R&D Activities in Japan for Coal Derived Fuels

1. Present Status in Japan 2. Coal Derived Fuels 3. Direct Coal Liquefaction 4. Coal Gasification and the Derived Fuels 5. Other Fuels from Coal 6. CCS and the Combination with Clean Coal Technology 7. Combination with Sustainable Energy 8. Conclusions

Masaki Onozaki The Institute of Applied Energy (IAE)

Ø East Japan Earthquake attacked the broad East area of Japan including Tokyo on the eleventh of March. Gigantic tsunami as well as the earthquake caused the terrible disaster. About twenty thousands people died.

JMA Seismic Scale 7 (the strongest); Thrown by the shaking Fukushima and impossible to move at will. The Daiichi Nuclear ground is considerably distorted by large Power Plant cracks and fissures. Greater than 4 m/s² 5+; Difficult to keep standing. TOKYO Occasionally, cracks appear in the ground, and landslides take place. Note; a part of description Source; http://en.wikipedia.org/wiki/ File:Shindomap_2011-03-11_Tohoku_earthqua ke.png Copyright; 2011 IAE. All rights reserved. IASS: Sustainable Methanol, November 24, 2011 Copy Prohibited 2 1. Present Status on Energy in Japan East Japan Earthquake and Fukushima Disaster

http://koramu2.blog59.fc2.com/ blog-category-43.html

http://www.boston.com/ http:// bigpicture/2011/03/ jishin.ldblog.jp/ massive_earthquake_hits_japa archives/ n.html 51674229.html

Copyright; 2011 IAE. All rights reserved. IASS: Sustainable Methanol, November 24, 2011 Copy Prohibited 3 1. Present Status on Energy in Japan East Japan Earthquake and Fukushima Disaster Ø Fukushima Daiichi Nuclear Power plants failed in the safety shutdown. Some coal-fired power plants were shut down due to the earthquake. Ø Most coal fired power plants were restored after several months. Nuclear power plants have been gradually shut down for scheduled inspection everywhere in Japan. It is difficult that these will come up to operation, judging from the sentiment of the people.

http://www.ogj.com/content/dam/ogj/print- http://www.asahi.com/photonews/gallery/ articles/Volume%20109/August%201/ 111113fukushima_daiichi/101.html z110801OGJpho01.gif Copyright; 2011 IAE. All rights reserved. IASS: Sustainable Methanol, November 24, 2011 Copy Prohibited 4 1. Present Status on Energy in Japan East Japan Earthquake and Fukushima Disaster Ø In Eastern Japan, order on electricity use restrictions was enforced from July 1 to cope with loss of power sources. The government had set out an electricity saving target of 15% for this summer, mandated compliance by large power users. Most people tried to save electricity so that we turned up the room temperature and cut the switch as much as possible. Ø The peak electricity demand was lower than last year by 16.5% for Tokyo Electric. The summer peak demand season ended without any planned outages.

Peak Electricity Demand compared with the same weekday of 2010

Source; IEE JAPAN, Japan Energy Brief No.15, Sep., 2011 Copyright; 2011 IAE. All rights reserved. IASS: Sustainable Methanol, November 24, 2011 Copy Prohibited 5 1. Present Status on Energy in Japan Strategic Energy Plan of Japan

Ø The latest strategic energy plan of Japan Primary Energy Supply in Japan towards 2030 revised in 2010 shows the following measures to reduce CO2 emission and increase the energy self efficiency. • 14 nuclear plants will be built by 2030. • Renewable energy will be introduced by implementation of feed-in- tariff system and so on. • Maintain and enhance energy efficiency.

Source; The Strategic Energy Plan of Japan, June, 2010, METI, Japan

Power Generation in Japan

Source; The Strategic Energy Plan of Japan, June, 2010, METI, Japan

Ø The strategic energy plan will be revised by next summer after intensive discussion in senior and junior level committees on energy policy. First, balances of supply and demand will be estimated on the basis of several scenarios. Ø The main issue might be balances of nuclear power, sustainable energy, and fossil fuel towards the future under the conditions such as energy security, CO2 emission, and independent grid.

Generated electricity

Ø Japan consumes 190 million ton / year of coal and is importing coal from the world, mainly from Australia.

10.8M t/yr

Russia 8.1M t/yr Canada 14.3M t/yr 0M t/yr China USA

Others U.S.A. Russia

Indonesia Indonesia 28.5M t/yr • TechnologiesSouth Africa for easy and stable Australia transportation China South 120.1M t/yr Africa • Compatible technologies with aAustralia diverse 0M t/yr range of coal varieties Canada 2008fy Source; White paper on Energy of Japan, 2010 Copyright; 2011 IAE. All rights reserved. IASS: Sustainable Methanol, November 24, 2011 Copy Prohibited 9

2. Coal Derived Fuels Production Routes of Low-carbon Synthetic Fuels

A Utility Methane Gas Natural CNG LPG Gas Vehicles

Gasoline B LPG Vehicles

Crude MTG Gasoline Oil Vehicles Transportation FT Oil Fuel Diesel Vehicles Conversion Diesel Processes Airplane COAL Heavy Oil Marine Methanol

DME Fuel for Stationary Ethanol Biomass A; Gas Fuel Equipment B; Substitute Oil BDF C C; Oxygenated Fuel Copyright; 2011 IAE. All rights reserved. IASS: Sustainable Methanol, November 24, 2011 Copy Prohibited 10 2. Coal Derived Fuels Production Routes of Low-carbon Synthetic Fuels

Ø CO2 emission factor of coal is 1.7 times that of methane. Ø Low-carbon fuel such as methanol, DME, and methane can be produced from coal in combination with CCS.

5 Lower-carbon fuel 0

Carbon emission, g-carbon / MJ(LHV)-fuel g-carbon emission, Carbon DME

Crude Oil Gasoline Methanol Propane Methane

各種燃料の低位発熱量(LHV)当りの炭素排出係数 2. Coal Derived Fuels Developed or Developing Technologies

Ø Many clean coal technologies for fuel production have been and been being developed over the past ten years, supported by Japanese government. Ø The fuel-related technologies are shown as follows.

Drying of Lignite Reforming of Low-rank Coal Briquetting of Lignite Slurry production from Lignite

Coal Flash Partial Hydropyrolysis

Coal Gasification Circulating Fluidized Bed Gasification Underground Coal Gasification Reforming of Coke Oven Gas Utilization of Synthetic Gas Direct DME Production Substitute Natural Gas Production

Coal Liquefaction Direct Bituminous Coal Liquefaction Direct Brown Coal Liquefaction Gas To Liquid (GTL) Copyright; 2011 IAE. All rights reserved. IASS: Sustainable Methanol, November 24, 2011 Copy Prohibited 12 3. Direct Coal Liquefaction

Coal Brown Coal Up-grading Field Test Liquefaction (BCL) 50 t/d PP Brown Coal

1981 – 1990 in Australia Bituminous Coal Gasoline Liquefaction (NEDOL) Bituminous 150 t/d PP & 40 bbl/d PDU Diesel Sub-Bit. 1991 – 2001 in Japan

Source; S. Wasaka, World1996 CTL 2008,– 2000 Paris in Japan Products Copyright; 2011 IAE. All rights reserved. IASS: Sustainable Methanol, November 24, 2011 Copy Prohibited 13 3. Direct Coal Liquefaction Achievements of NEDOL Process

150 t/d Pilot Plant in Japan (1996-2000)

Kashima

Achievement - Demonstration of NEDOL process concept Oil yield of 58 wt% - Continuous operation of 1,920 hrs - High feed-slurry coal concentration of 50 wt% - Demonstration of special developed equipment Source; S. Wasaka, World CTL 2008, Paris Copyright; 2011 IAE. All rights reserved. IASS: Sustainable Methanol, November 24, 2011 Copy Prohibited 14 3. Direct Coal Liquefaction Comparison of Coal Liquefaction Processes

Country USA USA Germany China Japan Process EDS CTSL New IG NEDOL BCL Sub- Sub- Bituminou Bituminou Sub-bit. & Coal bituminou brown coal bituminous s s s Bituminous Stage of 250t/d PP 3t/d PDU 200t/d PP 6000t/d DP 150t/d PP 50t/d PP development Operation period 1977~1982 1992 1981~1987 2009~ 1996~1998 1981~1990 Liquefaction reactor Bubble Ebulｌated Bubble Bubble Bubble Bubble type column bed column column column column Catalyst Nil Iron Iron Iron Iron Reaction oC 450 450 480 450 450 Condition MPa 17 17 30 17 15 Solid / liquid Vacuum Solvent Vacuum Vacuum Solvent separation distillation deashing distillation distillation deashing Solvent / Coal ratio (by weight) 2.0 ~ 2.9 2.0 1.0 1.5 2.0 wt%,daf 55 52 ~ 74 50 ~ 58 54 ~ 62 52 ~ 64 Liquefactio bbl/t- n yield 3.6 3.8 ~ 5.0 3.4 ~ 4.2 4.0 ~ 4.7 3.8 ~ 4.8 coal Bottoms recycling Yes Yes No No Yes Source; S. Wasaka, World CTL 2008, Paris Copyright; 2011 IAE. All rights reserved. IASS: Sustainable Methanol, November 24, 2011 Copy Prohibited 15 3. Direct Coal Liquefaction Flow diagram of NEDOL Process

Coal Liquefaction Distillation Preparation Gas Atmospheric Catalyst Tower Separators Coal Naphtha

Bituminous Gas Oil & Sub-Bit. Mixer H2 Reactors Slurry Heat exchanger Letdown Heater Valve Vacuum Residue Preheater Tower Pulverizer Naphtha Separators

H2 Reactor Stripper

Preheater Recycle Solvent Hydrogenated Solvent Solvent Hydrogenated Source; S. Wasaka, World CTL 2008, ParisSolvent Hydrogenation Copyright; 2011 IAE. All rights reserved. IASS: Sustainable Methanol, November 24, 2011 Copy Prohibited 16 3. Direct Coal Liquefaction Flow diagram of NEDOL Process

Liquefaction Letdown Valves Coal Liquefaction Distillation PreparationReactors Gas Catalyst Atmospheric Tower Separators Naphtha Coal

Bituminous Gas Oil & Sub-Bit. Mixer H2

Reactors - Large press. Slurry Difference - New Material Heat - Controlled by exchanger Letdown - High-SpeedHeater slurry quenching H2 Valve flow Vacuum Residue Preheater Tower Slurry Heat Solvent PulverizerExchangers Hydrogenation Naphtha Separators

- Fuel reduced Slurry Preheating H2 Furnace Hydrogenation Catalyst Reactor - No serious Stripper indications - Ni-Mo Cat. developed of Fouling Preheater - Heavy oil converted or Scaling into Recyclehydrogen Solventdonor Hydrogenated Solvent Solvent Hydrogenated Solvent Hydrogenation solvent Source; S. Wasaka, World CTL 2008, Paris Copyright; 2011 IAE. All rights reserved. IASS: Sustainable Methanol, November 24, 2011 Copy Prohibited 17 3. Direct Coal Liquefaction Slurry Heat Exchangers and Vacuum Tower

Tested at 50t/d PP Tested at 150t/d PP Siuth Banko (Indonesia) Siuth Banko Xianfeg (China) Yallourn (Australia) Yallourn Wyoming (USA) Wyoming Adaro (Indonesia) Illinois#6 (USA) Taiheiyo (Japan) (Japan) Taiheiyo (Australia) Wandoan Yilan Yilan (China) Tanito-Harum(Indonesia) Tanito-Harum(Indonesia) Shenhua (China) (Japan) Ikeshima

Tested at 0.1t/d BSU Tested at 1t/d PSU

66 68 70 72 74 76 78 80 82 84 Carbon content (wt%, daf coal) Low rank Lignite sub-bit. Sub-bit. Low rank bit. Bit. Coal for BCL Coal for NEDOL Process Source; S. Wasaka, World CTL 2008, Paris Copyright; 2011 IAE. All rights reserved. IASS: Sustainable Methanol, November 24, 2011 Copy Prohibited 19 3. Direct Coal Liquefaction Demonstration Plant of NEDOL Process

Ø The technology of Direct Coal Liquefaction had been established through the operation of the pilot plants. Ø There are several issues to deploy the process. 1) uncertainty of future oil price, 2) huge investment, 3) properties of product oil with high aromaticity

5,000 t-coal/day

Ø There are several types of gasifiers. Ø The system is arranged due to the Ø The composition of the outlet gas and the purposes such as power generation, range of feasible coal depend on the types hydrogen production, CO+H2, of gasifiers as well as the kinds of coal. Methane, and so on.

Heat Synthetic Gas Low-rank Coal Recovery CO, H2, CO2, CH4 (CO, H2, CH4)

Coal Treatment Gas Acid Gas (Drying, CO Shift Pulverizing) Cleaning Removal

O2, Steam, H2, Air Slag H2S, CO2

Coal Gasification Processes developed by Japanese Farms Licensor/Maker Trade Name Type Mitsubishi Heavy Industries (MHI) Pressurized two stage entrained beds Hitachi, J-Power EAGLE Pressurized two stage entrained beds Nippon Steel Engineering (NSC) ECOPRO Coal Flash Partial Hydropyrolysis, `Pressurized two stage entrained beds IHI TIGAR Two stage circulating fluidized beds

Copyright; 2011 IAE. All rights reserved. IASS: Sustainable Methanol, November 24, 2011 Copy Prohibited 21 4. Coal Gasification and the Derived Fuels Synthetic Fuels XTL process Chemical FT fermentation Hydrogenation Users Feed Synthesis Synthesis stock reforming＋ Power Natural methanol・ GTL generation, Gas DME City gas

Unconventional Asphalt Desulfurization, crude oil, to liquid hydrocracking residue refinery Syn Crude Tar Sand Oil (SCO)

gasification＋ Coal methanol・ Indirect coal Direct coal DME liquefaction liquefaction Power generation, Coke Oven MTG reforming＋ CTL Steel mill Gas methanol・ DME Power BTL generation, Biomass Bio-ethanol BDF Thermal WTL ETBE supply Copyright; 2011 IAE. All rights reserved. IASS: Sustainable Methanol, November 24, 2011 Copy Prohibited 22 4. Coal Gasification and the Derived Fuels GTL

Ø Nippon GTL and JOGMEC established by the six Japanese private sectors have been developing GTL technology with a 500BPD demonstration plant. Ø The process consists of CO2 reforming of natural gas containing CO2, FT synthesis with high-efficient Co based catalyst, and hydrocracking.

http://www.chiyoda-corp.com/ technology/en/future/ co2_reforming.html

Source; Nippon GTL http://www.nippon-gtl.or.jp/pdf/ gtl_test_07.pdf#search='JOGMEC GTL 2011' Copyright; 2011 IAE. All rights reserved. IASS: Sustainable Methanol, November 24, 2011 Copy Prohibited 23 4. Coal Gasification and the Derived Fuels Reforming of Coke Oven Gas (COG)

Ø Nippon Coke & Engineering, Babcock- H2 46.58 mol % Hitachi, JCOAL, and IAE developed a non- N2 2.07 mol % catalytic reforming technology of crude coke CH4 25.28 mol % CO 5.20 mol % oven gas (COG). CO2 2.15 mol % Ø 1/10 scaled pilot tests have been carried ------out. Tar 4.68 mol % about 30 wt % Moisture 9.84 mol % Hot COG, Total 100 mol % 1050 K

Tar recovery Coke ovens Ammonium removal Benzol removal Hydrogen sulfide removal Synthetic gas

cold COG, room temp. 2 – 3 MPa Screw compressor Copyright; 2011 IAE. All rights reserved. IASS: Sustainable Methanol, November 24, 2011 Copy Prohibited 24 4. Coal Gasification and the Derived Fuels Reforming of Coke Oven Gas (COG)

Ø The synthetic gas with R=2, which is suitable with methanol production, can be obtained by adjusting operating conditions including the amount of oxygen. Ø The reforming technology doubles CO+H2 gas by use of tar in the crude COG. Note; R = ((H2) – (CO2)) / ((CO) + (CO2)) CH0.8(tar)+1/2O2→CO+0.4H2

Hot COG, 1050 K CH0.8(tar)+H2O→CO+1.4H2

Washer Coke ovens Heat exchangers Synthetic gas

Oxygen and steam 1300 - Methanol 1500 K Production 2 – 3 MPa Tar Converter slug compressor Copyright; 2011 IAE. All rights reserved. IASS: Sustainable Methanol, November 24, 2011 Copy Prohibited 25 5. Other fuels from Coal

Ø JGC Coal Fuel Process (JCF ® ) is a process for producing coal and water slurry fuel from low-rank coal and enables easier handling, like fuel oil. Slurry fuel is a mixture of powdered coal and water with a small amount of additive, which maintains a stable state. Ø A demonstration test with about 30 ton/day is currently underway in Indonesia.

Source; Web site of JGC, http://www.jgc.co.jp/en/04tech/04coal/jcf.html

Ø A low-rank coal upgrading technology (UBC ®) has been developed by Kobe Steel to enable long-distance transportation of low-rank coal. This process, an adaptation of the slurry dewatering technique in the brown coal liquefaction process, consists of 3 stages: 1) slurry preparation/dewatering, 2) solid-liquid separation/solvent recovery, and 3) briquetting. Ø A demonstration test with 600 ton/day ended in Kalimantan, Indonesia.

130-160C

100mm

Source; Web site of JGC, http://www.jgc.co.jp/en/04tech/04coal/jcf.html Copyright; 2011 IAE. All rights reserved. IASS: Sustainable Methanol, November 24, 2011 Copy Prohibited 27 6. CCS and the Combination with Clean Coal Technology

Low-carbon synthetic fuels and chemicals can be practically and economically produced, using coal gasification and CCS.

Coal Producing Countries Consuming Countries 1 Steaming Coal

CO2 Methanol Liquid Fuels Capture Ash Gasification DME 2 and Storage Low Rank SNG Coal Liquefaction LNG CO2 In Existing 3 Capture LNG Facilities and Ash Storage NH3 and Urea

Infrastructure of LNG Domestic Markets Transportation and Storage

Copyright; 2011 IAE. All rights reserved. IASS: Sustainable Methanol, November 24, 2011 Copy Prohibited 28 6. CCS and the Combination with Clean Coal Technology Total System of Zero-emission Coal-fired Power Generation

Feasibility studies of total system of near zero-emission coal-fired power generation was carried out. It includes several ways of CO2 transportation.

and recovery> Storage>

CO2 conc. : 7-40% Liquefaction Ship/Pipeline Storage

CO2 CO2

IGCC and Absorption/ Storage Pump coal-fired Separation Tank Power Plant Compressor CO2

1. IGCC and Coal-fired 3. Transportation 4. Injection and Storage Power Plant ・Transportation ・Injection 2. CO2 Recovery – Pipeline, Ship – Subsea completion – CO2: liquid, gas, hydrate – Dry completion ・Injection Facilities for – ERD Note ； a part of research ship transportation ・Storage Site Selection achievements of “NEDO 2008～2010 – Onshore Innovative Zero-emission Coal Power – Storage Potential Generation Project, Feasibility of Total – Offshore – Various factors System” 5. Evaluation; Economics, Contribution, and Standards Source; CCT Workshop, University of Tokyo, 2011 Copyright; 2011 IAE. All rights reserved. IASS: Sustainable Methanol, November 24, 2011 Copy Prohibited 29 7. Combination with Sustainable Energy Green Fuel Production Ø IAE and TIT tried to realize a green-fuel production process without CO2 emission from coal and natural gas to methanol. Ø The feasibility study showed that the cost of methanol produced in Australia might be about 35 yen/kg (0.33€/kg) after development of components.

Copyright; 2011 IAE. All rights reserved. IASS: Sustainable Methanol, November 24, 2011 Copy Prohibited 30 7. Combination with Sustainable Energy Hydrogen Production from Water with Solar Energy Professor Kodama, Niigata University, has been developing, the technology of “SINGLE PROCESSED” water splitting in a fluidized bed reactor combined with beam-down concentrating system Improved kinetics of the reaction energy efficiency can be obtained as follows: Ø Fine particles of the metal oxide work as the redox materials. Ø High temp. reaction and low temp. reaction of two-step cycle proceed simultaneously in the different positions in the reactor. Concentrated Solar Flux Ø Recuperation from annulus section to draft-tube section. Reflective Tower O2/ N2 H2

Concentrated Solar High Temp. Quartz Window 1400℃

O2/N2 1400℃ Low Temp. ℃ Heat Heat H2 Reacting 1000 Particles Draft Tube 1000 ℃ International Patent Heliostats ：PCT/JP2010/071485 Gas Inlet H2O H2O Distributor N2 H2O H2O N2 by courtesy of Professor Kodama Copyright; 2011 IAE. All rights reserved. IASS: Sustainable Methanol, November 24, 2011 Copy Prohibited 31 8. Conclusions

Ø In Japan, coal is imported from coal producing countries via long-distance transportation. The technologies required under the circumstances such as coal slurry and briquetting have been being developed. Ø Production of low-carbon fuel from higher-carbon fuel like coal will be the important field for technology development. Combination of sustainable energy as well as CCS should be considered to realize them. Ø Methanol will be one of potential future fuels in consideration of CO2 reduction and long-distance transportation.

Acknowledgement A part of work was done in financial support of New Energy and Industrial Technology Development Organization, NEDO.