WO2012010080A1 - Appareil et procédé utilisables en vue de la désulfuration et de la dénitration des gaz de combustion - Google Patents

Appareil et procédé utilisables en vue de la désulfuration et de la dénitration des gaz de combustion Download PDF

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Publication number
WO2012010080A1
WO2012010080A1 PCT/CN2011/077318 CN2011077318W WO2012010080A1 WO 2012010080 A1 WO2012010080 A1 WO 2012010080A1 CN 2011077318 W CN2011077318 W CN 2011077318W WO 2012010080 A1 WO2012010080 A1 WO 2012010080A1
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oxygen
flue gas
acid
desulfurization
active
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PCT/CN2011/077318
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English (en)
Chinese (zh)
Inventor
白敏菂
白敏冬
张芝涛
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大连海事大学
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Publication of WO2012010080A1 publication Critical patent/WO2012010080A1/fr

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    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B13/00—Oxygen; Ozone; Oxides or hydroxides in general
    • C01B13/02—Preparation of oxygen
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
    • B01D53/32—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols by electrical effects other than those provided for in group B01D61/00
    • B01D53/323—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols by electrical effects other than those provided for in group B01D61/00 by electrostatic effects or by high-voltage electric fields
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
    • B01D53/34—Chemical or biological purification of waste gases
    • B01D53/46—Removing components of defined structure
    • B01D53/60—Simultaneously removing sulfur oxides and nitrogen oxides
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2251/00—Reactants
    • B01D2251/10—Oxidants
    • B01D2251/102—Oxygen
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2252/00—Absorbents, i.e. solvents and liquid materials for gas absorption
    • B01D2252/10—Inorganic absorbents
    • B01D2252/103—Water
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2257/00—Components to be removed
    • B01D2257/30—Sulfur compounds
    • B01D2257/302—Sulfur oxides
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2257/00—Components to be removed
    • B01D2257/40—Nitrogen compounds
    • B01D2257/404—Nitrogen oxides other than dinitrogen oxide
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2258/00—Sources of waste gases
    • B01D2258/02—Other waste gases
    • B01D2258/0283—Flue gases
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2259/00—Type of treatment
    • B01D2259/80—Employing electric, magnetic, electromagnetic or wave energy, or particle radiation
    • B01D2259/818—Employing electrical discharges or the generation of a plasma
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02A—TECHNOLOGIES FOR ADAPTATION TO CLIMATE CHANGE
    • Y02A50/00—TECHNOLOGIES FOR ADAPTATION TO CLIMATE CHANGE in human health protection, e.g. against extreme weather
    • Y02A50/20—Air quality improvement or preservation, e.g. vehicle emission control or emission reduction by using catalytic converters

Definitions

  • the present invention relates to the field of gas ionization discharge, plasma chemistry, and environmental engineering application technology, and relates to a method for oxidative desulfurization and denitration of hydroxyl radicals in an oxygen-active particle and an initiator injection into a flue.
  • Another advanced gas ionization discharge method is known as electron beam synergistic active absorbent and redox reagent NH 3 method.
  • an industrial test of 30xl0 4 m 3 /h flue gas was carried out on a 200MW unit in Chengdu, China.
  • the test flue gas temperature is 58 °C.
  • the desulfurization rate is over 80%, and the denitration rate is only 18%.
  • the test results show that the problem of ammonium salt recovery in pulse desulfurization and denitrification is solved.
  • the recovery rate is over 95%, which is about 90% higher than that of pulsed desulfurization and denitrification.
  • the problem of low flue gas denitration rate is not solved.
  • N 2 in the flue gas by the plasma reactor (origin) field is dissociated, ionized oxygen reacts with the new NO x, while the removal of NO x and side turn generates a new NO x, gas ionization visible removal discharge can not solve the problem of low efficiency of NO x in;
  • Electron beam method such as vacuum system, is huge, and X-ray radiation is seriously polluted;
  • the flue gas desulfurization and denitrification reaction has a low temperature, and a large heat exchanger with a temperature drop after first cooling is required; the energy consumption is further increased;
  • the object of the present invention is to overcome the deficiencies of the prior gas ionization discharge flue gas desulfurization and denitration methods, and to provide a method for oxidizing desulfurization and denitration of hydroxyl radicals into the flue by using oxygen active particles.
  • This The method is to inject a small flow rate, high concentration of oxygen active particles (0 2 +, 0 3, etc.) into the flue, and the oxygen active particles react with 0 2 + in the flue gas to form a high initial reaction rate constant of 2.2 X 10 6 L/mol.
  • the invention solves the problems existing in the current flue gas desulfurization and denitrification, realizes a new method of desulfurization and denitrification by using the catalyst, the absorbent and the reducing agent, does not produce any recontaminated by-products, and does not have any negative influence on the environment.
  • the oxygen radical oxidative desulfurization and denitration method of injecting oxygen-active particles into the flue is to inject oxygen-active particles [0 2 + , 0 3 , 0 ( ⁇ ⁇ ), 0 ( 3 ⁇ ), etc. into the flue of lm ⁇ 20 m long.
  • the oxygen-active particles react with water in the flue gas to form hydroxyl radicals and enthalpy, and in 1 to 10 s, ⁇ oxidizes and removes S0 2 , 1 ⁇ 0 ! in the flue gas ( and forms acid mist droplets
  • the charged coagulation and electric acid mist remover integrates a mixture of sulfuric acid and nitric acid, wherein:
  • the flue gas temperature is in the range of 40 ⁇ 120°C and the water content is in the range of 5 ⁇ 16% by volume.
  • the oxidative desulfurization and denitrification rate of bismuth reaches 80% respectively. ⁇ 98%, 85% ⁇ 99.8%.
  • the oxygen active particle generator is a strong ionization discharge electric field composed of a discharge electrode, a grounding electrode, a dielectric layer and a spacer, and the electric field strength thereof reaches 200Td ⁇ 400Td, and the average energy of the electron in the electric field reaches 6eV ⁇ 9eV.
  • Oxygen-active particles are injected into the flue to oxidize desulfurization and denitration equipment of hydroxyl radicals, which package a flue or reactor, an oxygen active particle generator, an acid mist remover, a charge condenser, etc., in which;
  • the charge condenser is composed of an ion source and an alternating condensation electric field disposed in the flue.
  • the ion source output ion concentration reaches 10 8 /cm 3 to 10 12 /cm 3 : the alternating electric field strength is 4Td ⁇ 100Td, frequency is 40Hz ⁇ 1.5kHz;
  • FIG. 1 The scheme of plasma chemical reaction between the oxygen molecules of 0 2 + and 0 3 injected into the flue 2 (or reactor) and the water molecules containing S0 2 and NO x flue gas 1 of the present invention is shown in FIG. 1 . Shown.
  • the invention adopts a strong electric field ionization discharge method to prepare a small flow rate and a high concentration of 0 2 +, 0 3 and other oxygen active particles 3 [0 2 +, 0 ( ! D), 0 ( 3 P), 0 3 , etc.
  • channel 2 (or reactor) the plasma reaction of 0 2 + in the oxygen-active particles with the water containing S0 2 and NO x flue gas 1 produces a high concentration (60 mg/L to 300 mg/L) and a high initial reaction.
  • a constant constant (2.2 X 10 6 L/mol.s) of H0 2 -peroxyhydroxy ion initiator, 0 2 +, 0 3 and other oxygen-active particles 3 react with initiator H0 2 to form a high concentration ⁇ ⁇ (30 mg / L ⁇ 150mg / L), the length of the flue ⁇ ⁇ lm ⁇ 20m oxidative removal of the flue gas S0 2, NO x, achieved without catalyst, absorbers, reducing agents and other conventional desulfurization and denitration method synergy, ⁇ oxidative desulfurization containing S0 2, NO x in the flue gas 1 is S0 2, NO x, and generating a mist, the removal rate of 80% ⁇ 98%, 85% ⁇ 99.8%, by generating a mist having charge properties and coagulation
  • the acid mist 8 recovered as an acid solution 9 in which H 2 S0 4 and HN0 3 are mixed, it can be seen from Fig. 1 that formation of scale and high concentration in the flue
  • This program will provide an effective and feasible new technology and method for solving the existing problems of flue gas desulfurization and denitrification technology.
  • the specific steps to implement the invention are: 1. Preparation of oxygen-active particles.
  • the key technology of the present invention is to newly develop an oxygen-active ion generator 5 which produces oxygen active particles 3 having a high concentration of 0 2 + and 0 3 , and its structure is shown in FIG. It is composed of a discharge plate 14, a grounding electrode 12, a dielectric layer 16, and a spacer 15.
  • the discharge electrode plate is formed by sintering a discharge electrode made of a metal material and an extremely thin (330 ⁇ m) dielectric layer 16 of the outer layer, and can also be processed into a discharge electrode plate 14 by a stainless steel thin plate, and the dielectric layer 16 is attached on the discharge side.
  • the grounding pole 12 is processed into a cavity plate by titanium or stainless steel, and a coolant is introduced into the cooling liquid inlet 13 to regulate the temperature of the plasma reaction process, and a thin dielectric layer 16 can also be sprayed on the surface of the grounding electrode.
  • dielectric material is pure ultrafine ⁇ 1 2 0 3 powder.
  • dielectric barrier discharge ionization method of the strong electric field having a concentration of oxygen to the inlet 17 reaches the input 02 80mg / L ⁇ 400mg / L of reactive oxygen species, 0.01mm between the discharge electrode plate dielectric layer and the ground electrode In the ⁇ 0.5mm discharge gap, the electric field strength is established in the range of 200Td ⁇ 400Td.
  • the average energy of the electron from the electric field is 7eV ⁇ 12eV, and most of the electrons have the most useful energy (8.4 e - ⁇ 2.5 eW).
  • the plasma reaction mode for generating oxygen-active particles is as shown in A of Fig. 2, and its plasma reaction formula:
  • the concentration of oxygen-active particles 3 [0 3 , 0 2 +, 0 ( ⁇ ⁇ ), 0 ( 3 ⁇ ), etc. is supplied to the flue to a concentration of 80 mg/L to 400 mg/L. 2. Formation of initiator H0 2 - in flue 2. 0 2 + in the oxygen-active particles reacts with water containing S0 2 , NO x flue gas 1 to form H0 2 —initiator, and its plasma reaction mode is shown as B in Fig. 2 Shown, its plasma chemical reaction formula:
  • H 2 0 2 and H0 2 - are in an equilibrium reaction state, and the concentration of the initiator H0 2 in the flue reaches 60 mg L to 300 mg L.
  • the oxygen-active particles 3 such as 0 2 + and 0 3 injected into the flue are subjected to a plasma chemical reaction at a ⁇ 0 2 hair styling agent to form a high-concentration active particle group mainly composed of ruthenium.
  • the plasma reaction mode for the formation of krypton in flue 2 is shown in Figure 2, and its plasma reaction formula:
  • the concentration of strontium reaches 30mg/L ⁇ 150mg/L.
  • NO x in the flue gas 1 is S0 2
  • An ion generating portion is provided in the charging condenser 23, and the unipolar ion concentration is 10 8 /cm 3 to 10 12 /cm 3 , so that the acid mist particles can be sufficiently charged in the charging condenser 23 The charge is coagulated and the particle size of the acid mist remover 8 is easily captured.
  • the fine acid mist drops through the charged coagulation and becomes the particle size that can be trapped by the acid mist remover 8.
  • the oxide ⁇ ⁇ S0 2 NO x formation of fine droplets, the field intensity of the alternating electric field equivalent 4 ⁇ l, 00Td, frequency of charge and a particle size of coagulation 40Hz ⁇ 1.5kHz 0. 5 ⁇ ! ⁇ ⁇ range of charged acid particles, easy to remove the acid mist trap.
  • the temperature and humidity regulator 19 is used to adjust the temperature and humidity of the S0 2 and NO x flue gas 1 so as to meet the requirements of the flue gas enthalpy oxidative desulfurization and denitrification chemical reaction, and the moisture content of the flue gas should be in the range of 5 to 16 vol%. Within, usually should be controlled at 10 ⁇ 12% by volume; the temperature is controlled at 40 ⁇ 120 °C.
  • the electric acid removal mist collector 8 collects the charged coagulation and forms a large particle size acid mist to become the acid liquid 9.
  • the electric field intensity of the electric acid mist removing device should be controlled at 0.8 ⁇ 30kV/cm, and the defogger efficiency should reach 98.0. ⁇ 99.8%.
  • reaction generation ⁇ 3 ⁇ 40 reaction generation ⁇ , oxidative removal of S0 2 , ⁇ (3 ⁇ 4 and formation of tiny acid mist droplets, this The reaction belongs to a new field of advanced oxidation technology applied to flue gas desulfurization and denitrification. Because of its fast chemical reaction rate, it is more than 7 orders of magnitude higher than the current desulfurization and denitration method.
  • the chemical reaction time of flue gas desulfurization and denitrification is only 1 ⁇ 10s, so the process is shortened and the equipment is reduced, which will greatly reduce equipment investment and Operating cost, greatly reducing energy consumption; achieving no external catalyst, absorbent and reducing agent; achieving simultaneous desulfurization and denitrification by thousand methods, and correspondingly reducing operating costs; realizing resource desulfurization and denitrification, production by-product is chemical product sulfuric acid and Nitric acid, which does not produce other by-products and pollutants, solves the problem that the by-products of desulfurization and denitrification are difficult to handle, and there is no problem of sewage treatment, thus achieving zero pollution and zero waste discharge to the environment, meeting the requirements of advanced oxidation technology. It is conducive to solving the problem of shortage of sulfur resources and high energy consumption of nitric acid production in China.
  • the invention can also be used alone for gas denitration or desulfurization.
  • Figure 1 is a schematic diagram of an advanced oxidative desulfurization and denitration scheme for injecting oxygen-active particles into a flue.
  • Figure 2 is a model diagram of the chemical reaction of oxidative desulfurization and off-gas plasma in the flue.
  • Figure 3 is a schematic view showing the structure of a plasma source.
  • Figure 4 is a flow chart showing the process of oxidative desulfurization and denitrification of hydroxyl radicals in the flue and acid formation.
  • Fig. 5 is a graph showing the effect of the molar ratio of oxygen-active particles to S0 2 and NO x on desulfurization and denitrification.
  • Figure 6 is a graph of the effect of flue gas temperature on desulfurization and denitrification.
  • Figure ⁇ is a graph of the effect of the initial concentration of S0 2 and ⁇ on the desulfurization and denitrification in the flue gas.
  • Figure 8 is a graph showing the effect of water volume concentration in flue gas on desulfurization and denitrification.
  • Figure 9 is a graph of the effect of flue gas flow on desulfurization and denitrification.
  • Oxygen 5. Oxygen active particle generator; 6. High frequency high voltage power supply; 7. DC high voltage power supply;
  • the oxygen-active particle generator 5 of the oxygen-active particles 3 such as 0 2 +, 0 3 has a structure as shown in FIG.
  • the oxygen-reactive particle formation and desulfurization and denitration plasma chemical reaction model of the present invention is shown in Fig. 2.
  • the specific embodiment is shown in FIG.
  • a considerable amount of one thousandth of the amount of oxygen is injected into the oxygen active particle generator 5, and the high frequency and high voltage is applied to the discharge electrode plate 14 by the high frequency high voltage power source 6 of the oxygen active particle generator.
  • a strong ionization electric field with a refractive electric field strength of 200 to 400 Td is formed in the discharge gap between the grounding electrode 12 and the grounding electrode 12, and the oxygen activity of 0 2 +, 0 3 is formed after dissociation and ionization of the oxygen gas 4 to a concentration of 80 to 400 mg/L.
  • the enthalpy is removed in the flue 2 by removing the S0 2 and NO x flue gas 1 S0 2, NO x and generate submicron mist, and the mist is charged in the condenser 23 and the ion generating portion generating a concentration of 10 8 / cm 3 ⁇ 10 12 / cm 3 ions collectively Charged into the coagulation vessel and coagulation charged and an alternating electric field 23, the field frequency is 40Hz ⁇ 1.5kH Z, reduced field The intensity is 4 ⁇ 100Td, and the submicron acid mist is coagulated by an alternating electric field to form a particle size of 0.5 ⁇ ⁇ acid mist.
  • the electric acid mist eliminator 8 with electric field strength of 0.8 ⁇ 30kV/cm is integrated into the acid liquid 9, and the electric collection efficiency reaches 98.0 ⁇ 99.8%.
  • the recovered acid liquid 9 is chemically purified into sulfuric acid and nitric acid, and the resource recovery rate is reached. 50% ⁇ 98%.
  • the electric defogger is a cylindrical shape made of titanium steel with the outer casing grounded and a star corona pole placed in the middle.
  • the gas containing S0 2 and NO x flue gas 1 is desulfurized and denitrated, and the remaining active particles such as ruthenium are treated by the residual ruthenium breaker 25 into purified flue gas 11 and discharged by the CF type induced draft fan 10.
  • the Photon type (Austria) flue gas analyzer 22 was used to detect the S0 2 , NO x , 0 2 concentration, temperature, pressure difference and flow rate in the flue gas, and the acid was quantitatively analyzed by the ICS-1500 (USA) ion chromatograph 29 .
  • the liquid component was detected on-line using a self-made oxygen active particle concentration detector 30, and captured by a salicylic acid impregnated membrane-high performance liquid chromatography (HPLC) method.

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Abstract

La présente invention concerne un appareil utilisable en vue de la désulfuration et de la dénitration des gaz de combustion. Ledit appareil comprend un générateur d'ions oxygène actif, un agglomérateur électrostatique et un désembueur électrostatique pour brouillard chimique, le générateur d'ions oxygène actif comprenant une électrode de terre, une plaque d'électrode à décharge et une membrane. L'invention concerne également un procédé de désulfuration et de dénitration impliquant une oxydation des radicaux hydroxyle sous l'effet de l'injection d'ions oxygène actif dans les gaz de combustion. Ledit procédé comprend les étapes consistant à utiliser un générateur d'ions oxygène actif en vue de l'obtention de particules d'oxygène actif, puis à injecter ces particules dans les gaz de combustion pour les faire réagir avec lesdits gaz et produire des gouttelettes d'un brouillard chimique à base d'acide sulfurique et d'acide nitrique et, enfin, à agglomérer par voie électrostatique les gouttelettes de brouillard chimique ainsi formées qui sont ensuite recueillies sous la forme d'un liquide acide mixte. Ledit procédé permet une désulfuration et une dénitration simultanées sans recours ni à un catalyseur, ni à un absorbant ni à un agent réducteur et sans effet négatif sur l'environnement.
PCT/CN2011/077318 2010-07-19 2011-07-19 Appareil et procédé utilisables en vue de la désulfuration et de la dénitration des gaz de combustion WO2012010080A1 (fr)

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CN2010102359504A CN101961596A (zh) 2010-07-19 2010-07-19 氧活性粒子注入烟道中的羟基自由基氧化脱硫脱硝方法
CN201010235950.4 2010-07-19

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CN102764574A (zh) * 2012-07-16 2012-11-07 广东佳德环保科技有限公司 流光放电等离子体自由基注入烟气的脱硫脱硝方法
CN103204482A (zh) * 2013-04-12 2013-07-17 大连海事大学 一种制取硝酸的方法
CN103691264A (zh) * 2013-12-30 2014-04-02 大连海事大学 一种消除烟气中粒径小于二点五微米的二次颗粒前体物方法
CN103768942A (zh) * 2014-02-19 2014-05-07 大连海事大学 一种等离子体净化柴油机尾气方法
WO2020083097A1 (fr) * 2018-10-22 2020-04-30 上海必修福企业管理有限公司 Système et procédé de traitement d'émissions de moteur
CN111330423A (zh) * 2020-03-06 2020-06-26 昆明理工大学 一种同时去除氮氧化物和气态汞的方法
CN115445406A (zh) * 2022-09-30 2022-12-09 广东青扬环保科技有限公司 一种除尘脱硫脱硝一体化处理方法以及一体化处理装置

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