Towards co-production of chemicals, power and fuels in future pulp mills
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1 Jubilee Seminar in the occasion of the 90th anniversary of METLA - The Finnish Forest Research Institute Tuesday, 20 March 2007 Marina Congress Center, Helsinki Towards co-production of chemicals, power and fuels in future pulp mills Mikko Hupa and Bjarne Holmbom Åbo Akademi rocess Chemistry Centre Turku, Finland
2 Kraft ulp Mill Black liquor 15% solids Steam turbine Steam (power) rocess steam ulp Chips Digester Na 2 CO 3 Na 2 SO 4 CaCO 3 White liquor NaOH Na 2 S Black liquor concentration Lime kiln Causticizing CaO Black Liquor 75% solids Flue gas Recovery boiler Na 2 CO 3 Na 2 SO 4 Na Smelt 2 CO 3 Na 2 S Green liquor Na 2 CO 3 Na 2 S Dissolving tank Water
3 The aper Mill as a Biorefinery for roduction of Transportation Fuels Chips Hemicellulose Hemicellulose extraction Fermentation Ethanol Digester ulp Black liquor White liquor Gasification Syngas cleaning Syngas conversion Synthesis gas Hydrocarbons Methanol
4 Future ulp Mill ulp Ethanol Liquid fuels Specialty chemicals Clean power
5 Kraft ulp Mill pulping chemicals paper pulp stemwood chipping chips pulping round wood debarking black liquor forest harvesting bark pulping chemicals combustion heat & power emissions ash
6 Kraft ulp Mill & Biorefinery pulping chemicals paper pulp stemwood chipping chips pulping forest round wood harvesting debarking bark extraction knots extraction black liquor pulping chemicals combustion ---- heat & power emissions ash
7 Birch bark: betulinol and suberin Betulinol ~ 30% HO CH 2 OH Betulinol 1 4 Outer bark Inner bark Suberin ~ 30% olyester of hydroxy fatty acids Birch bark waste in Finland ~ 500,000 t/a
8 Spruce bark: stilbenes and tannins Spruce bark waste in Finland ~ 700,000 t/a Spruce bark Sequential Extraction Residue Stilbenes 5-10% Carbohydrates 10-20% Tannins 10-20%
9 Stilbenes both in bark and knots OH OH OH HO OH HO HO OH OH iceatannol Spruce bark Resveratrol Spruce bark & Red wine inosylvin ine knots
10 Kraft ulp Mill & Biorefinery pulping chemicals paper pulp stemwood chipping chips pulping forest round wood harvesting debarking bark extraction knots extraction black liquor pulping chemicals combustion ---- heat & power emissions ash
11 Lignans in icea abies % 6-24% Heartw. Sapw. 0.1 % 0.0 % 33 knots 7 trees Willför, S. et al. Holzforschung 57 (2003) % of the lignans MeO O O HO HO OH OMe Hydroxymatairesinol (HMR)
12 HMR from spruce knots MeO O O University of Turku & Åbo Akademi: Inhibits the growth of breast cancer recursor to the active metabolite enterolactone HO HO OH OMe Strong antioxidant Hormos Medical Inc., Turku US-FDA approval as dietary supplement in May : Linnea S.A., Locarno, world-wide production and marketing license
13 On the market in 2006 Recent research has shown that plant lignans have a positive influence on the development of breast, prostate and colon cancer which rely specifically on oestrogens in order to progress. Lignans also help to maintain good cardiovascular health and to moderate other oestrogendependent health problems such as menopause symptoms and osteoporosis.
14 aper mill in Northern Finland Spruce chips Farm in Southern Finland Separation of pure knots ure knot material Linnea SA, Locarno Extraction and purification HMR in capsules Dietary supplement markets
15 In other tree species other lignans! MeO HO HO O O MeO HO OH O O MeO HO OH O OMe OH OMe OH OMe OH HMR Nortrachelogenin Lariciresinol MeO HO OH OH OH OMe MeO HO OH O O OMe In many species also flavonoids and stilbenes Secoisolariciresinol Matairesinol Knots: the richest source of polyphenols in nature
16 More polyphenol products? Functional foods Cosmetics (sun creams) Technical antioxidants Natural biocides
17 Kraft ulp Mill & Biorefinery pulping chemicals paper pulp stemwood chipping chips pulping forest round wood harvesting debarking bark extraction knots extraction extraction black liquor separation pulping chemicals combustion ---- heat & power emissions ash
18 Black Liquor Recovery Boilers Daily Capacity Capacity, tds/d Maximum Delivery year
19 Flue Gas Emission Components 100 % 0 CO 2 Carbon Dioxide 1 % CO Carbon Monoxide / C x H y Hydrocarbons -5 SO 2 Sulfur Dioxide / NO x Nitrogen Oxides 1 ppm AH olyaromatic Hydrocarbons 1 ppb -10 As, Cr, Ni, V, b, Cd, Hg,... Heavy Metals Dioxins, Furans -15
20 Black Liquor Recovery Boiler Emissions SO (ppm) ~ 0 NO x (ppm) Red. S (ppm) ~ 0 articulate (mg/m 3 )
21 EU Directive on Incineration of Waste Containing Fuels Heavy Metals ( EDD ) Hg 0.05 mg/m 3 n Cd+Tl 0.05 mg/m 3 n Sb+As+Co+Cr+ Cu+b+Mn+Ni+V 0.5 mg/m 3 n
22 alkali metals alkaline earth H metals EU Heavy Metals halogens noble gases He Li Be B C N O F Ne Na Mg Al Si S Cl Ar K Ca Sc Ti V Cr Mn Fe Co Ni Cu Zn Ga Ge As Se Br Kr Rb Sr Y Zr Nb Mo Tc Ru Rh d Ag Cd In Sn Sb Te I Xe Cs Ba La Hf Ta W Re Os Ir t Au Hg Tl b Bi o At Rn Fr Ra Ac Rf Ha Sg Ns Hs Mt UunUuuUub Uuq Uuh Uuo s-block d-block transition metals p-block lanthanides Ce r Nd m Sm Eu Gd Tb Dy Ho Er Tm Yb Lu actinides Th a U Np u Am Cm Bk Cf Es Fm Md No Lr f-block transition metals
23 Typical Recovery Boiler Steam System
24 Steam Temperatures in Black Liquor Recovery Boilers Steam temperature, oc Delivery year
25 History of Steam Conditions of Coal Fired ower lants in Japan Steam temperature (C) Steam pressure ( Ma ) Steam temperature Steam pressure Tachibanawan-1 ~~ Hekinan-Unit3 ~ Isogo- New Unit C 31.0 Year of Initial Operation
26 Corrosion Test by Alkali Salts Before heat treatment After heat treatment repared for SEM
27 Steel: A Time: 168 h Corrosion due to Alkali Salts 140 Corrosion layer thickness m Salt 10 Salt 9 Salt 8 Salt 7 Salt C Salt C525 C550 C575 C600 C (Skrifvars et al. 2007)
28 Corrosion due to Alkali Salts Steel: C Time: 168 h Corrosion layer thickness μm C 500 C525 C550 C 575 C 600 C Salt 10 Salt 9 Salt 8 Salt 7 Salt 6 Salt 5 (Skrifvars et al. 2007)
29 Additional Superheating in a Separate Furnace Fired with Clean Fuels Natural gas Bark gasif. gas Methanol
30 Gasification artial oxidation of biomass into combustible gases (H 2, CO, CH 4 etc.) Burning of the gases in GT for power, or Use of the gases for synthesis of hydrocarbons etc. (F-T)
31 Kraft ulp Mill & Biorefinery pulping chemicals paper pulp stemwood chipping chips pulping forest round wood harvesting debarking bark extraction knots extraction extraction black liquor separation heat & power pulping chemicals combustion ---- gasification emissions synthesis gas ash biofuels (l) synthesis
32 Gasification 20+ different reactor concepts suggested MTCI fluidized bed steam reformer Chemrec entrained-flow gasifier
33 MTCI Black Liquor Steam Reformer (ca present) roduct Gas Black Liquor Flue Gas roduct Gas + Air ulsed Combustors Bed Solids Fluidizing Steam
34 Chemrec BLGCC rocess (ca present) Black liquor Oxygen Gas cooler S-rich gas Gas turbine Gasifier Quench Water Fuel gas Condensate Steam turbine Steam Green liquor Absorber / Stripper HRSG
35 Gasification - Challenges Complete carbon conversion Cleaning of the gases Handling of the cooking chemicals (Na, S) Reactor materials Non-process elements and emissions
36 Kraft ulp Mill & Biorefinery pulping chemicals paper pulp stemwood chipping chips pulping forest round wood harvesting debarking bark extraction knots extraction extraction black liquor separation recycling residues pulping chemicals combustion ---- gasification heat & power emissions synthesis gas ash biofuels (l) synthesis
37 Conclusions: Specialty Chemicals Complicated molecular structures developed by evolution during millions of years Not easily synthesized by chemists Truly green chemicals with Nature s Wisdom Small volumes, but healthy margins
38 Conclusions: Biorefinery Fuels and Energy Biorefinery concepts highly interesting but not yet available technology Many unresolved technical challenges Much more research needed Optimization: Ethanol vs. synthetic fuels vs. power? We should not forget longer-term, curiositydriven research!
39 Annual Ring Study - Sampling N W E Latewood Earlywood S Wood discs from 2 meters height of a ~40-year-old Norway spruce tree were used. Annual growth rings in different compass direction One annual growth ring (1994) Microtoming ranovich et al. 2006
40 Annual Growth Ring Earlywood Latewood mg/kg wood Mannans Galactans mm ranovich et al. 2006
41 Calcium Distribution within the Annual Growth Ring mg/kg wood 1994 WEST Ca EARLYWOOD LATEWOOD mm ranovich et al. 2006
42 Acknowledgements Kevin Whitty, Kari Saviharju, Nikolai DeMartini, Thomas Grace, Jim Frederick Markku Auer, Andrey ranovich, Bengt-Johan Skrifvars, Christian Mueller, Mikael Forssén, Maria Zevenhoven Åbo Akademi ChemCom Consortium: Andritz, Foster Wheeler, Kvaerner ower, Metsä-Botnia, Vattenfall, International aper Finnish Recovery Boiler Committee Academy of Finland Centre of Excellence rogram Åbo Akademi rocess Chemistry Centre Graduate School in Chemical Engineering (GSCE) Tekes
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