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State of the Art in Black Liquor Gasification Technology

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State of the Art in Black Liquor Gasification Technology State of the Art in Black Liquor Gasification Technology Kevin Whitty Larry Baxter University of Utah Brigham Young University Salt Lake City, Utah, USA Provo, Utah, USA ABSTRACT Black liquor, a biomass-based fuel formed in the paper making process, has traditionally been burned in recovery boilers to generate energy and recover the inorganic chemicals that comprise about a third of the fuel. Gasifying black liquor offers an attractive alternative to the recovery boiler that has the potential to double the power output, reduce operational costs, improve safety and increase the yield of paper in a mill. Over the years, more than a dozen companies have tried to develop a commercially viable process for gasifying black liquor. About half these technologies have centered on low temperature gasification in fluidized beds. The rest have focused on high temperature gasification, usually in entrained flow reactors. Many of the low temperature technologies encountered problems attaining good carbon conversion (improves with increasing temperature) while avoiding bed agglomeration (worsens with increasing temperature). Condensation of "tars" has also been problematic in low temperature gasification. The high temperature technologies have suffered from problems with liquor distribution and severe corrosion by the molten smelt. Nonetheless, two companies appear to be on the brink of commercializing black liquor gasification. MTCI's fluidized bed steam gasification process has been developed to the point where MTCI now has five commercial projects under way. Chemrec has sold an atmospheric version of their high temperature entrained flow gasifier, and development of the pressurized version is entering the final pre-demonstration phase. If progress in these technologies continues, gasifiers should be a proven alternative to the recovery boiler within the next decade. INTRODUCTION Black liquor is a biomass-based fuel that is formed in the process of making paper. The chief chemical cycle for a typical pulping process is depicted in Figure 1. In the digester, wood chips are cooked in a caustic solution called white liquor (mostly sodium hydroxide) to liberate the fibers that form the pulp and eventually paper. Roughly half the mass of the wood, containing lignin and other organic material, dissolves into the solution to form black liquor. In order to make the black liquor combustible, it is concentrated from about 15% solids to about 70% solids. The composition of this "strong black liquor" is roughly 30% water, 35% inorganic chemicals and 35% organic material that was dissolved out of the wood. Black liquor is burned in a large recovery boiler, which is the single most expensive piece of equipment in the mill. The recovery boiler serves the dual purposes of producing steam and recovering the inorganic chemicals in the liquor for recycle to the process. As the liquor burns, the inorganic Black Liquor 10-15% Flue Gas Black Liquor Black Concentration Liquor Chips 70-80% Recovery Boiler Digester Smelt Pulp Causticizing White Green Water Dissolving Paper Liquor Liquor Tank Figure 1. Pulping chemical cycle chemicals collect in the bottom as molten smelt, mostly sodium carbonate. The smelt runs out of the boiler into a tank where it is dissolved in water to form "green liquor." The green liquor is causticized to form white liquor, thus completing the chemical cycle. Because the energy content in black liquor is derived from wood, it is classified as a biomass- based, renewable energy source. Global black liquor production is roughly 180 million tons annually, corresponding to an energy input of 80,000 MW. An average mill produces about 1500 tds (tons dry solids) per day, and recovery boilers with capacities as large as 3850 tds/day (corresponding to a thermal input of 600 MW) are in operation. Gasification of black liquor offers an interesting alternative to the conventional recovery boiler- based process. The primary advantage of a black liquor gasification system is that it has the potential to significantly increase electrical power production and overall thermal efficiency in the mill. The exact magnitude of the energy benefits depends on the configuration of the gasification system and pulping process. Several studies have projected improvements in energy efficiency for model mills, and have found that electricity production for a black liquor gasification combined cycle (BLGCC) system can be more than double that of a recovery boiler system without any penalty to overall thermal efficiency [1,2]. In addition to increasing power production, gasification has the potential for better environmental performance and improved safety. A final incentive for pursuing black liquor gasification is that it opens up possibilities for advanced pulping methods that could increase the quantity of pulp produced per ton of wood. Inspired by these advantages, no less than a dozen serious attempts have been made to develop a commercial black liquor gasification system. The majority of these projects have been discontinued, highlighting the fact that black liquor gasification presents very serious technical challenges. Currently, there are only two companies actively pursuing commercialization of the technology. This paper summarizes the previous attempts at developing black liquor gasification and describes the two systems currently being actively developed. These two systems define the state of the art in black liquor gasification technology today. 2 HISTORY OF BLACK LIQUOR GASIFICATION Black liquor gasification technologies can be divided into two categories based on their operating temperature. Low temperature schemes operate below the melting point of the inorganic material in the black liquor (approx. 750°C) and all have used fluidized bed reactors. High temperature schemes operate above the melting point, and a variety of reactor types have been considered. The following two sections summarize past efforts to develop low and high temperature black liquor gasification solutions. The technologies in each section are presented in approximate chronological order. Low Temperature Gasification Technologies Several companies have tried to develop low temperature processes for black liquor gasification. All of these have used fluidized bed reactors, either bubbling or circulating, and the problems that were encountered were largely the same. VTT Circulating Fluidized Bed Gasifier (1988–1992). The Technical Research Center of Finland (VTT) worked on a circulating fluidized bed gasification process in the late 1980's and early 1990's as part of the Finnish Fuel Conversion Research Program [3,4]. A 1.5 tds/day pilot unit designed to operate at pressures up to 20 bar was built in Äänekoski, Finland. The unit was operated both at atmospheric pressure and at high pressure, but encountered a number of difficulties. Agglomeration of the bed material was problematic. Changing the bed material from Na2CO3 to Al2O3 made a slight improvement. Poor conversion of the liquor was also a problem. Efforts to address this by staging the gasification were made, but were largely unsuccessful. Circulating the bed was also difficult due to the low density of the black liquor char. The program was finally abandoned in 1992 due to a lack of funds. ABB Circulating Fluidized Bed Gasifier (~1990–1997). ABB's process for black liquor gasification centered on an atmospheric air-blown circulating fluidized bed operating at roughly 700ºC [3,5]. Preheated air was both the fluidizing medium and the oxidant for gasification. ABB operated a pilot unit in Sweden for several years. Performance was reported to be good, with less than 1% unburned carbon in the solids and high sulfur reduction efficiency (>95%). The fuel gas was run through a cyclone and bag filter to remove entrained particles, and had a heating value of roughly 4 MJ/Nm3. Agglomeration of the bed did not cause severe problems. This may be due to the fact that the pilot runs were generally short, less than a day. But it also may be due to high fluidization velocities and associated attrition keeping Fuel gas agglomeration in check. ABB Cyclones discontinued development in 1997 due to lack of funding and lack of a Gas cooler clear market. Babcock & Wilcox Circulating Scrubber fluidized bed Bag house Fluidized Bed Gasifier (1989– gasifier 1998). Babcock & Wilcox's low temperature gasifier design centered on an air-blown, bubbling fluidized bed, operated either at Air atmospheric or elevated Bed pressure [6]. The system design Blower Air solids incorporated a fluidized bed preheater Black liquor combustor to preheat the air and Mix Weak wash tank Green liquor fully convert unburned bed material and tars not destroyed in the gasifier. A bench-scale system Figure 2. Fluidized bed gasifier similar to ABB process 3 was built and tested at atmospheric pressure, with bed temperatures ranging between 482–538ºC [7]. The testing proved that black liquor could be gasified in a low temperature, bubbling bed gasifier. However, serious problems associated with carbon conversion and condensation of tars were encountered, and it was concluded that unless these problems can be solved, the process will not be a viable commercial alternative. The program was discontinued in 1998. High Temperature Gasification Technologies While many companies have pursued low temperature gasification, at least as many have pursued high temperature gasification. The mix of approaches for high temperature gasification is much more varied, and the problems encountered
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