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Title: Retention of elemental mercury in fly ashes in different atmospheres

Abstract

Mercury is an extremely volatile element, which is emitted from coal combustion to the environment mostly in the vapor phase. To avoid the environmental problems that the toxic species of this element may cause, control technologies for the removal of mercury are necessary. Recent research has shown that certain fly ash materials have an affinity for mercury. Moreover, it has been observed that fly ashes may catalyze the oxidation of elemental mercury and facilitate its capture. However, the exact nature of Hg-fly ash interactions is still unknown, and mercury oxidation through fly ash needs to be investigated more thoroughly. In this work, the influence of a gas atmosphere on the retention of elemental mercury on fly ashes of different characteristics was evaluated. The retention capacity was estimated comparatively in inert and two gas atmospheres containing species present in coal gasification and coal combustion. Fly ashes produced in two pulverized coal combustion (PCC) plants, produced from coals of different rank (CTA and CTSR), and a fly ash (CTP) produced in a fluidized bed combustion (FBC) plant were used as raw materials. The mercury retention capacity of these fly ashes was compared to the retention obtained in different activated carbons. Although themore » capture of mercury is very similar in the gasification atmosphere and N{sub 2}, it is much more efficient in a coal combustion retention, being greater in fly ashes from PCC than those from FBC plants. 22 refs., 6 figs., 3 tabs.« less

Authors:
; ;  [1]
  1. Instituto Nacional del Carbon (CSIC), Oviedo (Spain)
Publication Date:
OSTI Identifier:
20862162
Resource Type:
Journal Article
Resource Relation:
Journal Name: Energy and Fuels; Journal Volume: 21; Journal Issue: 1; Other Information: rmtarazona@incar.csic.es
Country of Publication:
United States
Language:
English
Subject:
01 COAL, LIGNITE, AND PEAT; RETENTION; CAPTURE; MERCURY; FLY ASH; COAL; AIR POLLUTION CONTROL; OXIDATION; ADSORBENTS; FOSSIL-FUEL POWER PLANTS

Citation Formats

M.A. Lopez-Anton, M. Diaz-Somoano, and M.R. Martinez-Tarazona. Retention of elemental mercury in fly ashes in different atmospheres. United States: N. p., 2007. Web. doi:10.1021/ef060143s.
M.A. Lopez-Anton, M. Diaz-Somoano, & M.R. Martinez-Tarazona. Retention of elemental mercury in fly ashes in different atmospheres. United States. doi:10.1021/ef060143s.
M.A. Lopez-Anton, M. Diaz-Somoano, and M.R. Martinez-Tarazona. Mon . "Retention of elemental mercury in fly ashes in different atmospheres". United States. doi:10.1021/ef060143s.
@article{osti_20862162,
title = {Retention of elemental mercury in fly ashes in different atmospheres},
author = {M.A. Lopez-Anton and M. Diaz-Somoano and M.R. Martinez-Tarazona},
abstractNote = {Mercury is an extremely volatile element, which is emitted from coal combustion to the environment mostly in the vapor phase. To avoid the environmental problems that the toxic species of this element may cause, control technologies for the removal of mercury are necessary. Recent research has shown that certain fly ash materials have an affinity for mercury. Moreover, it has been observed that fly ashes may catalyze the oxidation of elemental mercury and facilitate its capture. However, the exact nature of Hg-fly ash interactions is still unknown, and mercury oxidation through fly ash needs to be investigated more thoroughly. In this work, the influence of a gas atmosphere on the retention of elemental mercury on fly ashes of different characteristics was evaluated. The retention capacity was estimated comparatively in inert and two gas atmospheres containing species present in coal gasification and coal combustion. Fly ashes produced in two pulverized coal combustion (PCC) plants, produced from coals of different rank (CTA and CTSR), and a fly ash (CTP) produced in a fluidized bed combustion (FBC) plant were used as raw materials. The mercury retention capacity of these fly ashes was compared to the retention obtained in different activated carbons. Although the capture of mercury is very similar in the gasification atmosphere and N{sub 2}, it is much more efficient in a coal combustion retention, being greater in fly ashes from PCC than those from FBC plants. 22 refs., 6 figs., 3 tabs.},
doi = {10.1021/ef060143s},
journal = {Energy and Fuels},
number = 1,
volume = 21,
place = {United States},
year = {Mon Jan 15 00:00:00 EST 2007},
month = {Mon Jan 15 00:00:00 EST 2007}
}
  • To study mercury (Hg) retention in solid sorbents, researchers generally employ similar laboratory-scale devices. However, despite their similarities, these devices are generally used under different experimental conditions. The Hg concentration in the gas phase, gas flow, and sorbent-bed characteristics are variables that influence the contact time, mass transfer, and kinetics and may greatly modify the quantities of Hg retained when the same sorbents are compared. These differences in the experimental conditions do not impede an evaluation of the sorbents as long as the results obtained points toward the same qualitative conclusions. However, the extent of variation needs to be definedmore » to avoid misinterpretation. To illustrate the range of interpretations, the results of a preliminary approach using four experimental devices in two laboratories have been compared in this work. All the experiments were carried out under a nitrogen atmosphere and Hg{sup 0} in the gas phase. The same sorbents were employed in all the devices. These were fly ashes obtained from the combustion of coals of different rank and with different unburned carbon contents. From the results obtained it can be inferred that it is necessary to strictly control the influence of the experimental variables to infer a correct interpretation of the results.« less
  • The objective of this study was to evaluate the effect of unburned carbon particles present in fly ashes produced by coal combustion on mercury retention. To achieve this objective, the work was divided into two parts. The aim of the first part of the study was to estimate the amount of mercury captured by the fly ashes during combustion in power stations and the relationship of this retention to the unburned carbon content. The second part was a laboratory-scale study aimed at evaluating the retention of mercury concentrations greater than those produced in power stations by fly ashes of differentmore » characteristics and by unburned carbon particles. From the results obtained it can be inferred that the unburned carbon content is not the only variable that controls mercury capture in fly ashes. The textural characteristics of these unburned particles and of other components of fly ashes also influence retention.« less
  • Nine fly ash samples were collected from the particulate collection devices of four full-scale pulverized coal utility boilers burning eastern bituminous coals and three cyclone utility boilers burning either Powder River Basin coals or PRB blends. As-received fly ash samples were mechanically sieved to obtain six size fractions. Unburned carbon content, mercury content, and Brunauer-Emmett-Teller surface areas of as-received fly ashes and their size fractions were measured. In addition, UBC particles were examined by scanning electron microscopy, high-resolution transmission microscopy, and thermogravimetry to obtain information on their surface morphology, structure, and oxidation reactivity. It was found that the UBC particlesmore » contained amorphous carbon, ribbon-shaped graphitic carbon, and highly ordered graphite structures. The mercury contents of the UBCs in raw ash samples were comparable to those of the UBC-enriched samples, indicating that mercury was mainly adsorbed on the UBC in fly ash. The UBC content decreased with a decreasing particle size range for all nine ashes. The mercury content of the UBCs in each size fraction, however, generally increased with a decreasing particle size for the nine ashes. The mercury contents and surface areas of the UBCs in the PRB-CYC ashes were about 8 and 3 times higher than UBCs in the EB-PC ashes, respectively. It appeared that both the particle size and surface area of UBC could contribute to mercury capture. The particle size of the UBC in PRB-CYC ash and thus the external mass transfer was found to be the major factor impacting the mercury adsorption. Both the particle size and surface reactivity of the UBC in EB-PC ash, which generally had a lower carbon oxidation reactivity than the PRB-PC ashes, appeared to be important for the mercury adsorption. 26 refs., 16 figs., 2 tabs.« less
  • Mercury capture by coal-combustion fly ash is a function of the amount of Hg in the feed coal, the amount of carbon in the fly ash, the type of carbon in the fly ash (including variables introduced by the rank of the feed coal), and the flue gas temperature at the point of ash collection. In their discussion of fly ash and Hg adsorption, Lu et al. (Energy Fuels 2007, 21, 2112-2120) had some fundamental flaws in their techniques, which, in turn, impact the validity of analyzed parameters. First, they used mechanical sieving to segregate fly ash size fractions. Mechanicalmore » sieving does not produce representative size fractions, particularly for the finest sizes. If the study samples were not obtained correctly, the subsequent analyses of fly ash carbon and Hg cannot accurately represent the size fractions. In the analysis of carbon forms, it is not possible to accurately determine the forms with scanning electron microscopy. The complexity of the whole particles is overlooked when just examining the outer particle surface. Examination of elements such as Hg, present in very trace quantities in most fly ashes, requires careful attention to the analytical techniques. 36 refs., 3 figs., 1 tab.« less
  • Low halogen content in tested Powder River Basin (PRB) coals and low loss of ignition content (LOI) in PRB-derived fly ash were likely responsible for higher elemental mercury content (averaging about 75%) in the flue gas and also lower mercury capture efficiency by electrostatic precipitator (ESP) and wet-FGD. To develop a cost-effective approach to mercury capture in a full-scale coal-fired utility boiler burning PRB coal, experiments were conducted adding hydrogen bromide (HBr) or simultaneously adding HBr and selected fly ashes in a slipstream reactor (0.152 x 0.152 m) under real flue gas conditions. The residence time of the flue gasmore » inside the reactor was about 1.4 s. The average temperature of the slipstream reactor was controlled at about 155{sup o}C. Tests were organized into two phases. In Phase 1, only HBr was added to the slipstream reactor, and in Phase 2, HBr and selected fly ash were added simultaneously. HBr injection was effective (>90%) for mercury oxidation at a low temperature (155{sup o}C) with an HBr addition concentration of about 4 ppm in the flue gas. Additionally, injected HBr enhanced mercury capture by PRB fly ash in the low-temperature range. The mercury capture efficiency, at testing conditions of the slipstream reactor, reached about 50% at an HBr injection concentration of 4 ppm in the flue gas. Compared to only the addition of HBr, simultaneously adding bituminous-derived fly ash in a minimum amount (30 lb/MMacf), together with HBr injection at 4 ppm, could increase mercury capture efficiency by 30%. Injection of lignite-derived fly ash at 30 lb/MMacf could achieve even higher mercury removal efficiency (an additional 35% mercury capture efficiency compared to HBR addition alone). 25 refs., 5 figs., 1 tab.« less