New flue gas desulphurisation process

90 VGB PowerTech 10/2011

Intervex – A new process for desulphurisation of flue gasesLars Tiberg and Mats Eriksson

Authors

Lars Tiberg, Ph. D. Radscan Intervex ABVästeras/Sweden

Mats ErikssonGällivare/Sweden

Kurzfassung

Intervex – Ein neues Verfahren zur Rauchgasentschwefelung

Ein neues Verfahren zur Rauchgasentschwefe-lung wird vorgestellt. In einen Reaktor werden Rauchgase im Gegenstrom durch ein körniges Kalksteinbett geleitet. Wasser wird oberhalb des Bettes gleichmäßig versprüht. Der Kalk-stein wandert langsam von oben nach unten und der Grobanteil wird rezirkuliert. Schwe-feloxide aus dem Rauchgas bilden Calcium-sulfit und Calciumsulfat und werden mit dem Wasser ausgewaschen.

Eine erste Pilotanlage für ein 20-MW-Kessel ist seit mehreren Jahren in Betrieb. Für diese kann auf interessante Betriebsergebnisse ver-wiesen werden.

So kann ein hoher Abscheidegrad von Schwe-fel, Chlor, Fluor und Flugasche bei geringem Druckverlust festgestellt werden. Der Ausnut-zungsgrad des Kalksteins liegt bei 75 %. Der Kalkstein ist preiswert und die Investitionskos-ten für die Anlage sind niedrig.

The basic process

In the Intervex desulphurisation process, gran-ular limestone is used as reactant, water is sprayed over the granular bed and the flue gas is led upwards through the bed.

The reaction between limestone, CaCO3 and sulphur dioxide SO2 takes place in the pres-ence of water:

CaCO3 + SO2 + 2 · H2O = CaSO3 · 2H2O + CO2 (1)

In the presence of oxygen, the calcium sul-phite will oxidise to calcium sulphate, gyp-sum:

CaSO3 · 2H2O + ½ O2 = CaSO4 · 2H2O (2)

The oxidation is rapid in acidic environment.-

To avoid that a layer of calcium sulphate is formed on the limestone, a small content of chloride ions should be present in the water. The chloride ions react with the limestone to form calcium ions in the spray water, and these calcium ions react with sulphur dioxide to form calcium sulphite in the water phase:

CaCO3 + 2HCl = Ca2+ + CO2 + H2O + 2Cl- (3)

SO2 + 3H2O = 2H3O+ + SO32- (4)

2H3O+ + 2Cl- = 2HCl + H2O (5)

Ca2+ + SO32- + 2H2O = CaSO3 · 2H2O (6)

It is obvious that the chloride ion works as a catalyst as it takes part in the reaction but is not consumed.

Some calcium sulphate is precipitated on the limestone granules, therefore it is necessary to circulate the stone through the bed to remove this layer.

Development steps

In the classical wet process, limestone is fine-ly pulverised, which is emulsified in water. The emulsion meets the flue gases containing sulphur oxide in a scrubber tower. The reac-tion takes place in three steps – (1) dissolution of SO2 gas in water, (2) transport in the water to the limestone grain and (3) reaction be-

tween the two. The total reaction is rather sluggish and the process demands large reac-tion volumes.

If however, the limestone is just moistened with water, and the flue gas is led in contact with it, the reaction will be very fast. We ob-served this during our development work and since then, we have tried to design a desul-phurisation process for this fast reaction.

In our first process, we used a limestone bed as heat exchanger, i.e. two parallel reactors were applied, which alternatively cooled flue gas and heated combustion air. When the flue gas was cooled by limestone, a very thin layer of water condensed on the stone surface, and in this layer, sulphur oxide contained in the flue gas immediately formed calcium sulphite, i.e. gypsum. The process had two functions: desulphurisation and recovery of heat from the flue gases. We could regain heat from the flue gases down to a temperature about 50 °C. This double function made the process quite attractive.

In the process, the flue gas was led upwards through the limestone bed whereas the lime-stone was transported downwards, creating a counter flow process. From the bottom of the reactor, the exit stone was led to a tumbler to wear off sulphite. The cleaned stones were transported to the top of the reactor and again fed into the reactor.

A drawback of this process was the limited capacity of the limestone surface to take up sulphur dioxide, i.e. a layer of only about 2 micrometer could built up before the stone was saturated and had to be cleaned. One cu-bic meter of limestone (5 to 30 mm) would only take up 6 kg of sulphur dioxide between the tumbling treatments. The transport and tumbling of the limestone became too exten-sive and too costly.

Another problem was designing a process where flue gas and air were to be alternatively led through two reactors. During the exchange of reactors, for a short time, only flue gas was led into the boiler furnace with an oxygen shortage which might cause an explosive situ-ation.

Our second process was designed avoiding the explosion risk. We called it Rotovex. A number of reactors were placed in a ring and a rotating valve in the centre would lead flue gas and

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combustion air successively up and down through the reactors. In this way the leakage of flue gas into the combustion chamber would be rather constant never exceeding about 10 %. This process may still be of interest for large plants, but it has still the drawback of very big transport volumes of limestone.

In our third process the heat exchange was abandoned. We sprayed water over the bed, but sparsely to let the limestone dry up before it reached the exit. The idea was to get a dry waste that could easily be freed from fly ash and calcium sulphite – sulphate powder. How-ever, it was too difficult to avoid that wet ma-terial occasionally reached the outlet and greatly disturbed waste treatment.

Our forth process seems to be a hit. We have increased the water spray to get a wet outgoing material. We introduced a quench before the limestone reactor to give an even cooling of the whole reactor. With increasing water flow, we got more calcium sulphite formation in the water phase and the transport of the limestone through the reactor could be reduced to 10 % of what we had used earlier. F i g u r e 1 shows a flow scheme of the process.

Counter flow reactor design

The advantages of counter flow processes are well known to chemists and physicists. The incoming, most active reagents meet the out-going product to be cleaned, i.e. very low con-tents of contaminants can be reached. The outgoing reagents meet the flue gas with the highest content of contaminants whereby the reagents will be fully used up.

Our Intervex reactor ( F i g u r e 2 ) has a coni-cal bottom part, a cylindrical middle part and a conical top. Limestone is fed from a top hop-per through a central feed tube that extends around 2 meters down in the reactor. From the tube end, the stone material flows down to form a cone with a slide angle of around 38 degrees to the horizontal plane. The flue gas is introduced from a ring chamber around the bottom end of the cylindrical middle part of the reactor. From the ring chamber, a number of ducts extend towards the centre of the reactor like spokes in a wheel. The ducts are simply steel plates that are bent in an angle of around 60 degrees with the angle upwards and they are open downwards. The flue gas can flow from

the ring chamber towards the centre and they can flow from the ducts out in the stone bed and upwards towards the bed surface. As the ducts are mounted parallel to the upper conical bed surface, the distance from the ducts to the surface is constant over the cross section of the reactor. As a consequence, the gas velocity will also be constant over the cross section of the reactor. The reaction zone extends from the spokes up to the conical top surface.

The limestone material is slowly transported down through the reactor. The velocity is con-trolled by the exit feeder. A set of concentric funnels in the bottom cone under the spokes guides the stones to make the downward flow velocity equal over the reactor cross section. The material coming out from the bottom is sieved to three fractions: the finest material < 1 mm goes to the waste treatment, stones 1 to 5 mm are taken out from the process and stones > 5 mm are again transported to the top of the reactor.

Water is spayed over the bed via a number of nozzles that distribute the water evenly over the stone bed.

We have tested several stainless steel grades in the reactor. For the ring chamber and spokes,

Fresh limestone

To container

To container

Vibration exit feeder

To water cleaning

Freshwater

Freshwater

Limestone 1-5 mmTo container

Centrifuge

FlexowellelevatorFlue gas out

Flue gas in

DemisterQuench

M

SO2

01

Sleve

Spiral dewaterer

Buffer tank

M MM

MM

M

M

M

MM

LIC

01

LIC02

LIC01

Figure 1. Flow scheme.

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high alloy steels are necessary, but for the inside of the reactor, including the funnels, lower alloyed grades are sufficient.

With an even gas flow upward and an even stone flow and water flow downwards, our In-tervex reactor gives optimum conditions for a high contaminant reduction and a high yield of the reagents. Not only sulphur, but also chlorides, fluorides and fly ash are reduced to low levels.

Waste treatment

The waste from the process consists of fly ash, calcium sulphite, calcium sulphate and lime-stone fine material. From the outlet under the reactor, limestone and waste material pass a vibrating feeder with ample air contact where most of the calcium sulphite is oxidised to cal-cium sulphate (gypsum). A small, acidic bleed off the quench is pumped to the feeder to en-

hance oxidation. Some waste limestone is in the form of stones < 5 mm and some in the form of a fine powder. The stone is sieved away and can be reused in other processes. All other wastes come as sludge. We have tested two methods to take care of it.

In one method which is used in Gällivare, we pump the sludge to a sedimentation tank. From the top end we take out a rather clean

Table 1. Technical data for intervex desulphurisation plants.

Gällivare 20 MW peat 200 MW coal

Gas flow Nm3/s 14 92

SO2 contents mg/Nm3 500 1500

Fly ash contents m/Nm3g 100 150

Reactor diameter m 5,8 15

Bed depth m 2,5 3,5

Pressure drop quench Pa 300 300

Pressure drop reactor pA 550 650

Exit SO2 contents mg/Nm3 9 25

Exit fly ash contents mg/Nm3 7 7

Spray flow m3/h 16 106

Stone flow m3/h 1 20

Water consumption m3 /h 2,5 16,5

Limestone consumption kg/h 54 1060

Limestone yield % 75 75

Figure 2. The Intervex reactor.

fluid. The fluid is reused as spray water. From the bottom end, a rather thick sludge is pumped to the dry fly ash container where it is used to moisten fly ash when it is to be transported to the ash deposit.

Alternatively, the sludge is dewatered in a cen-trifuge. The dry product will contain around 15 % of water. The dewatered product can be used in concrete production.

15200

4400

3200

4000

1110

1

Quench

13000

3782

1

Figure 4. Section 13 m reactor.

Figure 3. The Gällivare Intervex plant.

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The Gällivare plant – results

In 2002, we started building an Intervex plant in Gällivare in northern Sweden for a 20 MW peat-fired boiler. Gällivare is situated 100 km north of the polar circle which means long transports routes, long winters and sometimes very cold weather. The reactor has a diameter of 5.8 m and is designed for a flue gas flow of 14 Nm3/s. At that time we used the concept with restricted water spraying over the lime-stone reactor bed that would keep the bottom and exit feed dry. Since then, we have intro-duced a quench upstream of the Intervex reac-tor and increased water spraying to get a wet waste product. We have developed the sedi-mentation system for waste and the moisten-ing system for the dry fly ash. We improved many components and the reactor design to eliminate the risk for clogging. In autumn 2009, we made the last, important improve-ments to the reactor and since then the process has operated according to our specifications, although some failures occurred at external components during the last year.

In 2009 we also made a test on completion when the plant was operated for 20 days with a strict control of the performance. The fol-lowing results were documented:

Flue gas flow 9 to 11 Nm3/s

Contents of SO2 200 to 400 mg/Nm3

Degree of desulphurisation 97.5 %

Availability 97.4 %

Limestone yield 55 %

Reusable limestone 1 to 5 mm 20 %

Overall limestone yield 75 %

Since the test, Gällivare Heat and Power has taken over the plant. F i g u r e 3 shows a view of the plant and Ta b l e 1 provides some data.

We now regard the process ready for the mar-ket.

The final process

Future Intervex plants will differ from the Gällivare plant in some ways: future plants

will not need an electrostatic precipitator. A cyclone or a falling chamber will be suffi-cient.

The waste sludge will most often be dewatered in a centrifuge instead of the sedimentation process.

F i g u r e 4 shows a drawing of a 13 m reactor (for a 160 MW coal boiler).

We assume a reactor for a 200 MW coal-fired boiler as maximum size for one unit. It will have a diameter of 15 m and a total height of 30 m to the top hopper.

The following advantages of the Intervex process are important:

The reagent – limestone 5 to 30 mm – is −cheap compared to caustic lime for the dry processes or the very finely ground lime-stone of the wet process.

The pressure drop is lower and the electric- −ity consumption is lower than in other proc-esses.

The investment cost is lower than for most −other processes.

High degrees of emission reduction are −reached. □

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