Sulfur speciation and partitioning during thermochemical conversion of cellulosic biomass to biofuel
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1 Sulfur speciation and partitioning during thermochemical conversion of cellulosic biomass to biofuel Singfoong Cheah Daniel Carpenter Calvin Feik Shealyn Malone National Renewable Energy Laboratory Golden, CO, USA May 14, 2012 NREL is a national laboratory of the U.S. Department of Energy, Office of Energy Efficiency and Renewable Energy, operated by the Alliance for Sustainable Energy, LLC.
2 Outline o Biomass conversion pathways o Sulfur speciation in syngas and pyrolysis vapors o High temperature sulfur sorbent 2
3 Bioconversion Technologies Feedstocks Lignocellulosic biomass (wood, agri waste, grasses, etc.) Gasification Pyrolysis & Liquefaction Intermediates Syngas Bio-oils Catalytic syn FT or MTG HydroCracking/Tr eating Fuels Mixed alcohols Diesel* Gasoline* Sugar/starch crops (corn, sugar cane, etc.) Hydrolysis Lignin Sugars aq phase processing Diesel* Gasoline* Cat. pyrolysis Hydrogen aq phase reforming Ethanol, Fermentation Butanol, Hydrocarbons Natural oils (plants, algae) Transesterification Hydrodeoxygenation Biodiesel Green diesel * Blending Products 3
4 4 Biomass feedstock composition wood chips wheat straw switch grass component wt% lignin 28 cellulose 41 hemicellulose 25 H 2 O 5 ash 0.4 sulfur 0.03 component wt% lignin 15 cellulose 33 hemicellulose 25 H 2 O 5 ash 13 sulfur 0.09
5 5 Where does the sulfur go? Organosulfur in matrix Salt particle Discrete mineral particle Devolatilization Aqueous solution in pores Gases such as H 2 S, COS, thiophene During pyrolysis and gasification, char and ash particles are formed Syngas containing H 2 S is formed during gasification Pyrolysis vapor containing organosulfur molecules is formed during pyrolysis
6 kmol Sulfur speciation in syngas kmol Experimental data: H 2 S depends on gasifier temperature Model: no temperature dependence Model: temperature dependence if sulfur reacts with olivine or reactor wall need experimental data Experimental Data Carpenter et al ,000 H2S (g) Temp (C) Thermodynamics estimate: assume no 2 reaction inside gasifier COS (g) Temp (C) H2S (g) Fe0.877S FeS COS(g) Thermodynamics estimate: assume reaction inside gasifier 6
7 Sulfur speciation in pyrolysis vapors Experimental: 550 ppmv in bio-oil from corn stover 650 C pyrolysis--based on ultimate analysis of the oil (Carpenter 2008 tech memo) Experimental: Methyl-mercaptan, ethyl-mercaptan, thiophene, benzothiophene, dibenzothiophene (MBMS measurements Carpenter 2008 tech memo) Pyrolysis vapor composition is not equilibrium composition Predicted in model Predicted in model 7
8 8 Biochar preliminary results Motivation: To elucidate factors controlling sulfur distribution in char and syngas Potassium chloride Corn stover, pyrolysis char, 500 ºC Sulfur rich region is also enriched with potassium, but low in oxygen and carbon Further study of char from gasification will be conducted Elemental maps sulfur potassium oxygen carbon
9 catalyst activity (%) 9 Development of high temperature sulfur sorbent Measure H 2 S with sorbent and blank in space, both with actual biomass syngas and simulated syngas. Conduct experiments with sorbent upstream of reforming catalyst results show the sorbent protects the catalyst. Analyze what happen to the sorbent afterwards. Figure caption: H 2 S levels in syngas from corn stover after blank vessel and vessel containing Mn sorbent H 2 S introduction 40 MnO dry syngas MnS Time (min) No sorbent with sorbent
10 10 Importance of organosulfur species in pyrolysis vapors Catalyst deactivation Affect what catalysts and upgrading path can be used. High temperature sorbents developed for H 2 S not suitable for organosulfur Petroleum industry : o Produce H 2 S from organosulfur using hydrotreating, MoS 2 type catalyst. o Then adsorb H 2 S (low temperature process) o Discard or regenerate Biomass options o Hydrotreating o New organosulfur sorbents o Send to refinery o Need further understanding of other inorganics in pyrolysis vapors
11 11 Acknowledgments Funding provided by the Office of the Biomass Program, U.S. Department of Energy, under contract number DE- AC36-99GO10337
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