Amorphous silica membranes have molecular sieving properties for the separation of hydrogen from gas mixtures at high temperature. Consequently, they are considered to be applied in separation of a shifted syngas coming out of a water-gas-shift-reactor into the syngas and hydrogen. This separation is a key to an Integrated Gasification Combined Cycle (IGCC) plant, which would allow reducing the carbon footprint in power generation industry. The main objective of this thesis was to carry out a preliminary assessment of suitability of currently available amorphous silica membranes for this separation. However, the separation properties of amorphous silica membranes reported in the open literature vary by orders of magnitude. Therefore, in the first part of this thesis the separation properties of hypothetical silica membrane with different pore size distributions were predicted from first principles. Considering different possible gas transport mechanisms, it was concluded that gas transport in amorphous silica membranes is dominated by the activated and non-activated Knudsen diffusion. The activation energy for transport of different species was predicted using the concept of suction energy. Then, with arbitrary pore size distributions gas permeance of hypothetical silica membrane was predicted for different gas species. Since the pore size distribution of amorphous silica membrane cannot be known a priori, the developed model was used to determine the pore size distribution based on experimentally measured single gas permeances of three different species (kindly provided by Natural Resources Canada, CANMET Energy Technology Center (CETC) laboratory in Ottawa) by minimizing the error of the calculated permeance ratios with respect to the experimental values. The results indicate that, depending on how the objective function is defined, more than one pore size distribution can be found to satisfy the experimental permeance ratios. It is speculated that by increasing the number of experimentally determined permeances, a more unique pore size distribution for the tested silica membrane can be obtained. However, even at this early stage, the developed model provides a rational explanation for the effect of membrane densification on the properties of silica membranes. More specifically, a simultaneous decrease in membrane permeance and selectivity due to membrane densification, reported in the literature, is explained by shrinking the size of pores beyond a certain critical value, which depends on the kinetic diameter of gas molecules that are being separated. Comparing theoretically determined permeances, which match experimentally observed permeance ratios, revealed that the experimental permeances are considerably smaller than the theoretical values. The ratio of the two provided the basis for a scaling factor, a new concept that was introduced in this thesis. To simulate membrane module performance, a novel approach was introduced. More specifically, co- and counter-current flow configurations as well as cross-flow configuration were modeled by assuming no change in feed composition over an infinitesimally small element of membrane area. This led to a system of linear, rather than differential equations, which was readily solved numerically.

Strong dependency on fossil fuels and the associated price and supply chain risk increase the need for more efficient utilisation of existing non-renewable energy sources. Carbon capture and hydrogen purification technologies are expected to play a key role in the future low-carbonised energy matrix. Integrated Gasification Combined Cycles (IGCCs) are one of the emerging clean coal technologies which pave the way for producing power from coal with a higher net power efficiency than conventional PC-fired boiler power plants. It is also advantageous that in an IGCC power plant a carbon capture unit can be applied to a stream having a very high CO2 partial pressure ahead of gas combustion that would not be available in case of a PC-fired boiler power plant, leading to less energy penalty involved in carbon capture. At the same time, the production of ultrapure hydrogen is both a sought target and an appropriate environmental solution because it is commonly utilised as feedstock in refineries’ hydrotreaters and hydrocrackers as well as energy carrier in fuel cells. A high purity of hydrogen has been commercially produced out of raw synthesis gas using a Hydrogen Pressure Swing Adsorption (H2 PSA) process. In this thesis, it was aimed to design and optimise a bespoke H2 PSA system tailored for a decarbonised syngas feed originating from a carbon capture unit. Therefore, a novel H2 PSA has been studied that is applied to an advanced IGCC plant for cogenerating power and ultrapure hydrogen (99.99+ mol%) with pre-combustion CO2 capture. In designing the H2 PSA, it is essential to increase the recovery of ultrapure hydrogen product to its maximum since the power consumption for compressing the H2 PSA tail gas up to the gas turbine operating pressure should be minimised to save the total auxiliary power consumption. Hydrogen recovery was raised by increasing the complexity of the PSA step configuration that allows a PSA cycle to have a lower feed flow to one column being used for adsorption and more pressure equalisation steps. An in-depth economic analysis was carried out and discussed in detail. The industrial advanced IGCC performances have also been improved by process integration between the H2 PSA unit and other units in the plant.

Submitted by ELZIMAR TADEU DE FREITAS FERREIRA null (elzimar@feg.unesp.br) on 2016-08-17T20:29:45Z No. of bitstreams: 1 Tese de doutorado de Elzimar Tadeu de Freitas Ferreira.pdf: 3358273 bytes, checksum: 0b61e834c1870d60b5531502a4c3e8b9 (MD5) / Approved for entry into archive by Ana Paula Grisoto (grisotoana@reitoria.unesp.br) on 2016-08-19T18:18:10Z (GMT) No. of bitstreams: 1 ferreira_etf_dr_guara.pdf: 3358273 bytes, checksum: 0b61e834c1870d60b5531502a4c3e8b9 (MD5) / Made available in DSpace on 2016-08-19T18:18:10Z (GMT). No. of bitstreams: 1 ferreira_etf_dr_guara.pdf: 3358273 bytes, checksum: 0b61e834c1870d60b5531502a4c3e8b9 (MD5) Previous issue date: 2016-07-08 / Agência Nacional de Energia Elétrica (ANEEL) / Atualmente, a grande preocupação relacionada ao meio ambiente e redução do uso de combustíveis fósseis levou a comunidade acadêmica/científica a se concentrar em novas tecnologias de conversão de energia que possam garantir sua produção nos níveis necessários ao atendimento das necessidades humanas, mas considerando também os meios para minimizar os impactos ambientais. Propõe-se estabelecer o estado da arte da estrutura de geração termelétrica, conceituando a estrutura tecnológica de ciclos térmicos no mundo, caracterizada em centrais termelétricas distribuída e centralizada. São precedidos estudos termodinâmicos em centrais termelétricas de diferentes configurações, nas escalas industrial, municipal e nacional. Para fins de avaliação do desempenho de uma central térmica, é apresentado o desenvolvimento de uma modelagem térmica, utilizando ciclos combinados com gaseificação integrada (IGCC) e suas variações, usando balanço de massa, balanço de energia e balanço de exergia. Na geração distribuída em nível industrial, foi realizada uma análise no setor de papel e celulose, mostra-se que seu subproduto, o licor negro, um passivo ambiental, será mais bem aproveitado se passar por um processo de gaseificação e antes da queima em ciclo combinado em um sistema de cogeração. Na geração distribuída em escala municipal, o estudo de uma configuração de planta piloto foi elaborado para operar em empreendimento vinculado a alguma forma às cidades. Para o projeto de uma instalação piloto, dentre as opções de tecnologias envolvidas, as mais recomendadas seriam o ciclo IGCC (gaseificação do resíduo sólido urbano) e diferentes concepções de ciclos híbridos (incineração de resíduo sólido urbano, integrada a conjuntos a gás acionados com biogás de aterro ou gás natural). Na geração centralizada em escala nacional, empregaram-se centrais de grande porte que são usualmente encontradas na literatura. Nesta parte do estudo verificou-se a utilidade de um ciclo IGCC, com tecnologia avançada de co-gaseificação de resíduo sólido urbano e carvão aplicada a um gaseificador entrained-flow, sistema ASU (Air Separation Unit), com injeção de oxigênio e captura de CO2 pré-combustão, como alternativa eficiente de geração de energia frente às tecnologias convencionais, como a incineração e o aterro sanitário para o tratamento de materiais residuais. / Currently, the major concern related to the environment and reduction of fossil fuels has led the academic/scientific community to focus on new energy conversion technologies that can guarantee production levels necessary to meet human needs, but also that consider the means to minimize environmental impacts. In this work, it is proposed to establish the state of the art of thermoelectric generation structure, conceptualizing the technological structure of thermal cycles in the world, in the context of distributed and centralized thermal power plants, as well as their technological characteristics. Thermodynamic studies are performed in thermal power plants of different configurations, considering scales in industrial, municipal and national levels. For the purpose of evaluating the performance of a thermal power plant, it is presented the development of a thermal modeling for combined cycles with an integrated gasification (IGCC) and their variations, using mass, energy and exergy system balances. In distributed generation at the industrial level, an analysis in the paper and pulp sector was held. It is shown that its by-product, the black liquor, an environmental liability, would be better used if sent through a process of gasification before being burned in a combined cycle cogeneration system. In distributed generation at the municipal level, the study of a pilot plant configuration is designed to operate in an enterprise linked to some form to the cities. For the design of a pilot plant, from the options of technologies involved, the most recommended would be the IGCC cycle (gasification of municipal solid waste) and different conceptions of hybrid cycles (municipal solid waste incineration, integrated to gas cycles powered with landfill biogas or natural gas). For the centralized generation at the national level, it was employed large-scale plants that are usually found in the literature. In this part of the study it is demonstrated the utility of an IGCC cycle, with advanced technology co-gasification of municipal solid waste and coal applied to an entrained-flow gasifier, ASU system (Air Separation Unit), with oxygen injection and capture of CO2 in a pre combustion mode as an efficient alternative compared to power generation with conventional technologies such as incineration and the use of a landfill for the treatment of waste materials. / ANEEL: PD-0553-0022/2012

Given the growing worldwide interest in fossil fuels on one hand and mitigation of climate change on the other hand, it is necessary to research into new technologies as Carbon Capture and Storage. This technology became a matter of interest as an option to diminish greenhouse gas emissions of power plants. It is essential to find out about the costs of Carbon Capture and Storage and expected future costs of power plants with CCS. Impact of this techology is not only in the sphere of capital and operational costs, but it also influences power plant efficiency and fuel consumption in negative way. Analysis of reductions in the costs of this technology as a result of learning-by-doing is observed on Experience Curves. This study observes influence of CCS on costs of mainly PC, IGCC and NGCC type of power plant. CCS technology has positive impact not only on environment, but it is possible to assess Enhanced Oil, Methane or Gas Recovery, which can partly offset costs of this technology.

Integrated Gasification Combined Cycle (IGCC) power plants have been considered as one of the best options for energy production in an environmental friendly manner. IGCC power plants are demonstrating better results, both in terms of plant performance and economics, when compared to a Pulverised Coal (PC) power plant with CO2 capture. The additional components required for an IGCC power plant when it is desired to operate in CO2 capture mode, give research potential with respect to an improved IGCC power plant performance. The IGCC power plant design framework studied and developed was based in DOE/NETL report and is presented. The conventional and CO2 capture IGCC power plants have been benchmarked in rigorous process flow diagrams developed using the commercial software Honeywell UniSim Design R400. As an essential part of the Innovative Gas Separations for Carbon Capture project (IGSCC EPSRC – EP/G062129/1) predictive simulation tools were produced to investigate the IGCC performance. The case studies considered include different gasification options for non-capture and carbon capture IGCCs, with a two stage Selexol process for the CO2 capture cases. Particular effort has been made to produce an accurate simulation component to describe the behaviour of the syngas in the Selexol solvent. The two stage Selexol configuration was investigated in detail and novel schemes are presented. No similar approaches have been reported in the literature, in terms of the proposed configuration and the capture efficiency. Moreover, innovative CO2 capture schemes incorporating combined units of physical absorption and membranes have been examined with respect to the power plant’s performance. In this thesis, contrary to other studies, all simulations cases have been conducted in unified flow diagrams. The results presented include overall investigations and can be a helpful tool for engineers and stakeholders in the decision making process.

In recent years, Integrated Gasification Combined Cycle Technology (IGCC) has become more common in clean coal power operations with carbon capture and sequestration (CCS). Great efforts have been spent on investigating ways to improve the efficiency, reduce costs, and further reduce greenhouse gas emissions. This study focuses on investigating two approaches to achieve these goals. First, replace the subcritical Rankine steam cycle with a supercritical steam cycle. Second, add different amounts of biomass as feedstock to reduce emissions. Finally, implement several types of CCS, including sweet- and sour-shift pre-combustion and post-combustion. Using the software, Thermoflow®, this study shows that utilizing biomass with coal up to 50% (wt.) can improve the efficiency, and reduce emissions: even making the plant carbon-negative when CCS is used. CCS is best administered pre-combustion using sour-shift, and supercritical steam cycles are thermally and economically better than subcritical cycles. Both capital and electricity costs have been presented.

Certain types of fuel used for combustion in land-based gas turbines can contain traces of ash when introduced into a gas turbine. Examples include synfuel, from the gasification of coal, and heavy fuel oil. When these ash particles travel through the hot gas path of the gas turbine they can deposit on turbine vanes and blades. As deposits grow, they can reduce turbine efficiency and damage turbine hardware. As turbine inlet temperatures increase, ash deposition rates increase as well.Experiments were conducted in the Turbine Accelerated Deposition Facility (TADF) at Brigham Young University to better understand ash deposition behavior at modern turbine inlet temperatures. Experiments were conducted that varied deposition duration, gas temperature, surface temperature, ash type and characteristics, and film-cooling blowing ratio. Analysis included measuring and calculating the capture efficiency, deposit surface roughness, deposit density, and deposit surface temperature. Test results indicate that capture efficiency increases with time and as the gas temperature increases. Previous studies have shown that the capture efficiency increases with increasing surface temperature as well, but the results from this study show that at a gas temperature of 1400°C, the capture efficiency of the ash used in these tests initially increased but then began to decrease with increasing surface temperature. It was also shown that different ashes, with differing ash chemistries and densities, deposit at very different rates and produce different surface structures. The film-cooling tests showed that film cooling does reduce the capture efficiency at modern turbine temperatures, but has a smaller relative effect than at lower temperatures. Tests performed with heavy fuel oil ash and increased SO2 levels (similar to those found in heavy fuel oil combustion environments) indicate that the increased sulfur levels result in the formation of more sulfur compounds in the deposit and change which elements are dissolved by water, but has little effect on the amount of deposit that dissolves. CFD simulations were performed to model the fluid dynamics and particle trajectories in the TADF. The resulting particle impact data (particle impact velocity, temperature, diameter, etc.) were used in sticking models to evaluate the models' performance at high temperatures. Results indicate that while the models can be fit fairly well to specific data, they need to be able to better account for changing surface conditions and high temperature particle behavior to accurately model deposition at high temperatures.

Orientador: José Luz Silveira / Resumo: As maiores restrições ambientais impostas por autoridades de todo o mundo, no sentido de buscar a redução dos níveis de emissões de poluentes, bem como a crescente escassez de recursos minerais como o petróleo, impõe a alguns países a real necessidade de investir em novas tecnologias que melhor aproveitem os recursos disponíveis com menos agressão ao meio ambiente aliado a maior geração de receita. Nesse sentido a tecnologia IGCC – Integrated Gasification Combined Cycle é apresentada como uma possibilidade para atingir estes objetivos, inclusive para países como o Brasil que dispõe de grandes reservas petrolíferas e que tem a necessidade de aumentar a produção de insumos como hidrogênio, vapor e energia elétrica. Este trabalho apresenta uma breve revisão da bibliografia sobre o refino de petróleo, sobre a gaseificação dos resíduos provenientes do refino e sobre a tecnologia IGCC em seus aspectos gerais, abordando os principais componentes do sistema e como esta tecnologia pode ser utilizada em uma planta de refino. Na sequência, as aplicações da tecnologia IGCC são exemplificadas com três exemplos reais em funcionamento no mundo. A refinaria do vale do Paraíba é utilizada como estudo de caso para a implantação de uma planta IGCC, utilizando 100% do coque verde de petróleo produzido como matéria prima para a gaseificação, tendo como objetivo a produção exclusiva de energia elétrica para a geração de dividendos à refinaria. A análise termodinâmica da planta apresentou eficiênci... (Resumo completo, clicar acesso eletrônico abaixo) / Abstract: The greater environmental restrictions imposed by authorities around the world, in the sense of seeking to reduce levels of pollutant emissions, as well as the growing scarcity of mineral resources such as oil, impose on some countries the real need to invest in new technologies that best utilize available resources with less aggression to the environment combined with greater revenue generation. In this sense the Integrated Gasification Combined Cycle (IGCC) technology is presented as a possibility to achieve these objectives, including for countries such as Brazil that has large oil reserves and that has the need to increase its production of inputs such as hydrogen, steam and electricity. This paper presents a brief review of the literature on oil refining, gasification of waste from refining and IGCC technology in its general aspects, addressing the main components of the system and how this technology can be used in a refining plant. Following, the applications of the IGCC technology are exemplified with three real examples in operation in the world. The Paraíba Valley Refinery is used as a case study for the implementation of an IGCC plant, using 100% of the Petcoke produced as a raw material for gasification, with the objective of producing exclusively electric energy for generation of dividends to the refinery. The thermodynamic analysis of the plant presented net efficiency in electricity production of 41,2% with a production capacity of 260 MW. The economic analysis... (Complete abstract click electronic access below) / Mestre

Die vorliegende Arbeit befasst sich mit Untersuchungen zur Trockenentschwefelung von Brenngasen durch Partialoxidation von H2S an Herdofenkoks. Hierzu wurden Versuche in der Technikumsanlage VTE 2004 mit einem simulierten PHTW Gas durchgeführt. Es zeigte sich, dass der COS-Abbau nicht wie bisher angenommen durch die COS-Partialoxidation sondern durch die COS-Hydrolyse erfolgt. Die COS-Hydrolyse gewinnt dabei mit abnehmender Raumbelastung an Bedeutung. Der Entschwefelungsgrad erhöht sich mit steigendem Sauerstofffaktor und abnehmender Raumbelastung. Sauerstofffaktoren >4 sind aufgrund des vollständigen H2S-Umsatzes und der nicht ablaufenden COS-Partialoxidation nicht sinnvoll. Die Gewinnung des abgeschiedenen Schwefels auf dem Herdofenkoks konnte nachgewiesen werden. Abschließende Berechnungen ergaben, dass sich mit den erreichten Schwefelkonzentrationen im Reingas das Verfahren im aktuellen Entwicklungsstand für die Vorentschwefelung im IGCC-Kraftwerk eignet.

The reliable operation of Integrally Geared Centrifugal Compressors (IGCCs), used in the coal-fired power generation industry of South Africa, is essential for economic, environmental and safety considerations. However, due to the unavailability of individual stage performance curves, the ability of a compressor owner to identify underperforming stages to maintain these compressors proactively remains limited. This study addresses the stage performance prediction of an IGCC when only the compressor’s overall performance characteristic, in conjunction with the impeller diameters and tip speeds, are known. The study is limited to IGCCs used in the coal-fired power generation industry of South Africa. Based on the limited inputs, two performance modelling methods were considered for this application, namely stage stacking and 1-dimensional modelling. However, stage stacking requires known operating points on each stage performance curve from which the rest of the curve can be extrapolated while 1-dimensional models require detailed stage design information to model stage performance. This study developed a revised stage stacking procedure which in contrast to the traditional stage stacking procedure, does not require a known operating point on each stage’s performance curve, for it assesses the relative stage performance at the compressor’s surge flow rate. The relative maximum pressure ratio of each stage is acquired through the application of similarity principles while a simplified 1-dimensional impeller analysis model is used to assess relative impeller head coefficients. The modelling process was developed based on performance and design data for IGCCs obtained from a compressor manufacturer. Performance data of four IGCCs, consisting of 13 stages, were obtained, including the design data for ten impellers. Hence, the IGCCs satisfy the requirements of geometric and aerodynamic similarity, unveiling a linear relationship between the stage impeller tip speed and maximum pressure ratio. A simplified 1-dimensional performance model was used to assess relative impeller head coefficients. A verification procedure ensured the integrity of the findings of the 1-dimensional model was maintained by comparing the model results to findings obtained using commercial compressor performance modelling software. A sensitivity analysis was conducted on the 1-dimensional performance model to ascertain which input parameters could be scaled as a function of the impeller tip diameter. For the four IGCCs for which data were obtained, the stage-discharge pressure and isentropic efficiency curves were calculated using the developed model. The maximum variation between the measured and calculated pressure and isentropic efficiency curves equaled 8.20% and 10.84%, respectively. The prediction accuracy of the developed modelling procedure is similar to map-based models found in literature and is considered adequate for identifying an underperforming stage. Thus, the developed model could serve as a valuable conditioning monitoring tool for site-based compressor owners. / Dissertation (MEng)--University of Pretoria, 2019. / Mechanical and Aeronautical Engineering / MEng / Unrestricted