Tesi sul tema "Carbon dioxyde (CO2)"
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Dębek, Radoslaw. "Novel catalysts for chemical CO2 utilization". Thesis, Paris 6, 2016. http://www.theses.fr/2016PA066215/document.
Testo completoThe growing emissions of carbon dioxide forced implementation of different CO2 emissions reduction strategies, which may be divided into two main groups: (i) carbon capture and storage (CCS) and (ii) carbon capture and utilization (CCU) technologies. The latter approach allows to recycle CO2. One of the processes that converts CO2 into added-value products is dry reforming of methane (DRM). The DRM process has not yet been commercialized due to the high endothermicity of the reaction and lack of cheap, active and stable catalysts.The materials which have beneficial properties in DRM reaction and may include desired catalysts components i.e. Ni, MgO and Al2O3 are hydrotalcites. The main goal of this PhD thesis was to evaluate catalytic performance of different hydrotalcite-based catalytic systems containing nickel in methane dry reforming process. This PhD was divided into three parts: (i) the comparison of the influence of nickel introduction into HTs-based catalytic system, (ii) the evaluation of wide range of nickel content in hydrotalcite brucite-like layers on materials catalytic properties and (iii) the evaluation of the effect of Ce and/or Zr promoters. In order to address these issues a number of different hydrotalcite-based catalysts was synthesized by co-precipitation. The physico-chemical properties of the prepared materials were evaluated by means of elemental analysis (XRF or ICP-MS), XRD, FTIR, low temperature N2 sorption, H2-TPR, CO2-TPD, TEM, SEM and TG experiments. The materials were subsequently tested in the DRM reaction. Most of catalytic tests were carried out at 550°C, but higher temperatures (650 and 750°C) were also studied
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.
Testo completoIn 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
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.
Testo completoAt 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
Bouziane, Abderlkader. "Simulation et étude expérimentale d’une machine frigorifique au CO2 transcritique munie d’un éjecteur". Thesis, Lyon, INSA, 2014. http://www.theses.fr/2014ISAL0014.
Testo completoCarbon dioxide is being advocated to reduce the environmental impact of the refrigeration systems. However, the thermodynamic properties of CO2 imply supercritical refrigerating cycle with low energy performance when the hot source temperature is near that of the environment. The expansion losses of an isenthalpic throttling process have been identified as one of the largest irreversibilities of transcritical refrigeration cycles, which contribute to the low efficiency of such cycles. In order to recover the expansion losses and increase the cycle efficiency, it has been proposed to replace the expansion valve with an ejector expansion device. This work is devoted to the numerical and experimental study of the ejector expansion devices used in a transcritical vapor compression system using carbon dioxide as the refrigerant. The numerical study includes a one-dimensional model of the CO2 two-phase ejector. The developed model is a good tool for predicting the operation conditions of the ejector and the overall characteristics of the flow (mass flow, velocity, enthalpy.. The model is a good tool to optimizing the geometry of the ejector, although it can be improved. The ejector was manufactured and incorporated into an instrumented test bench. Experimental study showed that the transcritical CO2 refrigeration system using an ejector as the expansion device outperformed a conventional expansion-valve transcritical CO2 system in COP and cooling capacity by approximately 17 % and 12,5 %, respectively. The experimental results were used to validate the one-dimensional model, a satisfactory agreement was found between the numerical and experimental results, especially in terms of mass flow with a difference of 9 %
Couchaux, Gabriel. "Relation structure-propriété pour la cinétique de la réaction amine-CO2 en solution [i.e.solutions] aqueuses". Thesis, Université de Lorraine, 2013. http://www.theses.fr/2013LORR0206/document.
Testo completoThe post-combustion process by amine scrubbing is currently the most mature to reduce carbon dioxide emissions from industry. However, if there are numerous demonstrators, the investment and operating cost of this process are still too important to develop it in a large scale. The kinetics of reaction between the amine and the carbon dioxide is one of the major factor which influence the costs. The objectives of this work are to study and understand the kinetics of the amine-CO2 reaction and to set up of a predictive structure-property model. This approach is adapted to the large number of possible amines which can be candidates for the process. In a first time we study five kinds of amines (primary, acyclic secondary, cyclic secondary, tertiary and multi-amines) representatives of candidate molecules. Among those molecules, two behaviours can be distinguished: one the one hand amines which form carbamates and on the other hand those which do not form carbamates. Measurements have been realised at 25 °C in diluted solutions by stopped-flow technique to characterize the intrinsic kinetics of each of the 87 studied amines using two kinetic constants. For each kind of amine, the main structural factors, electronic and geometric, which impact the kinetics of reaction have been identified. Then, from a statistical model using molecular descriptors to describe the different parameters of each amine, a structure-property relationship has been set up with the different kinetic constants. A descriptor of the steric hindrance has been developed
Poor, Kalhor Mahboubeh. "Étude DFT du mécanisme de formation du dimethyl carbonate à partir de CO2 et de CH3OH à l'aide de Me2Sn(OMe)2". Thesis, Lyon 1, 2009. http://www.theses.fr/2009LYO10325.
Testo completoCarbon dioxide occupies a special place in the amplification of the anthropogenic greenhouse effect. In particular, its use in the synthesis of organic carbonates from alcohols, constitute an alternative to the current application of phosgene or carbon monoxide. The insertion of CO2 into the Sn-OCH3 bond of dialkyldimethoxystannanes is recognized as the first step to dimethyl carbonate (DMC) formation from methanol and carbon dioxide. The identification of the subsequent steps is crucial for activity improvements and is still under debate as the tin species have the propensity for oligomerization. We have used density functional theory calculations to provide insight into the reaction mechanism. The CO2 insertion into the Sn-OCH3 bond is promoted by the concerted Lewis acid-base interaction of CO2 with tin and the oxygen atom of the methoxy ligand. The major reaction pathway to DMC is proposed to occur via an intramolecular rearrangement of the monomeric species, Me2Sn[OC(O)OCH3]2. The process results in the transfer of a methyl group from one methyl carbonate to the other via a 4-membered or 6-membered ring forming the Sn-CO3 moiety. In a second stage, methanol reacts with one intermediate and leads to DMC formation and a trimer compound which may allow the regeneration of the reactant. Also a decanuclear tin complex is produced due to the lateral reaction. Finally a catalytic cycle for DMC production in methanol can be elaborated. DFT calculations are in agreement with the experimental data and allow a comparative analysis of reaction channels
Ricaurte, Fernandez Marvin José. "Séparation du co2 d’un mélange co2-ch4 par cristallisation d’hydrates de gaz : influence d’additifs et effet des conditions opératoires". Thesis, Pau, 2012. http://www.theses.fr/2012PAUU3031/document.
Testo completoThe separation of CO2 from a gas mixture by crystallization of gas hydrates is a process that could eventually provide an attractive alternative to the conventional techniques used for CO2 capture. The aim of this thesis was to evaluate the potential of this "hydrate" process to separate CO2 from a CO2-CH4 gas mixture, rich in CO2. We have studied in particular the selectivity of the separation toward CO2 and the hydrate crystallization kinetics. The effects of thermodynamic and kinetic additives (and some additive combinations) on these two parameters for different operating conditions (pressure, temperature, concentrations) were evaluated. Hydrate formation and dissociation experiments were performed in "batch mode” in a high pressure reactor, and with an experimental pilot rig designed and built entirely during this thesis. A semi-empirical model was also developed to estimate the water to hydrate conversion and the composition of the different phases (hydrates, liquid and vapor) at equilibrium. The results show that the combination of sodium dodecyl sulfate (SDS) used as a kinetic promoter, with tetrahydrofuran (THF) used as a thermodynamic promoter, provides interesting results in terms of both the amount of hydrates formed and the hydrate formation kinetics. The selectivity of the separation toward CO2 remains too low (an average of four CO2 molecules trapped in the hydrate structure for one of CH4) to consider using this "hydrate" process on a larger scale to separate CO2 from such a gas mixture
Scondo, Alexandre. "La réaction phosphine imide en milieu CO2 supercritique". Thesis, Vandoeuvre-les-Nancy, INPL, 2008. http://www.theses.fr/2008INPL077N/document.
Testo completoIn the aim to propose a substitution process to the use of phosgene for the production of isocyanates and their derivatives, we devoted this work to the study of the phosphine imide reaction in supercritical CO2. In this context, we have chosen a standard reaction and investigated the influence of operational parameters on the kinetic of this reaction in CO2 using a high pressure 100 ml reactor. Analyses of the samples were performed using high performance liquid chromatography. These observations permits to develop a first order kinetic model, and we have compared the results obtained using this model with the observations we realized in a high pressure 1l reactor. We have compared the kinetics obtained in CO2 with those observed in dimethylformamide. We have also studied in dimethylformamide and CO2 the influence of the "catalyst" which permits to obtain isocyanates. We've finally performed the synthesis of a compound of pharmaceutical interest, which increase the bioavailability of Busulfan, in CO2 using phosphine imide reaction and we have followed the kinetic of this reaction
Qiu, Kehui. "Transfert de silicium et de carbone entre un gaz CO-SiO-CO2 et un alliage Fe-Si-C : étude de laboratoire". Châtenay-Malabry, Ecole centrale de Paris, 1993. http://www.theses.fr/1993ECAP0301.
Testo completoAllard, Vincent. "Effects of elevated atmospheric CO2 concentrations on carbon and nitrogen fluxes in a grazed pasture". Vandoeuvre-les-Nancy, INPL, 2003. http://docnum.univ-lorraine.fr/public/INPL_T_2003_ALLARD_V.pdf.
Testo completoJensen, Rojas Erik. "Effect of CO2 on carbon metabolism through the study of a low CO2-inducible protein and the production of storage compounds in diatoms". Thesis, Aix-Marseille, 2019. http://www.theses.fr/2019AIXM0286.
Testo completoDiatoms are photosynthetic microalgae found in most aquatic environments and, as all photosynthetic organisms, they use carbon from environmental CO2 as building brick for other more complex organic molecules. Diatoms have different mechanisms to adapt to varying environmental CO2 concentrations. Aquatic environments are generally low in CO2 and, to cope with this, diatoms use CO2-concentrating mechanisms (CCMs) to increase CO2 concentrations around the enzyme RuBisCO. In the first part of this thesis the role of a low CO2-inducible protein, LCIP63, found in the marine diatom Thalassiosira pseudonana was described. The results showed that LCIP63 is a new subclass of carbonic anhydrase (CA), that we called iota (ɩ), and is also a new component of the CCM of T. pseudonana. Additionally, LCIP63 is widespread among marine phytoplankton, including other diatom species. In the second part, structural characterization of LCIP63 was performed using different biophysical approaches. The shape of one oligomeric form of LCIP63 was determined, however no link between function and structure of LCIP63 was established. The third part deals with the adaptation of seawater and freshwater environments to high CO2 concentrations. The accumulation of the two main reserve compounds, lipids and chrysolaminarin, was studied in several diatom species acclimated to high CO2. Last, we studied the effect of LCIP63 overexpression on carbon partition in T. pseudonana. Finally, the results obtained in this thesis were globally discussed and new perspectives for future research are proposed
Dumas, Arnaud. "Apport des photodiodes à avalanche HgCdTe pour la télédétection du CO2 atmosphérique par lidar DIAL à 2 micromètres". Electronic Thesis or Diss., Université Paris-Saclay (ComUE), 2016. http://www.theses.fr/2016SACLX105.
Testo completoThe Short Wavelength Infrared (SWIR) region (1.5-2 μm) is well adapted for diffe- rential absorption lidar technique (DIAL) for several reasons : (i) it covers absorption bands with suitable intensity for the main greenhouse gases (CO2, CH4, H2O, etc.) (ii) the extinction due to particles is low (iii) it belongs to the eye safe domain. However, one main drawback has long been the lack of efficient photodetectors for such frequencies. A major enhancement occurred in the early 2000s when it was understood that HgCdTe avalanche photodiodes (APD) present close to unity excess noise factor on top of high gain and very low dark current. These features make this technology an almost ideal amplifier, especially useful for ultra low flux applications such as lidar.In this thesis, we analyze the performances of a custom large diameter (200μm) monopixel HgCdTe-APD based detector (designed at CEA-LETI) in the framework of atmospheric CO2 measurements with the DIAL technique. The laser emitter, a custom solid-state Ho :YLF laser developed at the Laboratoire de Météorologie Dynamique, is tunable in the 2050-2054nm range and produces 10 mJ pulses at a repetition rate of 2kHz. This emitter is associated to a detection chain adapted to the HgCdTe APD based detector to provide the first atmospheric DIAL measurements using the HgCdTe APD technology.Experiments confirmed the outstanding sensitivity of the detector (75 noise photons per characteristic time given a 20MHz bandwidth) and highlight the huge potential of this technology for any application relying on low light flux detection in SWIR. With the system previously mentioned, we reach an precision of 10-20 % on CO2 mixing ratio for a time-space resolution of 100 m and 4 s for measurements in the atmospheric boundary layer. Regarding the detector impulse response, we have shown evidence of a negative influence of reverse bias on the long term settling time of the APD. This phenomenon limits the dynamic range of useful signals and contraints the DIAL system. Thanks to numerical simulation taking into account this behaviour, we derive numerically expected biases on DIAL measurements
Mirabaud, Anaïs. "Développement d'une chimie hôte-invité pour la valorisation du CO2 via une catalyse éco-compatible". Thesis, Lyon, École normale supérieure, 2015. http://www.theses.fr/2015ENSL1052/document.
Testo completoThe utilization of carbon dioxide (CO2) as a key component in organic transformations has recently drawn much attention as a greener alternative to fossil fuel based resources. The objectives of this work aim at studying the synthesis of cyclic carbonates from the coupling of CO2 with epoxide. Numerous catalysts have been proposed for this reaction among which the ammonium halides providing the nucleophile to initiate the reaction by opening the epoxide. Herein, we propose a new approach based on host-guest chemistry, to improve catalytic reactivity by increasing the nucleophilicity of the halide anion. For this purpose, cavitand molecular receptors able to bind quaternary ammonium ions are used, releasing the anionic nucleophile for the initial epoxide ring-opening reaction. At CO2 atmospheric pressure, our catalytic systems demonstrated a great potential by the dramatic activation of tetramethylammonium halides, whereas when used alone, these catalysts had never shown any activity. The influence of the cavitand structure was investigated through experiments run under 10 bar of CO2 pressure, and revealed that a double activation was possible with cavitand bearing Brönsted acidic hydroxyl functions and optimal recognition properties. The heterogeneization of such catalytic systems was finally studied with the grafting of either ammoniums or cavitands on silica based materials
Wolff, Niklas von. "Reaction mechanisms of CO₂ activation and catalytic reduction". Thesis, Université Paris-Saclay (ComUE), 2016. http://www.theses.fr/2016SACLS580.
Testo completoThe use of CO₂ as a C1 chemical feedstock for the fine chemical industry is interesting both economically and ecologically, as CO₂ is non-toxic, abundant and cheap. Nevertheless, transformations of CO₂ into value-added products is hampered by its high thermodynamic stability and its inertness toward reduction. In order to design new catalysts able to overcome this kinetic challenge, a profound understanding of the reaction mechanisms at play in CO₂ reduction is needed. Using novel N/Si+ frustrated Lewis pairs (FLPs), the influence of CO₂ adducts and different hydroborane reducing agents on the reaction mechanism in the catalytic hydroboration of CO₂ were investigated, both by DFT calculations and experiments. In a second step, the reaction mechanism of a novel reaction for the creation of C–C bonds from CO₂ and pyridylsilanes (C₅H₄N–SiMe₃) was analyzed by DFT calculations. It was shown that CO₂ plays a double role in this transformation, acting both as a catalyst and a C1-building block. The fine understanding of this transformation then led to the development of a novel approach for the synthesis of sulfones and sulfonamides. Starting from SO₂ and aromatic silanes/amine silanes, these products were obtained in a single step under metal-free conditions. Noteworthy, sulfones and sulfonamides are common motifs in organic chemistry and found in a variety of highly important drugs. Finally, this concept was extended to aromatic halides as coupling partners, and it was thus shown for the first time that a sulfonylative Hiyama reaction is a possible approach to the synthesis of sulfones
Caville, Sylvain. "Spectroscopie embarquée pour la distribution verticale d'ammoniac (NH3) et de dioxyde de carbone (CO2)". Electronic Thesis or Diss., Reims, 2024. http://www.theses.fr/2024REIMS008.
Testo completoAmmonia (NH3) is an atmospheric pollutant, emitted at 80 % by agriculture, which contributes to the eutrophication and acidification of natural environments. It is also a precursor of fine particles (PM2.5) that are harmful to human health. Despite this major scientific and societal role, our knowledge about atmospheric ammonia is still very limited. Measuring the vertical profile of NH3 is one of the keys to improving this knowledge. For this reason, the main objective of this thesis is to develop an ammonia measurement instrument that can be embedded in a tethered balloon to measure these vertical profiles. To begin, a state of the art of NH3 measurement was carried out through the data analysis of the AMICA campaign (Multi-Instrumental Analysis of Ammonia Concentrations) in autumn 2021. It highlighted the need to design an instrument without a sampling system to avoid bias due to NH3 adsorption. To assess the infrared spectroscopy techniques (DAS and WMS) intended for NH3 detection, a first instrument aimed at atmospheric CO2 measurements (main anthropogenic greenhouse gas) was developed and used to carry out vertical profiles. As NH3 is much more difficult to detect than CO2 , a long-path optical cell was designed to improve the instrument’s sensitivity. On a more general level, the tools developed and implemented during this thesis can be applied to the measurement of all the atmospheric species of interest, and in particular those that exist in trace quantities
Destro, Gianluca. "Chemistry of CO₂ for the synthesis of radio-labelled compounds". Thesis, Université Paris-Saclay (ComUE), 2019. http://www.theses.fr/2019SACLS228.
Testo completoRadioisotope labeling is a relevant topic both from a fundament research perspective and for health applications in academy and pharmaceutical and agrochemical industries. In this context, carbon-14 plays a basic role in drug development and ADME and toxicological studies. Traditional synthesis with radiocarbon (¹⁴C), based on lengthy and multistep approaches, have hampered the sustainable of the strategy. The aim of this thesis is to develop novel labeling techniques by isotope exchange. At first, our efforts were focused on the developement of a copper catalyzed dynamic carbon isotope exchange (CIE) using ¹³CO₂ and ¹⁴CO₂, a fundamental and readily available source of radiocarbon on (hetero)aromatic carboxylic acids. The concept of CIE was further extent to another relevant drug scaffolds such as phenyl acetic acids. Hence, it was described a transition metal-free approach able to exchange ¹³CO₂, le ¹⁴CO₂ and ¹¹CO₂, to the best of our knowledge this would be the first example. At last, another CIE with a different primary radiocarbon source such as cyanyde was envisioned. CIE technology expands the concept of late-stage carbon radiolabeling, with substrates bearing carboxylic acid and nitrile moieties, reducing the synthetic costs and limiting the generation of radioactive waste. This new process is still at its infancy and more work need to be done
Sahin, Nihat Ege. "Réduction électrochimique du dioxyde de carbone sur des électrocatalyseurs à base de cuivre". Thesis, Poitiers, 2016. http://www.theses.fr/2016POIT2313/document.
Testo completoThe 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
Membrive, Olivier. "Caractérisation de la distribution verticale des gaz à effet de serre CO2 et CH4 par mesures sous ballons. Application à la validation d'observations satellites". Thesis, Paris 6, 2016. http://www.theses.fr/2016PA066509/document.
Testo completoMonitoring and understanding the evolution of the two most important anthropogenic greenhouse gases(carbon dioxide (CO2) and methane (CH4)) are some of the major challenges in climate science. Over the past decades,the increased availability and diversity of observations (surface networks, aircraft campaigns, satellite observations)and the improvement of atmospheric transport models has allowed to increase our understanding of biogeochemicalcycles of CO2 and CH4. Nevertheless, precise vertical observations are still very rare. However, these become crucialto both properly characterize the vertical transport of the gases, as well as to fully evaluate total or partial columnsof gases retrieved from space observations.In this thesis, we present an innovative instrument called “AirCore” allowing to collect a continuous air samplealong an atmospheric column while descending from high altitude. The analysis of CO2 and CH4 mole fractions inthe collected sample combined with the measurements of an ambient parameters (Pressure, temperature...) allows toretrieve vertical profiles from the surface up to 30 km. Initially invented at NOAA, several new AirCores giving accessto various vertical resolutions have been developed at LMD and flown with success during the CNES Strato-Sciences2014, 2015, and 2016 balloon campaigns. Excellent agreement was found between profiles acquired with differentAirCores during the same flights demonstrating the repeatability of the measurements and allowing to validate thecalculation of the vertical resolution. Comparisons with measurements from independent laser diode spectrometersflown on the same gondola have confirmed that AirCore profiles capture the vertical variability of CO2 and CH4.The vertical profiles retrieved from AirCores have been allowed to validate the CH4 partial columns retrieved fromIASI/Metop at LMD and revealed that the information on the full atmospheric column is required. Comparisons havebeen performed with tropospheric profiles obtained during aircraft campaigns (HIPPO) as well as vertical profilesextracted from atmospheric transport models (LMDz,TM5) and forecast systems (CAMS). Results demonstrated theimportance of a good characterization of the stratosphere for satellite
Venet, Saphir. "Stockage du CO2 et séparation CO2/CH4 par des matériaux de silice à porosité et fonctionnalité contrôlées : étude expérimentale et modélisation de dynamique moléculaire". Thesis, Pau, 2018. http://www.theses.fr/2018PAUU3027/document.
Testo completoThis work aims to evaluate the performance of silica-based materials and to rationalize their synthesis according to their desired adsorption properties (capacity and/or selectivity) by combining experimental approaches and the management of the molecular animal. These materials are ideally suited for CO2 adsorption capacity but also CO2/ CH4 selectivity. The different stages of this work were:- the synthesis and functionalization of the silica materials,- their textural and chemical characterization,- the determination of CO2 adsorption capacities, of their CO2/ CH4 selectivity.- the characterizations by various spectroscopic and microscopic techniques of tests to try to locate the adsorption of CO2 and to measure its mobility,- microscopic identification by the factor of physic-Factors influence the preferential adsorption of CO2 and its diffusivity in the role of hydrophilic / hydrophobic character in silica by functional.These objectives required the preparation of high specific surface materials through a simple sol-gel process. These materials have been modified in order to obtain a degree of functionalization with -CH3 groups sufficient to modify the hydrophilic nature of the material while maintaining a sufficient specific surface area. The influence of pore size was also probed.The adsorption capacities of the gases under pressure were carried out for pure gases but also on CO2/ CH4 mixtures in different proportions. The CH4/ CO2 selectivity, often estimated from the pure body isotherms and / or the IAST method, was in this case determined from the direct measurement of the isotherms of the gas mixtures. It has become apparent that water plays a crucial role in adsorption capacity and selectivity. This parameter is one of those studied through molecular dynamics simulations. The influence of the introduction of hydrophobic groups has also been explored.The results obtained by molecular dynamics are on the whole in good agreement with the experimental data. These two parallel experience / theory approaches have highlighted the selectivity of one of the materials for applications where the gaseous effluent is little loaded with CO2
Ponsard, Louise. "Conversion catalytique du CO pour la synthèse de monomères oxygénés". Thesis, université Paris-Saclay, 2021. http://www.theses.fr/2021UPASF002.
Testo completoThe production and exploitation of fossil-based chemicals leads to increased emissions of greenhouse gases, responsible for unprecedented climate change. Small molecules (CO and CO₂), currently seen as waste products, could be considered as appealing carbon sources for the transition of our linear economy to a circular economy. Carbon monoxide (CO) is a small molecule released by the chemical industry as gaseous waste, and is accessible through the electroreduction of CO₂. In this manuscript, the utilization of CO from both industrial and electrochemical sources is disclosed, constituting here a carbon source for the synthesis of oxygenated monomers. During this PhD thesis, new catalytic systems were developed for the synthesis of new monomers through the carbonylation of oxygenated heterocycles. The utilisation of CO produced by CO₂-electroreduction in a carbonylation reaction for the synthesis of beta-lactone from epoxides was also shown feasible. The formation of acrylic acid by β-propiolactone isomerisation is reported herein, in mild conditions. The mechanism of this reaction was elucidated by DFT calculations. Finally, the study of the reaction of carbonylation of acrylic acid was proved to be an efficient strategy for the synthesis of oxygenated monomers
Barral, Cuesta Abel. "The carbon isotope composition of the fossil conifer Frenelopsis as a proxy for reconstructing Cretaceous atmospheric CO2". Thesis, Lyon, 2016. http://www.theses.fr/2016LYSE1148.
Testo completoThe Cretaceous was a period characterized by strongly marked climate change and major carbon cycle instability. Atmospheric CO2 has repeatedly been pointed out as a major agent involved in these changing conditions during the period. However, long-term trends in CO2 described for the Cretaceous are not consistent with those of temperature and the large disturbance events of the carbon cycle described for the period. This raises a double question of whether descriptions of the long-term evolution of atmospheric CO2 made so far are accurate or, if so, atmospheric CO2 was actually a major driver of carbon cycle and climate dynamics as usually stated. In this thesis the close relationship between the carbon isotope composition of plants and atmospheric CO2 is used to address this question. Based on its ecological significance, distribution, morphological features and its excellent preservation, the fossil conifer genus Frenelopsis is proposed as a new plant proxy for climate reconstructions during the Cretaceous. The capacity of carbon isotope compositions of Frenelopsis leaves (d13Cleaf) to reconstruct past atmospheric CO2, with regards to both carbon isotope composition (d13CCO2) and concentration (pCO2), is tested based on materials coming from twelve Cretaceous episodes. To provide a framework to test the capacity of d13Cleaf to reconstruct d13CCO2 and allowing for climate estimates from carbon isotope discrimination by plants (?13Cleaf), a new d13CCO2 curve for the Cretaceous based on carbon isotope compositions of marine carbonates has been constructed. Comparison with d13Cleaf-based d13CCO2 estimates reveals that although d13CCO2 and d13Cleaf values follow consistent trends, models developed so far to estimate d13CCO2 from d13Cleaf tend to exaggerate d13CCO2 trends because of assuming a linear relationship between both values. However, given the hyperbolic relationship between ?13Cleaf and pCO2, by considering an independently-estimated correction factor for pCO2 for a given episode, d13Cleaf values may be a valuable proxy for d13CCO2 reconstructions. ?13Cleaf estimates obtained from d13CCO2 and d13Cleaf values were used to reconstruct the long-term evolution of pCO2. The magnitude of estimated pCO2 values is in accordance with that of the most recent and relevant model- and proxy-based pCO2 reconstructions. However, these new results evidence long-term drawdowns of pCO2 for Cretaceous time intervals in which temperature maxima have been described
Thong, Deng Honda. "Extraction et mise en forme (en liposomes) de phospholipides issus d'un co-produit par voie supercritique". Thesis, Bordeaux 1, 2011. http://www.theses.fr/2011BOR14351/document.
Testo completoThe demand in phospholipids is increasing because of their use in defferent domains, i.e. pharmaceutics, food industry, and cosmetics. Nowadays, the main sources of phospholipids come from soya and egg yolk classically extracted using organic solvents. The present work was undertaken in order to add value to waste products of fishery and to extract the lipids using a green technology. We developed an alternative green technique for lipid extraction based on the use of GRAS solvents as CO2 and ethanol. The extractions were carried out by flowing supercritical CO2. Varying the operating conditions (pressure, temperature, proportion and nature of the co-solvent, type of reactors) allowed obtaining extracts with different purities and contents in phospholipids. Finally, we explored the possibility of producing liposomes by coupling the phospholipid extraction using supercritical fluids and the vesicle formation in a continuous process
Messabeb, Hamdi. "Caractérisation thermodynamique des équilibres liquide-vapeur des systèmes CO2 – eaux salées dans des conditions de hautes températures et hautes pressions". Thesis, Pau, 2017. http://www.theses.fr/2017PAUU3013/document.
Testo completoThis work was supported by Total and ‘’Agence National de la recherche’’ as a part of SIGARRR project (Simulation of the impact of annex gases co-injected with CO2 during its geological storage on the Reservoir-Rocks Reactivity. The aim of the thesis was to obtain experimental CO2 solubility data in salty aqueous solutions of sodium chloride and calcium chloride at different molalities (1, 3 and 6 mol/kg) under high temperature (323K < T < 423K) and high pressure (5 MPa < P < 20 MPa).Following a bibliographical study on experimental methods used for the carbon dioxide solubility determination, three characterization methods were tested: Aqueous phase analysis by ion chromatography Solubility estimation from mass balance, amounts of CO2 and liquid initially loaded into the cell and experimental parameters (density of liquid phase, molar volume of gas phase, and total volume of the equilibrium cell…). A liquid sample trapping in sodium hydroxide solution followed by a titrationA sensitivity study was carried out on the Solubility estimation method from mass balance. This study identified the level of accuracy of autoclave volume measurement to obtain reliable and accurate solubility data high-pressure.A sampling protocol was developed to withdraw aqueous samples and trap them into soda solution at high pressure. Two titration procedures were set up; liquid samples of CO2-H2O and CO2-H2O-NaCl systems were analyzed by potentiometric titration and samples of CO2-H2O-CaCl2 system were analyzed by conductimetric titration. 84 solubility data were obtained during this study, which include 45 new experimental data. Experimental measurement were compared to the results of simulation performed with PHREEQC software using a ‘’Pitzer.dat’’ database.The salting out effect observed was evaluated for each system under all temperature and pressure conditions
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.
Testo completoMethane 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
Fleury, Christelle. "Optimisation d'un procédé par CO2 pressurisé pour la pasteurisation et la préservation de compléments alimentaires liquides". Thesis, Bordeaux, 2017. http://www.theses.fr/2017BORD0595/document.
Testo completoAccording to the law, food dietary supplements belong to food products and must then be pasteurized to kill potentially pathogenic microorganisms. Pressurized carbon dioxide can be a low-temperature alternative to usual thermal treatments. In this study, a high pressure carbon dioxide process is optimized to pasteurize dietary supplements highly contaminated with 3 microorganism species.This work reviews the effect of operating parameters on microbial inactivation and active ingredients thanks to a central composite design. Temperature and, at a lower extent, the pressure-duration interaction were identify as influent. Concerning active ingredients, total phenolic concentration is fully preserved whereas vitamin C retention rate is at least of 70%. Results were analyzed taking into account the synergistic effect of temperature and pH, temperature and atmospheric or N2 pressure, contamination level and the composition of the food matrix.Pasteurization was evaluated from the mass transfer and characteristic times point of view in a gaz-liquid contactor. The sensitivity analysis underlines that CO2 solubility in water is the main factor that affects the dissolution kinetic, beyond contactor constraints. Experiments led with 2 different batch set-ups and a mini‑continuous reactor illustrate that point.Finally this work studies the shelf-life of our CO2-pasteurized products and estimates the added value of such a treatment compared to a thermal one
Wang, Mingxi. "Synthèse RAFT-MADIX de copolymères à gradient amphiphiles à base de pivalate de vinyle et leurs propriétés dans le CO2 supercritique". Thesis, Toulouse 3, 2019. http://www.theses.fr/2019TOU30276.
Testo completoIn the field of polymer science, the identification of CO2-philic (co)polymers and rationalization of their solubility properties in supercritical carbon dioxide (scCO2) have represented challenges over the past twenty years. In the present work, we propose an easy to implement and use methodology to measure cloud point pressures in scCO2 without the need for a specific setup. Based on the analysis of images issued from the video recording of solution changes occurring while the pressure is changed, this alternative analytical method demonstrates higher repeatability, higher accuracy than direct visual determination and enables in the case of complex architectures like block copolymers to infer additional information from cloud point measurements. The thesis then encompasses the synthesis and the resulted phase behavior and interfacial properties of amphiphilic gradient copolymers at the water/CO2 interface by comparing with block copolymer counterparts. Thanks to the determination of reactivity ratios and simulation of the composition profile of copolymer chains, a series of well-controlled vinyl pivalate (VPi)-based spontaneous gradient copolymers were synthesized by RAFT/MADIX polymerization in a 'one-pot' process. These copolymers were varied using N,N-dimethylacrylamide (DMA) and acrylic acid (AA) as hydrophilic segments, and using monofunctional xanthate (Xa) and difunctional xanthate (DiXa) as chain transfer agents. The corresponding block copolymers were also prepared for comparison by RAFT/MADIX in two steps. Building on the newly-proposed methodology of cloud point measurement, the solubility of all those copolymers could be mapped in function of their composition, microstructure and architecture
Dumas, Arnaud. "Apport des photodiodes à avalanche HgCdTe pour la télédétection du CO2 atmosphérique par lidar DIAL à 2 micromètres". Thesis, Université Paris-Saclay (ComUE), 2016. http://www.theses.fr/2016SACLX105/document.
Testo completoThe Short Wavelength Infrared (SWIR) region (1.5-2 μm) is well adapted for diffe- rential absorption lidar technique (DIAL) for several reasons : (i) it covers absorption bands with suitable intensity for the main greenhouse gases (CO2, CH4, H2O, etc.) (ii) the extinction due to particles is low (iii) it belongs to the eye safe domain. However, one main drawback has long been the lack of efficient photodetectors for such frequencies. A major enhancement occurred in the early 2000s when it was understood that HgCdTe avalanche photodiodes (APD) present close to unity excess noise factor on top of high gain and very low dark current. These features make this technology an almost ideal amplifier, especially useful for ultra low flux applications such as lidar.In this thesis, we analyze the performances of a custom large diameter (200μm) monopixel HgCdTe-APD based detector (designed at CEA-LETI) in the framework of atmospheric CO2 measurements with the DIAL technique. The laser emitter, a custom solid-state Ho :YLF laser developed at the Laboratoire de Météorologie Dynamique, is tunable in the 2050-2054nm range and produces 10 mJ pulses at a repetition rate of 2kHz. This emitter is associated to a detection chain adapted to the HgCdTe APD based detector to provide the first atmospheric DIAL measurements using the HgCdTe APD technology.Experiments confirmed the outstanding sensitivity of the detector (75 noise photons per characteristic time given a 20MHz bandwidth) and highlight the huge potential of this technology for any application relying on low light flux detection in SWIR. With the system previously mentioned, we reach an precision of 10-20 % on CO2 mixing ratio for a time-space resolution of 100 m and 4 s for measurements in the atmospheric boundary layer. Regarding the detector impulse response, we have shown evidence of a negative influence of reverse bias on the long term settling time of the APD. This phenomenon limits the dynamic range of useful signals and contraints the DIAL system. Thanks to numerical simulation taking into account this behaviour, we derive numerically expected biases on DIAL measurements
Li, Lun. "Séquestration biologique du carbone par les cyanobactéries". Phd thesis, Université Claude Bernard - Lyon I, 2010. http://tel.archives-ouvertes.fr/tel-00878524.
Testo completoMembrive, Olivier. "Caractérisation de la distribution verticale des gaz à effet de serre CO2 et CH4 par mesures sous ballons. Application à la validation d'observations satellites". Electronic Thesis or Diss., Paris 6, 2016. http://www.theses.fr/2016PA066509.
Testo completoMonitoring and understanding the evolution of the two most important anthropogenic greenhouse gases(carbon dioxide (CO2) and methane (CH4)) are some of the major challenges in climate science. Over the past decades,the increased availability and diversity of observations (surface networks, aircraft campaigns, satellite observations)and the improvement of atmospheric transport models has allowed to increase our understanding of biogeochemicalcycles of CO2 and CH4. Nevertheless, precise vertical observations are still very rare. However, these become crucialto both properly characterize the vertical transport of the gases, as well as to fully evaluate total or partial columnsof gases retrieved from space observations.In this thesis, we present an innovative instrument called “AirCore” allowing to collect a continuous air samplealong an atmospheric column while descending from high altitude. The analysis of CO2 and CH4 mole fractions inthe collected sample combined with the measurements of an ambient parameters (Pressure, temperature...) allows toretrieve vertical profiles from the surface up to 30 km. Initially invented at NOAA, several new AirCores giving accessto various vertical resolutions have been developed at LMD and flown with success during the CNES Strato-Sciences2014, 2015, and 2016 balloon campaigns. Excellent agreement was found between profiles acquired with differentAirCores during the same flights demonstrating the repeatability of the measurements and allowing to validate thecalculation of the vertical resolution. Comparisons with measurements from independent laser diode spectrometersflown on the same gondola have confirmed that AirCore profiles capture the vertical variability of CO2 and CH4.The vertical profiles retrieved from AirCores have been allowed to validate the CH4 partial columns retrieved fromIASI/Metop at LMD and revealed that the information on the full atmospheric column is required. Comparisons havebeen performed with tropospheric profiles obtained during aircraft campaigns (HIPPO) as well as vertical profilesextracted from atmospheric transport models (LMDz,TM5) and forecast systems (CAMS). Results demonstrated theimportance of a good characterization of the stratosphere for satellite
Sinyakova, Tatyana. "Experimental and theoretical studies of infrared spectroscopic signatures of key atmospheric molecules : carbon dioxide CO2 and monodeuterated methane CH3D". Thesis, Besançon, 2016. http://www.theses.fr/2016BESA2064.
Testo completoPresent Ph.D work has focused on experimental and theoretical studying of spectroscopic signatures of key atmospheric molecules: CO2 and CH3D. It was divided into experimental part, devoted to high-pressure measurements of IR CO2 spectra, and theoretical part, namely calculation of collisional line-widths for CH3D perturbed by various gases. In the first part, I reported room-temperature high-pressure CO2 absorption measurements in the spectral interval 600-9650 cm-1 (probed in planetary atmosphere studies) with the double goals: to provide accurate and extensive data and to trace evolution of the line-mixing effects with gradual pressure variations. In the second part, I presented semi-classical calculations of CH3D-N2 and -142 line-broadening coefficients using exact trajectory model in the parallel v3 and perpendicular vs, v6 bands of CH3D-N2 as well as in the parallel v3 band of CH3D-112 for large intervals of rotational quantum numbers required for spectroscopic databases
Perret, Alexandre. "Etude des propriétés de transport du CO2 et de l'éthanol en solution hydroalcoolique par dynamique moléculaire classique : Application aux vins de Champagne". Thesis, Reims, 2014. http://www.theses.fr/2014REIMS024/document.
Testo completoThe work presented in this manuscript is devoted to the study of the diffusion of dissolved carbon dioxide and ethanol in a hydroalcoholic solution model representing Champagne wines. The first part of this work deals with the different formalisms of molecular diffusion, as well as theoretical and experimental methods used to account for this phenomenon of transport. Particular attention is paid to the classical force field molecular dynamics that is used in this work with the GROMACS software. This theoretical approach provides a new perspective in research on champagne and particularly on the role of each of the main species in CO2 diffusion. NMR spectroscopy, and an experimental method based on the study of the bubbles growth rate, were also used. In the second part, the theoretical and experimental results are presented and compared with each other to validate the protocol of molecular dynamics simulations. The viscosities of the model solution and of the champagne, as well as the hydrodynamic radii of CO2 and ethanol, are also investigated. The last part of the manuscript focuses on the partnership with the Bull company and the study of the GROMACS software performance. The expertise of and the tools developed by the Bull company are used to study the scalability and the parallel behavior of GROMACS for modeling champagne
Kilaparthi, 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.
Testo completoThis 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
Liu, Xuan. "Novel vinyl ester-based copolymers : RAFT/MADIX synthesis and properties in supercritical carbon dioxide media". Thesis, Toulouse 3, 2015. http://www.theses.fr/2015TOU30092.
Testo completoSupercritical fluid is a substance whose temperature and pressure are both above their critical values which are defined as the critical point. Similarly to the triple point which defines the zero-variance point for the solid, gas and liquid states, the critical point (Pc) denotes the point where the gas, liquid and supercritical phases coexist and it can be experimentally observed through a critical opacity. Properties of SCFs are different from those of ordinary liquids and gases. Close to the critical density, SCFs display properties that are to some extent intermediate between those of a liquid and a gas. For example, a SCF may be relatively dense and dissolve certain solids while being miscible with permanent gases and exhibiting high diffusivity and low viscosity. In addition, SCFs are highly compressible and the density (and therefore solvent properties) can be "tuned" over a wide range by varying pressures and temperatures. Among supercritical fluids, scCO2 certainly has excellent potential for practical development not only because of its low critical conditions (Tc = 31 °C, Pc = 74 bar), but also due to some other factors such as: CO2 is non-toxic. Its threshold air concentration for working conditions is as high as 5000 ppm. By means of comparison, a daily exposition to 10 ppm of chloroform is considered hazardous. CO2 is non-flammable. This constitutes another very competitive advantage compared to halogenated solvents. Its high pressure vapour-superior to 60 bar-allows its complete removal from processed materials. Thus, CO2 is one of the two solvents fully approved by the Food and Drug Administration (FDA), along with water. CO2 has a low reactivity and is inert towards oxidation. It is also a non-transferring species for radicals. Heat and mass transfer are significantly enhanced in scCO2 due to its properties of low viscosity and densities. Its low surface tension allows wetting structured materials better than liquids usually do. However, besides the cost of high-pressure vessels, CO2 still has intrinsic physical disadvantages: A low cohesive energy density which confers a weak solvent strength to CO2. CO2 is a Lewis acid through its electron-deficient carbon. It thus reacts reversibly with strong Lewis bases such as primary and secondary amines. But this can be turned into an advantageous property for the capture of CO2 by amine-based solvents and surfactants, polymers and solvents that possess CO2-responsive moieties such as guanidines and amidines. CO2 is a poison for Ziegler-Natta and palladium-based catalysts due to the formation of CO. Due to the non-polar and weak Van der Waals forces of CO2, most lipophilic and hydrophilic species (such as amino acids, proteins and many catalysts) are often insoluble in scCO2. Obviously, it is a limitation for the application of supercritical carbon dioxide. Recently, in order to overcome this disadvantage, the most effective approach is to use suitable surfactants to produce water-in-CO2 microemulsions or reverse micelles. Consan and Smith tested the solubility of over 130 commercially available surfactants in scCO2 at 50 °C and 10-50 MPa. All of them were rarely soluble or only slightly soluble in scCO2, so they could not be employed as surfactants in scCO2
El, yazidi Abdelhadi. "Estimation des flux de CO2 et de CH4 en France en utilisant les concentrations atmosphériques du réseau ICOS et les techniques d'assimilation de données". Thesis, Université Paris-Saclay (ComUE), 2018. http://www.theses.fr/2018SACLV067/document.
Testo completoSince the industrial revolution, the economic and the demographic growths have increased exponentially,leading to an enhancement of the fossil fuels combustion, such as coal, oil, and natural gas. Consumingthese source of energy amplifies the greenhouse gas emissions, mainly carbon dioxide (CO2) and methane(CH4), whose accumulation in the atmosphere lead to the increase of the greenhouse effect. According tothe 5th assessment report of the Intergovernmental Panel on Climate Change (IPCC), it is extremely likely(95-100% of certainty) that the observed increase in the greenhouse effect is related to the increase of theanthropogenic emissions. However, the estimations of the GHG budget at the regional and the nationalscales remains highly uncertain. The aim of this thesis is to improve the estimation of the CO2 and CH4fluxes in France, using data assimilation techniques and atmospheric measurements provided by theIntegrated Carbon Observation System (ICOS) network.The first phase focuses on analyzing the measured CO2, CH4, and CO (Carbon monoxide) atmosphericconcentrations provided by surface monitoring stations. This study is concerned with the problem ofidentifying atmospheric data influenced by local emissions that can result in spikes in the GHG time series.Three methods are implemented on continuous measurements of four contrasted atmospheric sites. The aimof this analysis is to evaluate the performance of the used methods for the correctly detect the contaminateddata. This work allows us to select the most reliable method that was proposed to perform daily spikedetection in the ICOS Atmospheric Thematic Centre Quality Control (ATC-QC) software.Secondly, we simulate the atmospheric concentrations of CO2 and CH4 using the chemistry transport modelCHIMERE in a domain centered over France for the year 2014. The objective of this study is to evaluate thesensitivity of simulated concentrations using different input data (sensitivity to the meteorological transportand sensitivity to the surface fluxes). This work led to the quantification of both the transport and surfacefluxes errors based on the combination of different simulations. Thus, the most reliable combination of thebest input data was selected for the flux inversion study.Lastly, the measured CO2 and CH4 concentrations are used by the PYMAI inversion system (Berchet et al.,2013 and 2015) in order to estimate the CO2 and CH4 fluxes in France. The Inversion is performed for onemonth in winter (January) and one month in summer (July), using the transport model CHIMERE. Theinversion results have provided very interesting results for the regional estimation of the CO2 and CH4surface fluxes in France with an uncertainty reduction that may attain 35% of the national totals
El, yazidi Abdelhadi. "Estimation des flux de CO2 et de CH4 en France en utilisant les concentrations atmosphériques du réseau ICOS et les techniques d'assimilation de données". Electronic Thesis or Diss., Université Paris-Saclay (ComUE), 2018. http://www.theses.fr/2018SACLV067.
Testo completoSince the industrial revolution, the economic and the demographic growths have increased exponentially,leading to an enhancement of the fossil fuels combustion, such as coal, oil, and natural gas. Consumingthese source of energy amplifies the greenhouse gas emissions, mainly carbon dioxide (CO2) and methane(CH4), whose accumulation in the atmosphere lead to the increase of the greenhouse effect. According tothe 5th assessment report of the Intergovernmental Panel on Climate Change (IPCC), it is extremely likely(95-100% of certainty) that the observed increase in the greenhouse effect is related to the increase of theanthropogenic emissions. However, the estimations of the GHG budget at the regional and the nationalscales remains highly uncertain. The aim of this thesis is to improve the estimation of the CO2 and CH4fluxes in France, using data assimilation techniques and atmospheric measurements provided by theIntegrated Carbon Observation System (ICOS) network.The first phase focuses on analyzing the measured CO2, CH4, and CO (Carbon monoxide) atmosphericconcentrations provided by surface monitoring stations. This study is concerned with the problem ofidentifying atmospheric data influenced by local emissions that can result in spikes in the GHG time series.Three methods are implemented on continuous measurements of four contrasted atmospheric sites. The aimof this analysis is to evaluate the performance of the used methods for the correctly detect the contaminateddata. This work allows us to select the most reliable method that was proposed to perform daily spikedetection in the ICOS Atmospheric Thematic Centre Quality Control (ATC-QC) software.Secondly, we simulate the atmospheric concentrations of CO2 and CH4 using the chemistry transport modelCHIMERE in a domain centered over France for the year 2014. The objective of this study is to evaluate thesensitivity of simulated concentrations using different input data (sensitivity to the meteorological transportand sensitivity to the surface fluxes). This work led to the quantification of both the transport and surfacefluxes errors based on the combination of different simulations. Thus, the most reliable combination of thebest input data was selected for the flux inversion study.Lastly, the measured CO2 and CH4 concentrations are used by the PYMAI inversion system (Berchet et al.,2013 and 2015) in order to estimate the CO2 and CH4 fluxes in France. The Inversion is performed for onemonth in winter (January) and one month in summer (July), using the transport model CHIMERE. Theinversion results have provided very interesting results for the regional estimation of the CO2 and CH4surface fluxes in France with an uncertainty reduction that may attain 35% of the national totals
Brochard, Laurent. "Poromechanics and adsorption : application to coal swelling during carbon geological storage". Thesis, Paris Est, 2011. http://www.theses.fr/2011PEST1067/document.
Testo completoPas de résumé en anglais
Alves, Margot. "Carbon dioxide and vegetable oil for the synthesis of bio-based polymer precursors". Thesis, Bordeaux, 2016. http://www.theses.fr/2016BORD0129/document.
Testo completoAlthough it is a thermodynamically and kinetically stable molecule, carbon dioxide can beconverted into five- and six-membered cyclic carbonates by coupling with epoxides or oxetanes, respectively, using appropriate catalysts. Cyclic carbonates are used as green solvents, electrolytes for Liion batteries or intermediates for the synthesis of polymers. However, the catalytic performance must be further enhanced in particular for the coupling of CO2 with epoxidized vegetable oils or oxetanes. In this context, we developed a new highly efficient bicomponent homogeneous organocatalyst composed of anammonium salt as the catalyst and fluorinated single or double hydrogen bond donors as co-catalysts. First,a screening of onium-based catalysts and hydrogen-bond donors was performed. Performances of thecatalysts and optimization of the reaction was realized through detailed kinetics studies using in-situ FTIR/Raman spectroscopy under pressure. We demonstrated that fluorinated alcohols showed unexpected co-catalytic activity due to synergisms between the onium salt and fluorinated co-catalysts enabling the fast and selective addition of CO2 on to model epoxides and epoxidized vegetable oils under solvent-free and mild experimental conditions. The use of this powerful dual catalyst was then extended to the first organocatalytic coupling of CO2 with less reactive oxetanes to produce hydroxyl telechelic oligocarbonates that were used asprecursor of CO2-based polyurethanes by chain-extension with a diisocyanate. In addition, a fine comprehension of the mechanisms was investigated by DFT calculations highlighting that the co-catalytic performance of the onium salt/fluorinated alcohol binary catalyst arose from the strong stabilization of the intermediates and transitions states by hydrogen-bonding. To date, through comparative studies, we evidenced that this new catalyst is one
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.
Testo completoKanchev, Hristiyan. "Gestion des flux énergétiques dans un système hybride de sources d’énergie renouvelable : Optimisation de la planification opérationnelle et ajustement d’un micro réseau électrique urbain". Thesis, Ecole centrale de Lille, 2014. http://www.theses.fr/2014ECLI0001/document.
Testo completoThe presented research works aim to develop an energy management system for a cluster of distributed micro gas turbines and controllable PV generators called «active generators». The general principles of electricity generation from renewable and non-renewable energy sources are first presented. The operation of actual electric grids is also recalled in order to highlight the challenges and expected innovations in future Smart Grids. Then, the integration of a novel method for maximum and limited power point tracking in a PV-based active generator is presented. The modeling of micro-gas turbines in a microgrid energy management system is also presented. The main contribution of this thesis concerns the design of an operational planning of generators one day ahead by the means of a dynamic programming-based algorithm, taking into account the PV power production and the consumption forecasts. The proposed method calculates the production planning of generators by performing a global optimization of an objective function. An adjustment algorithm is proposed and executed every ½ hours through a communication network in order to take into account the uncertainty in forecasted values. An urban microgrid is used for testing the developed algorithms through Supervisory Control and Data Acquisition (SCADA) with hardware-in-the-loop and real-time simulations. Comparisons of the microgrid operation in identical situations with different objective functions are performed, as well as evaluations of economic and environmental indicators
Ricci, Olivia. "Capture et stockage géologique du CO2 à partir de biomasse : quelles perspectives économiques ?" Electronic Thesis or Diss., Orléans, 2011. http://www.theses.fr/2011ORLE0506.
Testo completoIn a context of unbridled growth of global energy demand and environmental pressure in the fight againstglobal warming, this thesis studies one of the proposed technologies to reduce carbon dioxide (CO2)emissions: carbon capture and geological storage (CCS). We therefore consider the application of thistechnology to the production of bioenergies (BCCS) because this technology allows purifying theatmosphere while providing a clean energy alternative to fossil fuels. The first part of this work analyzesthe economic and environmental potential of BCCS. First, an economic and environmental assessment ofBCCS in the bioethanol production in France is conducted. Then, using the bottom-up optimization modelTIAM-FR, we study the global and regional potential of this technology in the electricity sector. Finally,the economic incentives that need to be provided to ensure BCCS deployment are highlighted. In thesecond part, a general equilibrium model is used to evaluate environmental policies. We construct thetheoretical model by introducing the CCS and BCCS as well as a wide range of economic instruments.The model is then calibrated to compare the effectiveness of environmental policy instruments at a globallevel and at a French level
Gac, Jean-Philippe. "Etude multi-échelles des échanges air-mer de CO2 et de l'acidification océanique en Manche Occidentale". Electronic Thesis or Diss., Sorbonne université, 2021. http://www.theses.fr/2021SORUS223.
Testo completoThe anthropogenic impact of the raise of atmospheric CO2 has been observed on the global oceanic scale, resulting in the Ocean Acidification (OA). Largely present in the coastal ecosystems, a decrease of their population could have significant socio-economic consequences. Coastal ecosystems represent only 7% of the global ocean but host a third of the total primary production of the oceans, playing a key role in the global carbon cycle. They are highly diversified and influenced by continental inputs, which complexifies the study of the CO2 cycle. This PhD thesis investigated at different spatial and temporal scales the variability of the carbon cycle in megatidal environments of the North Western European Shelves. From 2015 to 2019, we installed an autonomous sensor of pCO2 (Sunburst SAMI-CO2) on a cardinal buoy located off Roscoff, in the south of the English Channel. Coupled with additional proximal and offshore observations of the carbon cycle and biogeochemical parameters, we were able to describe precisely this ecosystem and assess the tidal, diurnal and interannual variability. Secondly, we followed the variability of these parameters at the decadal scale, based on regular sampling from 2008 to 2018 in two coastal environments very close geographically (Brest and Roscoff, NWES), but with different freshwater influence. Finally, since methane is increasingly considered as a key player in the understanding of the coastal ecosystem functioning and Climatically-Actives Gas cycles, we quantified the driving processes of CO2 and CH4 air-sea exchanges in two mega-tidal estuaries influencing our study region
Trotignon, Raphaël. "In search of the carbon price : The european CO2 emission trading scheme : from ex ante and ex post analysis to the protection in 2020". Thesis, Paris 9, 2012. http://www.theses.fr/2012PA090052.
Testo completoThis thesis is an evaluation of the first two phases of the EU ETS. It is articulated around the progressive construction of a simulation model, ZEPHYR-Flex, which aims at being able to replicate the observed price and emissions trajectories between 2005 and 2012, and to project them until 2020 under different sets of assumptions. The ex post analysis of the first eight years of the system reveals that to understand its development, it is necessary to study in details the role played by three flexibility mechanisms: trading, spatial flexibility (offsets), and time flexibility (banking/borrowing). In a first stage, we build a technical-economic framework for the core trading mechanism of the model. The role of offsets is then scrutinized and a scenario for their use up to 2020 is calculated on this basis. Next, the time flexibility and the related banking and borrowing behavior are introduced into the model which can then replicate the past price and emission trajectory. The model and the lessons from the first two phases are then used in different prospective scenarios to 2020. Among the scenarios tested, only a strengthening of the cap in line with the 2050 European reduction target is able to restore confidence and anticipations, two factors needed for the efficiency of the EU ETS in the long term. The issue of correctly articulating the EU ETS with other climate-energy policies is also underlined
Renner, Marie. "The Emergence of Carbon Capture and Storage Techniques in the Power Sector". Thesis, Paris 10, 2015. http://www.theses.fr/2015PA100045/document.
Testo completoThis thesis analyses the techno-economic and social conditions required for the emergence of Carbon Capture and Storage (CCS) techniques in the power sector, in compliance with CCS role in long-term mitigation scenarios. The research combines two complementary approaches: the positive one deals with the economic and social determinants necessary to trigger CCS investments, and addresses two significant issues: (1) for which CO2 price is it worth investing in CCS plants, and (2) when is CCS use socially optimal? The normative approach gives recommendations on how CCS can best be deployed as part of a least cost approach to climate change mitigation. Notably, recommendations are provided about the optimal combination of CCS policy supports that should be implemented. This Ph.D. dissertation is composed of four chapters. The first two chapters embrace the investor’s vision and highlight the determinants necessary for CCS commercial emergence. The last two chapters embrace the public decision-makers’ vision. Based on the fact that, although cost-effective, one technology may not be deployed because of social acceptance issues, Chapter 3 deals with CCS public acceptance and optimal pollution. Chapter 4 goes further and addresses the optimal CCS investment under ambiguity by providing a decision criterion with simulations on the European Union’s 2050 Energy Roadmap
Lebel-Simon, Murielle. "Mesures simultanées par DRASC de température et de concentration de CO2 dans un moteur. Application à l'étude des variations cycle à cycle liées aux gaz résiduels". Rouen, 1994. http://www.theses.fr/1994ROUES010.
Testo completoBaccour, 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.
Testo completoCarbon 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
Foltran, Stéphanie. "Le CO2 supercritique pour la synthèse de carbonates cycliques catalysée par des liquides ioniques : étude des propriétés thermodynamiques et des mécanismes réactionnels par spectroscopie vibrationnelle et modélisation moléculaire". Thesis, Bordeaux 1, 2012. http://www.theses.fr/2012BOR14619/document.
Testo completoThis thesis aims to understand the thermodynamic properties and reaction mechanisms generated in the cycloaddition reaction of epoxides in supercritical CO2 medium catalyzed by ionic liquids for the green synthesis of cyclic carbonates. Thermodynamic properties (solubility, swelling, phase diagram) of epoxide/CO2 binary mixtures were determined for commercial mono-epoxides and vegetable based epoxidized oils. Kinetics study in-situ by FTIR and Raman spectroscopy were performed to determine the influence of the nature of the ionic liquids studied and of different parameters such as temperature and pressure on the reaction. Molecular modeling using DFT method has helped us to propose a reaction mechanism consistent with the experimental results and to understand what are the respective roles of the anion and cation of the ionic liquid in the reaction
Lagier-Jaegler, Anicia. "Evaluation des impacts simultanes de la localisation, de l'efficacite et du type de produits fabriques sur les performances environnementales et financieres d'une chaine logistique". Phd thesis, Ecole Nationale Supérieure des Mines de Saint-Etienne, 2011. http://tel.archives-ouvertes.fr/tel-00844739.
Testo completoSáinz-García, Álvaro. "Dynamique de stockage souterrain de gaz : aperçu à partir de modèles numériques de dioxyde de carbone et d'hydrogène". Thesis, Toulouse 3, 2017. http://www.theses.fr/2017TOU30187/document.
Testo completoClimate change mitigation is one of the major challenges of our time. The anthropogenic greenhouse gases emissions have continuously increased since industrial revolution leading to global warming. A broad portfolio of mitigation technologies has to be implemented to fulfill international greenhouse gas emissions agreements. Some of them comprises the use of the underground as a storage of various substances. In particular, this thesis addresses the dynamics of carbon dioxide (CO2) and hydrogen (H2) underground storage. Numerical models are a very useful tool to estimate the processes taking place at the subsurface. During this thesis, a solute transport in porous media module and various multiphase flow formulations have been implemented in COMSOL Multiphysics (Comsol, 2016). These numerical tools help to progress in the understanding of the migration and interaction of fluids in porous underground storages. Three models that provide recommendations to improve the efficiency, monitoring and safety of the storages are presented in this manuscript: two in the context of carbon capture and storage (CCS) and one applied to underground hydrogen storage (UHS). Each model focus on a specific research question: Multiphase model on CCS. The efficiency and long-term safety of underground CO2 storage depend on the migration and trapping of the buoyant CO2 plume. The wide range of temporal and spatial scales involved poses challenges in the assessment of the trapping mechanisms and the interaction between them. In this chapter a two-phase dynamic numerical model able to capture the effects of capillarity, dissolution and convective mixing on the plume migration is applied to a syncline-anticline aquifer structure. In anticline aquifers, the slope of the aquifer and the distance of injection to anticline crest determine the gravity current migration and, thus, the trapping mechanisms affecting the CO2. The anticline structure halts the gravity current and promotes free-phase CO2 accumulation beneath the anticline crest, stimulating the onset of convection and, thus, accelerating CO2 dissolution. Variations on the gravity current velocity due to the anticline slope can lead to plume splitting and different free-phase plume depletion time is observed depending on the injection location. Injection at short distances from the anticline crest minimizes the plume extent but retards CO2 immobilization. On the contrary, injection at large distances from anticline crest leads to large plume footprints and the splitting of the free-phase plume. The larger extension yields higher leakage risk than injection close to aquifer tip; however, capillary trapping is greatly enhanced, leading to faster free-phase CO2 immobilization. Reactive transport model on convective mixing in CCS. Dissolution of carbon-dioxide into formation fluids during carbon capture and storage (CCS) can generate an instability with a denser CO2-rich fluid located above the less dense native aquifer fluid. This instability promotes convective mixing, enhancing CO2 dissolution and favouring the storage safety
Ricci, Olivia. "Capture et stockage géologique du CO2 à partir de biomasse : quelles perspectives économiques ?" Thesis, Orléans, 2011. http://www.theses.fr/2011ORLE0506/document.
Testo completoIn a context of unbridled growth of global energy demand and environmental pressure in the fight againstglobal warming, this thesis studies one of the proposed technologies to reduce carbon dioxide (CO2)emissions: carbon capture and geological storage (CCS). We therefore consider the application of thistechnology to the production of bioenergies (BCCS) because this technology allows purifying theatmosphere while providing a clean energy alternative to fossil fuels. The first part of this work analyzesthe economic and environmental potential of BCCS. First, an economic and environmental assessment ofBCCS in the bioethanol production in France is conducted. Then, using the bottom-up optimization modelTIAM-FR, we study the global and regional potential of this technology in the electricity sector. Finally,the economic incentives that need to be provided to ensure BCCS deployment are highlighted. In thesecond part, a general equilibrium model is used to evaluate environmental policies. We construct thetheoretical model by introducing the CCS and BCCS as well as a wide range of economic instruments.The model is then calibrated to compare the effectiveness of environmental policy instruments at a globallevel and at a French level
Guérin, Frédéric. "Emission de gaz à effet de serre (CO2,CH4) par une retenue de barrage hydroélectrique en zone tropicale (Petit-saut, Guyane française) : expérimentation et modélisation". Toulouse 3, 2006. https://tel.archives-ouvertes.fr/tel-00079947.
Testo completoThe emissions of carbon dioxide (CO2) and methane (CH4) and the carbon cycle in the Petit-Saut reservoir and in the Sinnamary River (French Guiana) were studied with an aim of developing a coupled physical/biogeochemical model. The development of this model required the study of three processes controlling these emissions: (i) CO2 and CH4 production during the mineralization in anoxic condition of organic matter (OM) from soils and plants, (ii) aerobic CH4 oxidation in the water column of the lake and (iii) the processes involved in gas exchange at the air-water interface. Over 10 years, atmospheric emissions were shown to be very significant, in particular the first three years having followed the reservoir impoundment and then decreased with time. While 50% of the CO2 emissions take place at the surface of the lake, the emissions of CH4 are mainly localized downstream from the turbines. The atmospheric emissions result from the degradation of OM (soil and biomass originating from the tropical forest) flooded during impoundment and their reduction with time rises from the exhaustion of the OM stock. 10 years after impoundement, 20% of the carbon stock were mineralized and emitted to the atmosphere in the form of CO2 and of CH4. Aerobic CH4 oxidation transforms more than 95% of the CH4 diffusing upward from the hypolimnion into CO2 in the water column of the lake and 40% of the CH4 entering the river downstream of the dam. In the whole Petit Saut system, this process is responsible for the oxidation of 90% of the produced CH4 and 30% of the total CO2 emissions. The CH4 and CO2 which reach the water surface of the reservoir and of the river downstream of the dam are emitted to the atmosphere by diffusive flux. The study of this process of gas transfer to the interface air-water shows that, in tropical environment, diffusive fluxes are enhanced by the elevated temperatures and the rainy phenomena. The model is based on the hydrodynamic model SYMPHONY 2D and the biogeochemical model developed during this study starting from the kinetic data of the studied processes. The simulated vertical profiles of temperature, oxygen, CO2 and CH4 are well reproduced. This model poses the bases of an operational tool of modeling for the Petit-Saut reservoir like for other reservoirs in tropical environments