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Export Gases and Their Utilization Potential Technical and Economical Evaluation of Selected Processes for Chemical Syngas Generation

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Export Gases and Their Utilization Potential Technical and Economical Evaluation of Selected Processes for Chemical Syngas Generation Dissertation Export Gases and their Utilization Potential Technical and Economical Evaluation of selected Processes for Chemical Syngas Generation Submitted to the Institute of Process Technology and Industrial Environmental Protection Montanuniversität Leoben Author: DI Doris Wall Mat.Nb.: 9335178 Advisors: Em.O.Univ.Prof.Dipl.-Ing.Dr.mont. Werner L. Kepplinger Univ.Prof.Dipl.-Ing.Dr.tech. Johannes Schenk Leoben, 2012 AFFIDAVIT I declare in lieu of oath, that I wrote this thesis and performed the associated research myself, using only literature cited in this volume. Ich erkläre an Eides statt, dass ich diese Arbeit selbständig verfasst, andere als die angegebenen Quellen und Hilfsmittel nicht benutzt und mich auch sonst keiner unerlaubten Hilfsmittel bedient habe. i ACKNOWLEDGEMENTS For supporting me throughout this thesis I would like to give special thanks to… … my advisor Em.O.Univ. Prof. Dr. Werner Kepplinger for his professional guidance and his time for motivating and inspiring discussions. … my advisor Univ. Prof. Dr. Johannes Schenk for his expertise and his valuable input. … Siemens VAI Metals Technologies GmbH for facilitating and financial funding of this thesis project within the K1-MET program, and especially to DI Robert Millner and DI Kurt Wieder for their professional support. … Linde AG Engineering Division, especially to Dr. Johann Ferstl, DI Josef Schwarzhuber, DI Horst Weiss, DI Martin Lang, DI Robert Baumer and DI Ulrich Lahne for supporting me with expert knowledge and calculations related to export gas treatment and final purification. … BASF SE, especially to Dr. Heinrich-Josef Blankertz, DI Martin Gall and DI Alexander Weck for advices and support in literature review about syngas generation and the synthesis of chemicals. … Günther for his time and patience and for promoting me to write and finish this thesis. … Felix and Moritz for their patience and for showing me what really matters in life. … my friend Doris for her willing ear and for the motivating words. ii ABSTRACT Over the last four decades alternative smelting reduction processes for iron making have been introduced to economically compete with the classical blast furnace route. Besides process optimization to lower material and energy consumption and to cause less environmental impact, a focus has been set on an economic and environmental friendly utilization of by-products. The excess gases are typically used as fuel for heat and power plants within the iron and steel work . But due to their comparatively low calorific value, the material recycling becomes a matter of interest. For example the export gas from the alternative smelting reduction process COREX® has been recycled as reducing gas for direct reduction of iron ores and as feedstock for microbiological ethanol production. Due to the high share of CO and H2 and the low content of N2, as a result of the gasification of coal with oxygen, COREX® and FINEX® export gases are presumed to be a valuable feedstock for the synthesis of basic chemicals, but technical feasibility has not been proven yet. This thesis will provide thermo-chemical process designs for export gas utilization into specific syngases for the production of main intermediate chemicals (CO, oxo chemicals, acetic acid, methanol, Fischer-Tropsch liquids, ammonia and H2) including CO2 balance and production cost estimate for environmental and economic evaluations of the process technologies. The literature review provides an overview of conventional synthesis and syngas production technologies for the synthesis of the main intermediate chemicals, including the market potential and the production cost estimates for the standard feedstock natural gas. Based on common gas process technologies, thermo-chemical process designs (CHEMCAD) have been set up for the conversion of COREX® and FINEX® export gases into the specific syngases. For the calculations of the production costs, a model has been developed related to the cost calculation scheme for natural gas based syngas production. The CO2 balance – as a factor for environmental impact – includes process related CO2 emissions as well as CO2 emissions related to the import of electric energy, steam and heat. Economic analyses showed that export gas treatment is a feasible option to produce CO product and oxogas (H2:CO-ratio ≤1) including the downstream synthesis of acetic acid and oxo-chemicals respectively. The economic advantage is related to the high content of CO in the export gases even considering compression and export gas treatment costs. H2-rich syngas production (H2:CO-ratio ≥2) from export gas is less economic compared to syngas generated by steam reforming of natural gas. The CO2 balance showed high process related emissions for carbon monoxide shift, resulting in higher overall CO2 emissions for export gas based oxo- and syngas production ( H2:CO-ratio ≥1) compared to the feedstock natural gas. As no shift reaction is required for CO production, the bulk of CO 2 emissions result from the import of electric energy for gas compression and cryogenic separation of N2 and CO, leading to net CO2 emission savings for export gas utilization compared to natural gas based syngas production. With the substitution of the smelting reduction carrier gas N2 by recycling of CO2 from the Rectisol absorber or with polygeneration concepts combining two or more chemical syngas production processes, a reduction of the utility demand and the capital expenditures can be expected, reducing overall production costs for export gas based syngas production. iii KURZFASSUNG In den letzten vier Jahrzehnten wurden alternative Schmelzreduktionsverfahren entwickelt, die gegenüber der klassischen Hochofenroute wirtschaftliche Vorteile erzielen sollten. Neben der Prozessoptimierung zur Reduktion von Roh- und Hilfsstoffen und des Energiebedarfes wird bei diesen Verfahren zusätzlich auch auf die ökonomische und umweltfreundliche Nutzung der Nebenprodukte geachtet. Anfallende Überschussgase werden derzeit hauptsächlich als thermischer und elektrischer Energieträger im Hüttenverbund eingesetzt, jedoch wird aufgrund des relativ geringen Heizwertes die stoffliche Verwertung zunehmend interessanter. COREX® Exportgas wird beispielsweise als Direkt- reduktionsgas weiter genutzt und dient als Rohstoff für die mikrobiologische Ethanol Produktion. Aufgrund der hohen Anteile an CO und H2, und dem vergleichsweise niedrigen Gehalt an N2 – bedingt durch die Vergasung von Kohle mit reinem Sauerstoff – stellen COREX® und FINEX® Exportgase auch einen wertvollen Rohstoff zur Synthese von chemischen Grundstoffen dar. Die technische Realisierbarkeit wurde jedoch noch nicht umfassend untersucht. Im Rahmen dieser Dissertation wurden thermochemische Prozessmodelle zur Aufbereitung von Exportgasen zu speziellen Synthesegasen für die Erzeugung von Grundchemikalien (CO, Oxo- Chemikalien, Essigsäure, Methanol, Fischer-Tropsch-Treibstoffe, Ammoniak und H2) entwickelt. Im Vergleich von Produktionskosten und CO2 Bilanzen wurden die entwickelten Prozesse ökonomisch und ökologisch bewertet. Die Literaturrecherche gibt einen Überblick über konventionelle Syntheseverfahren und über die Technologien zur Erzeugung der dazu benötigten Synthesegase. Dargestellt werden das Marktpotential und eine auf Erdgas basierende Produktionskostenschätzung der Grundchemikalien und deren Synthesegase. Auf Basis herkömmlicher Synthesegas-Prozesstechnologien wurden die Prozesse zur Synthesegasaufbereitung aus COREX® und FINEX® Exportgasen thermochemisch simuliert (CHEMCAD). Das Berechnungsmodell zur Abschätzung der Produktionskosten lehnt sich an das Kalkulationsschema der auf Erdgas basierenden Synthesegasproduktion an. Die CO2-Bilanz der einzelnen Prozesse berücksichtigt neben prozessbedingten Emissionen auch CO2-Emissionen aufgrund von thermischer und elektrische Energie- und Dampfbereitstellung. Der wirtschaftliche Vergleich zwischen Exportgas und Erdgas als Synthesegasrohstoff zeigt, dass die Exportgasaufbereitung zu CO und Oxogas (H2:CO ≤1) und die nachfolgende Synthese von Essigsäure beziehungsweise Oxo-Chemikalien aufgrund des hohen CO Anteils günstiger ist als die auf Erdgas basierende Synthesegasproduktion. Die Aufbereitung zu H2-reichen Synthesegasen (H2:CO≥2) ist aufgrund des niedrigen H2:CO-Verhältnisses im Exportgas jedoch weniger wirtschaftlich. Exportgas-CO2-Bilanzen weisen hohe prozesstechnische Emissionen bedingt durch die CO-Shift auf, und resultieren in deutlich höheren Gesamtemissionen bei Oxo- und Synthesegas Erzeugung (H2:CO ≥1) im Vergleich zur Verarbeitung von reformiertem Erdgas. Da zur Erzeugung von reinem CO keine CO-Shift erforderlich ist, sind die CO2-Emissionen bei der Exportgasaufbereitung hauptsächlich energetisch bedingt (Kompression und kryogener Trennprozess) und geringer als bei der Synthesegaserzeugung aus reformiertem Erdgas. Dies führt zu einer Netto-Emissionseinsparung. Durch die Substitution von Schmelzreduktionsträgergasen mit CO2 aus der Rectisolwäsche, oder durch die Kombination der Herstellung von zwei oder mehreren Synthesegasen, kann eine Reduktion von Energie- und Hilfsmaterialien erwartet werden, die in Summe zur Senkung der Produktionskosten und zur Verringerung der CO2-Emissionen führen würde. iv ABBREVIATIONS ASU air separation unit ATR autothermal reforming CFB circulating fluidized bed COG coke oven gas CR combined reforming DR direct reduction DRI direct reduced iron HC hydrocarbons HTFT high temperature Fischer-Tropsch HTS high temperature shift ISBL inside battery limits LHV low heating
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