CN1923341A - Device and method for coal-burning boiler fume ozone oxidation and simultaneous desulfurization and denitrification - Google Patents
Device and method for coal-burning boiler fume ozone oxidation and simultaneous desulfurization and denitrification Download PDFInfo
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Abstract
本发明公开了一种燃煤锅炉烟气臭氧氧化同时脱硫脱硝装置及其方法。方法包括以下步骤：1)在锅炉烟道4的静电除尘器5前或后110～150℃低温段喷入臭氧O3，喷入臭氧与锅炉烟气中的氮氧化物摩尔比例为0.5～1.5，将锅炉烟气中不溶于水的低价态氮氧化物氧化成为易溶于水的高价态氮氧化物，二氧化硫氧化生成三氧化硫，反应时间至少为0.5秒；2)将经过上一步骤处理的锅炉烟气送入碱液洗涤塔7，在碱液洗涤塔中对烟气进行洗涤，同时吸收烟气中的高价态氮氧化物和硫氧化物。本发明的有益效果是：本发明提供的烟气同时脱硫脱硝新方法，可以同时达到80％以上的脱硝效率和95％以上的脱硫效率，经估算投资比传统SCR+WFGD方式便宜30～60％，运行成本节省60％左右。
The invention discloses a coal-fired boiler flue gas ozone oxidation and simultaneous desulfurization and denitrification device and a method thereof. The method comprises the following steps: 1) spraying ozone O 3 into the low temperature section of 110-150°C before or after the electrostatic precipitator 5 of the boiler flue 4, and the molar ratio of the injected ozone to the nitrogen oxide in the boiler flue gas is 0.5-1.5 , to oxidize the water-insoluble low-valence nitrogen oxides in the boiler flue gas into water-soluble high-valence nitrogen oxides, and oxidize sulfur dioxide to form sulfur trioxide. The reaction time is at least 0.5 seconds; 2) After the previous step The treated boiler flue gas is sent to the lye washing tower 7, where the flue gas is washed and the high-valent nitrogen oxides and sulfur oxides in the flue gas are absorbed. The beneficial effects of the present invention are: the new method for simultaneous desulfurization and denitrification of flue gas provided by the present invention can simultaneously achieve a denitration efficiency of more than 80% and a desulfurization efficiency of more than 95%, and the estimated investment is 30-60% cheaper than the traditional SCR+WFGD method , saving about 60% of running cost.
Description
技术领域technical field
本发明涉及环境保护技术领域，尤其涉及一种燃煤锅炉烟气臭氧氧化同时脱硫脱硝装置及其方法。The invention relates to the technical field of environmental protection, in particular to a coal-fired boiler flue gas ozone oxidation simultaneous desulfurization and denitrification device and a method thereof.
背景技术Background technique
能源利用过程中产生的硫氧化物、氮氧化物对我国的大气环境造成了日益严重的危害。目前已有的脱硫技术可分为干法、半干法和湿法等几类。干法、半干法投资运行费用低，但往往存在脱硫效率不高的缺点，大型锅炉燃烧设备如电站锅炉等往往不能达到环保要求。目前电站锅炉广泛采用的是石灰石/石膏湿法烟气脱硫技术(WFGD)，该方法脱硫效率高，运行稳定，但存在耗水量大，排放废水二次污染，投资和运行成本较高等缺点。The sulfur oxides and nitrogen oxides produced in the process of energy utilization have caused increasingly serious harm to our country's atmospheric environment. At present, the existing desulfurization technology can be divided into several categories such as dry method, semi-dry method and wet method. Dry method and semi-dry method have low investment and operation costs, but often have the disadvantage of low desulfurization efficiency, and large-scale boiler combustion equipment such as power plant boilers often cannot meet environmental protection requirements. At present, limestone/gypsum wet flue gas desulfurization technology (WFGD) is widely used in power plant boilers. This method has high desulfurization efficiency and stable operation, but has disadvantages such as large water consumption, secondary pollution of discharged wastewater, and high investment and operating costs.
氮氧化物的控制技术主要有两类：第一类属炉内燃烧过程控制方式，主要有低NOx燃烧器技术，OFA(Over fire air)技术，低氧燃烧技术，再燃烧技术等通过燃烧过程调整来控制NOx的排放，可以将NOx控制在中等排放水平，一般脱硝效率在30～50％左右。但一方面这些技术容易造成燃烧稳定性下降，燃烧器区域容易形成局部还原性气氛，造成灰熔点下降，引起水冷壁的粘污结渣现象，影响锅炉的正常安全运行。另一方面随着环保要求的进一步提高，很难实现NOx更进一步的排放控制。第二类技术为烟气脱硝技术，目前美国、日本、欧洲等国家应用最为广泛的技术为选择性催化还原技术(SCR)。SCR技术脱硝效率高，运行稳定，但高灰布置情况下烟气中较高的粉尘颗粒容易引起催化剂的磨损、堵塞等问题，飞灰中的重金属会引起催化剂的中毒，运行和投资费用非常昂贵。我国环保工作起步较晚，二氧化硫的控制才刚刚开始，今后氮氧化物势必提上日程，若采用发达国家逐项治理的思路，采用湿法烟气脱硫WFGD装置脱硫，选择性催化SCR脱硝的方法势必增加巨额的投资、运行费用，而一些老机组甚至存在布置困难等问题，因此开发低成本、高效率的同时脱硫脱硝技术就显得尤为重要。There are two main types of nitrogen oxide control technologies: the first type belongs to the combustion process control method in the furnace, mainly including low NOx burner technology, OFA (Over fire air) technology, low oxygen combustion technology, re-burning technology, etc. through the combustion process Adjust to control the emission of NOx , NOx can be controlled at a medium emission level, and the general denitrification efficiency is about 30-50%. But on the one hand, these technologies are likely to cause a decrease in combustion stability, and a local reducing atmosphere is likely to be formed in the burner area, resulting in a decrease in ash melting point, causing fouling and slagging of the water wall, and affecting the normal and safe operation of the boiler. On the other hand, with the further improvement of environmental protection requirements, it is difficult to achieve further emission control of NOx . The second type of technology is flue gas denitrification technology. At present, the most widely used technology in the United States, Japan, Europe and other countries is selective catalytic reduction technology (SCR). SCR technology has high denitrification efficiency and stable operation, but in the case of high ash layout, the high dust particles in the flue gas are likely to cause problems such as catalyst wear and blockage, and the heavy metals in the fly ash will cause catalyst poisoning, and the operation and investment costs are very expensive. . my country's environmental protection work started relatively late, and the control of sulfur dioxide has just begun. In the future, nitrogen oxides will definitely be put on the agenda. If we adopt the idea of item-by-item treatment in developed countries, we will use wet flue gas desulfurization WFGD device desulfurization and selective catalytic SCR denitrification method It is bound to increase huge investment and operating costs, and some old units even have problems such as difficult layout. Therefore, it is particularly important to develop low-cost, high-efficiency desulfurization and denitrification technologies.
目前在研究的烟气同时脱硫脱硝技术有炉内干法同时脱硫脱硝技术，电催化同时脱硫脱硝技术等。其中电催化同时脱硫脱硝技术脱除效率高，运行成本低，正在成为人们研究的热点。目前的电催化技术包括电子束技术，脉冲放电等离子体技术，水蒸气氨气电晕放电活化等技术。主要利用高能电子和烟气中的中性分子(N2，O2，H2O等)碰撞，产生一些活性自由基(O，OH，O3，HO2等)，这些自由基与烟气中的SO2和NOx分子反应生成SO3，高价态氮氧化物，硝酸，硫酸等，在NH3存在的条件下生成硫酸铵、硝酸铵等副产品。优点是干法脱除，不产生废水废渣，能同时脱硫脱硝，副产物可以资源化利用。但由于自由基存活时间非常短，需要将自由基的产生与烟气反应器合二为一，针对整个烟道进行放电，而锅炉烟气中含有大量的N2、CO2、H2O、粉尘等物质，放电条件恶劣，同时N2、CO2消耗大量的输入能量，造成能量利用率低，整体运行费用昂贵。The flue gas simultaneous desulfurization and denitrification technologies currently under study include furnace dry simultaneous desulfurization and denitrification technology, electrocatalytic simultaneous desulfurization and denitrification technology, etc. Among them, electrocatalytic simultaneous desulfurization and denitrification technology has high removal efficiency and low operating cost, and is becoming a research hotspot. The current electrocatalysis technology includes electron beam technology, pulse discharge plasma technology, water vapor ammonia corona discharge activation and other technologies. Mainly use high-energy electrons to collide with neutral molecules (N 2 , O 2 , H 2 O, etc.) in the smoke to generate some active free radicals (O, OH, O 3 , HO 2 , etc.), The SO 2 and NO x molecules in the reaction react to generate SO 3 , high-valence nitrogen oxides, nitric acid, sulfuric acid, etc., and generate by-products such as ammonium sulfate and ammonium nitrate in the presence of NH 3 . The advantages are dry removal, no waste water and waste residue, simultaneous desulfurization and denitrification, and by-products can be used as resources. However, due to the very short survival time of free radicals, it is necessary to combine the generation of free radicals with the flue gas reactor to discharge the entire flue, and the boiler flue gas contains a large amount of N 2 , CO 2 , H 2 O, Dust and other substances, the discharge conditions are harsh, and N 2 and CO 2 consume a large amount of input energy, resulting in low energy utilization and high overall operating costs.
发明内容Contents of the invention
本发明的目的是针对各种电催化技术针对整个烟道放电，能耗较高的问题，提供一种燃煤锅炉烟气臭氧氧化同时脱硫脱硝装置及其方法。The purpose of the present invention is to provide a simultaneous desulfurization and denitrification device and method for the ozone oxidation of coal-fired boiler flue gas in view of the problem of high energy consumption for the entire flue discharge of various electrocatalytic technologies.
燃煤锅炉烟气臭氧氧化同时脱硫脱硝装置具有依次相连接的锅炉炉膛、尾部烟道、碱液洗涤塔，碱液洗涤塔上部设有除雾器，碱液洗涤塔下部设有储液槽，碱液洗涤塔顶部与烟囱相接，碱液洗涤塔底部与硝酸盐硫酸盐浓缩结晶装置相接，尾部烟道依次与臭氧发生装置、干燥过滤制氧装置相接，在所述尾部烟道上设有静电除尘器。The coal-fired boiler flue gas ozone oxidation simultaneous desulfurization and denitrification device has a boiler furnace, tail flue, and lye washing tower connected in sequence. The upper part of the lye washing tower is equipped with a demister, and the lower part of the lye washing tower is equipped with a liquid storage tank. The top of the lye washing tower is connected to the chimney, the bottom of the lye washing tower is connected to the nitrate and sulfate concentration and crystallization device, and the tail flue is connected to the ozone generating device and the drying and filtering oxygen making device in turn. There is an electrostatic precipitator.
燃煤锅炉烟气臭氧氧化同时脱硫脱硝方法包括以下步骤：The method for simultaneous desulfurization and denitrification by ozonation of coal-fired boiler flue gas comprises the following steps:
1)在锅炉烟道(4)的静电除尘器(5)前或后110～150℃低温段喷入臭氧O3。喷入臭氧与锅炉烟气中的氮氧化物摩尔比例为0.5～1.5，将锅炉烟气中不溶于水的低价态氮氧化物氧化成为易溶于水的高价态氮氧化物，二氧化硫氧化生成三氧化硫，反应时间至少为0.5秒；1) Ozone O 3 is sprayed into the low-temperature section at 110-150°C before or after the electrostatic precipitator (5) of the boiler flue (4). The molar ratio of the ozone sprayed into the boiler flue gas and the nitrogen oxides in the boiler flue gas is 0.5 to 1.5, and the low-valence nitrogen oxides that are insoluble in water in the boiler flue gas are oxidized into high-valence nitrogen oxides that are easily soluble in water, and sulfur dioxide is oxidized to form Sulfur trioxide with a reaction time of at least 0.5 seconds;
2)将经过上一步骤处理的锅炉烟气送入碱液洗涤塔(7)，在碱液洗涤塔中对烟气进行洗涤，同时吸收烟气中的高价态氮氧化物和硫氧化物。2) The boiler flue gas treated in the previous step is sent to the lye washing tower (7), and the flue gas is washed in the lye washing tower, while absorbing high-valent nitrogen oxides and sulfur oxides in the flue gas.
所述碱液是氢氧化钠、氢氧化钾、氢氧化钙、氧化钙、碳酸钙、氨水其中至少一种。The lye is at least one of sodium hydroxide, potassium hydroxide, calcium hydroxide, calcium oxide, calcium carbonate and ammonia water.
本发明的有益效果是：本发明提供的烟气同时脱硫脱硝新方法，可以同时达到80％以上的脱硝效率和95％以上的脱硫效率，经估算投资比传统SCR+WFGD方式便宜30～60％，运行成本节省60％左右The beneficial effects of the present invention are: the new method for simultaneous desulfurization and denitrification of flue gas provided by the present invention can simultaneously achieve a denitration efficiency of more than 80% and a desulfurization efficiency of more than 95%, and the estimated investment is 30-60% cheaper than the traditional SCR+WFGD method , saving about 60% in operating costs
附图说明Description of drawings
图1是燃煤锅炉烟气臭氧氧化同时脱硫脱硝装置I结构示意图；Fig. 1 is a schematic diagram of the structure of a coal-fired boiler flue gas ozone oxidation simultaneous desulfurization and denitrification device I;
图2是燃煤锅炉烟气臭氧氧化同时脱硫脱硝装置II结构示意图；Figure 2 is a schematic diagram of the structure of coal-fired boiler flue gas ozone oxidation simultaneous desulfurization and denitrification device II;
图中：锅炉炉膛1、干燥过滤制氧装置2、臭氧发生装置3、尾部烟道4、静电除尘器5、储液槽6、碱液洗涤塔7、除雾器8、烟囱9、硝酸盐硫酸盐结晶处理装置10。In the figure:
具体实施方式Detailed ways
本发明针对局部空气或氧气放电产生臭氧后喷入烟道对氮氧化物与硫氧化物进行氧化，尾部结合湿法洗涤装置进行同时脱除，若已安装湿法脱硫装置则可以与之进行有效结合，实现同时脱硫脱硝。The present invention aims at local air or oxygen discharge to generate ozone and spray it into the flue to oxidize nitrogen oxides and sulfur oxides. The tail is combined with a wet scrubbing device for simultaneous removal. If a wet desulfurization device has been installed, it can be effectively Combined to achieve simultaneous desulfurization and denitrification.
O3作为自由基的一种在电子束、脉冲等离子体放电中广泛存在，而O3生存周期相对较长，因此可将少量空气或氧气首先电离生成O3，然后送入锅炉烟道，就中大大降低系统的电耗，经估算O3仅需对总烟气量3％左右的气体进行放电就能够满足要求。As a kind of free radical, O 3 widely exists in electron beam and pulsed plasma discharge, and the life cycle of O 3 is relatively long. Therefore, a small amount of air or oxygen can be ionized first to generate O 3 , and then sent into the boiler flue, just It is estimated that O 3 only needs to discharge about 3% of the total flue gas to meet the requirements.
下面结合附图和具体实施例进一步详细描述本发明。The present invention will be further described in detail below in conjunction with the accompanying drawings and specific embodiments.
如图所示，燃煤锅炉烟气臭氧氧化同时脱硫脱硝装置具有依次相连接的锅炉炉膛1、尾部烟道4、碱液洗涤塔7，碱液洗涤塔上部设有除雾器8，碱液洗涤塔下部设有储液槽6，碱液洗涤塔顶部与烟囱9相接，碱液洗涤塔底部与硝酸盐硫酸盐浓缩结晶装置10相接，尾部烟道4依次与臭氧发生装置3、干燥过滤制氧装置2相接，在所述尾部烟道4上设有静电除尘器5。As shown in the figure, the coal-fired boiler flue gas ozone oxidation simultaneous desulfurization and denitrification device has a
燃煤锅炉烟气臭氧氧化同时脱硫脱硝方法包括以下步骤：The method for simultaneous desulfurization and denitrification by ozonation of coal-fired boiler flue gas comprises the following steps:
1)在锅炉烟道4的静电除尘器5前或后110～150℃低温段喷入臭氧O3，喷入臭氧与锅炉烟气中的氮氧化物摩尔比例为0.5～1.5，将锅炉烟气中不溶于水的低价态氮氧化物氧化成为易溶于水的高价态氮氧化物，二氧化硫氧化生成三氧化硫，反应时间至少为0.5秒；1) Before or after the
2)将经过上一步骤处理的锅炉烟气送入碱液洗涤塔7，在碱液洗涤塔中对烟气进行洗涤，同时吸收烟气中的高价态氮氧化物和硫氧化物。2) The boiler flue gas treated in the previous step is sent to the
锅炉烟气排放的NOx中，NO占95％以上，其它为NO2，N2O等，而NO不溶于水，是难于处理的气态污染物质之一，而高价态的NO2，NO3，N2O5可以与水反应生成HNO2、HNO3，极易被湿法洗涤装置脱除。通过在锅炉烟道110～150℃温度区间喷入臭氧，O3/NO摩尔比例取0.5~1.5，可以将NO氧化为易溶于水的高价态物质，通过湿法洗涤塔进行脱除，部分SO2也可以被氧化生成SO3，湿法洗涤对SO2的脱除已相当有效，SO3比SO2更易溶解与水，在臭氧氧化尾部配合湿法洗涤装置就可以实现高效同时脱硫脱硝，脱硝效率与喷入臭氧量相关。如果已配备石灰石/石膏湿法烟气脱硫设备，或者水膜除尘器，则可以对其进行适当改造后与该方法进行整合，节省投资成本。Among the NOx emitted by boiler flue gas, NO accounts for more than 95%, and the others are NO 2 , N 2 O, etc., and NO is insoluble in water, which is one of the gaseous pollutants that are difficult to treat, while high-valence NO 2 , NO 3 , N 2 O 5 can react with water to generate HNO 2 and HNO 3 , which are easily removed by wet scrubbing equipment. By spraying ozone into the boiler flue at a temperature range of 110-150°C, and taking the O 3 /NO molar ratio of 0.5-1.5, NO can be oxidized into high-valence substances that are easily soluble in water, and removed by a wet scrubber. SO 2 can also be oxidized to produce SO 3 . Wet scrubbing is quite effective in removing SO 2 . SO 3 is more soluble in water than SO 2 . It can achieve efficient simultaneous desulfurization and denitrification with a wet scrubbing device at the end of the ozone oxidation. The denitrification efficiency is related to the amount of ozone injected. If limestone/gypsum wet flue gas desulfurization equipment or water film dust collector is already equipped, it can be properly modified and integrated with this method to save investment costs.
具体过程为：在锅炉尾部烟道110～150℃温度区间喷入臭氧，喷入位置可以在静电除尘器之前或之后，臭氧喷入量根据烟气中NO浓度按O3/NO摩尔比0.5～1.5∶1选取，氧化后的氮氧化物和硫氧化物通过湿法洗涤塔进行脱除，吸收液为碱液，吸收液循环利用，富集的硫酸盐硝酸盐浓缩结晶后出售或进一步处理。下面结合附图进一步说明：The specific process is: spray ozone in the temperature range of 110-150°C in the tail flue of the boiler. The injection position can be before or after the electrostatic precipitator. 1.5:1 selection, the oxidized nitrogen oxides and sulfur oxides are removed through a wet scrubber, the absorption liquid is lye, the absorption liquid is recycled, and the enriched sulfate nitrate is concentrated and crystallized for sale or further treatment. Further explain below in conjunction with accompanying drawing:
实施例1Example 1
燃煤锅炉烟气臭氧氧化同时脱硫脱硝布置方案I，如图1所示。空气经干燥净化后送入干燥过滤制氧装置，产生的氧气送入臭氧发生装置以制备高浓度臭氧，臭氧送入空气预热器后静电除尘器前的温度约为150℃的含尘烟道，喷入量根据烟气氮氧化物浓度，按臭氧与氮氧化物摩尔比1.1∶1时时调整，保证至少0.5s反应时间。喷口采用多孔网格喷射，喷入位置在空预器烟气出口1m处。处理后的烟气经静电除尘器后进入湿法洗涤塔，吸收液循环利用，烟气经湿法洗涤塔、除雾器处理后送入烟囱，吸收的硫酸盐与硝酸盐进行浓缩结晶处理。洗涤塔采用碱液作为吸收剂，洗涤塔为喷淋塔或填料塔。作为吸收剂的碱液是氢氧化钠，也可以是水、氢氧化钾、氢氧化钙、氧化钙、碳酸钙或氨水中的一种或多种。Layout scheme I for simultaneous desulfurization and denitrification by ozone oxidation of coal-fired boiler flue gas is shown in Figure 1. After the air is dried and purified, it is sent to the dry and filtered oxygen generator, and the generated oxygen is sent to the ozone generating device to prepare high-concentration ozone. The injection amount is adjusted from time to time according to the concentration of nitrogen oxides in the flue gas, and the molar ratio of ozone to nitrogen oxides is 1.1:1 to ensure a reaction time of at least 0.5s. The nozzle adopts porous grid injection, and the injection position is 1m away from the flue gas outlet of the air preheater. The treated flue gas enters the wet scrubber after passing through the electrostatic precipitator, and the absorption liquid is recycled. The flue gas is sent to the chimney after being treated by the wet scrubber and demister, and the absorbed sulfate and nitrate are concentrated and crystallized. The washing tower uses lye as the absorbent, and the washing tower is a spray tower or a packed tower. The lye used as absorbent is sodium hydroxide, and can also be one or more of water, potassium hydroxide, calcium hydroxide, calcium oxide, calcium carbonate or ammonia water.
实施例2Example 2
燃煤锅炉烟气臭氧氧化同时脱硫脱硝置方案II，如图2所示。将臭氧送入静电除尘器之后约110℃左右的低尘烟气环境，臭氧喷入量根据烟气氮氧化物浓度，按臭氧与氮氧化物摩尔比1.0动态调整，喷入点位置保证距洗涤塔入口0.5s以上停留时间。臭氧采用多孔网格状喷射方式进行，氧化后的烟气进入碱液洗涤塔进行吸收，吸收液循环利用，烟气经洗涤、除雾后送入烟囱排放，吸收的硫酸盐与硝酸盐进行浓缩结晶处理。洗涤塔采用碱液作为吸收剂，洗涤塔为喷淋塔或填料塔。作为吸收剂的碱液是氢氧化钠，也可以氢氧化钾、氢氧化钙、氧化钙、碳酸钙或氨水中的一种或多种。Coal-fired boiler flue gas ozone oxidation and simultaneous desulfurization and denitrification scheme II, as shown in Figure 2. Send ozone into the low-dust flue gas environment at about 110°C after the electrostatic precipitator. The amount of ozone injected is dynamically adjusted according to the concentration of nitrogen oxides in the flue gas, and the molar ratio of ozone to nitrogen oxides is 1.0. The position of the injection point is guaranteed to be away from the washing machine. The residence time at the tower entrance is more than 0.5s. Ozone is sprayed in a porous grid shape. The oxidized flue gas enters the lye washing tower for absorption, and the absorption liquid is recycled. After the flue gas is washed and defogged, it is sent to the chimney for discharge, and the absorbed sulfate and nitrate are concentrated. Crystallization treatment. The washing tower uses lye as the absorbent, and the washing tower is a spray tower or a packed tower. The lye used as absorbent is sodium hydroxide, or one or more of potassium hydroxide, calcium hydroxide, calcium oxide, calcium carbonate or ammonia.
最后，还需要注意的是，以上列举的仅是本发明的具体实施例。显然，本发明不限于以上实施例，还可以有许多变形。Finally, it should also be noted that what is listed above are only specific embodiments of the present invention. Obviously, the present invention is not limited to the above embodiments, and many variations are possible.
本发明可用其他的不违背本发明的精神和主要特征的具体形式来概述。因此，无论从哪一点来看，本发明的上述实施方案都只能认为是对本发明的说明而不能限制本发明，权利要求书指出了本发明的范围，而上述的说明并未指出本发明的范围，因此，在与本发明的权利要求书相当的含义和范围内的任何改变，都应认为是包括在权利要求书的范围内。The present invention may be embodied in other specific forms without departing from the spirit and main characteristics of the invention. Therefore, no matter from which point of view, the above-mentioned embodiments of the present invention can only be regarded as descriptions of the present invention and cannot limit the present invention, and the claims have pointed out the scope of the present invention, and the above description does not point out the scope of the present invention. Therefore, any change within the meaning and scope equivalent to the claims of the present invention should be considered to be included in the scope of the claims.
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