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Title: TOXIC SUBSTANCES FROM COAL COMBUSTION-A COMPREHENSIVE ASSESSMENT

Abstract

The Clean Air Act Amendments of 1990 identify a number of hazardous air pollutants (HAPs) as candidates for regulation. Should regulations be imposed on HAP emissions from coal-fired power plants, a sound understanding of the fundamental principles controlling the formation and partitioning of toxic species during coal combustion will be needed. With support from the National Energy Technology Laboratory (NETL), the Electric Power Research Institute, and VTT (Finland), Physical Sciences Inc. (PSI) has teamed with researchers from USGS, MIT, the University of Arizona (UA), the University of Kentucky (UK), the University of Connecticut (UC), the University of Utah (UU) and the University of North Dakota Energy and Environmental Research Center (EERC) to develop a broadly applicable emissions model useful to regulators and utility planners. The new Toxics Partitioning Engineering Model (ToPEM) will be applicable to all combustion conditions including new fuels and coal blends, low-NOx combustion systems, and new power generation plants. Development of ToPEM will be based on PSI's existing Engineering Model for Ash Formation (EMAF). The work discussed in this report covers the Phase II program. Five coals were studied (three in Phase I and two new ones in Phase II). In this work UK has used XAFSmore » and Moessbauer spectroscopies to characterize elements in project coals. For coals, the principal use was to supply direct information about certain hazardous and other key elements (iron) to complement the more complete indirect investigation of elemental modes of occurrence being carried out by colleagues at USGS. Iterative selective leaching using ammonium acetate, HCl, HF, and HNO3, used in conjunction with mineral identification/quantification, and microanalysis of individual mineral grains, has allowed USGS to delineate modes of occurrence for 44 elements. The Phase II coals show rank-dependent systematic differences in trace-element modes of occurrence. The work at UU focused on the behavior of trace metals in the combustion zone by studying vaporization from single coal particles. The coals were burned at 1700 K under a series of fuel-rich and oxygen-rich conditions. The data collected in this study will be applied to a model that accounts for the full equilibrium between carbon monoxide and carbon dioxide. The model also considers many other reactions taking place in the combustion zone, and involves the diffusion of gases into the particle and combustion products away from the particle. A comprehensive study has been conducted at UA to investigate the post-combustion partitioning of trace elements during large-scale combustion of pulverized coal combustion. For many coals, there are three distinct particle regions developed by three separate mechanisms: (1) a submicron fume, (2) a micron-sized fragmentation region, and (3) a bulk (>3 {micro}m) fly ash region. The controlling partitioning mechanisms for trace elements may be different in each of the three particle regions. A substantial majority of semi-volatile trace elements (e.g., As, Se, Sb, Cd, Zn, Pb) volatilize during combustion. The most common partitioning mechanism for semi-volatile elements is reaction with active fly ash surface sites. Experiments conducted under this program at UC focused on measuring mercury oxidation under cooling rates representative of the convective section of a coal-fired boiler to determine the extent of homogeneous mercury oxidation under these conditions. In fixed bed studies at EERC, five different test series were planned to evaluate the effects of temperature, mercury concentration, mercury species, stoichiometric ratio of combustion air, and ash source. Ash samples generated at UA and collected from full-scale power plants were evaluated. Extensive work was carried out at UK during this program to develop new methods for identification of mercury species in fly ash and sorbents. We demonstrated the usefulness of XAFS spectroscopy for the speciation of mercury captured on low-temperature sorbents from combustion flue gases and developed XAFS parameters for such analyses. We demonstrated that all mercury sorption processes appeared to involve chemisorption rather than physisorption. This work aimed to develop a model that predicts the vaporization of metals during coal combustion and to incorporate this model into the existing Engineering Model for Ash Formation (EMAF). The model is based on theoretical analysis for metal vaporization, experimental data and data correlations. The existing program, EMAF, was substantially modified to accommodate the vaporization sub-model.« less

Authors:
; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ;
Publication Date:
Research Org.:
Physical Sciences Inc
Sponsoring Org.:
USDOE
OSTI Identifier:
891188
DOE Contract Number:  
AC22-95PC95101
Resource Type:
Technical Report
Country of Publication:
United States
Language:
English
Subject:
01 COAL, LIGNITE, AND PEAT; 29 ENERGY PLANNING, POLICY AND ECONOMY; CARBON DIOXIDE; CARBON MONOXIDE; CHEMISORPTION; CLEAN AIR ACTS; COAL; COMBUSTION; COMBUSTION PRODUCTS; EVAPORATION; FLY ASH; MERCURY; MICROANALYSIS; OXIDATION; PACKED BEDS; POWER GENERATION; POWER PLANTS; SORPTION; SPECTROSCOPY; TRACE AMOUNTS

Citation Formats

C.L. Senior, F. Huggins, G.P. Huffman, N. Shah, N. Yap, J.O.L. Wendt, W. Seames, M.R. Ames, A.F. Sarofim, S. Swenson, J.S. Lighty, A. Kolker, R. Finkelman, C.A. Palmer, S.J. Mroczkowski, J.J. Helble, R. Mamani-Paco, R. Sterling, G. Dunham, and S. Miller. TOXIC SUBSTANCES FROM COAL COMBUSTION-A COMPREHENSIVE ASSESSMENT. United States: N. p., 2001. Web. doi:10.2172/891188.
C.L. Senior, F. Huggins, G.P. Huffman, N. Shah, N. Yap, J.O.L. Wendt, W. Seames, M.R. Ames, A.F. Sarofim, S. Swenson, J.S. Lighty, A. Kolker, R. Finkelman, C.A. Palmer, S.J. Mroczkowski, J.J. Helble, R. Mamani-Paco, R. Sterling, G. Dunham, & S. Miller. TOXIC SUBSTANCES FROM COAL COMBUSTION-A COMPREHENSIVE ASSESSMENT. United States. doi:10.2172/891188.
C.L. Senior, F. Huggins, G.P. Huffman, N. Shah, N. Yap, J.O.L. Wendt, W. Seames, M.R. Ames, A.F. Sarofim, S. Swenson, J.S. Lighty, A. Kolker, R. Finkelman, C.A. Palmer, S.J. Mroczkowski, J.J. Helble, R. Mamani-Paco, R. Sterling, G. Dunham, and S. Miller. Sat . "TOXIC SUBSTANCES FROM COAL COMBUSTION-A COMPREHENSIVE ASSESSMENT". United States. doi:10.2172/891188. https://www.osti.gov/servlets/purl/891188.
@article{osti_891188,
title = {TOXIC SUBSTANCES FROM COAL COMBUSTION-A COMPREHENSIVE ASSESSMENT},
author = {C.L. Senior and F. Huggins and G.P. Huffman and N. Shah and N. Yap and J.O.L. Wendt and W. Seames and M.R. Ames and A.F. Sarofim and S. Swenson and J.S. Lighty and A. Kolker and R. Finkelman and C.A. Palmer and S.J. Mroczkowski and J.J. Helble and R. Mamani-Paco and R. Sterling and G. Dunham and S. Miller},
abstractNote = {The Clean Air Act Amendments of 1990 identify a number of hazardous air pollutants (HAPs) as candidates for regulation. Should regulations be imposed on HAP emissions from coal-fired power plants, a sound understanding of the fundamental principles controlling the formation and partitioning of toxic species during coal combustion will be needed. With support from the National Energy Technology Laboratory (NETL), the Electric Power Research Institute, and VTT (Finland), Physical Sciences Inc. (PSI) has teamed with researchers from USGS, MIT, the University of Arizona (UA), the University of Kentucky (UK), the University of Connecticut (UC), the University of Utah (UU) and the University of North Dakota Energy and Environmental Research Center (EERC) to develop a broadly applicable emissions model useful to regulators and utility planners. The new Toxics Partitioning Engineering Model (ToPEM) will be applicable to all combustion conditions including new fuels and coal blends, low-NOx combustion systems, and new power generation plants. Development of ToPEM will be based on PSI's existing Engineering Model for Ash Formation (EMAF). The work discussed in this report covers the Phase II program. Five coals were studied (three in Phase I and two new ones in Phase II). In this work UK has used XAFS and Moessbauer spectroscopies to characterize elements in project coals. For coals, the principal use was to supply direct information about certain hazardous and other key elements (iron) to complement the more complete indirect investigation of elemental modes of occurrence being carried out by colleagues at USGS. Iterative selective leaching using ammonium acetate, HCl, HF, and HNO3, used in conjunction with mineral identification/quantification, and microanalysis of individual mineral grains, has allowed USGS to delineate modes of occurrence for 44 elements. The Phase II coals show rank-dependent systematic differences in trace-element modes of occurrence. The work at UU focused on the behavior of trace metals in the combustion zone by studying vaporization from single coal particles. The coals were burned at 1700 K under a series of fuel-rich and oxygen-rich conditions. The data collected in this study will be applied to a model that accounts for the full equilibrium between carbon monoxide and carbon dioxide. The model also considers many other reactions taking place in the combustion zone, and involves the diffusion of gases into the particle and combustion products away from the particle. A comprehensive study has been conducted at UA to investigate the post-combustion partitioning of trace elements during large-scale combustion of pulverized coal combustion. For many coals, there are three distinct particle regions developed by three separate mechanisms: (1) a submicron fume, (2) a micron-sized fragmentation region, and (3) a bulk (>3 {micro}m) fly ash region. The controlling partitioning mechanisms for trace elements may be different in each of the three particle regions. A substantial majority of semi-volatile trace elements (e.g., As, Se, Sb, Cd, Zn, Pb) volatilize during combustion. The most common partitioning mechanism for semi-volatile elements is reaction with active fly ash surface sites. Experiments conducted under this program at UC focused on measuring mercury oxidation under cooling rates representative of the convective section of a coal-fired boiler to determine the extent of homogeneous mercury oxidation under these conditions. In fixed bed studies at EERC, five different test series were planned to evaluate the effects of temperature, mercury concentration, mercury species, stoichiometric ratio of combustion air, and ash source. Ash samples generated at UA and collected from full-scale power plants were evaluated. Extensive work was carried out at UK during this program to develop new methods for identification of mercury species in fly ash and sorbents. We demonstrated the usefulness of XAFS spectroscopy for the speciation of mercury captured on low-temperature sorbents from combustion flue gases and developed XAFS parameters for such analyses. We demonstrated that all mercury sorption processes appeared to involve chemisorption rather than physisorption. This work aimed to develop a model that predicts the vaporization of metals during coal combustion and to incorporate this model into the existing Engineering Model for Ash Formation (EMAF). The model is based on theoretical analysis for metal vaporization, experimental data and data correlations. The existing program, EMAF, was substantially modified to accommodate the vaporization sub-model.},
doi = {10.2172/891188},
journal = {},
number = ,
volume = ,
place = {United States},
year = {2001},
month = {6}
}