Source: FOREST AND WILDLIFE RES CENTER submitted to NRP
FUELS AND VALUE-ADDED PRODUCTS FROM PYROLYSIS OILS FROM DEVELOPMENT OF A UNIQUE AUGER REACTOR
Sponsoring Institution
National Institute of Food and Agriculture
Project Status
COMPLETE
Funding Source
Reporting Frequency
Annual
Accession No.
0208355
Grant No.
(N/A)
Cumulative Award Amt.
(N/A)
Proposal No.
(N/A)
Multistate No.
(N/A)
Project Start Date
Jul 1, 2006
Project End Date
Jun 30, 2010
Grant Year
(N/A)
Program Code
[(N/A)]- (N/A)
Recipient Organization
FOREST AND WILDLIFE RES CENTER
(N/A)
MISSISSIPPI STATE,MS 39762
Performing Department
DEPT OF FOREST PRODUCTS
Non Technical Summary
Pulpwood and industrial wood chip values have dropped sharply in recent years as the pulp and paper industry has contracted due to global competition. Utilization of these biomass sources is now feasible. Pyrolysis of wood biomass produces bio-oil which is suitable to produce chemicals and fuels. We have developed a laboratory scale auger pyrolysis reactor unit that produces high-quality bio-oil. However, the current reactor is very slow and the yield is lower than optimal. Modifications to the reactor to improve throughput and bio-oil yield and quality will be made in a new design. This design will automate the feed system, reduce the residence time and increase the heating rate. This new reactor will allow the MSU bio-oil research group to produce the bio-oil necessary to supply the numerous research projects currently funded and those expected to be funded in the future. We also anticipate patents on the innovative technology that we are developing.
Animal Health Component
50%
Research Effort Categories
Basic
(N/A)
Applied
50%
Developmental
50%
Classification

Knowledge Area (KA)Subject of Investigation (SOI)Field of Science (FOS)Percent
4020650200050%
4020650202050%
Goals / Objectives
The objective of this project is to develop an auger reactor demonstrating pyrolysis oil yields of greater than 65%. The goal is to improve the bio-oil quality above that attained by an ROI reactor by increasing heating rate, lowering residence time, practicing particulate filtration and by modifying other process parameters. The modifications should be such that they reduce capital required for an auger reactor below previous requirements.
Project Methods
We propose to redesign and fabricate a new auger pyrolysis reactor. The main purpose is to reduce residence time but other drawbacks to the current design will also be eliminated in the new design. Improved thermodynamic delivery of heat to the biomass feed stock will be achieved both by shortening the main pyrolysis pipe and by developing a confidential method to increase ablative and heat carrier to the heating zone. The modifications will reduce the space within which the vapors can circulate; therefore, the residence time over which both feed stock and vapors are pyrolyzed. Residence time can be reduced if the current batch feed required by the twin airlock system is replaced with a constant feed rate mechanism. This will be achieved by adding a rotary valve airlock as the feed system. A constant feed rate will be achieved with air exclusion accomplished. A rotary valve airlock will also be added to remove the char in order to exclude air introduced when char is released though the current twin airlock ahead of the char hopper.

Progress 07/01/06 to 06/30/10

Outputs
OUTPUTS: PROGRESS: 2006/01 TO 2010/12 OUTPUTS: A novel auger pyrolysis reactor design was developed and incorporated into a laboratory scale reactor that has been successfully operated for 2 years. This reactor is able to pyrolyze 360 lbs of biomass per day to produce 72 liters per day of bio-oil. Yield is 65% for pine feedstock. The bio-oil is of high quality containing only 25%, or less of water. This design has been modified to allow scale up to 10 ton per day or larger. PARTICIPANTS: Faculty scientists at the Forest Products Department at MSU were Philip Steele, Leonard Ingram, Fei Yu and E.M. Hassan. Faculty scientists campus-wide were Chuck Pittman, Chemistry; Mark Bricka, Priscilla Hill, Adrienne Minerick and Keisha Walters, Chemical Engineering; Sandun Fernando, Eugene Columbus and Radha Srinivasan, Agricultural and Biological Engineering; Arunkumar Rangaswami and Michael Parsons, Institute for Clean Energy Technology. Outside the University, we worked with George Huber, University of Massachusetts and James Dumesic, University of Wisconsin. Selected scientists were provided training in statistical and chemical analytical instruments as the needs of the project required. TARGET AUDIENCES: Target audiences are petroleum refineries, electrical generating facilities and those who heat agricultural buildings, such as greenhouses, hog and chicken houses. In addition, landowners who grow biomass in the form of agricultural and forestry biomass were targeted as entities that would provide biomass feedstocks for pyrolysis of bio-oil. During the duration of the project 61 presentations to various audiences were made to disseminate the technology resulting from this project. PARTICIPANTS: Faculty scientists, researchers and students at Mississippi State University involved in developing the auger reactor technology were P. Steele, B. Mitchell and D. Parish.Industrial cooperators include K. Moss and his staff and A. Manesh and his staff. Outside the university we worked with G. Huber, University of Massachusetts and James Dumesic, University of Wisconsin. TARGET AUDIENCES: TARGET AUDIENCES: Target audiences are petroleum refineries, electrical generating facilities and those who heat agricultural buildings, such as greenhouses, hog and chicken houses. In addition, landowners who grow biomass in the form of agricultural and forestry biomass were targeted as entities that would provide biomass feedstocks for pyrolysis of bio-oil. During the duration of the project 61 presentations to various audiences were made to disseminate the technology resulting from this project. PROJECT MODIFICATIONS: Not relevant to this project.

Impacts
IMPACT: 1/2006 to termination 12/2010 The auger reactor design developed under this project was incorporated into both laboratory scale and industrial scale versions. A patent was developed for the industrial scale version. This large-scale version was licensed to an industrial cooperator that has fabricated and is testing a 10-ton per day prototype. Cooperator plans to fabricate a commercial scale reactor of 50 tons per day by the end of 2012. The laboratory scale version was licensed to American Science and Technology to be utilized in their research into bio-oil upgrading. The MSU Lignocellulosic Boiler Fuel technology was also licensed to our industrial cooperator as the fuel to be marketed. MSU is fabricationg a 4-ton per day pilot scale system as a portion of our 4000 sq ft pilot building pyrolysis demonstration. These milestones indicate that the funding for this project has led to successful commercialization of the technology developed. This project has made a significant contribution to the commercialization of bio-oil production.

Publications

  • Badamkhand, S., P.H. Steele, L.L. Ingram, Jr., M.G. Kim. 2009. An exploratory study on the removal of acetic and formic acids from bio-oil. BioResources. 4(4):1319-1329.
  • Badamkhand, S., P.H. Steele, M.G. Kim. 2009. Use of lignin separated from bio-oil in oriented strand board binder phenol-formaldehyde resins. BioResources 4(2):789-804.
  • Badger, P., S. Badger, M. Puettmann, P.H. Steele, J.E. Cooper. 2010. Techno-economic analysis: Preliminary assessment of pyrolysis oil production costs and material energy balance associated with a transportable fast pyrolysis system. BioResources 6(1):34-47.
  • Patterson, D.W., J.I. Hartley, M.H. Pelkki, P.H. Steele. 2010. Effects of 9 months of weather exposure on slash bundles in the mid-South. Forest Products Journal 60(3):221-225.
  • Patton, R., P. Steele and F. Yu. 2010. Coal vs. charcoal-fueled diesel engines: A review. Energy Sources, Part A, 32:315-322.
  • Tripathi, M.M., E.M. Hassan, F. Yueh, J.P. Singh, P.H. Steele, L.L. Ingram, Jr. 2010. Study of the effect of ultraviolet exposure on bio-oil by laser-induced fluorescence spectroscopy. Energy and Fuels 24(11):6187-6192.
  • Yu, F., P.H. Steele, R. Ruan. 2010. Microwave pyrolysis of corn cob and characteristics of the pyrolytic chars. Energy Sources, Part A: Recovery, Utilization, and Environmental Effects 32:475-484.


Progress 01/01/09 to 12/31/09

Outputs
OUTPUTS: A mobile pyrolysis reactor of design similar to the Generation II auger reactor was developed. This reactor can be transported to biomass resource sites to produce bio-oil at distributed locations. Further research in development of a boiler fuel from esterified bio-oil was performed to refine the formula for this bio-fuel. Tests of esterified bio-oil combustion were performed in both a new boiler and an older boiler with retrofit injection system. These tests showed that combustion of esterified bio-oil as a boiler fuel is feasible. Further research on catalytic hydroprocessing of bio-oil to liquid hydrocarbons has allowed us to develop a novel catalyst that reduces both water and oxygen in hydrocracked bio-oil to zero. This breakthrough will allow these hydrocarbons to be fractionated into their gasoline, diesel and jet fuel components for immediate blending. Alternatively, the mixed hydrocarbon can be introduced in to petroleum refineries to produce standard fuels for combustion engines. PARTICIPANTS: Faculty scientists at the Forest Products Department at MSU were Philip Steele, Leonard Ingram, Fei Yu and E.M. Hassan. Faculty scientists campus-wide were Chuck Pittman, Chemistry; Mark Bricka, Priscilla Hill, Adrienne Minerick and Keisha Walters, Chemical Engineering; Sandun Fernando, Eugene Columbus and Radha Srinivasan, Agricultural and Biological Engineering; Arunkumar Rangaswami and Michael Parsons, Institute for Clean Energy Technology. Outside the University, we worked with George Huber, University of Massachusetts and James Dumesic, University of Wisconsin. Selected scientists were provided training in statistical and chemical analytical instruments as the needs of the project required. TARGET AUDIENCES: Target audiences are petroleum refineries, electrical generating facilities and those who heat agricultural buildings, such as greenhouses, hog and chicken houses. In addition, landowners who grow biomass in the form of agricultural and forestry biomass were targeted as entities that would provide biomass feedstocks for pyrolysis of bio-oil. PROJECT MODIFICATIONS: Nothing significant to report during this reporting period.

Impacts
MSU has recently entered into several MOUs and licensing agreements based on both the pyrolysis reactor and bio-oil upgrading project research. Agreements have been made with two industrial companies to employ our pyrolysis reactor design. An agreement with a company to employ our hydrotreating catalyst is being negotiated. These milestones indicate that the funding for this project has led to successful commercialization of the technology developed.

Publications

  • Hassan, E.M., P.H. Steele, L.L. Ingram Jr. 2009. Characterization of fast pyrolysis bio-oils produced from pretreated pine wood. Applied Biochemistry and Biotechnology 154:182-192.
  • Steele, P., S. Gajjela, F. Yu, E. M. Hassan, and G. Gresham. 2009. Hydrocarbon production via biomass pyrolysis and hydrodeoxygenation. In Proceedings: Clean Technology Conference & Expo 2009, May 3-7, Houston, TX, pp. 82-85.
  • Bhattacharya, P., P.H. Steele, E.B.M. Hassan, B. Mitchell, L. Ingram, C.U. Pittman Jr. 2009. Wood/plastic copyrolysis in an auger reactor: Chemical and physical analysis of the products. Fuel 88:1251-1260.
  • Steele, P.H. Yu, F. Gajjella, S. 2009. Past, present and future of pyrolytic production of bio-oil. In Proc. of the International Conference on Woody Biomass Utilization. August 4-5, 2009. Mississippi State University. Forest Products Society, Madison, WI.
  • Tripathi, M.M., E.M. Hassan, F.Y. Yueh, J.P. Singh, P.H. Steele, L.L. Ingram Jr. 2009. Reflection-absorption based near infrared spectroscopy for predicting water content in bio-oil. Sensors and Actuators B: Chemical 136(1):20-25.


Progress 07/01/07 to 06/30/08

Outputs
OUTPUTS: A Generation II pyrolysis reactor that attains bio-oil yields of 65% of dry biomass weight has been developed. Two paths to upgrading bio-oils have been developed: hydrodeoxygenation to hydrocarbons and esterification to lignocellulosic biodiesel. These upgraded fuels production methods are being refined and scaled up. PARTICIPANTS: Faculty scientists at Forest Products Department at MSU were Philip Steele, Leonard Ingram, Fei Yu and E.M. Hassan. Faculty scientists campus wide were Chuck Pittman, Chemistry; Mark Bricka, Priscilla Hill, Adrienne Minerick and Keisha Walters, Chemical Engineering; Sandun Fernando, Eugene Columbus and Radha Srinivasan, Agricultural and Biological Engineering; Arunkumar and Michael Parsons, Institute for Clean Energy. Outside the university we worked with George Huber, University of Massachusetts; James Dumesic, University of Wisconsin. Selected scientists were provided training in statistical and chemical analytical instruments as the needs of the project required. Craig Boden and Sanjeev Gajjela. TARGET AUDIENCES: Target audiences are petroleum refineries, electrical generating facilities and those who heat agricultural buildings, such as greenhouses, hog and chicken houses. In addition, landowners who grow biomass in the form of agricultural and forestry biomass were targeted as entities that would provide biomass feedstocks for pyrolysis of bio-oil. PROJECT MODIFICATIONS: Nothing significant to report during this reporting period.

Impacts
Raw bio-oil was produced in the MSU Generation II auger pyrolysis reactor. This bio-oil was upgraded by catalytic hydrotreating and hydrocracking in an autoclave under heat and pressure. The outcome of this phase of the research is a hydrocarbon that is allowing us to discuss petroleum refining of this product in combination with petroleum crude to produce a typical suite of petroleum refinery products to be used as transportation and other fuel types. Raw bio-oil was produced and upgraded via esterificaton to a space heating and boiler fuel as a replacement for No. 2 fuel oil. An electrical generating company plans tests of this product to fuel their electrical generators that currently utilize No. 6 fuel oil when natural gas supplies are in short supply.

Publications

  • Ingram, L. L., Mohan, D., Steele, P. H., Strobel, D. Mitchell, B. K., Mohammad, J., Cantrell, K. and Pittman, Jr, C. U. 2008. Pyrolysis of wood and bark in an auger reactor: Physical properties and chemical analysis of the produced bio-oils. Energy and Fuels, 22(1): 614-625
  • Mitchell, B. K., Ingram, L. L., Soria, J. A., Steele, P. H., and Strobel, D. 2008. Chemical and physical characteristics of bio-oils from pine and oak feed stocks. In: Proceedings, Woody Biomass Utilization: Challenges and Opportunities, 60th Meeting of the Forest Products Research Society, June 25-27, Newport Beach, CA. Forest Products Society, Madison, WI. 103 pp.
  • Steele, P. H., Mitchell, B. K., Cooper, J. E., and Arora, S. 2008. Bundled slash: A potential new biomass resource for fuels and chemicals. Applied Biochemistry and Biotechnology, 148 (1): 1-13.
  • Yu, F., Ruan, R., Steele, P. H. 2008. Consecutive reaction model for the pyrolysis of corn cob. Transactions of the American Society of Agricultural and Biological Engineers, 51(3): 1023-1028.
  • Shmulsky, R. and Armstrong, J. (2008). Accreditation: Elevating programs, the profession, and SWST. Wood and Fiber Science, 40(4): 481-483.
  • Bhattacharya, P., Steele, P. H., Ingram, L. L., Pittman, C. U. 2008. Development of fuel and value-added chemicals from pyrolysis of wood/waste plastic mixture. American Chemical Society, 53(1): 340-342.
  • Mohan, D., Shi, J., Nicholas, D. D., Pittman, Jr., C. U., Steele, P. H., Cooper, J. E. 2008. Fungicidal values of bio-oils and their lignin-rich fractions obtained from wood/bark fast pyrolysis. Chemosphere, 71(3): 456-465.
  • Patterson, D. W., Pelkki, M., Steele, P. H. 2008. Productivity of the John Deere slash bundler in removing in-forest residues from pine harvest sites in the mid-South: four case studies. Forest Products Journal, 58(7/8): 31-36.


Progress 01/01/07 to 12/31/07

Outputs
OUTPUTS: The initial Generation I (Gen I Reactor) auger reactor has been used as the basis for design and development of a Gen II Reactor currently being constructed. This reactor will increase the maximum processing volume from 2 kg/hr to 4 kg/hr. Higher heating rate will allow yield of 50 to 60% of bio-oil (dry weight basis) from biomass. Both reactors feature a novel system that produces bio-oil with low water content. This feature improves bio-oil stability, heat value and upgrading characteristics. Several southern forestry feed stocks have been characterized for bio-oil production: pine, white oak, sweet gum, red oak and cottonwood; agricultural feed stocks characterized include corn stover and switch grass. Harvested residue was collected by a John Deere slash bundler and cured to produce bio-oil of good quality. Yield values from this study indicate that, regardless of stand age, the yield of harvest slash is 20% of the volume of the commercial timber harvested. A method to transesterify bio-oil to a heating fuel with neutral pH, low water content and increased heating value has been developed. A demonstration project based on this technology will be demonstrated in 2008. The usual coking that occurs during hydrodeoxygenation (HDO) has been largely overcome by development of a new catalyst and HDO procedure. Wood preservative compounds were successfully developed from raw bio-oils. Methods to produce products from pyrolysis char were investigated. PARTICIPANTS: Philip Steele: Professor, Department of Forest Products, Mississippi State Mississippi; Leonard Ingram: Professor, Department of Forest Products, Mississippi State Mississippi; Dinesh Mohan: Dr. Dinesh Mohan, Scientist, Environmental Chemistry Division, Industrial Toxicology Research Centre, Mahatma Gandhi Marg, Lucknow-226001, India. David Strobel, Retired; Brian Mitchel, Research Assistant II, Department of Forest Products, Mississippi State University; Fei Yu, Post-Doctoral Research Associate, Department of Forest Products, Mississippi State University; Sanjeev Gajjala, Graduate Research Assistant, Department of Forest Products, Mississippi State University; Javeed Mohammad, Graduate Research Assistant, Department of Chemical Engineering, Mississippi State University; Kelley Cantrell, Technician, Department of Forest Products, Mississippi State University; Charles Pittman, Jr., Professor, Department of Chemistry, Mississippi State University; Moon Kim, Professor, Department of Forest Product, Mississippi State University; Sandun Fernando, Assistant Professor, Department of Agricultural and Biological Engineering, Mississippi State University. TARGET AUDIENCES: Forest products industries, farming organizations, forestry companies, timberland owners, petroleum refineries, enviromental protection agencies, forestry organizations, logging companies, heating fuel distributors. PROJECT MODIFICATIONS: Not relevant to this project.

Impacts
The development of a bio-oil transesterification method has led to funding of a precommercial demonstration project. A semi-batch reactor will produce the upgraded bio-oil that will fire a Combined Heat and Power (CHP) furnace as a portion of the CHP project demonstrating heating of commercial space. Success with development of the Gen I reactor has led to competitive funding of a project to demonstrate pyrolysis of CCA-treated wood at disaster sites. A mobile reactor will be designed, built and demonstrated. Funding for projects to explore additional bio-oil upgrading technologies has been received for projects to be completed during 2008-2009. Additional southern forestry and agricultural feed stocks will similarly be tested as feed stocks for raw bio-oils from which to produce fuels.

Publications

  • Mohan, D., C.U. Pittman, M. Bricka, F. Smith, B. Yancey, J. Mohammad, P. H. Steele, M.F. Alexandre-Franco, B. Gomez-Serrano, H. Gong. 2007. Sorption of arsenic, cadmium, and lead by chars produced from fast pyrolysis of wood and bark during bio-oil production. J. of Colloid and Interface Science. 310(2-7):57-73.


Progress 07/01/06 to 12/31/06

Outputs
A novel auger pyrolysis reactor has been designed and fabricated. Process control software modules are now being installed with reactor startup scheduled in April 2007. Following startup, and inevitable modifications, we will measure yield improvement by the improved thermodynamics of the device. An invention disclosure has been filed with with the Office of Intellectual Property of Mississippi State University to protect the innovative aspect of the design. Following startup, the reactor will be used to produce bio-oil for our funded projects. This production of bio-oil from various forestry feed stock types, its characterization, utilization of the char byproduct, and catalytic production of new fuels and chemicals from the produced bio-oils will comprise the research to be performed in the time remaining for this research project.

Impacts
The development of a novel auger reactor will reduce the capital cost of a typical pyrolysis reactor by about 50%. This will decreased the cost of bio-oil significantly. In addition, the auger design lends itself to production of mobile units that can be brought to the resource. This distributed production offers the potential for reduction of transportation costs. For pulp and paper production, tranportation costs for hauling forest biomass to a large centralized production facility, comprises a large proportion of total manufacturing cost. Distributed bio-oil production will also stimulate the creation of bio-oil production facilities in rural communities and will assist in their economic development.

Publications

  • Cooper, J. E. 2005. Radio frequency scanning technology for estimating lumber strength and locating anomalies in southern pine lumber and poles. Dissertation: Department of Forest Products, Mississippi State University. 121 p.
  • Mohan, D., C. U. Pittman and P. H. Steele. 2006. Single, binary and multi-component adsorption of copper and cadmium from aqueous solutions on Kraft lignin, a biosorbent. Journal of Coloid and Interface Science, Issue 297, p 489-504.
  • Mohan, D., C. U. Pittman and P. H. Steele. 2006. Pyrolysis of wood/biomass for bio-oil: a critical review. Energy and Fuels 20(3):848-889
  • Steele, P. H. and J. E. Cooper. 2006. Utilization of electrical impedance tomography to detect internal anomalies in southern pine logs. Pages 1802-1809 in D.O. Thompson and D.E. Chimenti, editors, Review of Quantitative Nondestructive Evaluation Vol. 25.
  • Steele, P.H., J. E. Cooper, B. Mitchell. 2006. Identifying knot wood in green and kiln-dried southern pine lumber with dielectric scanning. Five pages in Proceedings, Digital Imaging IX, and ASNT Topical Conference. Mashantucket, CT. July 24-26, 2006.