Air Quality and Stationary Source Emission Control (1975) / Chapter Skim
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11 Flue Gas Desulfurization
11 Flue Gas Desulfurization
Pages 385-484
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From page 385... ...
systems reliable and operable for scrubbing stack gas effluents from the combustion of high sulfur coal of the eastern United States? It is important to consider this question both in light of the recent large increase in knowledge of FGD technologies and also with sober regard to the disappointments anad failures that have contributed to the new knowledge.
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From page 386... ...
The NAE panel did its work at a time when the chemistry of sulf ur oxides scrubbing appeared f ar simpler than it does today. The panel considered 16 stack gas control procedures.
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From page 387... ...
387 onsidered to Lstrial-scale rell ~as the NAE ~peration at ;her or not ~ular unit, and this unit is aid to the panel as ocess t t~ and ;O,~ ~ local and a o v E u 1 ~a8 o o o .,, u~ ~n .
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From page 388... ...
The trend of thinking for wet scrubbing processes has been toward providing an electrostatic precipitator for removal of most of the f ly ash ahead of the scrubber, instead of relying upon the scrubber for particulate control. This is because f ly ash can interf ere with both scrubber chemistry (see section 2.
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From page 389... ...
This is not necessarily a complete list. Carbide Lime Paddy's Run (see 2.01)
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From page 390... ...
. Equivalent sOlet Electricity 2 Water Capacity Bed Loop Chiyoda (sulfuric acid- Fuel limestone double alkali)
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From page 391... ...
understanding of the mechanical and process pert ormance of the scribing hardware selected as well as I the proper materials of construction, (c} Adequate correlations; between performance of bench scale, pilot scale, and commercial scale scrubbers of the selected hardware and chemistry! and {d} - adequate numbers of chemists who share and agree upon the relevant chemical knowledge as well as adequate numbers of chemical engineers who understand the scrubbing hardware, in the employ of engineering firms Cat supply scrubbing systems.
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From page 392... ...
The remaining "low sulfur coal" delivered, containing ~ ess than 1 percent sulfur, were mostly taken by the steel industry. The discussion in Sections 2.0 and 3.0 is written on the assumption that most locations in the eastern United States are such as to require operation of a scrubber in the closed loop mode.
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From page 393... ...
0 and 3. 0 will concentrate upon (a}, availability of chemical knowledge, and (c)
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From page 394... ...
394 ~nal78i8 Of ~^-_-~" "~n~lMon8.-if =-^-~_ to form ~8ulfite 1On react With sulfur dioxide Ca O3.o.5 H o = C 2 O3 + il2O = 2 HSO3_1 2 (1)
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From page 395... ...
tends to cause additional sulfite ions to enter the~ -~ solution by reation (~ }, and the ions further react with Sulfur dioxide. Typically, about 3 percent of the entering calcium sulfite particles might be expected to dissolve as the liquor f lows through the scrubber.
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From page 396... ...
If the pH of the scrubbing liquor is too high, because 1 ime is present in excess, lime wil 1 react directly with sulfur dioxide and carbon dioxide in the f lue gas undergoing treatment to form a hard scale consisting of calcium sulfite and calcium carbonate.
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From page 397... ...
Lowering of the pa of the scrubbing liquor promotes oxidation by increasing the concentration of bisulfite ions, making more of these ions available for reaction with oxygen in Ache flue gas A greater amount of excess air, leading to higher oxygen level, is believed to promote oxidation. Presence of fly ash is known some1:i~nes to promote oxidation {see Section 2.053, and it is reaeonable to expect Oat t}`e effects nay be~greater for some ash compositions then for others.
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From page 398... ...
The Volubility of calcium sulfite is also increased, tending to promote greater efficiency of sulfur dioxide removal, but also creating a higher level of sulfite ions in the liquor, a factor tending to promote oxidation. It is probable that sodium ions would affect performance in similar ways their 1975?
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From page 399... ...
Chloride ions cause a greater drop to occur in pH of liquor flowing through the scrubber. This is apparently the result of a lowered solubility of calcium sulfite, whose dissolution is important to the capability of the liquor to absorb sulfur dioxide.
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From page 400... ...
above that a scrubber design of marginal contacting ef f iciency, that might be adequate for a liquor low in chloride ion content, may lead to trouble at a high chloride ion level, because maldistribution of gas and liquor f lows could lead to a region of excessively low pH, where the local f low of f lue gas exceeds the capability of the local f low of liquor to remove all of the sulfur dioxide in the gas. me Tennessee Valley Authority has measured hydrogen chloride content of flue gas from a wide variety of the coals that MA burns, to find that most of its coals produce a flue gas containing in the vicinity of 50 to 7 5 ppm of HC 1 tHollinden 1 97 5)
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From page 401... ...
The level to which the chloride ion concentration builds in the scrubbing liquor, before input of HC 1 balances the discharge of chloride salts, is greatest for closed loop operation. Since the quantity of water discharged in the sludge depends directly upon the quantity of sludge, the chloride ion level is inversely proportional to the sulfur content of the coal.
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From page 402... ...
5 percent sulfur. The level of Sulfur dioxide in the flue gas is about 1800 to 2000 ppm' reflecting a greater than usual degree of excess air, viz., about 80 percent excess air in contrast to the usual 20 to 30 percent.
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From page 403... ...
2. 02 Mitsui Miike Industrial Boiler A second lime scrubbing system (a Mitsui Miike Industrial boiler in Japan, di scharging combustion products roughly equivalent to a 160utility boiler)
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From page 404... ...
—2 Mild to Powl Plant 1111' 111.~ ~.
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From page 405... ...
1:J ~ Clear Water Return / Line to Plant /~ Spare Line | //,~ Slurry Line | ~ ~f, from Plant l 71 .. Dnd.B :.\ ~fore-After .
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From page 406... ...
Tests with a 1 ime high in magnesium showed better sulf ur dioxide removal. 2.04 EPA's 10-MW Pilot Lime Scrubber Operation in the unsaturated mode has been observed in EPA' s 1 0-MOO pilot scale time scrubbing system (at TVA' s Shawnee Station} for 39 2 hours with a closed water loop (Princiotta 1975~.
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From page 407... ...
The operation was effectively closed loop In respect to build-up of chloride and magnesium ion levels, which ran about 5000 ppm and 2300 ppm respectively. (The mist eliminator of this scrubber is arranged so that it can be washed with fresh water that does not combine with the primary flow of scrubbing liquor.
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From page 408... ...
Oxidation level was 5 to 7 percent; appreciate] y higher than at Paddys Runs Since both chloride arid magnesium ions tend to promos, oxidations not much can be said concerning the comparison of the oxidation levels in the 1~NW bei~,C,~ SCa.
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From page 409... ...
The higher L/G would be expected to hold down oxidation. (c} The residence time of liquor in the reaction tank was 2 minutes versus 25 minutes at Paddys Run.
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From page 410... ...
in . ~ In light of the above facts, the probability would appear to be greater than 90 percent that a lime scrubbing unit could be ordered with a reasonable prospect for reliable performance An a closed loop unsaturated mode for use In a power plant burning a medium sulfur coal (1 to percent sulfur)
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From page 411... ...
or high (beyond 3 percent} sulfur content without provision of an electrostatic precipitator. Fly ash has been convincingly demonstrated to promote oxidation in the 1-MOO Colbert Station scrubber.
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From page 412... ...
2.10 Conclusion ~~ Respect to Adequacy of Performance comparisons The comparisons between bench scale scrubbers at 0.1-MN and 1 MW, the pilot scale scrubber at 10-MW, and Paddys Run are insufficiently exact to provide a basis for confident design, even if the chemical knowledge base were adequate. Table 11-3 summarizes performance comparisons for scrubbers treating f lue gas from coal combustion.
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From page 413... ...
. ~ Wr,~ benisons Ply ~ iatS In Or in TABLE 11-3 Comparisons among Bench, Pilot, and Corrunercial Lime Scrubbers Operating in Closed Loop, Unsaturated Mode on Flue Gas from Coal-Fired Boilers , ...
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From page 414... ...
Such experiments could include studies of effects of carbide lime and addition of fly ash (preferably by taking gas from a coal-fired power station ahead of a precipitator)
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From page 415... ...
`5~ consideration mi. gthhtstpeikging of f lue gas ash from o her with HC, and,°r f Y h tests should bear in mind that the L/G at Paddys Bun are markedly lower than the L/G ' s of the bench scale scrubbers, and it might be f ound necessary to increase the L/G at Paddys Run, if this should be possible.
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From page 416... ...
03} will operate in any event consideration might be given to a study looking toward its revision for an attempt to operate in the closed loop unsaturated or borderline mode. The revision ought to bring pa under firm controls to separate the main scriber loop from loops serving venturi scrubbers whose job is to remove fly ash, and no doubt to effect other improvements as well.
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From page 417... ...
Advocates of the horizontal scrubber also feel that it could operate well into the supersaturated mode without trouble from deposits. 2.13 open versus Closed Water Loop As noted earlier, the point of view here has been that substantially all locations an the eastern United States where a lime scrubber might be situated are such as to require operation of the scrubber in the closed loop mode.
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From page 418... ...
The Fulham Station scrubber in England {see 3.01 below} is reported to have operated with lime in a supersaturated mode in the late 1930s. Operators of EPA's 10-M lime scrubber believe their work to have demonstrated a viable practice in a supersaturated mode, although the operation was marred by trouble at the mist eliminator and has not yet simulated load variations.
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From page 419... ...
Although the volubility of calcium carbonate in water is small -- indeed, far smaller than the volubility of calcium sulfite, which provides alkalinity to the lime scrubber -- nevertheless, the liquor is unsaturated in respect to this species. As the calcium carbonate enters solution, carbonate ions react with sulfur dioxide to form bisulfite ions and to release carbon dioxide gas: CaCO3 = ca+2 + CON —2 (1?
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From page 420... ...
Oxidation of sulfite to sulfate is inherently a more serious problem for ~ closed loop limestone scrubber than for the lime system. This is because the pH in the limestone system is buffered by presence of limestone at a pH in the vicinity of 5.
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From page 421... ...
3. O ~ Fulham Station Full scale limestone scrubbers began to be used in England in ~ 933 ~ and experience was acquired there for both open and closed loop operation.
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From page 422... ...
As a result of pilot tests in the closed loop mode, developers of the Fulham Station system provided higher rate of flow of scrubbing liquor relative to flow of flue gas (higher L/G) and a larger burden of circulating limestone than the levels of these variables that have been used in commercial limestone scrubbers built recently in the United States.
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From page 423... ...
and ~N ~ibmtehte Without 423 velocity, lower solids burden, and shorter reaction tank residence time than the Fulham Station design that was reported to be successful in closed loop operation (see 3.
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From page 424... ...
Alternation of the system to approximate the Fulham station experience would be costly, if not infeasible. 3.04 EPA's 10-M Pilot Limestone Scrubber The operators of EPA's 10-M pilot limestone scrubbing system (at TVA's Shawnee Station} have developed a mode of operation on flue gas high in sulfur dioxide and HC1 in the closed loop mode.
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From page 425... ...
Attempts to operate the EPA pilot unit in the unsaturated, closed loop mode have f ailed to date ~ but the failure may be explained by the long liquor residence time in the reaction tank of the pilot scrubber. 3.05 EPA's 0.1-M Bench Limestone Scrubber EPA's 0.1-M oil-fired bench scale limestone scrubbing system {300 ft3,min)
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From page 426... ...
The scrubbing liquor was supersaturated in respect to calcium sulfate and low in chloride ion. The plant' s operators are aware of the possibility of operating in an unsaturated mode, and the unit normally operates successfully in this mode as a lime scrubber.
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From page 427... ...
~ {~} he Fu~ham Station mode, tested at 10 ~ulations in ~ Mw :hat may be i. (2} The Widows Creek mode, projected for Ben made ~ TVA' s Widows Creek Station and He mist ~ demonstrated at 1-Mw ~ulating ~ (3} The unsaturated mode with high p for the f: magnesium ion level, observed at 0.1-Mw t eliminator ~ essful until ~ It would appear that the earliest comparison ich a ~ of bench scale and commercial perf ormance will carbonate !
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From page 428... ...
13, the point Of view here has been that substantial ly all locations in the Eastern United States would require operation of a limestone scrubber in the closed loop mode. open loop systems have come onstream in Japan recently, or are about to come onstream, fox coal-fired boilers, the objective being to produce gypsum for wallboard manufacture.
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From page 429... ...
. Production Rate, 103 Tons/Year Wet, Separate Collection Wet, Common Collection Dry and Disposal and Disposal Scrubber Sludge 381 Coal Ash 338 719 763 - 50% Solids 763 1 422 - 80% Solids 676 1185 1439 J 50% Solids The EPA has also estimated the land requirements at 377 acres for sludge and fly ash disposal and 108 acres for fly ash disposal only.
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From page 430... ...
(a} The sludges typically contain calcium sulfite, calcium sulfate, calcium carbonate and f ly ash in varying compositions. Fly ashes typically contain silica, alumina and hematite.
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From page 431... ...
:y were ~f wet (50 [ualitative I fly ash. calcium .cium ring ~cally ~ematite.
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From page 432... ...
Each of the three companies have different additives but they are basically intended for the same purpose. Costs of chemical fixation are reported to be S 1 S/ton on a dry solids basis {50 percent solids stream to be treated}.
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From page 433... ...
and 0.15 f ixation rioration applied will ~lined ~n ~ceived a of f ixed As is utilities , but there ished ter runoff rcial nd Will g leachate loped by ,d IUCS}. In .sing the .
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From page 434... ...
will be at the limestone scrubber installation at Mohave Unit No. 1, where IU Conversion Systems will convert the sludge into a building material.
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From page 435... ...
Roughly 5 to 10 percent of the incoming sulfur {sulfur dioxide} is oxidized to sulf ate and may be discharged as sodium sulfate {dissolved in water) , or as dry sodium sulfate.
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From page 436... ...
Ges flow ~ 474,000 SCFM inlet / 584,000 SCFM outlet / ·/ ·/ FIGURE 11-3: Inlet vs. Outlet Grain Loading 170 ME Horizontal Module Southern California Edison Plant s~ ma ap hit -...
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From page 437... ...
have published particulate removal data for TVA Shawnee operations, for limestone and lime scrubbing. The Bechtel report contains data on overall particulate removal efficiencies for several different scrubbers -- venturi and spray scrubbers, TCA scrubber with five grids and a marbel bed scrubber.
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From page 438... ...
FIGURE 11-4: Particle Size Distributions at TCA Scrubber Inlet and Outlet - TVA Shawnee Plant FIGURE ~ Efficient ~ Kit ~ Shawnee' ~ .~'' .
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From page 439... ...
100 Ant 439 60 40 20 10 8 6 4 11 a: a: 1 He 0.8 0.6 En UJ cz: LL 0.4 0.2 _ 0.1 1 1 1 1 1 1 1 1 0~ 34 0.06 0.1 0.2 0.4 0.6 1 2 4 \ PARTICLE DIAMETE R (microns) FIGURE 1~-5: TCA Scrubber Particulate Removal Efficiency as a Function of Particle Size - TVA Shawnee Plant.
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From page 440... ...
Very few data are available on the fly ash content of the particulates leaving the FGD system. What data are available suggest that the fly ash represents about 60 percent of the total and the remainder (40 percent} comes from entrainment from the slurry liquor.
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From page 441... ...
Also note that investment and operating costs for disposal of fly ash and byproduct credit have been excludede The effect of excluding product credits from annual operating C08t estimates is shown below.
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From page 442... ...
442 t l ill f // .~ I r ~ C 0 C ~ o U 0 ~ ~~ t g t.° '-I, to 2 '—g x it, U)
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From page 443... ...
.H li: tog Or O~ ~ 0 - t _ ~ fat 0 N · I ·~ U)
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From page 444... ...
Investment requirements for disposal of fly ash excluded. Construction labor shortages' with accompanying overtime pay incentive not considered.
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From page 445... ...
_ . ~ All Cat-Ox installations require particulate removal to 0 005 gr/scf a 1 ready ~'ee~e ~i Ag tonverter i Be1 aUse eXi s t i ng units are a d
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From page 446... ...
Experimental data now becoming available indicates that addition of magnesium to the scrubber liquor can improve sulfur dioxide removal efficiency substantially (e.
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From page 447... ...
to MA it. t: I' |,,' I' .f Excluding Credit for Byproducts Limestone process Total annual Years operating Mills/ life cost,$ kWh Coal-fired power units 50% SO2 removal;onsite solids disposal 200 MW new,3.5% sulfur 200 MW existing, 3.5% sulfur 500 MW existing, 3.5% sulfur 500 MW new,2.0% sulfur 500 MW new,3.5% sulfur 500 MW new,5.0% sulfur 1000 MW existing, 3.5% sulfur 1000 MW new,3.5% sulfur 30% SO2 removal;onsite solids disposal 500 MW new,3.5% sulfur 90% SO2 removal;offsite solids disposal 500 MW new,3.5% sulfur 90% SO2 removal (existing unit without existing particulate collection facilities)
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From page 448... ...
. Investment and operat~ng cost for dz~posaL of fly ash excluded.
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From page 449... ...
. _~; A: TABLE 11-8 Installation Cost, Bruce Mansfield Plant,Flue Gas Desulfurization System Scrubber System Chemico Contract Foundations, Electrical, I&C' Linings, Oil Storage, Control Room, Erection Sludge Ponds with Lining Lime Dock, Handling and Storage Facilities $32,000,000 32,200,000 2,500,000 11,700,000 Chimney with LIning 7,600,000 $86,000.000 Subtatal Distributables Contingency Escalation Engineering Owner's Cost Including Alleviance for ~ as During Construction 8,300,000 3,000,000 5, 000, 000 1,500,000 .
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From page 451... ...
~ 7. ~ Retrofit Flue Gas Desulfurization Systems Cost estimation f or retrof i*
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From page 452... ...
Radian then studied in some detail the power plants in the state of Ohio, using as a criterion that any unit with an availabl e area less than 20 square feet/MW can be retrofitted only with great dif f iculty (if at all} . The data on utility plant size and plot availability was taken from the f irst Kellogg study.
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From page 453... ...
i Fly f airly tail the power as a mailable area retrofitted ill)
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From page 454... ...
8. 0 INSTITUTIONAL BARRIERS TO THE ~PLICATTON OF SULFUR OXIDE CONTROL SYSTEMS There have been two recent studies discussing institutional barriers to the installation of FGD systems.
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From page 455... ...
455 ast units. ~ in f urthez rQ1 costs ncept.
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From page 456... ...
Currently there are about 15 vendors that have some established expertise in f lue gas desulfurization and of these three or four have substantial experience and the capability to expand their services rapidly. This would suggest that the data given in Appendix 11, showing new scrubber installations, provides a reasonable estimate of the possible rate of installation -- some 20 or so installations per year.
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From page 457... ...
- ~ -2 It t8 noteworthy that Me beneficial effect .of magnesium ions was not mentioned during hearings held in March through May of 1974 by Hearing Examiners of the Ohio -Ebvironmental Protection Agency. Indeed, testimony was heard concerning the question whether or not adequate supplies of limestone of low magnesium content were available.
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From page 458... ...
Any examination of this question ought to consider the hypothesis (Reller 1975} that emissions of sulfuric acid vapor and mist in New York City have declined nowhere nearly in proportion to the decline in sulfur content of the fuel. The data that it was possible to gather in the time available tend to confine the hypothesis, and point to need for experimental studies to determine sulfur dioxide emissions from representative space heating equipment in New York City while it burns oz1 containing 0.3 per cent sulfur, the level presently in use.
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From page 459... ...
. Sulfur dioxide reacts why atomic- oxygen to yield concentrations of-sulfur trioxide-that : parsdoxi<:al-ly~ exceed - the therms—amic eq~libri~um yield for reaction of sulfur dioxide with elemental oxygen at the temperature of the fla—.
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From page 460... ...
This temperature is tensed the dew-point;of the flue gas, and is a function of both the concentration of sulfuric acid vapor in the gas and also the concentration of water vapor. Muller's relation for~dew~point reread sulfur trioxide of flue gas appears to have been confirmed by the best available data and-to have general support a~nong~workers on the sub Ject Lisle and Sensedbaugh 1965, Dies ekes i 197S)
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From page 461... ...
The lower stack temperatures possible in coal-fired units at.usual amounts of excess air easy in part reflect a smaller production of sulfur trioxide, but also, they seem to-reflect an uptake of sulfuric acid vapor by adsorption upon fly ash or reaction with alkaline material in fly ash. Missions of sulfuric acid vapor or mist are generally lower for coal-fired boilers, unless the comparison is with an oil-fired unit at low excess air.
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From page 462... ...
2 3 4 5 6 PERCENT SULFU R IN FUEL FIGURE App. 11-A1: Sulfur Trioxide Levels in Flue Gas from Careful Laboratory Studies of Combustion of Oils (the Triangles)
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From page 464... ...
11-A2 is the average of Sulfur trioxide readings for a sample of gas taken from the co ~ ustion chamber and a sample taken from a scoots exit chamber at about 6SO F The tests used 25 percent excess air.
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From page 466... ...
As before, in connection with Figure App. 11-A2, one is led to the conclusion that sulfur trioxide emissions fron the firing of oil at 0.3 percent sulfur will not be negligibly small at the levels of excess air usual in small combustion equipment.
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From page 467... ...
ll-A3. Sulfur Trioxide in Flue Gas from Botlers at Low Excess Air.
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From page 468... ...
12) on an old oil-fired boiler sometimes receives sulfuric acid mist at 50 ppm when oil at 2 percent sulfur is used.
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From page 469... ...
ler A with ~on, lead to Vapor opriate "food, in the lity boilers flat low levels ie following a confidential lue Gas epyg} 0.8 t.7 2.6 3.s on tests on Aeration at and good hat failure fuel rate .development filler. The : - t 5 Lion at 3 list V .
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From page 470... ...
The Company enjoys a considerable revenue from sale of the vanadium-rich fly ash, and indeed, supplies a signif icant fraction of the nation ' s requirement for vanadium. .045 Control of Small Combustion Equipment I control of sulfuric acid vapor emissions from Small oil-fired combustion devices may not be easy.
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From page 471... ...
a for about 37 .culate Emissions Ig age nicer of that dew~points g are generally far below those of oil firing at usual levels of excess air. The dif f erences may arise not so much f rom a lower production of Sulfur diovide in a coal flame as from a tendency for the vapor pressure of sulfuric acid to be considerably lower an the presence of fly ash.
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From page 472... ...
' s coal-fired stations, that general ly produce a f lue gas containing between about 5 and 10 ppm of sulfur trioxide. Although the 10-MW limestone scrubber displays excellent efficiency for removing fly ash, the efficiency for removing sulfuric acid mist is poor (Princiotta 1 9 7 5)
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From page 473... ...
Although excellent efficiency For lly city fist The hypothesis (Heller 1975) that sulfate particulate levels in the air of New York City and other urban communities have remained high because of significant emissions of sulfuric acid vapor even from the firing of oil at 0.3 percent sulfur is sufficiently credible to warrant an experimental test.
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From page 474... ...
! `' APPENDIX 11-B This appendix contains tables presenting a summary of electric utility flue gas desulfurization facilities in the United States and a breakdown of the installed EGO systems and those under construction.
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From page 475... ...
; presenting ! gas de~ited States, 'GD systems .,,-l , ~ .
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From page 476... ...
1 Hawthorne 3 & 4 Lawrence 4 & 5 LIME SCRUBBING DuQuesne Light R Phillips R 115 N R Louisville Gas & Electric R Paddles Run No ~ FUEL TYPE _ % ASH Coal 5-15 0 37 167 N 820 R 240 R/N 525 410 65 Oil Coal 10 Coal 10-20 Coal Coal Coal 10 Coal '& 2.75 2 ~ n(1)
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From page 477... ...
burning low sulfur Montana coal at least part of time.
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From page 478... ...
1 ~ '1l~t ~ ¢~ou~oocuuoucomo !
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From page 480... ...
Erikeson, Erik (1971) The Fate of Sulfur Dioxide and NOx in the Atmosphere, chapter in Power Gen eration and Enviroronental Change, David A
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From page 481... ...
`(197;4) Sulfur Dioxide Scrubbing T - :K`ology,- testimony presented befo,r.
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From page 482... ...
W., Applicability of Sulfur Dioxide Control Process to POwer Plants, EPA R272- 100.: Kellogg , M Id, Evaluation of the Controllability of Power Plants lIaving a Significant impact on Air Quality Standards, SPAT 450~3-74-002.
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From page 483... ...
SOCTAP (Sulfur oxide control Technology Assessment Panel} (1973} Project" Utilization of Stack Gas Keening Systems by Ste~-EleCtric Plants, Final Report, April. Van Mersbergen, Ronald 11972, testimony for Illinois Pollution Control Board, Chicago, Illinois, January 5.
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From page 484... ...
Williams, D.J. (1964} Oxidation of Sulfur Dioxide in Combustion Processes, Coal Research in CSIRO, No.
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