- and electrochemical properties were studied in detail, before testing their activity with respect to catalytic CO2 reduction. The most remarkable result comes from the unique ability of these species to release one of their carbonyl ligands in a controlled fashion, which led to the discovery of novel Mn dicarbonyl complexes which are selective catalysts for CO2 reduction, and also to new molecules which are applicable in the release of small quantities of CO for therapeutic purposes.Chapter III covers the study of the complex [Mn(phen-dione)(CO)3(X)]n+ (X = Br, n = 0 ou CH3CN, n = 1). This complex was synthesised with the aim in mind of obtaining complexes soluble in aqueous media. While this objective was ambitious, it was soon found that these species showed no catalytic activity for CO2 reduction in the target aqueous medium. Nevertheless, electrocatalytic activity was demonstrated in hydro-organic media and photocatalytic applications in organic media proved promising. This work allowed us to gain a better understanding of the physicochemical properties and catalytic mechanisms of a Mn complex containing a redox-active ligand.The results presented in Chapter IV are based on the study of another new Mn carbonyl complex family. The study concentrated mainly on the complex [Mn(pyperNH)(CO)3(CH3CN)]+. The pyperNH ligand, with its aromatic system and NH functional group, plays a major role and is redox-active. After a section dedicated to its synthesis and characterisation, this chapter devotes a large part to the role that different experimental parameters can play on the efficiency of the catalytic CO2 reduction reaction. The Mn complexes described in this chapter have remarkable redox properties. A preliminary study of the catalytic activity of these complexes for CO2 reduction has allowed us to have an initial idea about the potential role of the N-H functional group of the ligand on the catalytic mechanism and reaction selectivity. This research was extended beyond the pyperNH ligand into a complex class of similar ligand structures, and the preliminary results obtained are original and promising, and open the way towards new perspectives
Routier, Mathilde. "Catalyse photochimique de la réduction du dioxyde de carbone par des porphyrines de fer." Paris 7, 2014. http://www.theses.fr/2014PA077066.
Full textThe transition from fossil fuels to renewable energy sources is a major challenge in today's society. The first step to address this challenge is to find a way to store and carry this energy, which can be done under the form of chemical bonds through the activation of small molecules like CO2, 02 and H2O. In this context, our work was focused on the catalytic photoreduction of carbon dioxide by three iron porphyrins showing remarkable electrocatalytic properties. We have first studied a homogeneous molecular photochemical approach. A careful analysis of the results, comparing the three porphyrins and the effect of the addition of a weak BrOnsted acid, allowed us to propose a reaction mechanism correlating the different behaviour of the porphyrins with their molecular structures. Furthermore, a detailed analysis of the experimental conditions required for the catalysis revealed that they induced the degradation of the porphyrins. To overcome these limits, we studied the use of a photosensitizer, resulting in improved catalytic performances and higher system stability. We also studied a homogeneous molecular photoelectrochemical approach, using p-type Si photoelectrodes. We observed the reduction of CO2 with a photovoltage of 350 mV, thus validating this strategy, but the process is limited by the sensitivity of the photoelectrodes towards 02. We are currently developing new electrodes made of copper oxide to obtain better catalytic performances and a higher stability
Gotico, Philipp. "Stratégies bio-inspirées pour la réduction catalytique et la valorisation du dioxyde de carbone." Thesis, Université Paris-Saclay (ComUE), 2019. http://www.theses.fr/2019SACLS283/document.
Full textThe criticality of global warming urges for the advancement of science to reduce carbon dioxide (CO₂) emissions in the atmosphere. At the heart of this challenge is the development of sustainable catalysts that can help capture, activate, reduce, and eventually valorize CO₂. This PhD work tried to respond to this call by developing molecular mimics inspired by natural systems in the larger scheme of artificial photosynthesis. Firstly, it involved tracking the journey of a photon of visible light and how it is transformed to a reducing power able to reduce CO₂. Secondly, in search for more efficient and stable catalysts, new mimics were synthesized inspired by the exceptional performance of CO dehydrogenase enzymes (CODH) in reducing CO₂. Lastly, further understanding of CODH also led to a proof-of-concept that directly valorizes the photo-produced CO for the synthesis of isotopically-labelled amide bonds, a common motif in pharmaceutically-relevant drugs
Bitar, Ziad. "Electrocatalyse de la réduction sélective du dioxyde de carbone sur électrodes à diffusion de gaz." Thesis, Grenoble, 2014. http://www.theses.fr/2014GRENV030/document.
Full textThis thesis concerns the valorization of CO2 by electrochemical means. It is largely devoted to the preparation and physico-chemical study of gas diffusion electrodes (GDE) in order to better understand the mechanisms and key parameters for electrocatalytic reduction of CO2 using this type of porous electrode. This study revolves around two main axes, the first is related to metal catalysts and the second is focused on molecular catalysts.The first axis deals with the preparation, characterization and electrochemical properties of Cu, Co, In, Zn, Bi, Pb and Fe catalysts supported on porous carbon powder. Their implementation to form GDE and their electrocatalytic activity toward CO2 reduction were studied. In aqueous medium, the GDE containing indium allowed obtaining the highest Faraday yields for electroreduction of CO2 to formic acid. In comparison with a metallic indium foil, the GDE-In/C showed improved catalytic performance and improved resistance to the electrolyte's impurities. We demonstrated that in the aqueous phase, a continuous flow of CO2 through a GDE resulted in an improved reactivity of the supported catalyst. This highlights the advantage of using dispersed metal particles on GDE rather than metal foil electrodes.The second axis of this study focuses on three dimeric ruthenium complexes with the general formula [Ru(L)(CH3CN)(CO)2]2(PF6)2. The study of the redox properties of these catalyst precursors containing variously substituted L (bipyridine) ligands, allowed the formation of polymer bonds of Ru-Ru by electroreduction to be demonstrated. The ligand with a pyrrole functional group allows for the prior formation of a polypyrrole film, conferring improved catalyst stability and enhancing the catalytic performance. Different ways of immobilizing the complex on porous carbon have been used to obtain modified GDE. This study provided insight into the interaction between the molecular catalyst and the catalyst carrier during the CO2 reduction. We have demonstrated that the electrocatalytic activity of the catalyst deposited on the GDE is maintained in an aqueous medium.Alongside this fundamental work, a laboratory pilot was developed to perform the electrocatalytic reduction of CO2 in the gas phase, in order to overcome limitations encountered in an aqueous medium, such as CO2 solubility and reaction products separation. This under development study has not only identified obstacles, including the nature of the ion exchange membrane, but has also identified the nature and proportion of the polymer electrolyte used in the formulation of the catalyst layer. This work has provided fundamental knowledge and concrete answers which probably allow one day that such a process as CO2 valorization may be viable on an industrial scale
Ruiz, Valencia Azariel. "A new microbiological way for CO2 reduction : from discovery to development." Thesis, Montpellier, Ecole nationale supérieure de chimie, 2019. http://www.theses.fr/2019ENCM0002.
Full textAt the European Institute of Membranes, a new microbiological process for CO2 reduction into formate was discovered. The first objective of this PhD work was to reproduce the CO2 reduction tests in reference conditions, with a new biocatalyst vial ordered to the same strain provider as for the prior trials at the Lab. However, these tests did not allow to reiterate the results obtained previously, i.e. formate production. A strain mutation was suspected and the strain that was stored during the preliminary tests was thus implemented. Nevertheless, new reproducibility problems were encountered. A biochemical analysis revealed finally that the strain assumed to catalyze the CO2 reduction was in consortium with other bacteria. In parallel, a reliable methodology based on CO2 labelling by 13C and NMR monitoring was developed at the Lab to follow 13CO2 assimilation. The different strains were isolated and tested separately regarding CO2 reduction. The NMR analysis demonstrated that the principal contamination, whose presence was unexpected, was the true biocatalyst of the 13CO2 reduction into 13C-formate.The 13C-formate was then quantified by a GC-MS method that was developed at the Lab. The effects of different reaction parameters on the reaction performances were thereafter investigated. These tests allowed notably to evidence an intracellular enzymatic system that could catalyze the CO2 reduction and to identify the possible electron donor. Indeed, addition of Poly-3-HydroxyButyrate (PHB) in the bacterial suspension enhanced significantly the formate production, suggesting that this energy storage polymer could be the electron source required for the CO2 reduction.Nevertheless, this intracellular PHB stock, formed during the bacteria culture step, is finite and can be exhausted during the reaction. This explains why the ability of the biocatalyst to recover electrons from a polarized cathode for CO2 reduction was assessed. Preliminary tests demonstrated the feasibility of this bio-electrochemical approach by the establishment of a CO2-dependant reduction current in a bio-electrolyzer. Current densities from 1.2 to 3.2 A·m-2 were obtained, which corresponds to volumetric flows of reduced CO2 ranging from 12 to 30 mL CO2·(g dry-cell)-1·d-1. Up to now, this new bioprocess was operated over 25 day. Regarding literature, this bioprocess is particularly interesting because (i) the volumetric flow of reduced CO2 is significant and (ii) no adding of cofactor, organic molecules, H2 or photons to the reaction medium is required
Innocent, Babette. "Etude des mécanismes réactionnels de l'électro-réduction du dioxyde de carbone sur le plomb en vue de sa transformation en des composés organiques." Poitiers, 2008. http://www.theses.fr/2008POIT2308.
Full textThe aim of this work was to promote the reduction of CO2 through its electrochemical conversion (electrosynthesis) on a lead electrode into high added value products. Depending on the nature of electrolyte, the electro-reduction of carbon dioxide leads to different products. Various electrolytes (aqueous or organic, protic or aprotic) were used to study two mechanisms: hydrogenation (formation of formate) and electrodimerization (synthesis of oxalate). Cyclic voltammetry studies have been carried out for electrochemically characterizing CO2 reduction on Pb. The electrochemical investigation of the electrode – electrolyte interface has shown that the process of CO2 electro-reduction is a mass transfer control both in the organic and aqueous media. Electrochemical experiments (cyclic voltammetry, chronoamperometry) coupled with in situ infrared reflectance spectroscopic techniques (SPAIRS, SNIFTIRS) have also shown that in aqueous medium (7
Davoust, Romain. "Trajectoires carbone en Europe à l'horizon 2050 sous une stabilisation mondiale à 450 ppmv CO2-équivalent : réductions, valeurs carbone et coûts d'abattement optimaux." Paris 9, 2011. http://basepub.dauphine.fr/xmlui/handle/123456789/7235.
Full textGlobal warming will be a major issue in the 21st century. Limiting temperature increase to +2⁰C above pre-industrial levels should help to preserve ecosystems. According to current estimates, this sustainable development objective requires a stabilisation of Greenhouse Gases (GHG) concentrations at 450 ppmv CO2-equivalent. Over the next decade, the world should reduce its GHG emissions by a factor 2 compared to 1990 levels. Europe has committed to reduce its Greenhouse Gases emissions by 20% in 2020 compared to 1990 and by 30% in case of a fair international agreement. In the long term, EU is targeting an abatement of at least 80% by 2050, which is a required level under the 450 ppmv CO2-equivalent constraint. The thesis models carbon effort in Europe to reach -80% GHG by 2050. Over the projection, the OCTET model (Optimal Carbon Trajectories for Emission Targets) projects a set of temporally optimal CO2 pathways. Efficient reduction strategies are built for the next decades (2020, 2030, 2040) depending on international uncertainty. The thesis calculates carbon price profiles in Europe under a factor 5 reduction as well as reduction costs. In a word, this thesis seeks to explore the implications of a low-carbon European society and to advise the European abatement policy over the 2050 horizon
Duong, Hong Phong. "Highly selective electrocatalysts for carbon monoxide conversion to multi-carbon products." Electronic Thesis or Diss., Sorbonne université, 2023. http://www.theses.fr/2023SORUS467.
Full textCarbon dioxide (CO2) valorization by electrolysis has shown its potential as an environmentally friendly and efficient method to synthesize value-added products like hydrocarbons and alcohols. However, the detrimental issue associated with carbonation in alkaline electrolyte limited the possibility to scale up CO2 electrolysis. Lately, a two-step concept, in which CO2 was firstly reduced into carbon monoxide (CO) with an industrially relevant Faradaic efficiency (FE) of 90% by a solid oxide electrochemical cell, then CO would be subsequently electrochemically reduced into ethylene with a high FE of 60% has been realized. As a result, there has recently been great attention focused on finding selective heterogeneous electrocatalysts to reduce CO into essential multi-carbon products. In this thesis, several copper-based electrocatalysts exhibiting high activity for CO conversion into ethylene, n-propanol and ethanol will be presented. The first chapter focuses on an original dendritic copper catalyst showing excellent selectivity for ethylene production from CO electrochemical reduction. The system exhibited the record FE for ethylene of 78% at an applied current density of 100 mA cm-2 with a record half-cell energy efficiency of 40.5%. In the second chapter, our attempt was focused on developing a nitride-derived silver- doped copper (CuAgN) electrocatalyst showing a high selectivity for CO electroreduction to n-propanol at the optimized condition (FE = 45%, an applied current density of 150 mA cm-2). In comparison with the bare copper nanoparticles, copper nitride and silver-doped copper nanoparticles, the CuAgN material possessed much higher electrochemically active surface area and CO conversion selectivity for n-propanol. Interestingly, the selectivity for C2+ liquid products of CuAgN was largely dependent on the concentration of KOH electrolyte. By employing in-situ characterization and computational modelling, a mechanism for n-propanol production was proposed as the presence of Ag could promote C1-C2 coupling reactions on the CuAg catalyst surface. Finally, according to the literature, C1-C2 coupling reactions were proposed as the key of C3+ products formation, thus the presence of a C2 substrate like acetaldehyde was presumed to boost C3+ products formation. The third chapter demonstrates the effect of an ab initio addition of acetaldehyde as a C2 substrate to CO electrolysis on the selectivity of the CuAgN, D-Cu catalysts, and commercial copper or silver nanoparticles
Le, Cong Tanh. "Etude expérimentale et modélisation de la cinétique de combustion de combustibles gazeux : méthane, gaz naturel et mélanges contenant de l’hydrogène, du monoxyde de carbone, du dioxyde de carbone et de l’eau." Orléans, 2007. http://www.theses.fr/2007ORLE2034.
Full textGuidal, Valentin. "Conception et réactivité de nouveaux complexes de lanthanides et de cobalt contenant des ligands rédox-actifs : application aux réductions multi-électroniques." Thesis, Grenoble, 2014. http://www.theses.fr/2014GRENV022/document.
Full textThe redox chemistry of lanthanide complexes is attracting increasing interest because of the potential of divalent lanthanide complexes to promote unusual redox chemistry. For example they are able to activate small molecules such as CO2 and N2 in mild conditions. Due to the unique coordination and bonding properties of the lanthanide ions, their compounds could provide an attractive alternative to transition metals for the catalytic transformation of small molecules. However, metal-based multi-electron processes remain uncommon in lanthanide chemistry especially in comparison with the d-block metals; the chemistry of low-valent lanthanides being dominated by single-electron transfers. In this context, the first aim of this project was to investigate the association of lanthanides with a redox-active ligand acting as an independent electron reservoir within the same molecule. Accordingly, we examined the use of highly π-delocalized Schiff base ligands to study the reductive chemistry of lanthanide ions. This led to the isolation of electron-rich complexes which are stabilized by storing two or four electrons on the ligands through the formation of C-C bonds. Interestingly, these C-C bonds can be cleaved by oxidizing agents and the electrons released can participate in multi-electron redox reactions. This process was observed within different tridentate and tetradentate Schiff-base ligand scaffolds, allowing a tuning of the properties of the compounds. The ability of these complexes to react with CO2 has been studied, which lead to the identification of some neodymium complexes capable of reducing CO2. The second part of this work was dedicated to the study of cobalt complexes bearing redox-active and highly π-delocalized Schiff base ligands able to store electrons through the formation of C-C bonds. Seminal studies on Schiff base complexes of cobalt had been carried out in the 1990's and they demonstrated the ability of these complexes to activate CO2. With the aim to identify the active species responsible for CO2 activation, we have revisited these systems and highlighted a redox-isomeric equilibrium between a Co(I) and a Co(II) complexes where the electron can be localized on the cobalt or on the ligand. We also investigated the parameters influencing this equilibrium. In particular we have investigated the effect of the ligand architecture on the redox reactivity of cobalt complexes. Such studies pave the way to the development of new complexes for the electrocatlytic reduction of CO2
Raux, Charles-Gabriel. "Quel coût pour le secteur électrique d'une politique de restriction des émissions de carbone en France ?" Paris 2, 2010. http://www.theses.fr/2010PA020032.
Full textPerazio, Alessandro. "Electrolyzer and Catalyst Engineering for Acidic CO2 Reduction." Electronic Thesis or Diss., Sorbonne université, 2023. http://www.theses.fr/2023SORUS438.
Full textThe project focuses on the electrochemical reduction of CO2 with heterogeneous catalysts. Thanks to the "gas-fed flow cell" configuration developed in the group, high current densities can be achieved at moderate overpotentials. The first part of the project is more focused on the overall efficiency of the electrolyzer. To optimize it, we work to find the best acidic electrolyte for the system and, in parallel, we try to increase the fraction of CO2 that is converted into the desired products. The second part of the project focused on optimizing the reactor voltage, aiming to minimize the energy consumption of the reduction process. Finally, the last part was devoted to the surface modification of the catalyst in order to obtain better selectivity for the most valuable carbon products
Tu, Thi Hoai Thu. "Potentiel de réduction des émissions de GES du transport routier de fret." Thesis, Paris Est, 2019. http://www.theses.fr/2019PESC2026/document.
Full textThe purpose of this thesis is to identify policies that would allow to mitigate road freight GHG emissions at the lowest cost for the community. With this in mind, for six scenarios corresponding to different mitigation policies we estimate the mitigated emissions along with the economic cost, over the 2030-2050 period. The overall economic cost includes the cost for transport users, for public authorities, and an economic valuation of transport externalities. When available, we used sets of assumptions retained by the French Ministry of Transports for official traffic projections and for the unitary valuation of external costs. For every scenario, the economic cost by avoided ton of CO2 is highly sensitive to these assumptions, especially to the unitary value of external costs (valuation of co-benefits). In the central set of assumptions, several scenarios result in a negative economic cost of GHG mitigation, id est a benefit to the community in addition to GHG cuts.This is notably the case for the carbon tax, as long as it remains lower than the external costs of freight road transportation. However, when the tax rate is rising, the resulting increase in transport prices leads shippers to reduce their activity, which limits the desirable tax rate increase. Increasing the maximum authorized weight of heavy trucks from 40 to 60 tons would be a very beneficial measure towards transport users by allowing a substantial transport costs reduction. This scenario is also beneficial for the community, when accounting for the avoided external costs, the financial loss for public authorities and infrastructure costs (the required reinforcement of roads and bridges and increased maintenance costs). The installation of catenaries on motorways to supply hybrid heavy trucks is efficient to reduce CO2 emissions, and the economic cost per avoided ton of CO2 remains moderate. Quite the opposite, the economic cost is high in the scenario of electrification of urban freight (where diesel trucks are replaced by electric trucks for urban goods delivery), if electric trucks only have a maximum payload of 2 tons. On the contrary, it turns into an economic benefit if, thanks to technological progress, electric trucks have a payload of 6 tons in 2030, for a range of 100 km.The replacement of diesel trucks by natural gas vehicles reduces transport costs and is therefore beneficial towards carriers and loaders, but public authorities support a loss of taxation revenues. However, when accounting for the avoided external costs, the overall economic cost happens to be limited.Finally, shippers can reduce GHG emissions for a reasonable economic cost by reducing the frequency of shipments, this measure also being beneficial for the community.However, none of these measures is capable to achieve by itself the official goal of dividing by 4 the level of GHG emissions at a reasonable cost for the community, implying that additional measures have to be considered jointly
Adam, Florence. "Étude de la fissuration lors de la réduction de l'hématite en magnétite à basse température." Nancy 1, 1988. http://www.theses.fr/1988NAN10059.
Full textSergent, Nicolas. "Dioxyde d'étain : Synthèse, Caractérisation et Etude des Interactions avec Différents Gaz Polluants - Application à la Catalyse DeNOx." Phd thesis, Université Jean Monnet - Saint-Etienne, 2003. http://tel.archives-ouvertes.fr/tel-00002302.
Full textTrillat, Jean-Frédéric. "Réduction de NO par CO sur catalyseurs bimétalliques Pd-Mn : application à la conversion de mélanges complexes en post-combustion automobile (moteurs à essence)." Lyon 1, 1997. http://www.theses.fr/1997LYO10029.
Full textYu, Xiang. "Photocatalytic conversion of methane and reduction of CO2 with H2O." Thesis, Lille 1, 2019. http://www.theses.fr/2019LIL1R022/document.
Full textPhotocatalysis is one of the key technologies for clean energy and environmental applications. The number of applications based on photocatalysis has increased dramatically for the past two decades. Photocatalytic activation of C-H bonds is an emerging field. Methane is a promising source of energy with a huge reserve and is considered to be one of the alternatives to non-renewable petroleum resources because it can be converted to valuable hydrocarbon feedstocks and hydrogen through appropriate reactions. However, due to its high stability, high energy is usually consumed for its conversion, which remains a problem to be solved. Methane conversion and reaction mechanism occurring on metal-heteropolyacid-titania nanocomposites were investigated in Chapters 3 and 4. Oxidation of methane has been carried out for more than a century. Since oxygen is a very reactive molecule, methane can react very rapidly with molecular oxygen and is prone to total oxidation till CO2. Therefore, it is difficult to obtain a desired product with high yield and high selectivity. We report here direct and selective photocatalytic highly-selective oxidation of methane to carbon monoxide under ambient conditions. The composite catalysts on the basis of zinc, tungstophosphoric acid and titania exhibit exceptional performance in this reaction, high carbon monoxide selectivity and quantum efficiency of 7.1% at 362 nm. The reaction is consistent with the Mars-Van Krevelen type sequence and involves formation of the surface methoxy-carbonates as intermediates and zinc oxidation-reduction cycling. In the past few decades, extensive research has focused on the direct conversion of methane to alcohols or higher hydrocarbons. The current processes of converting methane to alcohols or olefins are complex and expensive, because they require an intermediate step of reforming methane to syngas. Although the direct conversion of methane to more valuable products has significant environmental and potential commercial value, there is no commercial scale process available. We uncovered highly selective (>90%) quantitative photochemical direct conversion of methane to ethane at ambient temperature over silver-heteropolyacid-titania nanocomposites. The ethane yield from methane reaches 9 % on the optimized materials. High quantum efficiency, high selectivity and significant yield of ethane combined with excellent stability are major advantages of methane quantitative synthesis from methane using the photochemical looping approach. The rise in atmospheric carbon dioxide and the depletion of fossil fuel reserves have raised serious concerns about the subsequent impact of CO2 on the global climate and future energy supply. The use of abundant solar energy to convert carbon dioxide into fuel, such as carbon monoxide, methane or methanol, solves both problems simultaneously and provides a convenient method of energy storage. Chapter 5 addresses a new efficient catalyst for selective CO2 to CO conversion. The zinc containing phosphotungstic acid-titania nanocomposites exhibited exceptional high activity reaching 50 µmol CO/g·h and selectivity (73%) in the CO2 photocatalytic reduction to CO in the presence of water. The in-situ IR experiments suggest that reaction involves zinc bicarbonates containing hydroxyl groups. The decomposition of these zinc bicarbonate species under irradiation leads to the selective production of carbon monoxide and oxygen. In photocatalytic reactions, the difference in catalyst morphology usually has a significant effect on the photocatalytic performance. Chapter 6 studied the effect of monoclinic bismuth vanadate (BiVO4) crystals with controlled ratio of {010} and {110} facets for photocatalytic reduction of CO2 by H2O. The reaction under irradiation is significantly enhanced by selective photo-deposition of Cu and Co co-catalysts over different facets providing Z-scheme charge flow
Baccour, Mohamed. "Monolithes à porosité multi-échelle comme supports pour la réduction enzymatique du CO2 en molécules d'intérêts." Thesis, Montpellier, Ecole nationale supérieure de chimie, 2018. http://www.theses.fr/2018ENCM0004.
Full textCarbon dioxide (CO2) is a greenhouse gas that results, in part, from human activities and causes global warming and climate change. According to the International Energy Agency, global CO2 emissions from fossil-fuel combustion reached a record high of 31.3 gigatonnes in 2011. The concept of the methanol economy, advocated by Nobel laureate Prof. George A. Olah back in the 1990s, hinges on the chemical recycling of CO2 to methanol and derived, suggesting methanol as a key substitute fuel and starting material for valuable chemicals. The recycling conversion of CO2 could be a rational way to develop an anthropogenic short-term carbon cycle. With this aim, The design of functional porous architectures depicting hierarchical and interconnected pore networks has emerged as a challenging field of research. Particularly, porous monoliths offer many advantages and can be employed as flow-through reactors for separation, catalysis and biocatalysis. This study focuses on the design of monoliths with hierarchical porosity and high surface area. Firstly, silica monoliths with both homogeneous macro- and mesopores were prepared using sol-gel chemistry and spinodal decomposition using PEO polymers. Macropore (up to 30 microns) and mesopore (up to 20 nm) diameters of the monoliths were controlled by modifying various experimental parameters (PEO molecular weight, addition of surfactants, different basic post-treatments, different temperatures, etc.). Secondly, carbonaceous replica have been prepared through hydrothermal carbonization of sucrose, subsequent pyrolysis and silica etching. These materials present large interconnected flow-trough macropores, a bimodal mesoporosity, a high surface area (up to 1400 m2 g-1) and high meso- and macropore volumes.Different enzymes were immobilized onto the monoliths amongst which formate dehydrogenases. Flow-through reactors were engineered and continuous flow biocatalysis was performed. In such systems, straightforward processes for the in situ regeneration of the enzyme cofactor, i.e. 1,4-NADH wrer developped. Flow-through reactors and their use for the enzymatic reduction of carbon dioxide into formate were designed
Yu, Xiang. "Photocatalytic conversion of methane and reduction of CO2 with H2O." Electronic Thesis or Diss., Université de Lille (2018-2021), 2019. http://www.theses.fr/2019LILUR022.
Full textPhotocatalysis is one of the key technologies for clean energy and environmental applications. The number of applications based on photocatalysis has increased dramatically for the past two decades. Photocatalytic activation of C-H bonds is an emerging field. Methane is a promising source of energy with a huge reserve and is considered to be one of the alternatives to non-renewable petroleum resources because it can be converted to valuable hydrocarbon feedstocks and hydrogen through appropriate reactions. However, due to its high stability, high energy is usually consumed for its conversion, which remains a problem to be solved. Methane conversion and reaction mechanism occurring on metal-heteropolyacid-titania nanocomposites were investigated in Chapters 3 and 4. Oxidation of methane has been carried out for more than a century. Since oxygen is a very reactive molecule, methane can react very rapidly with molecular oxygen and is prone to total oxidation till CO2. Therefore, it is difficult to obtain a desired product with high yield and high selectivity. We report here direct and selective photocatalytic highly-selective oxidation of methane to carbon monoxide under ambient conditions. The composite catalysts on the basis of zinc, tungstophosphoric acid and titania exhibit exceptional performance in this reaction, high carbon monoxide selectivity and quantum efficiency of 7.1% at 362 nm. The reaction is consistent with the Mars-Van Krevelen type sequence and involves formation of the surface methoxy-carbonates as intermediates and zinc oxidation-reduction cycling. In the past few decades, extensive research has focused on the direct conversion of methane to alcohols or higher hydrocarbons. The current processes of converting methane to alcohols or olefins are complex and expensive, because they require an intermediate step of reforming methane to syngas. Although the direct conversion of methane to more valuable products has significant environmental and potential commercial value, there is no commercial scale process available. We uncovered highly selective (>90%) quantitative photochemical direct conversion of methane to ethane at ambient temperature over silver-heteropolyacid-titania nanocomposites. The ethane yield from methane reaches 9 % on the optimized materials. High quantum efficiency, high selectivity and significant yield of ethane combined with excellent stability are major advantages of methane quantitative synthesis from methane using the photochemical looping approach. The rise in atmospheric carbon dioxide and the depletion of fossil fuel reserves have raised serious concerns about the subsequent impact of CO2 on the global climate and future energy supply. The use of abundant solar energy to convert carbon dioxide into fuel, such as carbon monoxide, methane or methanol, solves both problems simultaneously and provides a convenient method of energy storage. Chapter 5 addresses a new efficient catalyst for selective CO2 to CO conversion. The zinc containing phosphotungstic acid-titania nanocomposites exhibited exceptional high activity reaching 50 µmol CO/g·h and selectivity (73%) in the CO2 photocatalytic reduction to CO in the presence of water. The in-situ IR experiments suggest that reaction involves zinc bicarbonates containing hydroxyl groups. The decomposition of these zinc bicarbonate species under irradiation leads to the selective production of carbon monoxide and oxygen. In photocatalytic reactions, the difference in catalyst morphology usually has a significant effect on the photocatalytic performance. Chapter 6 studied the effect of monoclinic bismuth vanadate (BiVO4) crystals with controlled ratio of {010} and {110} facets for photocatalytic reduction of CO2 by H2O. The reaction under irradiation is significantly enhanced by selective photo-deposition of Cu and Co co-catalysts over different facets providing Z-scheme charge flow
Fogeron, Thibault. "Synthèse de complexes inspirés des formiate déshydrogénases à Mo/W : application à la catalyse moléculaire de la réduction du CO2." Thesis, Sorbonne université, 2018. http://www.theses.fr/2018SORUS132.
Full textIn the context of global warming, the development of new sources of energy, clean and sustainable, is a key challenge of our society. The reduction of CO2 could allow the storage of renewable energies and offer an answer to the dramatic increase of CO2 in the atmosphere. Development of molecular catalysts offers the possibility of studying the structure-reactivity relationships. However, the library of existing homogeneous catalysts in the literature is quite limited. In order to find new potential catalysts, we decided to take inspiration from the active site of formate dehydrogenases (FDH). The synthesis of molecules mimicking this active site is an interesting challenge. In this thesis, we described the synthesis of two ligands inspired from the molybdopterin (chapter I). The synthesis of CoCp(dithiolène) complexes allows us to better characterize these ligands (chapter II). Moreover, the observation of the reactivity of these ligands allows us to understand their behaviour during electrocatalysis. The [MoO(dithiolene)2]2- complexes obtained from the bio-inspired ligands are,so far, the best mimics of the active site of FDH in the literature (chapter III). In this chapter, the generalization of synthetic procedure was also explored. Finally, [Ni(dithiolene)2]- synthesize from the bio-inspired ligands are the first dithiolene complexes able to reduce CO2 (chapter IV). They are among the few non-nobles metal complexes catalyzing the reduction of CO2 into formate
Blondiaux, Enguerrand. "Recyclage du CO2 : Une alternative à la pétrochimie pour la synthèse de molécules azotées." Thesis, Paris 11, 2015. http://www.theses.fr/2015PA112151/document.
Full textThe fossil carbon resources (oil, coal, gas) cover 85% of world energy portfolio and serve as raw materials for 95% of organic chemicals consumables (plastics, fertilizers, pesticides...). The decrease of oil resources and the accumulation of CO2 arising from their use thus pose environmental, energetic and availability of raw materials problems for the chemical industry. In this context, it is appropriate to propose new methods of chemical synthesis to build a sustainable industry based on the use of renewable carbon resources. Bypassing petrochemicals and valorize its carbon waste, CO2, to build molecular structures without energy purposes (polymers, fertilizers, synthetic textiles ...) represents a leading scientific challenge. From this perspective, new nitrogen molecules synthetic processes have been developed from CO2 as a carbon source, amines as nitrogen source and mild reductant such as hydrosilanes and hydroboranes as a hydrogen source. These processes are accelerated by the use of metal-free catalysts and enable the production of formamides, formamidines, aminals and methylamines, which are basic molecules of the chemical industry
Photinodellis, Roxane. "Politique climatique dans le secteur agricole : efficacité, coûts de surveillance, séquestration du carbone et risque." Electronic Thesis or Diss., université Paris-Saclay, 2024. http://www.theses.fr/2024UPASB011.
Full textThe aim of this thesis is to explore the trade-off between the effectiveness of net GHG mitigation policies and the costs associated with monitoring emissions and carbon sequestration. In the first contribution, our objective is to estimate the marginal cost andeffectiveness in terms of mitigating net GHG emissions for several policies partially covering emission sources and sinks. We find that subsidies for total carbon sequestrationand for carbon contained only in above-ground biomass are more cost-effective than aGHG tax. In the second contribution, at the scale of the plot, we examine the costs of participation in two types of carbon contracts, one model-based and the other results-based. For the latter type, we take into account the risk aversion of farmers regarding the uncertainty surrounding carbon sequestration results. The goal is to highlight the trade-offs regarding risk-sharing between the regulator and farmers, while defining theoretical conditions for farmer participation in these contracts. In the third contribution, at the scale of a French region, we compare the cost-effectiveness of different carbon contracts, whether results-based, model-based, or practice-based. This analysis takes into account some of the heterogeneity among farmers. Our results indicate that the most cost-effective contract form is to remunerate farmers per hectare for the implementation of intra-parcel agroforestry
Ané, David. "Stratégie d'exploitation et architecture de commande du système DEFONTAINE." Nantes, 2008. http://www.theses.fr/2008NANT2136.
Full textThis work, undertaken in collaboration with company DEFONTAINE SA, is within the framework of researches for innovating solutions for the reduction of CO2 car emissions. The studied system, that we will name DEFONTAINE system, was the subject of two other complementary theses, which concern the design of two electric machines : a linear actuator and a permanent magnet synchronous machine. Its goal is to fulfill the principal functions of a thermal engine flywheel, while avoiding its disadvantages. Indeed, if the flywheel reduces the acyclisms of the thermal engine at low speed, it becomes disadvantageous during the vehicle accelerations. Our work has consisted to model and to control the actuators of DEFONTAINE system, in order to supervise its operation. First of all, we characterized the acyclisms of a thermal engine in sight, in particular, to emulate them on test bench. Then, we considered the sensorless control of a traditional synchronous machine based on an improvement of the Matsui estimation method coupled to siliding mode observers. We have implemented a global approach of the identification and the corrector tuning of the various control loops. This approach was transposed to the synchronous machine with trapezoidal distribution of the DEFONTAINE system, within an extended vector control. Two test benches were built and we experimentally validated the control of the synchronous machine with sinusoidal distribution (motor and generator) and the extended vector control of the synchronous machine of DEFONTAINE system
El, Idrissi Nouaamane. "Novel nanocellulose-supported catalysts for carbon dioxide valorisation, ring-opening polymerisation and reduction reactions." Electronic Thesis or Diss., Université de Lille (2022-....), 2023. https://pepite-depot.univ-lille.fr/ToutIDP/EDSMRE/2023/2023ULILR068.pdf.
Full textThe use of functionalised nanocellulose as catalyst support has become topical in recent years, making it possible to reduce production costs and minimise the production of harmful toxic waste. This encourages the use of renewable resources by offering a greener alternative to traditional toxic catalysts while maintaining high catalytic performances. This thesis focuses on the conception of novel functionalized nanocellulose-based catalysts, which can be used in various chemical fields such as organic synthesis, CO2 conversion and ring-opening polymerization.In this study, a novel Co0/TEMPO-Cellulose biohybrid aerogel was prepared by a simple and green method. The structure of Co0/TEMPO-Cellulose aerogels was studied by TEM, SEM/EDX, FT-IR, DRX and XPS. These analyses show the formation of metallic cobalt (Co0) nanoparticles, indicate their immobilisation on the catalytic support and confirm their nanometric size (d < 4 nm). The catalytic activity of the aerogel was significantly higher than that of unsupported cobalt particles for the reduction of nitroarenes, due to the good dispersion of the Co0 nanoparticles on the catalytic support. The recyclability of the aerogel was studied, the catalyst retaining good catalytic activity even after 11 cycles without any significant loss of efficiency.In the continuation of our research on the conception of innovative and recyclable catalysts, 1,5,7-Triazabicyclo[4.4.0]dec-5-ene (TBD) is chemically immobilized on the surface of cellulose nanocrystals (CNC) to form a novel heterogeneous nanocatalyst (TBD-CNC) for the production of cyclic carbonates by the cycloaddition of CO2 to epoxides without the use of metals or halogens. The prepared catalysts were characterized by solid-state 13C NMR, FT-IR, XRD and elemental analysis to confirm TBD grafting onto CNC surface. TBD-CNC exhibited higher catalytic performance compared to the homogeneous mTBD catalyst possibly due to hydrogen bond co-activation. Under optimized reaction conditions, TBD-CNC efficiently converted the investigated mono-substituted and di-substituted epoxides, selectively producing the corresponding cyclic carbonates in high yields. Moreover, it is easily recovered by centrifugation and can be reused at least five times without losing its catalytic efficiency.TBD-CNC was also evaluated in the ring-opening polymerization of trimethylene carbonate (TMC), offering a promising alternative to traditional metal catalysts. The reaction was carried out in the presence of benzyl alcohol (BnOH) as co-initiator and TBD-CNC as organocatalyst. The prepared catalyst showed good catalytic performance for this polymerization, producing poly(trimethylene carbonate) (PTMC) with a high molar mass (Mn = 19 100 g.mol-1) and good dispersion (DM = 1.4).Copolymerization of CO2 with oxetane is a promising approach for the direct production of PTMC, the combination of iodine and TBD-CNC as a binary catalyst system proved successful for the synthesis of PTMC oligomers from CO2, achieving satisfactory levels of carbonate linkage (73% selectivity).The results of this work could be extended beyond these reactions, as similar catalytic systems can be developed for a wide range of chemical reactions, thus addressing green chemistry concerns related to environmental impact, economic efficiency and sustainable development.Keywords: nanocellulose, cobalt nanoparticles, nitroarenes reduction, TBD, CO2 valorisation, ring-opening polymerisation, cyclic carbonate, polycarbonate, recyclability
Ma, Bing. "Catalyse moléculaire de la réduction photochimique du CO2 à l’aide de complexes de cobalt en conditions homogène et supportée." Thesis, Université de Paris (2019-....), 2020. http://www.theses.fr/2020UNIP7006.
Full textPhotocatalytic solar fuel production is an effective means of chemical storage for solar energy and it provides a potential fruitful option for achieving a zero-emissions energy system. The cornerstone of a practical solar fuel production process is to design and optimize stable, efficient, and scalable photocatalysts, including a semiconductor material that accommodates photon absorption, efficient charge carriers generation, transport, and then catalytic reactions. Molecular catalysis plays an essential role in both natural and artificial photosynthesis. In this doctoral work, I have (i) investigated a bimetallic complex for selective CO2 reduction, illustrating that molecular catalysis is one of the promising way to activate metal cooperativity with outstanding intrinsic activities; (ii) synthesized inorganic material (semiconductive carbon nitride and graphitic acid) able to be functionalized with a molecular molecule (cobalt quaterpyridine) through a covalent amide bond. Effective heterogenization of the two components was thoroughly accessed. These hybrid systems showed high catalytic performance towards CO2 photoreduction. They illustrate that the development of molecular catalysts is worth to be explored for the invention of scalable catalytic systems that are needed for large scale, practical solar fuel production. In the mechanism of material-supported molecule catalysts, challenges still remain regarding both to molecular stability, heterogenization techniques, and control of the electronic interaction between these components
Liu, Yunsong. "Characterizing methane (CH4) and carbon dioxide (CO2) emissions through mobile platforms from local to national scale." Electronic Thesis or Diss., université Paris-Saclay, 2022. http://www.theses.fr/2022UPASJ021.
Full textMethane and carbon dioxide are the most abundant human-induced greenhouse gases (GHG) in the atmosphere. Their increasing atmospheric concentration is the main driver of climate change. Therefore, it is critical to monitor the evolution of their sources and sinks. Accurate characterization and quantification of their territorial emissions from different sectors are required in order to determine and manage efficient mitigation actions and policies. The main goal of this Ph.D. is to improve the characterization of CH4 and CO2 sectoral emissions from local to national scale through the development of mobile observation strategies including platforms such as car, drone and aircraft.This study consists of three parts. The first part aims at verifying a national CH4 inventory with a replicable method. I focus on surveying and quantifying significant methane emitters that represent 28% of national (Cyprus) methane emissions. These are essentially landfills and cattle farm areas. The approach is based on car-based mobile measurements and Gaussian plume dispersion modelling. The calculated methane emissions from landfills and enteric fermentation of cattle were about 160% and 40% larger, respectively, than the bottom-up sectoral estimates used in the national inventory. These mobile surveys show that an ensemble of in situ measurements targeting representative methane emission hotspots with consistent temporal and spatial coverage can largely improve national bottom-up emission inventories.The second part focuses on methods to quantify CH4 emissions for the oil and gas industry. It compares ten state-of-the-art commercial methane quantification systems through a series of controlled release experiments at an inert compressor station. The controlled releases covered a range of situations including various leak rates and wind conditions. The results indicated that ‘source-level' systems (close to single leak) generally underestimate emissions, while ‘site-level' systems (integrating emissions for the site) relying on atmospheric dispersion slightly overestimate emission rates. The analysis of this part highlights that unmanned aerial vehicles (UAV) have the potential to bridge the gap between ground-based and airborne observations but are strongly wind sensitive.The last part focused on the development of UAV GHG measurements. I have developed and validated a novel portable UAV-CO2 sensor system that is lightweight but remains sufficiently precise. Through a careful sensor characterization, correction and calibration procedure, we reach an in-flight precision of ± 2 ppm (1σ) at 1 Hz and ± 1 ppm (1σ) at 1 min. This system is relatively inexpensive and easy to reproduce, and has the potential to perform a wide range of field applications, such as urban and point source emissions monitoring.In short, this Ph.D. makes a step forward for future reconciliation of GHG emission estimates based on various observation systems and different approaches, and seeks methods that are easily duplicated and applicable to other regions and emission sectors. While mobile approaches presented here clearly represent important monitoring options, significant challenges remain in current capacity to estimate routinely anthropogenic GHG emission trajectories with sufficient precision and at large scale
Younes, Mourad. "Capture du CO2 par anti-sublimation : conception, simulation et réalisation d'un prototype." Paris, ENMP, 2003. http://www.theses.fr/2003ENMP1192.
Full textMissions of CO2 are increasing, leading to temperature increase of Earth. This led to the Kyoto Protocol which aims at the elaboration of policies of limitation of the emissions of greenhouse gases among which CO2. A large number of options exist to limit CO2 emissions associated with energy production, one of them is developed in this dissertation, the CO2 capture from flue gases. Usual techniques of CO2 capture are briefly analyzed. The major part of this work concerns the development of a new CO2 capture based on the CO2 frosting at low temperature. The CO2 frosting is performed by a refrigerating system composed of an integrated cascade, which offers evaporating temperatures lower than the CO2 frosting temperature. Several architectures are analyzed in order to choose the most energy efficient one. A prototype mock-up has been designed and realized for the validation of the global concepts of the CO2 frosting and defrosting. The components have been sized using computerized tools developed for the modeling of multi-stage integrated cascades. The system includes two low-temperature evaporators operating alternatively in frosting and defrosting modes to permit continuous system operation. The "cold" energy from defrosting is recovered by the refrigerant blend, which permits to improve the energy efficiency of the system
Brohe, Arnaud. "Réalisations et limites des marchés du carbone: évaluation et perspectives." Doctoral thesis, Universite Libre de Bruxelles, 2014. http://hdl.handle.net/2013/ULB-DIPOT:oai:dipot.ulb.ac.be:2013/209301.
Full textUne hypothèse forte des marchés du carbone dotés d’un système de plafonnement est qu’ils permettraient de garantir le respect des objectifs climatiques. Cette hypothèse ne s’est pas révélée exacte. En générant plus d’un milliard de crédits, dont un nombre important de crédits issus de projets, et en ne parvenant pas à empêcher des défections, le système mis en place par le Protocole de Kyoto n’est pas parvenu à garantir le plafonnement des émissions dans les pays développés. Il en va de même pour les systèmes liés à Kyoto comme le système communautaire d'échange de quotas d'émissions (SCEQE).
Dans la plupart des configurations des règles ad hoc et peu transparentes ont nui à l’objectif environnemental. La comptabilité commune de différents gaz à effet de serre, malgré des incertitudes importantes sur les pouvoirs de réchauffement globaux a également été néfaste à l'intégrité du système.
Le lien à des mécanismes de projets trouvant leur légitimité dans une preuve de l’additionnalité souvent floue demeure problématique. Notre analyse a ainsi mis en avant la problématique de l'enregistrement de projets hydrauliques dont la décision de construction est antérieure aux marchés du carbone.
En théorie, le mécanisme d’échange a pour conséquence que les acteurs confrontés à des coûts de réduction faibles soient encouragés à réduire leurs émissions. Dans la pratique, notre analyse montre que peu d’acteurs connaissent leur coût de réduction marginal, empêchant dès lors la concrétisation de cet idéal d’une réduction au moindre coût. Nous avons aussi mis en avant le fait qu’un prix identique par tonne de CO2 réduite n’est pas adapté au soutien de technologies nouvelles, souvent plus onéreuses au début de leur cycle de développement.
Finalement, un des principaux mérites des marchés du carbone a peut-être été leur acceptabilité auprès des décideurs politiques et économiques. Il est manifeste que les marchés permettent d'internaliser le carbone à un niveau international sans passer par une difficile harmonisation des politiques fiscales. C'est clairement une des raisons de leur adoption rapide et dans de nombreux pays.
Les marchés du carbone ont aussi joué un rôle important en matière de sensibilisation aux changements climatiques. Ils ont permis de faire progresser la comptabilité carbone et la compréhension des technologies sobres en carbone.
L’effondrement récent du prix du carbone montre que ce nouvel instrument qui, en théorie, est efficace pour atteindre un objectif de réduction prédéfini, ne permet pas, dans la pratique, par manque d’ambition ou en raison d’erreurs dans la conception, de financer la transition vers une nouvelle économie sobre en carbone. Il apparaît dès lors nécessaire de réformer cet instrument mais aussi de développer progressivement des alternatives afin de ne pas uniquement faire reposer la réussite de l’atteinte des objectifs climatiques sur les seuls marchés du carbone et ainsi augmenter la résilience des politiques climatiques aux aléas de marchés financiers, par ailleurs eux-mêmes soumis à de nombreux tourments depuis 2008.
Doctorat en Sciences
info:eu-repo/semantics/nonPublished
Toro, Molina Carol. "Comparaison du captage du CO2 en postcombustion par des solutions d'ammoniaque et d'amines organiques : Évaluation en contacteurs direct et indirect, par des approches cinétiques, thermodynamiques et par modélisation." Phd thesis, Ecole Nationale Supérieure des Mines de Paris, 2013. http://pastel.archives-ouvertes.fr/pastel-00935386.
Full textBazzi, Sakna. "Electrogenerated divalent samarium for CO₂ activation : applications in carboxylic acid synthesis." Thesis, Université Paris-Saclay (ComUE), 2019. http://www.theses.fr/2019SACLS397.
Full textCO₂ activation is considered one of the most attractive tools to convert this cheap, abundant and non-toxic gas into valuable chemical feedstocks such as carboxylic acids. The market value of these compounds is expecting a significant increase in the next few years, thus the urgent need for sustainable and eco-friendly production pathways. Divalent samarium complexes are known for their strong monoelectronic reductive power that made them the perfect choice for the reduction of some challenging functional groups. Indeed, in the literature, this reagent has been used in combination with CO₂ but only to achieve the reductive disproportionation of CO₂ while no example reported C-C bond formation via CO₂ activation using the Sm(II) complexes. Herein, we report the CO₂ activation initiated by electrogenerated divalent samarium. Taking advantage of our recently developed method for the in situ generation of Sm(II) species, the synthesis of benzoic acid derivatives was successfully achieved. Furthermore, electrocatalytic CO₂ activation conditions were established in this work and applied not only for the preparation of phenylacetic acids from benzyl chloride derivatives but also for the regioselective hydrocarboxylation of styrene and phenylacetylene analogs. This electrochemical Sm(II)-based protocol offers the next generation of sustainable system to transform CO₂ into highly valued molecules under mild conditions and without the addition of co-reductants
Nascimento, Lucelma Aparecida. "Stockage du carbone dans les sols et dynamique des paysages en Amazonie : l’exemple du Nord-Ouest de l’État de Mato Grosso – Brésil dans le cadre du REDD (Réduction des Émissions par Déforestation et Dégradation)." Thesis, Rennes 2, 2015. http://www.theses.fr/2015REN20028/document.
Full textThe land use changes altered the carbon storage potential in the soil. The deforestation and agricultural techniques have a significant impact on the global carbon cycle and contribute to greenhouse gases. The main objective of this thesis is to highlight the links between carbon storage, land use and the dynamics. For this study, we used satellite images over the period 1987 – 2011, to classify types of land occupations. In fact, not only to determine the amount of carbon in the soil, but also to check the connection between the amount of carbon and land management in different properties. Farms operate in the northwestern part of the state of Mato Grosso were chosen for their different operating modes: the Fazenda São Nicolau, in the Cotriguaçu community, where a reforestation policy was designed, the Fazenda Preciosa (representing the traditional agricultural model) and the Assentamento Vale do Amanhecer (recent deployment system based on the division of land among smallholders, with each having an operating strategy) in the of Juruena community. Therefore, detailed studies were developed through a regional soil mapping at scale 1: 100,000 in association with relief, hydrographic network, the geological substratum, climate changes, the vegetation and soils, and following the methodology and the techniques based on established organizational charts for these jobs. All this, in addition to mapping data about the physical partitions of these areas by remote sensing. Thus were carried out some analysis: the physical and chemical analysis, of the fluorescence spectrometry X-rays, the diffraction of X-rays, the geochemical environments - statistical analyzes as well as calculate the densities of the sampled soils in a geochemical context for Determination of the elements are associated with the carbon and organic matter. Studies on land use were also conducted. The Results show a range of carbon stock values between 0.01 and 8.89 kg / m2 distributed among diverse class of soil and selected for placement. Mappings of carbon stock classes allowed confront them with the land and the textural classes. The best correlations between carbon storage classes and certain types of high forest and carbon stock between the classes and the clayey textures were possible to find out that were found. Thus no way to land use seems to have a radical impact on carbon stocks; the cultural and historical practices of each farm better explain the results. This physicochemical approach primarily aimed at identifying the regions studied the soil types in their compositions that have higher levels of organic matter and nutrients where carbon storage is more assured. The results that were obtained in this research, lead us to propose a new model of studies to put into practice new ideas about REDD, as well as the organization's data of carbon storage in these different areas studied, which can be applied in other regions and objective interpretations that will of course be obtained in this body of work
Dunand-Sauthier, Marie-Noe͏̈lle. "Propriétés électrochimiques et photochimiques de complexes mono(2,2'-bipyridine) carbonyle de ruthénium (II) : applications à la réduction électrocatalytique du CO2 et à la photoimagerie." Grenoble 1, 1993. http://www.theses.fr/1993GRE10105.
Full textPigeon, Jonas. "Les technologies de Captage, Transport et Stockage du CO2 (CTSC) dans l'Axe-Seine : description des futurs possibles d un dispositif technique de réduction des émissions de gaz à effet de serre." Thesis, Le Havre, 2016. http://www.theses.fr/2016LEHA0013/document.
Full textCarbon Capture and Storage enables industrial facilities to capture their CO2 emissions in order to geologically store it and then reduce their impact on global warming. The Seine Waterway Axis (from Paris to Le Havre) counts a lot of industrial facilities emitting huge quantities of CO2. From 2006 local stakeholders of this territory are willing to develop CCS to a commercial scale in order to reduce CO2 emissions.In our research we aim to understand potential futures of CCS technology in the Seine Waterway Axis. In this Phd thesis we first analyse initial technoscientific promises related to Carbon Capture and Storage in using Science and Technology Studies theoretical framework. Then we focus on the Seine Waterway Axis territorial dynamics regarding sustainable development. Finnaly, we focus on narratives related to Carbon Capture and Storage in the Seine Waterway Axis in order to identify hybridations between CCS implementations and territorial dynamics. These cross analysis will enable us to describe potential future of CCS establishment in the Seine Waterway Axis
Décultot, Marie. "Intensification par pervaporation de la synthèse de carbonates organiques à partir d'alcools et de CO₂ Solubility of CO₂ in methanol, ethanol, 1,2-propanediol and glycerol from 283.15 K to 373.15 K and up to 6.0 MPa Organic carbonates synthesis improved by pervaporation for CO₂ utilisation." Thesis, Normandie, 2019. http://www.theses.fr/2019NORMIR08.
Full textCO₂ valorisation consists of using this greenhouse gas that is the most emitted into the atmosphere to produce molecules that are usually synthesized from oil. The combination of CO2 and alcohols produces organic carbonates with many applications. The equilibrium constants of the DEC (diethyl carbonate) and PC (propylene carbonate) synthesis reactions were experimentally evaluated for different operating conditions. A kinetic modelling was carried out based on mechanisms developed in the literature. The pervaporation of reaction mixtures models of DEC and PC allows effective dehydration that displaces the balance of the reaction. The experimental study of the reaction/pervaporation coupling made it possible to multiply by 8 the yields obtained without dehydration. According to the modelling, it is possible to significantly increase yields by improving reaction kinetics and pervaporation conditions
Aloisi, Alicia. "Synthèse de nouveaux ligands tripodes et de leurs complexes de coordination pour l’activation de petites molécules." Thesis, Université Paris-Saclay (ComUE), 2018. http://www.theses.fr/2018SACLS360/document.
Full textThe extensive use of fossile fuel is currently causing climate change. Anthropogenic emissions of CO₂ enhance the greenhouse effect, resulting in global warming. In order to mitigate this climate change, the share of renewable energy is increasing and hydrogen seems to be a good candidate to stock energy to compensate the seasonal variations of those energies. One way to store H₂ is the hydrogenation of CO₂ to synthesise liquid molecules as formic acid and methanol. Those liquids can be conveyed in an easier way. In case of a lack of energy, H₂ can be recovered through dehydrogenation of those molecules thinks to catalysts. In this thesis, we studied the synthesis of organometallic complexes able to activate those small molecules, thus, growing a fundamental knowledge. As a number of triphos-metal complexes are known to catalyse hydrogenation and dehydrogenation reactions, we focused on the elaboration of ligands alike. With those ligands in hand, several non-noble metal based complexes (Fe (II), Co (II) and Cu (I)) were synthesized, which are active in CO₂ hydroboration catalysis. A complex of ruthenium(II)was grafted on silica through one of this ligand, in order to recycle it when it used as a catalyst. On the second hand, we designed a new ligand which could favor metal-ligand cooperativity. H₂ was succesfully activated with a copper(I) complex coordinated by this ligand, demonstrating that cooperation of the ligand. Finally, the first known cobalt complex active in dehydrogenation of formic acid was synthesised
Réjasse, Florian. "Etude de la réactivité des dioxydes métalliques du groupe IVb en présence de carbone par une approche (micro)-structurale : Application à la modélisation des diagrammes de phases ternaires Me-C-O (où Me = Ti, Zr, Hf)." Thesis, Limoges, 2015. http://www.theses.fr/2015LIMO0099/document.
Full textDuring this work, the reactivity of group IVb dioxides (TiO2, ZrO2, HfO2) in contact with turbostractic carbon has been investigated in order to understand the reactional mechanisms of the carbothermal reduction. This way of synthesis has also allowed us to obtain oxycarbides phases in powder form to study the different stability domains of solids solutions with respect to the temperature of heat treatment. The addition of oxygen within the crystalline structure modifies the sintering behaviour of these materials and also their macroscopic properties. Consequently, the determination of solid solution boundaries requires an accurate methodology. A broad panoply of characterization techniques are coupled (Elemental analysis, XRD, Quantification of phases, TEM) to determine the compositions of oxycarbide phases. In order to complete this study, the reactivity of titanium carbide monoliths in contact with titanium dioxide has been studied during heat treatments of annealing under pressure in confined atmosphere. The identification of phases in equilibrium constitutes diagrammatic data which are necessary for the preliminary attempts of thermodynamic modeling of ternary phases diagrams Me-C-O (where Me = Ti, Zr, Hf) using the semi-empirical CALPHAD method
Zsoldos, Daniela. "Complexes mono et bis bipyridine carbonyle de ruthénium(II), précurseurs de polymères organométalliques : propriétés électrochimiques et applications à l'électrocatalyse de la réduction du CO2 en milieu aqueux." Université Joseph Fourier (Grenoble), 1997. http://www.theses.fr/1997GRE10027.
Full textCourtemanche, Marc-André. "Transition-metal-free reduction of carbon dioxide." Doctoral thesis, Université Laval, 2015. http://hdl.handle.net/20.500.11794/26219.
Full textSeulement neuf années se sont écoulées depuis la découverte que les ‘’Paires de Lewis Frustrées’’ (PLF) peuvent promouvoir le clivage de l’hydrogène, mais plus d’un millier d’articles scientifiques ont déjà été publiés sur le sujet. Au début des travaux décrits dans cette thèse, les catalyseurs pour la réduction du CO2 étaient excessivement rares et peu efficaces. La présente thèse porte donc sur le développement de nouveaux systèmes sans métal de transition pour la réduction catalytique du CO2 en molécules riches en énergie et plus précisément, en méthanol. D’abord, la préparation d’un nouveau système basé sur les PLF et sa capacité à activer le CO2 de façon réversible est présenté. En présence de catécholborane, le CO2 est catalytiquement réduit en méthoxyboranes, espèces facilement hydrolysables en méthanol. Surprenamment, un produit de décomposition est identifié comme étant responsable de l’activité catalytique. En effet, l’espèce ambiphile 1-Bcat-2-PPh2-C6H4 constitue le premier exemple d’un catalyseur sans métal de transition pour l’hydroboration du CO2. L’activité de ce catalyseur excessivement simple surpasse celle des meilleurs systèmes basés sur des métaux. Des études mécanistiques détaillées révèlent que l’activation simultanée du borane et du CO2 est d’une importance critique. Une investigation poussée révèle que la formation d’un adduit entre le catalyseur et le formaldéhyde résulte en un organocatalyseur d’autant plus actif. Il est aussi démontré que les phosphazènes, super bases organiques, sont des organocatalyseurs très actifs pour la transformation du CO2 en dérivés de formate ou de méthanol. De façon intéressante, le DMF (N, N-diméthylformamide) peut promouvoir l’hydrosilylation réductive du CO2 en absence de catalyseur. Une nouvelle stratégie d’hydrogénation a été développée en étudiant les aspects fondamentaux de l’hydrogénation par les PLFs, permettant ainsi la conception d’un système pour l’hydrogénation du CO2 en conditions ambiantes. Même si une voie de décomposition inattendue rend le processus stoéchiométrique, une optimisation du catalyseur pourrait générer le premier catalyseur sans métal pour l’hydrogénation du CO2.
Only nine years have passed since the seminal discovery that Frustrated Lewis Pairs (FLPs) could split dihydrogen and yet, more than a thousand research papers have already been published on the subject. As the work presented herein commenced, metal-free systems capable of catalytically transforming CO2 could be counted on a single hand while transition-metal based systems were almost as scarce. As such, the present thesis deals with the development of novel transition-metal-free systems for the catalytic reduction of CO2 to energy rich materials, most notably methanol. Firstly, the preparation of a new FLP system bearing three pendant phosphine groups Al(C6H4(o-PPh2))3 and its ability to activate carbon dioxide in a reversible fashion are presented. In the presence of catecholborane, CO2 is catalytically reduced to methoxyboranes, species which are readily hydrolyzed to methanol. Interestingly, a decomposition product is shown to be responsible for the catalytic activity Indeed, species 1-Bcat-2-PPh2-C6H4 is the first report of a catalyst for the metal-free hydroboration of carbon dioxide. The activity of this excessively simple catalyst surpasses that of the best transition metal systems while using the cheap and high hydrogen content borane BH3.SMe2. In-depth mechanistic studies reveals that simultaneous activation of both the borane and CO2 molecules is of critical importance. Further investigation reveals that the formation of an adduct between the catalyst and formaldehyde affords an even more potent organocatalyst. It is also shown that phosphazene superbases are very active organocatalysts for the transformation of CO2 to either formate or methanol derivatives. Unexpectedly, N, N-dimethylformamide (DMF) can promote the reductive hydrosilylation of CO2 in the absence of any catalyst. Finally, the challenging task of developing a metal-free system for the hydrogenation of CO2 was undertaken. A novel strategy was developed by studying the fundamental aspects of FLP mediated hydrogenations, allowing us to achieve CO2 reduction under ambient conditions. While an unexpected decomposition pathway hampered catalysis, optimisation of the catalyst design is expected to yield the first metal-free catalyst for the hydrogenation of CO2.
Favre, Nathalie. "Captage enzymatique du dioxyde de carbone." Phd thesis, Université Claude Bernard - Lyon I, 2011. http://tel.archives-ouvertes.fr/tel-00840947.
Full textKilaparthi, Sravan Kumar. "Carbon-based electrocatalysts for CO2 reduction, PET hydrolysate, and water splitting towards value-added products." Electronic Thesis or Diss., Université de Lille (2022-....), 2023. http://www.theses.fr/2023ULILN051.
Full textThis study tackles the major global challenges such as CO2 emissions, energy crisis and PET plastic waste mismanagement, which not only pollutes the environment but also contributes to CO2 emissions during incineration. The innovative approach presented in this thesis offers a dual solution, addressing both PET waste and CO2 emissions simultaneously.Two remarkable systems have been explored in this thesis. The first utilized Bismuth oxide carbonate (BOC) functionalized reduced graphene oxide (rGO) for cathodic CO2 electroreduction (CO2RR), while CuCoO on rGO was employed for anodic PET hydrolysate oxidation. Impressively, the anodic CuCoO@rGO catalyst displayed exceptional electro-activity, achieving an outstanding Faradaic efficiency (FE) of 85.7% at 1.5V vs. RHE. Simultaneously, the cathodic BOC@rGO catalyst demonstrated an impressive FE of 97.4% at -0.8 V vs. RHE, facilitating the production of formate from CO2RR. When integrated into an electrolyzer setup, this approach resulted in formic acid production at a low cell voltage of 1.9 V and a remarkable formate FE of 151.8% at 10 mA cm-2.Another system employed a 3D activated carbon felt (aCF) electrode as substrate and Bismuth has been deposited electrochemically on the CF (Bi@aCF) which acts as the cathode CO2RR and nickel cobalt phosphate-deposited carbon felt (NiCoPOx@CF) for the anodic PET hydrolysate oxidation process. This setup achieved a high FE of 94% during CO2RR at -0.8 V vs. RHE, producing formate, and a FE of 95% for anodic PET hydrolysate oxidation to formate at a low potential of 1.5 V vs. RHE. Remarkably, the two-electrode electrolyzer attained an extraordinary FE of 157% to produce formate at a cell voltage of 1.8 V. This breakthrough represents a novel pathway for upcycling PET waste, reducing CO2 emissions, and promoting environmental sustainability.Additionally, our experiments also delved into water electrolysis, where a novel strategy involving Ru embedded in a carbon nitride matrix was proposed. This approach, utilizing a covalent organic framework 2D CIN-1 structure with coordinated Ru+2, resulted in Ru oxide nanoparticles with low-valence Ru sites arranged in nanowires between layers of graphitic carbon nitride after pyrolysis. This material exhibited significantly lower overpotentials for both hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) compared to benchmark Pt and RuO2 catalysts, demonstrating remarkable catalytic stability. This discovery holds tremendous promise for advancing the field of water splitting and contributing to the development of sustainable energy solutions
Jankhah, Sepideh. "Reformage de l'éthanol au dioxyde de carbone." Mémoire, Université de Sherbrooke, 2007. http://savoirs.usherbrooke.ca/handle/11143/1386.
Full textAziz, Hermansyah. "Photochimie fine avec le dioxyde de carbone comme solvant." Vandoeuvre-les-Nancy, INPL, 1990. http://www.theses.fr/1990INPL056N.
Full textSimond, Mickaël. "Étude des interactions moléculaires dans les solvants d'intérêt pour le captage des gaz acides." Phd thesis, Université Blaise Pascal - Clermont-Ferrand II, 2013. http://tel.archives-ouvertes.fr/tel-01011515.
Full textVivin, Philippe. "Effets de l'augmentation atmosphérique en CO2 et de contraintes hydriques sur l'allocation de carbone et d'azote et sur l'ajustement osmotique chez Quercus robur L." Nancy 1, 1995. http://www.theses.fr/1995NAN10076.
Full textFadel, Mariam. "Designing a new electrochemical cell for the study of enzyme that reduces CO2." Thesis, Aix-Marseille, 2018. http://www.theses.fr/2018AIXM0491.
Full textCarbon monoxide dehydrogenase (CODH) catalyzes the reversible reduction of carbon dioxide by its active site. Thus, CODH participates in the first step of fuel production. Using an electrochemical method called protein film voltammetry, we study the enzymatic mechanism of CODH by immobilizing the enzyme at a graphite electrode surface where direct electron transfer is possible. Traditionally, to prevent depletion of the substrate at the electrode, electrochemists use rotating electrodes (RDE). However, since CODH is very active, even RDE cannot prevent depletion, which masks the important kinetic characteristics of the enzyme and complicates the analysis of the enzymatic response.We cannot solve the problem with RDE, since we already use it at maximum speed. Therefore, we must completely change our approach and design a new electrochemical cell. For this, we used computational fluid dynamics (CFD) simulations to explore various geometries to find a suitable one. We began by validating our numerical method with the well-defined theoretical solution of the real cell of RDE. After good validation, we determined the mass transport velocities within several proposed geometries of the flow cell of hydrodynamic channel and jet electrodes. Based on the optimization of geometric parameters, we have achieved our proper design of jet electrode. This new prototype has a uniformly accessible graphite electrode with a transport rate three times faster than the RDE at acceptable solution speeds. We have successfully built and implemented the system to characterize its transport performance. We found an excellent agreement between the numerical and experimental results
Mourier, Pierre. "La Chromatographie en phase supercritique avec le dioxyde de carbone." Grenoble 2 : ANRT, 1986. http://catalogue.bnf.fr/ark:/12148/cb37599852p.
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