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Japan`S Sunshine Project. 17.. 1992 Annual Summary of Coal

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ETDE/W-mV-^/JV^ U A R Z\ IM ’ S SUNSHINE R R O U EOT 1992 ANNUAL SUMMARY OF COAL L I QU E FACT I ON and GAS I F I CAT I ON VOLUME X VII 19 9 3 NEW SUNSHINE PROJECT PROMOTION HEADQUARTERS AGENCY OF INDUSTRIAL SCIENCE AND TECHNOLOGY MINISTRY OF INTERNATIONAL TRADE AND INDUSTRY NEW ENERGY AND INDUSTRIAL TECHNOLOGY DEVELOPMENT ORGANIZATION (NEDO) DISCLAIMER Portions of tins document may be illegible in electronic image products. Images are produced from the best available original DISCLAIMER This report was prepared as an account of work sponsored by an agency of the United States Government Neither the United States Government nor any agency thereof, nor any of their employees, make any warranty, express or implied, or assumes any legal liabili­ ty or responsibility for the accuracy, completeness, or usefulness of any information, appa­ ratus, product, or process disclosed, or represents that its use would not infringe privately owned rights. Reference herein to any specific commercial product process, or service by trade name, trademark, manufacturer, or otherwise does not necessarily constitute or imply its endorsement recommendation, or favoring by the United States Government or any agency thereof. The views and opinions of authors expressed herein do not necessar­ ily state or reflect those of the United States Government or any agency thereof. CONTENTS 1. RESEARCH AND DEVELOPMENT OF COAL LIQUEFACTION TECHNOLOGIES (1) Basic Studies on the Effects of Coal Properties on the Liquefaction of Coal and Liquefaction Process Development................ 1 (2) Studies on Catalysts for Coal Liquefaction.................. 8 (3) Basic Studies on Coal Liquefaction Reaction, Reforming and Utiliza­ tion of Liquefaction Products .......................... 17 (4) Basic Research on Initial Stage of Coal Liquefaction........... 30 (5) Studies on the Mechanism of Direct Hydrogenation Reaction and Pre­ vention of Coking.................................. 37 (6) Desso1ution Reaction of Coal by Hydrogen-Donating Aromatic Solvents and Development of Effective Catalyst ..................... 42 (7) Mechanistic Basis of the Coal Dissolution by Hydrogen Donnor Sol­ vents ;Mu1ti-Stage Coal Liquefaction for the Better Liquid Yield under Milder Conditions ............................. 49 2. RESEARCH AND DEVELOPMENT OF COAL GASIFICATION TECHNOLOGIES (1) Basic Research on Gasification Characteristics of Various Coals • ♦ • 56 (2) Fundamental Studies on Improvement of the Efficiency of Coal Gasi­ fication ................ 63 3. DEVELOPMENT OF BITUMINOUS COAL LIQUEFACTION (1) Enginieering, Construction and Operation of a 150t/d Bituminous Coal Liquefaction Pilot Plant • • . ........................... 70 (2) Supporting Research for Pilot Plant ©Research on lt/d Process Supporting Unit (PSU).............. 76 ©Evaluation of Advanced Materials by In-plant Test ........... 83 ©Study on the Synthetic Iron Sulfide Catalyst............... 90 (DA Study on Coal Liquefaction Conditions .................. 94 ©Study on Hydrogenation Catalyst for Recycled Solvent.......... 100 4. DEVELOPMENT OF BROWN COAL LIQUEFACTION (l)Research on Brown Coal Liquefaction with 50t/d Pilot Plant....... 106 ©Development of Techniques for Upgrading Coal Oil from Brown Coal and Blending the Upgraded Coal Oil with Oil Products........... 112 5. DEVELOPMENT OF COMMON BASE TECHNOLOGIES ©Development of Slurry Letdown Valves...................... 119 ©Coal Selection Studies for Chinese Coal Liquefaction........... 125 MIRTFR mgmmrmitamtmm (3) Development of Valuation on Coal Liquefaction Process ®Study on Upgrading Technology of Coal-Derived Distillates ..... 128 ©Study on Catalyst for Upgrading Technology of Coal Derived Distillates •••.••....................... • • • • 142 ©The Development of Technology for the Separation and Utilization of Heteroatomic Compounds from Coal-Derived Liquids .......... 144 (4) Study of Toxicological and Environmental Effects of Coal-derived Liquids..... • • •........................ • • * • • 151 6. DEVELOPMENT OF COAL-BASED HYDROGEN PRODUCTION TECHNOLOGY (l)Study Operation by a Pilot Plant ©Design, Construction and Operational Research of a Pilot Plant for Coal-Based Hydrogen Production...................... 156 ©Research on Cleaning and Handling of Low-Rank Coals .......... 163 (2)Research on Support for Pilot Plant ©Research on Support for Design and Operation of Pilot Plant • • • • 167 ©Development and Evaluation of Materials for Slagging Gasifiers- - - 172 7. DEVELOPMENT OF TECHNOLOGY FOR ENTRAINED FLOW COAL GASIFICATION ©Development of Entrained Flow Coal Gasification Power Generation Plant • •......................................... 178 ©Research and Development of Coal Cleaning System.............. 185 ©Coal Selection for Conversion - - - -..................... 188 ©Development of Coal Conversion Technology Data Processing System- - - 192 8. ASSESNENT OF COAL HYDROGASIFICATION ...................... 198 9. INTERNATIONAL CO-OPERATION (l)IEA Contribution...... 202 BASIC STUDIES ON THE EFFECTS OF COAL PROPERTIES ON THE LIQUEFACTION OF COAL AND LIQUEFACTION PROCESS DEVELOPMENT Yosuke Maekawa Government Industrial Development Laboratory, Hokkaido Objectives The main objective of this research is to elucidate the relationships between the chemical structure of coals and its liquefaction conditions on each raw coal. The rational scale-up of coal liquefaction reactor based on the studies using O.lt/d bench scale plant and cold model reactor is also one of the objectives in this research. Furthermore, the change of chemical structure of liquefaction products with reaction conditions is studied to establish more effi­ cient liquefaction conditions. Also, a study of coprocessing of coals and tar sand bitumens is added in this year and the study of the separation of useful components in products is also continued to enhance the efficiency of coal liquefac­ tion process. Work Program (1) Study on liquefaction characteristics of various coals (a) Retrogressive reaction in initial stage of liquefaction (b) Pretreatment of coals for liquefaction of high concen­ tration slurry (c) Improvement of the iron based catalysts (2) Liquefaction test by 0.1 t/d BSU (a) Data correction on liquefaction of different types of coal (b) Liquefaction of high concentration slurry (3) Studies on physical properties for engineering (a) Determination of gas holdup (b) Flow characteristics of slurry near the nozzle Summary (1975-1991) 1.Up to FY 1991 Since 1975 the studies on chemical structural analysis such as precise ultimate analysis, oxygen-containing func­ tional group analysis, chemical structural analysis of various coals and liquefaction products by 1,jC-NMR spectros­ copy were carried out. Also, new structural parameter, (fa*and Haru/Car) studied to understand the coal structures. The liquefaction mechanism, the relationship between coal ranks and characteristics for liquefaction were studied. The effect of pretreatment of coal such as the extent of pulverization of coal and oil agglomeration on the liquefaction reaction was also exam- 1 iron-sulfur catalyst were systematically investigated to perform coal liquefaction process. By using O.lt/d BSU, liquefaction tests of various kinds of coals and a secondary treated coal such as finely pulverized coals were also examined. Recently, coprocessing of various kinds of coals with mainly Canadian bitumens and liquefaction of oil agglomerates was tested for process performance. The O.lt/d BSU plant has already been finished to operate for about 8800 hours (Runs 43) since 1975. Also, studies on physical properties of coal derived products and data corrections for engineering under liquefaction condi­ tions were carried out. 2.For FY 1990 (1)Study on liquefaction characteristics of various coals (a)Retrogressive reaction in coal liquefaction Coal liquefaction is carried out under high pressure and high temperature to cleavage chemical bondings in coal structures. Therefore, it is easy to understand that the coal structures are degraded during the liquefaction. Howev­ er, it is also well known that more stable covalent bondings than the originals are simultaneously formed due to retro­ gressive reaction of the liquefaction. In order to lower the severity, noncovalent bondings in addition to the covalent bondings in coal structures should also be controlled. According to this, the retrogressive reaction is prevented and severity of the liquefaction conditions can be lowered. For evaluation the retrogressive reaction in coal particles, coal sample indivilly prepared to impregnate naphthalene and let it swelling with pyridine and then, liquefied with pyridine-naphthalene-tetralin mixed solvent under lOMPa initial Ng at 723K for 0 min. Objectives are to observe effect of mtermolecular cohesion against coal conversion and formation of semicoke. Table 1 shows effect Table 1 Effect of solvent on product distribution Solvent Xf s yFS-TI y-is yi None 75.8 42.1 33.7 Hexane 79.0 46.4 32.6 Pyridine 76.1 28.1 48.0 4.8 Tetralin 77.1 43.1 34.0 5.8 Naphthalene 69.2 29.7 39.5 7.3 of swelling with different solvents on product distribution. This suggests that penetration of the solvent into coal structure affects reactivity of coal. In other word, mobili­ ty of the solvent into the coal structure effects the reac­ tivity of coal, Swelling ratios of the coal by pyridine and hexane were found to be 2 and 0, respectively. It is clearly 2 suggested from Table 1 that pyridine has a role to relax the condensation cohesion and enhance the reactivity of coal.
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