Evaluation of Palladium-Based Sorbents for Trace Mercury Removal in Electricity Generation

Abstract

The development of warm-gas cleanup (WGCU) systems for synthesis gas (syngas) cleanup in in- tegrated gasification combined cycle (IGCC) power plants has the potential to lower the costs of generating power. WGCU includes the removal of mercury (Hg), present in coal, from the syngas. Carbon-based sorbents used for Hg removal are not suitable for high-temperature Hg removal in conjunction with the WGCU. The US Department of Energy’s National Energy Technology Laboratory’s (DOE/NETL) Office of Research & Development (ORD) has been developing various sorbent alternatives to address the problem of high-temperature Hg removal. This study presents analysis of the capture of Hg from syngas streams as a polishing step to attain US Environmental Protection Agency (EPA) Mercury and Air Toxics Standards (MATS) requirements for Hg (0.003 lb/GWhgross for new IGCC plants) using palladium (Pd) adsorbent being tested by DOE/NETL in association with Johnson Matthey (JM). For the present study, it was assumed that syngas is already cleaned to 5 parts per billion by weight (ppbw) Hg, and the Pd sorbent technology is used as a polishing step to achieve the EPA MATS requirements (0.003 lb/GWhgross, equivalent to 2 ppbw given representative process configuration and material flows). The incremental cost of Hg polishing and the additional capital cost needed were estimated for several scenarios/cases. These cases were differentiated by variance in the following parameters, which are important because they have direct im- pacts on additional capital costs ($/kW), and in turn impacts on the levelized cost of electricity (LCOE): 1) Pd cost (varied from $4,000 to $12,000/lb Pd); 2) Gas hourly space velocity (SV) (varied from 500 to 13,500 h-1); 3) Pd loading (varied between 2 w/w% Pd and 5 w/w% Pd); 4) Sorbent make-up rate (varied between 3%, 1%). The ranges were chosen in order to reasonably reflect, in the cases that are analyzed, the actual fluctuations that have been observed in past *Corresponding author. experience in these important parameters that affect cost (e.g., the Pd cost has kept to within the $4 to 12 k/lb range in recent years). In the case of SV, the high and low points of the range are extremes beyond which costs would either be unreasonable, or increase in cost benefit would be negligible. For a typical case (i.e., using mid-range values of the parameters, including SV of 8000 h-1, 2% Pd loading, 3% make-up rate, $9500/lb Pd cost), the increase in LCOE due to the Pd-polishing system is approximately 0.4% and the additional capital cost is ~$10/kW. As a comparison, the incremental capital cost of conventional Hg removal in an IGCC plant is ~$4 to 8/kW, and the increase in the LCOE is less than 0.4%. Results indicate that in the range of SVs from 3500 h-1 to 10,000 h-1, the Hg-polishing step is expected to function adequately and with increase of LCOE limited to about 1% - 2%. The use of a Pd sorbent-based polishing system to reduce trace Hg levels to the EPA MATS requirements for new IGCC power generation appears to be feasible and reasonably cost-effective.

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Munson, C. , Indrakanti, P. , Ramezan, M. , Granite, E. and Tennant, J. (2014) Evaluation of Palladium-Based Sorbents for Trace Mercury Removal in Electricity Generation. International Journal of Clean Coal and Energy, 3, 65-76. doi: 10.4236/ijcce.2014.34007.

Conflicts of Interest

The authors declare no conflicts of interest.

References

[1] Environmental Protection Agency (2011) National Archives and Records Administration: Federal Register. 9303.
[2] Environmental Protection Agency, 40 CFR Parts 60 and 63[EPA-HQ-OAR-2009-0234; EPA-HQ-OAR-2011-0044, FRL- 9148-5]RIN 2060-AP52 (2014) National Emission Standards for Hazardous Air Pollutants from Coal- and Oil-Fired Electric Utility Steam Generating Units and Standards of Performance for Fossil-Fuel-Fired Electric Utility, Industrial- Commercial-Institutional, and Small Industrial-Commercial-Institutional Steam Generating Units. http://www.epa.gov/airquality/powerplanttoxics/pdfs/proposal.pdf
[3] Environmental Protection Agency (2012) In 40 CFR Parts 60 and 63; Federal Register. Environmental Protection Agency, Washington DC, 71323.
[4] Poulston, S., Granite, E.J., Pennline, H.W., Myers, C.R., Stanko, D.P., Hamilton, H., Rowsell, L., Smith, A.W.J., Ilkenhans, T. and Chu, W. (2007) Metal Sorbents for High Temperature Mercury Capture from Fuel Gas. Fuel, 86, 2201-2203. http://dx.doi.org/10.1016/j.fuel.2007.05.015
[5] Wendt, J.O.L. and Lee, S.J. (2010) High-Temperature Sorbents for Hg, Cd, Pb, and Other Trace Metals: Mechanisms and Applications. Fuel, 89, 894-903. http://dx.doi.org/10.1016/j.fuel.2009.01.028
[6] Granite, E.J., Pennline, H.W. and Hargis, R.A. (2000) Novel Sorbents for Mercury Removal from Flue Gas. Industrial & Engineering Chemistry Research, 39, 1020-1029. http://dx.doi.org/10.1021/ie990758v
[7] Reed, G.P., Ergüdenler, A., Grace, J.R., Watkinson, A.P., Herod, A.A., Dugwell, D. and Kandiyoti, R. (2001) Control of Gasifier Mercury Emissions in a Hot Gas Filter: The Effect of Temperature. Fuel, 80, 623-634. http://dx.doi.org/10.1016/S0016-2361(00)00148-4
[8] Wu, S.J., Uddin, Md.A. and Sasaoka, E. (2006) Characteristics of the Removal of Mercury Vapor in Coal Derived Fuel Gas over Iron Oxide Sorbents. Fuel, 85, 213-218. http://dx.doi.org/10.1016/j.fuel.2005.01.020
[9] Zhang, H., Zhao, J., Fang, Y., Huang, J. and Want, Y. (2012) Catalytic Oxidation and Stabilized Adsorption of Elemen- tal Mercury from Coal-Derived Fuel Gas. Energy & Fuels, 26, 1629-1637. http://dx.doi.org/10.1021/ef201453d
[10] McNamara, J.D. and Wagner, N.J. (1996) Process Effects on Activated Carbon Performance and Analytical Methods Used for Low Level Mercury Removal in Natural Gas Applications. Gas Separation and Purification, 10, 137-140. http://dx.doi.org/10.1016/0950-4214(96)00005-9
[11] Granite, E.J., Myers, C.R., King, W.P., Stanko, D.C. and Pennline, H.W. (2006) Sorbents for Mercury Capture from Fuel Gas with Application to Gasification Systems. Industrial & Engineering Chemistry Research, 45, 4844-4848. http://dx.doi.org/10.1021/ie060456a
[12] Poulston, S., Granite, E.J., Pennline, H.W., Hamilton, H. and Smith, A.W.J. (2011) Palladium Based Sorbents for High Temperature Arsine Removal from Fuel Gas. Fuel, 90, 3118-3121. http://dx.doi.org/10.1016/j.fuel.2011.05.012
[13] Quinn, R., Mebrahtu, T., Dahl, T.A., Lucrezi, F.A. and Toseland, B.A. (2004) The Role of Arsine in the Deactivation of Methanol Synthesis Catalysts. Applied Catalysis A: General, 264, 103-109. http://dx.doi.org/10.1016/j.apcata.2003.12.034
[14] Coade, R. and Coldham, D. (2006) The Interaction of Mercury and Aluminium in Heat Exchangers in a Natural Gas Plants. International Journal of Pressure Vessels and Piping, 83, 336-342. http://dx.doi.org/10.1016/j.ijpvp.2006.02.022
[15] Nichols, H. and Rostoker, W. (1961) On the Mechanism of Crack Initiation in Embrittlement by Liquid Metals. Acta Metallurgica, 9, 504-509. http://dx.doi.org/10.1016/0001-6160(61)90145-6
[16] Cayan, F.N., Zhi, M., Pakalapati, S.R., Celik, I., Wu, N. and Gemmen, R. (2008) Effects of Coal Syngas Impurities on Anodes of Solid Oxide Fuel Cells. Journal of Power Sources, 185, 595-602. http://dx.doi.org/10.1016/j.jpowsour.2008.06.058
[17] Baltrus, J.P., Granite, E.J., Pennline, H.W., Stanko, D., Hamilton, H., Rowsell, L., Poulston, S., Smith, A. and Chu, W. (2010) Surface Characterization of Palladium-Alumina Sorbents for High-Temperature Capture of Mercury and Arsenic from Fuel Gas. Fuel, 89, 1323-1325. http://dx.doi.org/10.1016/j.fuel.2009.09.030
[18] Cost and Performance Baseline for Fossil Energy Plants. Vol. 1, DOE/NETL-2007/1281, May 2007.
[19] Preliminary Feasibility Analysis of RTI Warm Gas Cleanup (WGCU) Technology, Nexant, June 2007. http://www.canadiancleanpowercoalition.com/files/7112/7723/6492/CCS8%20-%20090520_Nexant_RTI_Rp_Public.pdf
[20] NETL Factsheet, RECOVERY ACT: Scale-Up of High-Temperature Syngas Cleanup Technology. http://www.netl.doe.gov/publications/factsheets/project/FE0000489.pdf
[21] Granite, E.J., Pennline, H.W., Rupp, E.C., Baltrus, J.P., Stanko, D.C., Howard, B.H., Guenther, C. and Tennant, J.—NETL; Hamilton, H., Poulston, S., Rowsell, L., Chu, W. and Smith, A.—Johnson Matthey; Wu, T., Datta, S., Lambrecht, B. and Wheeldon, J.—Southern Company (2011) Palladium Sorbents for High Temperature Capture of Mercury, Arsenic, Selenium and Phosphorus from Fuel Gas. Proceedings of the West Virginia University Seminar, Morgantown, 28 October 2011.
[22] Cost and Performance Baseline for Fossil Energy Plants, Vol. 1, Bituminous Coal and Natural Gas to Electricity. DOE/NETL-2010/1397, September 2013. http://www.netl.doe.gov/File%20Library/Research/Energy%20Analysis/OE/BitBase_FinRep_Rev2a-3_20130919_1.pdf

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