Method for high-temperature non-catalytic removal of nitrogen oxides from combustion products with multi-zone input of reducing agent

FIELD: chemistry.

SUBSTANCE: invention relates to high-temperature purification of combustion products of all types of organic fuel from nitrogen oxides (NOx) via selective non-catalytic reduction thereof. A method for high-temperature purification of combustion products in the exhaust duct of a thermal generating unit from nitrogen oxides via selective non-catalytic reduction thereof includes feeding an ammonia-containing reducing agent into selected zones of the exhaust duct that are bounded by the temperature range of 850 - 1100°C. The method is characterised by that the reducing agent is simultaneously fed into all said selected zones, where in each of said zones the reducing agent is fed with a flow coefficient of less than one relative to the stoichiometric flow rate. The number of the reducing agent input zones is preferably 2-5. The flow coefficient of the reducing agent fed into each purification zone is preferably in the range of 0.2-0.8. The reducing agent is preferably ammonia or carbamide.

EFFECT: providing a maximum degree of reduction of NOx without exceeding the stoichiometric ratio of the flow of the reducing agent.

5 cl, 1 dwg, 4 tbl

 

The use of

The invention relates to a high-temperature cleaning of products of combustion of all fossil fuels from nitrogen oxides (NOxby their selective non-catalytic reduction (SNCR) and can be used to reduce emissions of NOxinto the atmosphere with flue gases of heating units for various purposes, mainly steam boilers of thermal power plants.

The level of technology

Cleaning of flue gases by means of SNCR is usually carried out in Gaza leakagerough reductant. Known methods of high-temperature combustion product cleaning from nitrogen oxides by SNCR (US 4208386, B01D 53/56, 1980; US 4325924, B01D 53/56, 1982 [1]), using as the reducing agent urea. Thus the temperature range of the gas flow, in the zone in which the injected reductant, is 1900...2500°F (1000...1350°C). The disadvantage of these methods is the low efficiency of the cleaning process of the gas flow due to the significant temperature dependence of the efficiency of reduction of nitrogen oxides within the specified interval. In addition, a decrease or increase in temperature within the specified interval on the optimal leads to an increase in excess of the permissible limits of the content in the purified gas of the secondary pollutant is ammonia. The fact is that in the process of EC�in the operation of thermal units in case of considerable fluctuation of the heat load, consequently, the temperature of the cleaned gas stream. In the case of reducing the temperature of the gas stream in the zone of entry of the reducing agent decreases the efficiency of the SNCR process. To resolve this problem, use an additive to a reducing agent that reduces the temperature of the recovery process, NOxfor example , oxygen-containing organic compounds: aldehydes, ketones, ethylene glycol (US 4719092, B01D 53/56 [2]) or hydrogen-containing inorganic compounds: guanidine, melamine and other (US 4751065; US 4770863; US 4927612; US 4119702 (all - B01D 53/56) [3]). However, the input of these additives that reduce the temperature of the effective stroke of the recovery process, NOx, however, does not provide sufficient efficiency of the cleaning process while the stress of thermal units, and in some cases leads to the formation of secondary pollutants.

Known adopted as a prototype method of the invention high-temperature purification of combustion products in the flue thermal unit from nitrogen oxides by selective non-catalytic reduction, namely that within a limited temperature range 850...1100°C of the selected zone of the flue gas duct disposed therein between the heating surfaces is administered immixture reductant (Zellinger G., Tauschitz J. Betrieb-serfahrungen mit der nichtkatalytischen Stickstoffoxidreduktion in den Dampfkraftwerken der Osterreichischen Draukraftwerke AG //VGB Kraftwerkstechnik, 1989, Bd. 69, H. 12, S. 1194-2000 [4]). According to [4] each of these zones is designed to work at a certain heat load of the unit in which the temperature of the flue gases is closest to optimal for SNCR. The disadvantages of this technical solution are the complexity of the adjustment process of selecting the working area with the switching operation of the corresponding equipment, as well as the possibility of contamination of the flue gas with ammonia because of the need to work with the highest possible coefficient of discharge of a reducing agent with respect to its stoichiometric value.

Disclosure of the invention

The object of the invention is improving the efficiency of flue gas cleaning from nitrogen oxides with the exception of the emissions of secondary pollutants in the form of an excess of a reducing agent, and the technical result - ensuring the maximum degree of recovery of NOxwithout exceeding the stoichiometric ratio of reductant consumption.

A solution to this problem and the achievement of specified technical result is ensured by the fact that in the method of high-temperature purification of combustion products in the flue thermal unit from nitrogen oxides by SNCR, namely that within a limited temperature range 850...1100°C of the selected zone of the flue gas duct disposed therein between �poverhnosti heating injected immixture the reducing agent according to the invention the reducing agent is injected simultaneously into all these selected areas, and in each of these areas it is served with a flow ratio relative to the stoichiometric consumption, smaller units. The number of zones input reductant is predominantly 2...5; the ratio of reducing agent supplied to each cleaning zone set in the range 0,2...0,8; as a reducing agent ammonia or urea.

A causal relationship between the specified technical result and the distinctive features of the invention consists in the following. It is known that the optimum temperature corresponding to the maximum degree of reduction of nitrogen oxides using as the reducing agent leakagerough compounds is in the range of 900...1000°C, while the practical temperature range of the combustion products possible in the field of processing a wider and 850...1100°C. This temperature range is almost all thermal units when operating at various loads. But it is advisable to carry out input of the reducing agent is not in a narrow temperature zone with the optimal conditions for the recovery process, and in all possible temperature range in which can flow SNCR-process.

The efficiency of purification of gases in each zone in a multizone enter the reducing agent may be less than effektivnosti single-band scheme of the input. This is because the flue gas temperature in each zone, enter the reducing agent varies and may differ from the optimal process temperature. However, the total efficiency multi-zone purification will be higher compared to single-band. This is because increasing the length of the path of the gases, which in their recovery process, and also increases the response time for a given volume of gases. In addition, the implementation of multi-zone enter the reducing agent reduces the amount of emission of a secondary pollutant is also due to the increase in volume and reaction time.

The reducing agent is added at each cleaning zone with flow ratio (the ratio of actual flow rate to stoichiometric reductant necessary) to smaller units. The total amount of feed of reducing agent should be sufficient for the reduction of nitrogen oxides (no less than stoichiometric amount) contained in flue gases.

Brief description of the drawing

The drawing shows a schematic flow diagram of one possible example of the method of high-temperature combustion product cleaning from nitrogen oxides according to the invention.

Detailed description of the invention

The method according to the invention is illustrated in the example presented�Lenno in the drawing process flow diagram. In the area of the flue 1 thermal unit, discussed below in the examples of coal-fired steam boiler, with the initial temperature of the gases at this site of approximately 1100°C, set the heating surface, including a first platen superheater (SP) 2, the second stage 3 of the second SPP first and second stage 4 SP at which the products of combustion of organic fuel are cooled to a temperature of 850°C. For high temperature cleaning of combustion products of contained nitrogen oxides free from heating surfaces 2-4 space of the flue 1 is selected three temperature zones A, b, C, to enter in which a reducing agent is provided fittings 5-8 respectively. The reducing agent in pure form (ammonia, urea) or in a mixture with water vapor as a carrier simultaneously administered in the initial sections of all said zones by means of valves 5-8, wherein the ratio of reducing agent supplied to each zone cleaning, establish the range of 0.2...0.8. By mixing the reducing agent with the combustion reaction occurs reduction of nitrogen oxides. The results of the experimental testing of specified technological scheme is shown below for four different examples. In the first two examples use only one zone, in the next two - three. The content of nitrogen oxides and ammonia last� cleaning was measured in the cooled products of combustion (flue gases) at the outlet of the boiler prior to their release into the chimney.

Example 1. The flow of the cleaned gases through the flue 1 was 1100000 nm3/h With full load in zone B of the flue 1, located in the splitting between the steps 3, 4 second SPP, filed previously obtained with the use of 40% urea solution combined cycle reduction mix. Flue gas temperature in this zone averaged 1006°C. the Coefficient of discharge of urea was equal to 1. The test results are shown in table 1.

Table 1
NNThe urea consumption, l/hThe content of NOxin the flue gas after cleaning, mg/m3The degree of purification, %The content of NH3in the flue gas, mg/m3
1.0108000
2.19304905535
3.19005405027
4.18505305120

Example 2. The volume of treated gases 800000 nm3/h Under a load of 70% in the high temperature zone of the boiler, located in the area served previously obtained with the use of 40% urea solution combined cycle reduction mix. Flue gas temperature in this zone averaged 860°C. the Coefficient of discharge of urea was equal to 1. The test results are shown in table 2.

Table 2
NNThe urea consumption, l/hThe content of NOxin the flue gas after cleaning, mg/m3The degree of purification, %The content of NH3in the flue gas, mg/m3
1.085000
2.11006202738
3.1120630 2645
4.10806452433

Example 3. With a hundred percent load reduction mix was fed simultaneously in three zones A, b, C clean. The temperature of products of combustion in the first zone A averaged 1049°C, in the second zone B - average 1006°C, in the third zone C - an average of 963°C. the Coefficient of discharge of urea in each cleaning zone ranged from 0.2 to 0.5. Other test conditions are similar to that given in example 1. The test results are shown in table 3.

0
Table 3
NNThe urea consumption, l/hThe content of NOxin the flue gas after cleaning, mg/m3The degree of purification, %The content of NH3in the flue gas, mg/m3
Zone aAreaArea
1.00010800
2.390980570240783
3.390770770260765
4.580390770300722

Example 4. At 70% load reduction mix was fed simultaneously in three zones A, b, C clean. The temperature of products of combustion in the zone A averaged 1045°C, in zone B, on average, 933°C, in zone C - an average of 890°C. the Coefficient of discharge of urea in each cleaning zone ranged from 0.2 to 0.6. Other test conditions are similar to that given in example 1. The test results are shown in table 4.

Table 4
NNThe urea consumption, l/hThe content of NOx� flue gases after purification, mg/m3The degree of purification, %The content of NH3in the flue gas, mg/m3
Area AArea BArea C
1.00085000
2.330550220240723
3.220650770220742
4.220550330215753

The analysis is presented in tables 1-4 results purification of exhaust products of combustion oxides of nitrogen showed a significant increase in the degree of purification of gases in multi-stage input reductant compared with agnosto�anatum, a significant decrease in the content of ammonia in the purified flue gases, as well as consistently high degree of purification of gases when the load changes of the boiler.

1. Method of high-temperature purification of combustion products in the flue thermal unit from nitrogen oxides by selective non-catalytic reduction, namely that within a limited temperature range 850-1100°C of the selected zone of the flue gas duct disposed therein between the heating surfaces is administered immixture a reducing agent, characterized in that the reducing agent is injected simultaneously into all these selected areas, and in each of these areas it is served with a flow ratio relative to the stoichiometric consumption, smaller units.

2. A method according to claim 1, characterized in that the number of zones you enter the reducing agent is 2-5.

3. A method according to claim 1 or 2, characterized in that the ratio of reducing agent supplied to each zone cleaning, establish the range of 0.2-0.8.

4. A method according to claim 1 or 2, characterized in that as a reducing agent ammonia or urea.

5. A method according to claim 3, characterized in that as a reducing agent ammonia or urea.



 

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