Task Mercury Speciation and Capture in Scrubber Solutions. Semi-Annual Report July 1 - December 31, By Sumitra R. Ness
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1 DOEMC (DE972229) Task Merury Seiation and Cature in Srubber Solutions Semi-Annual Reort July 1 - Deember 31, 1996 By Sumitra R. Ness r* *""i m 1 h 1997 OST Work Performed Under Contrat No.: DE-FC21-93MC397 For U.S. Deartment of Energy Offie of Fossil Energy Morgantown Energy Tehnology Center P.O. Box 88 Morgantown, West Virginia "*=3" By Energy and Environmental Researh Center University of North Dakota P. O. Box 918 Grand Forks, North Dakota C O, DSBTRtBUTfON OF THIS DOCUM? IS UNEJMt& \fip T DTICQUAlITTIHSPSlCTlfi
2 DISCLAIMER Portions of this doument may be illegible in eletroni image roduts. Images are rodued from the best available original doument.
3 DISCLAIMER This reort was reared as an aount of work sonsored by an ageny of the United States Government. Neither the United States Government, nor any ageny thereof, nor any of their emloyees makes any warranty, exress or imlied, or assumes any legal liability or resonsibility for the auray, omleteness, or usefulness of any information, aaratus, rodut, or roess dislosed or reresents that its use would not infringe rivately owned rights. Referene herein to any seifi ommerial rodut, roess, or servie by trade name, trademark, manufaturer, or otherwise does not neessarily onstitute or imly its endorsement, reommendation, or favoring by the United States Government or any ageny thereof. The views and oinions of authors exressed herein do not neessarily state or reflet those of the United States Government or any ageny thereof. ACKNOWLEDGMENT This semiannual was reared with the suort of the U.S. Deartment of Energy (DOE) Federal Energy Tehnology Center, Cooerative Agreement No. DE-FC21-93MC397. However, any oinions, findings, onlusions, or reommendations exressed herein are those of the author(s) and do not neessarily reflet the views of the DOE. EERC DISCLAIMER LEGAL NOTICE This researh reort was reared by the Energy & Environmental Researh Center (EERC), an ageny of the University of North Dakota, as an aount of work sonsored by U.S. Deartment of Energy. Beause of the researh nature of the work erformed, neither the EERC nor any of its emloyees makes any warranty, exress or imlied, or assumes any legal liability or resonsibility for the auray, omleteness, or usefulness of any information, aaratus, rodut, or roess dislosed, or reresents that its use would not infringe rivately owned rights. Referene herein to any seifi ommerial rodut, roess, or servie by trade name, trademark, manufaturer, or otherwise does not neessarily onstitute or imly its endorsement or reommendation by the EERC.
4 TABLE OF CONTENTS LIST OF TABLES i 1. INTRODUCTION 1 2. OBJECTIVES 1 3. INITIAL SCOPE OF WORK 1 4. DISCUSSION 1 5. REVISED SCOPE OF WORK 2 LIST OF TABLES 1 Revised Test Matrix 3 i
5 TASK MERCURY SPECIATION AND CAPTURE IN SCRUBBER SOLUTIONS 1. INTRODUCTION Investigations into merury ontrol aross onventional srubber systems have reiitated questions onerning 1) the initial seiation between oxidized and elemental forms of merury in flue gas from oal-fired boilers and, subsequently, 2) the effets of srubber slurry omosition and H on the merury forms. Merury ature in srubber slurry is highly deendent on its form. Oxidized merury is highly water-soluble and an be removed by srubber slurry, whereas elemental merury is not and asses through the srubber to the stak. 2. OBJECTIVES The objetives of this rojet are to determine whether srubber solutions onvert either form of merury to another and whether merury ature is affeted by H. 3. INITIAL SCOPE OF WORK The merury benh-sale test unit in the Energy & Environmental Researh Center (EERC) Partiulate Researh Laboratory will be used to erform these tests. A benh-sale srubber will be onstruted to ahieve the desired liquid-to-gas ratios andor sulfur dioxide and merury removals. Major variables inlude high and low H and two of three slurry omositions (lime-based, limestone-based, and srubber solution from a loal utility). Simulated flue gas (S 2, NO x, C 2, H 2, 2, and balane Nj) siked with either or both elemental and oxidized merury from ommerially manufatured alibration tubes will be srubbed while inlet and outlet elemental merury onentrations will be measured using the on-line ontinuous emissions monitor, SemTeh. 4. DISCUSSION Simulated srubber slurry omonents and srubber slurry from a loal utility as well as laboratory equiment required for the rojet have been roured. Quantities andflowrates of the gases and merury siking have been determined. The benh-sale unit has been set u and should be oerational through the month of February Modifiations to the H maintenane system and extra heatinginsulation are still required. Benh-sale tests, whih were to roeed in August 1996, were ut on hold beause of downtime on the SemTeh merury analyzers and onversion systems whih were servied on- site over Thanksgiving The SemTeh analyzers have sine been in full use for other delayed 1
6 rojets. This rojet will now have full use of a SemTeh analyzer for the month of February Use of the on-line analyzer, suh as the SemTeh, for both elemental and oxidized merury was initially referred beause real-time hanges in merury ature ould be reorded as the srubber solution was sent. The main advantages of using the SemTeh were the ability to shake down oeration of the unit and investigate more variables for the same ost and in a shorter amount of time than with wet hemistry methods whih are time-averaged over 3-6 minutes and exensive; the rojet budget would only suort eight analyses. Other disadvantages of the wet hemistry methods were the ontinuing disute over whih methods (or whether any of the methods) adequately ature oxidized forms of merury. Therefore, it was determined that the rojet should be ostoned until issues with the SemTeh ould be adequately addressed. When the soe of work for this rojet was initially roosed, it was believed that the wet hemistry methods would be validated and the on-line analyzersonversion systems both would be suessfully oerational by the rojet start date. At this time, a revised soe of work is roosed and will be omleted by Marh 31, A disussion of the Partiulate Researh Lab's aabilities for merury siking, benh-sale studies, and the SemTeh follows. The SemTeh analyzer only measures elemental merury and uses a onversion system to onvert oxidized forms of merury to elemental merury. The oxidized fration is measured by differene between the total merury in onverted samles less the merury in unonverted samles. At this time, the SemTeh analyzer and its onversion system aear to be working within the range of instrument seifiations. However, the benh-sale meruri hloride siking system has not yet yielded reroduible results before and after a system shutdown but does yield reroduible results within a given day. It has not yet been determined if the data disreanies are beause of the meruri hloride siking system, the SemTeh onversion system, the SemTeh analyzer, or the wet hemistry methods used as baku data for the meruri hloride siking system alibrations. In ontrast, the elemental merury siking system and SemTeh analyzer results have been favorable. Sine elemental merury is redited to ass through the srubber solutions unaffeted as has been shown at the full sale, the fous is on the behavior of oxidized merury in the srubber solutions. However, there is some evidene at the full sale that oxidized merury is onverted into elemental merury aross wet srubbers. This effet is small (^1%) and, as of yet, not onfirmed. Therefore, both elemental merury and meruri hloride will not be siked in ombination beause of the ossibility of this effet. Based on the aabilities of the SemTeh analyzer and urrently favored wet hemistry methods, a revised soe of work has been determined. 5. REVISED SCOPE OF WORK Results whih have been determined by the many merury rojets at the EERC and other researh failities that affet the soe of work for this rojet are as follows: Results from wet hemistry methods are affeted by the resene of, but not quantities of (as found in tyial ombustion flue gas), HC1 and NO x and will be a onstant, not variable, omonent of the simulated flue gas. 2
7 The tris-buffer method, not EPA Method 29, is urrently favored for the most aurate merury seiation results. Meruri hloride mass balanes annot be obtained unless all surfaes line surfaes are heated to at least 25 F. Sine the srubber annot be oerated at this temerature, several modifiations are required to heat all of the srubber surfaes and omonents to at least 15 F. However, deosition of meruri hloride is still likely and may be a major obstale to obtaining definitive data from this study. A revised 2 3 test matrix has been develoed where H: - = low H and = high H Slurry:- = Lab Slurry and = Commerial Slurry Hg Seies:- = Hg and = Hg TABLE 1 Revised Test Matrix Run H Slurry Hg Seies The initial soe of work intended to use two slurries: one lime and one limestone. Sine ommerial srubber slurry inludes many oxidizing and hlorine-ontaining additives (for disinfetion, et.), it is referable to use it in lab haraterization. The revised soe of work shows one lab and one ommerial slurry. If the data warrant and enough time remains in the rojet, a seond lab slurry will be tested. The objetives for the revised soe of work are as follows: To determine if an effet in srubber slurry removal of merury is deendent uon H for both elemental merury and meruri hloride. 3
8 To determine if under the same onditions laboratory-reared slurries show the same results as ommerial slurries whih ontain antibaterial agents and other oxidizers. To determine if a detetable amount of meruri hloride is onverted to elemental merury in the srubber solution. All measurements for tests (and orresonding blanks) siked with elemental merury will be made with the SemTeh analyzer. All measurements for tests (and orresonding blanks) siked with meruri hloride will be made using the tris-buffer merury seiation method. The error of the SemTeh analyzer and onversion system is not great enough to onlusively detet a 1% onversion of meruri hloride to elemental merury, whereas the error of the tris-buffer method is aroximately equal to 1%. Therefore, it is ossible that the tris-buffer method may be able to show the resene of, but not quantitate, the onversion. Sulfur dioxide will be regulated at the inlet with mass flow ontrollers and heked at the outlet using a ortable eletrohem analyzer. The H of the slurry will be momtored with a H meter as well as litmus aer. Temeratures will be monitored throughout the system. All data will be reorded manually. The final reort for this rojet will be written in Marh
9 J:\BAY4TJQ4 FORM EIA-459E (188) U.S DEPARTMENT OF ENERGY FEDERAL ASSISTANCE MANAGEMENT SUMMARY REPORT 1. ProgramProjet Identifiation No. 2. ProgramProjet Title DE-FC21-93MC397 TASK 2. AIR QUALITY ASSESSMENT AND CONTROL 4. Name and Address Energy & Environmental Researh Center University of North Dakota PO Box 918, Grand Forks, ND (71) FY Months or Quarters Quarters 9. Cost a. Dollars Exressed In Status 1. Cost Chart Fund Soure DOE Total P Total A Variane P A P A P A P A 1st Thousands 2nd Quarter 3rd th Cum. to Date P= Planned A = Atual Total Planned Costs for ProgramProjet $2 Tot. Plan 2 b. Dollar Sale ">r\n I 8 ^ ^ \ 6 ^ ^ 4 2 ^^1 2 1st JAN FEB MAR. Cumulative Arued Costs Planned Atual Variane 2nd APR MAY JUN.' ', rd FORM APPROVED MB NO Page 1 of 2 3. Reorting Period through Program Start Date Comletion Date JUL AUG,'' SEP th OCT NOV DEC ' Major Milestone Status 2.7 Merury Cature Mehanisms on Solid Surfaes and Aerosols 2.8 Merury Seiation and Cature in Srubber Solutions 2.9 Imroved Methods for Chlorine and Flourine in Coal Units Planned Units Comlete P C C II^^^^^^^^^^^^^^^^^H IIIIH^^^^^H 12. Remarks 13, Signature of Reiient and Date V(\,_>-fj I I Signature of DOE Reviewing Reresentative and Date
10 FORM EIA-459E (18) U.S. DEPARTMENT OF ENERGY FEDERAL ASSISTANCE MANAGEMENT SUMMARY REPORT 1. ProgramProjet Identifiation No. 2. ProgramProjet Title IDE-FC21-93MC397 TASK 2. AIR QUALITY ASSESSMENT AND CONTROL 4. Name and Address Energy & Environmental Researh Center University of North Dakota Milestone ID. No. Subtask 2.7 a b d PO Box 918, Grand Forks, ND Desrition Merury Cature Mehanisms on Solids & Aerosols Task Initialization - roure sulies, determine establish test matrix Perform benh-sale exeriments Evaluate data and erform additional tests if neessary Submit draft toial reort and an artile for ubliation 3. Reorting Period FORM APPROVED OMB NO Page 2 of 2 1SHU3& through 12J2U3& 5. Program Start Date (71) Comletion Data Planned Atual Comletion Comletion Date Date Comments Subtask 2.8 a b d Subtask 2.9 a b IVet-Srubber Effets on Merury Seiation Modify merury benh-sale unit. Construt and shake down aenh-sale srubber Comlete benh-sale tests Comlete data redution and evaluation Submit draft toial reort and an artile for ubliation Imroved Methods for CI and F in Coal Evaluate ASTM roosed yrohydrolysis method Comare yrohydrolysis method to oxygen bomb ombustion method Submit draft toial reort and an artile for ubliation Delayed due to late finalization of Cooerative Agreement Projet withdrawn due to artial funding of the Cooerative Agreement
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