JPH0521608B2 - - Google Patents
Info
- Publication number
- JPH0521608B2 JPH0521608B2 JP61249889A JP24988986A JPH0521608B2 JP H0521608 B2 JPH0521608 B2 JP H0521608B2 JP 61249889 A JP61249889 A JP 61249889A JP 24988986 A JP24988986 A JP 24988986A JP H0521608 B2 JPH0521608 B2 JP H0521608B2
- Authority
- JP
- Japan
- Prior art keywords
- exhaust gas
- sulfamic acid
- acid compounds
- present
- radiation
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
- Expired - Lifetime
Links
- 239000007789 gas Substances 0.000 claims description 19
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical group [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 claims description 17
- 229910002091 carbon monoxide Inorganic materials 0.000 claims description 17
- IIACRCGMVDHOTQ-UHFFFAOYSA-N sulfamic acid Chemical class NS(O)(=O)=O IIACRCGMVDHOTQ-UHFFFAOYSA-N 0.000 claims description 16
- 239000002516 radical scavenger Substances 0.000 claims description 12
- 238000000034 method Methods 0.000 claims description 9
- 230000005855 radiation Effects 0.000 claims description 9
- 239000006227 byproduct Substances 0.000 claims description 8
- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 claims description 6
- 229910052739 hydrogen Inorganic materials 0.000 claims description 5
- 230000003009 desulfurizing effect Effects 0.000 claims description 4
- 239000001257 hydrogen Substances 0.000 claims description 3
- 230000001678 irradiating effect Effects 0.000 claims description 3
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 claims description 2
- 229910021529 ammonia Inorganic materials 0.000 claims description 2
- PAWQVTBBRAZDMG-UHFFFAOYSA-N 2-(3-bromo-2-fluorophenyl)acetic acid Chemical compound OC(=O)CC1=CC=CC(Br)=C1F PAWQVTBBRAZDMG-UHFFFAOYSA-N 0.000 description 6
- BFNBIHQBYMNNAN-UHFFFAOYSA-N ammonium sulfate Chemical compound N.N.OS(O)(=O)=O BFNBIHQBYMNNAN-UHFFFAOYSA-N 0.000 description 6
- 229910052921 ammonium sulfate Inorganic materials 0.000 description 6
- 235000011130 ammonium sulphate Nutrition 0.000 description 5
- 238000006477 desulfuration reaction Methods 0.000 description 5
- 230000023556 desulfurization Effects 0.000 description 5
- 238000006243 chemical reaction Methods 0.000 description 4
- 238000010894 electron beam technology Methods 0.000 description 4
- 230000000694 effects Effects 0.000 description 3
- 239000003337 fertilizer Substances 0.000 description 3
- 238000004519 manufacturing process Methods 0.000 description 3
- 239000000047 product Substances 0.000 description 3
- 238000002485 combustion reaction Methods 0.000 description 2
- 239000000428 dust Substances 0.000 description 2
- 238000005516 engineering process Methods 0.000 description 2
- 239000000618 nitrogen fertilizer Substances 0.000 description 2
- 238000004458 analytical method Methods 0.000 description 1
- 230000000052 comparative effect Effects 0.000 description 1
- 238000007796 conventional method Methods 0.000 description 1
- 238000000354 decomposition reaction Methods 0.000 description 1
- 238000001514 detection method Methods 0.000 description 1
- 239000012717 electrostatic precipitator Substances 0.000 description 1
- 238000002474 experimental method Methods 0.000 description 1
- 230000035784 germination Effects 0.000 description 1
- 150000002431 hydrogen Chemical class 0.000 description 1
- 230000006698 induction Effects 0.000 description 1
- 238000005259 measurement Methods 0.000 description 1
- 229910000069 nitrogen hydride Inorganic materials 0.000 description 1
- 125000004430 oxygen atom Chemical group O* 0.000 description 1
- 230000008635 plant growth Effects 0.000 description 1
- 238000011160 research Methods 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
- -1 sulfamic acid compound Chemical class 0.000 description 1
Classifications
-
- 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
Landscapes
- Treating Waste Gases (AREA)
Description
【発明の詳細な説明】
１ 産業上の利用分野
本発明はアンモニア添加と放射線照射により、
排ガスを脱硫・脱硝処理する方法に関するもので
ある。特に、本発明は、脱硫・脱硝処理の際に
OHラジカルの捕捉剤を存在させることによつて
生成する副生成物中のスルフアミン酸系化合物を
低減させるものである。[Detailed Description of the Invention] 1. Industrial Application Field The present invention provides
This invention relates to a method for desulfurizing and denitrating exhaust gas. In particular, the present invention provides
The presence of an OH radical scavenger reduces the amount of sulfamic acid compounds in by-products.
２ 従来の技術
従来技術として、NO−H2Ｏ−O2−N2系にお
いて、COまたはH2を添加した後、この系に放射
線を照射することによつて、OHラジカル、Ｏ原
子、およびHO2ラジカルを生成させて、NOおよ
びNO2を、NO2およびHNO3に変換して系中から
除去することができることが、本発明の出願前に
知られていた。2. Prior Art As a conventional technology, in a NO - H 2 O-O 2 -N 2 system, OH radicals, O atoms, and It was known prior to the filing of the present invention that HO 2 radicals can be generated to convert NO and NO 2 into NO 2 and HNO 3 and remove them from the system.
また、他の従来技術として、NH3添加による
排ガスの脱硫・脱硝処理方法において、NOxお
よび／またはSOxを含む排ガスに放射線照射を行
つてNOxおよび／またはSOxを硝安および／また
は硫安として除去することも本発明の出願前に知
られていた。 In addition, as another conventional technique, in a method for desulfurizing and denitrating exhaust gas by adding NH 3 , the exhaust gas containing NO x and/or SO x is irradiated with radiation to remove NO x and/or SO x with ammonium nitrate and/or ammonium sulfate. It was also known prior to the filing of the present invention to remove as
３ 発明が解決しようとする問題点
前者の従来技術の場合には、NO−H2Ｏ−O2
−N2系中のNOがHNO3に変換されて系中から除
去されるものであるので、肥料として価値のある
ものが、副生成物として得られるものではないと
いう問題点があつた。3 Problems to be solved by the invention In the case of the former prior art, NO-H 2 O-O 2
Since the NO in the -N 2 system is converted to HNO 3 and removed from the system, there was a problem that something valuable as a fertilizer was not obtained as a by-product.
また、後者の従来技術の場合には、肥料として
価値のある硝安および／または硫安が生成物とし
て得られるが、NH3の添加によつてわずかでは
あるが、スルフアミン酸系化合物も同時に生成す
ることが判明した。このスルフアミン酸系化合物
は、植物の発芽、生育に有害な物質であるため回
収された副生物をそのまま肥料として利用するこ
とは困難であつた。スルフアミン酸系化合物の分
解処理等も技術的には可能と考えられるが、その
工程が複雑となり不経済であるという問題点があ
つた。 In addition, in the case of the latter conventional technology, ammonium nitrate and/or ammonium sulfate, which are valuable as fertilizers, are obtained as products, but sulfamic acid compounds are also produced at the same time, albeit in small amounts, due to the addition of NH3 . There was found. Since this sulfamic acid compound is a substance harmful to the germination and growth of plants, it has been difficult to use the recovered by-product as it is as a fertilizer. Although decomposition treatment of sulfamic acid compounds is considered technically possible, the problem is that the process is complicated and uneconomical.
本発明は、前記問題点を解決するものであつ
て、このスルフアミン酸系化合物を放射線照射プ
ロセスの改善によつて抑制し、回収副生物をその
まま良質な窒素肥料として利用できることを目的
とするものである。 The present invention is intended to solve the above-mentioned problems, and aims to suppress the generation of sulfamic acid compounds by improving the radiation irradiation process, so that the recovered by-products can be used as they are as high-quality nitrogen fertilizer. be.
４ 問題点を解決するための手段
すなわち、本発明は、SOxおよび／またはNOx
を含む排ガスに放射線を照射し、照射前、照射中
または照射後の排ガスにNH3を添加し、SOxおよ
び／またはNOxを除去する方法において、得ら
れる副生物の硝安および／または硫安の純度を向
上させ、良質な窒素肥料として利用することがで
きるようにするために、照射反応工程において生
ずるOHラジカルを捕捉する、捕捉剤として一酸
化炭素または水素が用いられる。4 Means for solving the problem That is, the present invention solves the problem
In this method, the by-products ammonium nitrate and/or ammonium sulfate are removed by irradiating exhaust gas containing Carbon monoxide or hydrogen is used as a scavenger to capture the OH radicals generated during the irradiation reaction process in order to improve the purity and enable use as a high-quality nitrogen fertilizer.
一酸化炭素（CO）または水素（H2）の存在下
で、放射線を照射し、処理を行うことによつて、
副生物の硝安および／または硫安中の植物にとつ
て有害なスルフアミン酸系化合物を低減するもの
である。 By irradiation and treatment in the presence of carbon monoxide (CO) or hydrogen (H 2 ),
This reduces the amount of sulfamic acid compounds harmful to plants in ammonium nitrate and/or ammonium sulfate, which are by-products.
なお、上記の本発明を第１図に基いて説明す
る。 The above-mentioned invention will be explained based on FIG. 1.
燃焼用空気がブロアー１から供給されるボイラ
ー２中で、NOxおよびSOxを含有する排ガスが発
生する。この排ガスに、OHラジカルの捕捉剤
（COまたはH2）が、その添加装置３から適量添
付される。その後、この排ガスにNH3がライン
７から添付される。前記捕捉剤およびNH3の添
加量は、排ガス通路に設けられたCO分析計また
はH2分析計４、またはSOx分析計５およびNOx
分析計６の測定結果に基づいて調整される。 In the boiler 2, to which combustion air is supplied from the blower 1, exhaust gas containing NO x and SO x is generated. An appropriate amount of an OH radical scavenger (CO or H 2 ) is added to this exhaust gas from the addition device 3 . Thereafter, NH 3 is added to this exhaust gas from line 7. The amount of the scavenger and NH 3 added is determined by the CO analyzer or H 2 analyzer 4 installed in the exhaust gas passage, or the SO x analyzer 5 and the NO x analyzer 5.
Adjustments are made based on the measurement results of the analyzer 6.
この捕捉剤およびNH3が添加された排ガスは、
反応器８中に導入され、そこで電子ビーム発生装
置９からの電子ビームによつて照射処理される。
照射処理されたガスは集塵機１０に導入され、そ
こで副生物のスルフアミン酸系化合物を含有しな
い硝安および硫安が回収され、清浄化されたガス
がブロアー１１を通つて大気中に放出される。 The exhaust gas to which this scavenger and NH 3 have been added is
It is introduced into a reactor 8, where it is irradiated with an electron beam from an electron beam generator 9.
The irradiated gas is introduced into a dust collector 10, where ammonium nitrate and ammonium sulfate that do not contain by-products of sulfamic acid compounds are recovered, and the purified gas is discharged into the atmosphere through a blower 11.
５ 作用
本発明において、OHラジカルの捕捉剤として
COまたはH2を存在させた場合に、スルフアミン
酸系化合物が低減される作用は、次のようなもの
であると考えられる。5 Action In the present invention, as a scavenger for OH radicals
The effect of reducing sulfamic acid compounds in the presence of CO or H 2 is thought to be as follows.
スルフアミン酸系化合物は、放射線照射により
排ガス中に生成する活性種中のOHラジカルと
SO2との反応によつて生成することが判明した。 Sulfamic acid compounds combine with OH radicals in active species generated in exhaust gas due to radiation irradiation.
It was found to be produced by reaction with SO 2 .
また、SO2がOHラジカルと反応する物（OH
ラジカルの捕捉剤）を添加することにより、スル
フアミン酸系化合物の生成を抑制し、実質的にゼ
ロにすることができることが確認された。 In addition, SO 2 reacts with OH radicals (OH
It was confirmed that by adding a radical scavenger), the production of sulfamic acid compounds can be suppressed and reduced to substantially zero.
上記のことをより具体的に説明するために、ス
ルフアミン酸系化合物（NH2SO3Ｈ）の生成にお
ける推定反応メカニズムを式で表わすと下記のご
とくである。 In order to explain the above more specifically, the estimated reaction mechanism in the production of sulfamic acid compounds (NH 2 SO 3 H) is expressed as follows.
SO2＋OH→
SO3Ｈ (2)
NH3＋OH→
NH2＋H2Ｏ (3)
SO3Ｈ＋NH2→
NH2SO3Ｈ (4)
一方、COを添加すると、(2)，(3)式より速く下
記の(5)式が進行し、(2)〜(4)式を経て生成するスル
フアミン酸系化合物の生成が抑制される。 SO 2 +OH→ SO 3 H (2) NH 3 +OH→ NH 2 +H 2 O (3) SO 3 H+NH 2 → NH 2 SO 3 H (4) On the other hand, when CO is added, equations (2) and (3) The following formula (5) proceeds more quickly, and the production of sulfamic acid compounds produced through formulas (2) to (4) is suppressed.
CO＋OH→CO2＋Ｈ (5)
Ｈ＋O2→HO2 (6)
なお、COに捕捉されたOHラジカルから(6)式
に示す反応により別種のHO2ラジカルが生成し、
これが脱硫・脱硝に寄与する結果、CO無添加の
場合に比べ、脱硫率、脱硝率は向上する。このた
め、本発明は、より経済的、実用的であることが
分つた。 CO + OH → CO 2 + H (5) H + O 2 → HO 2 (6) In addition, another type of HO 2 radical is generated from the OH radical captured by CO by the reaction shown in equation (6),
As a result of this contributing to desulfurization and denitrification, the desulfurization rate and denitrification rate are improved compared to the case without the addition of CO. Therefore, the present invention was found to be more economical and practical.
６ 実施例
次に本発明についてその具体的な実施例により
説明する。6 Examples Next, the present invention will be explained using specific examples.
実施例 １
SO2200ppm、NOx185ppm、CO Oppmを含有
し、流量15／minの排ガスにNH3585ppmを加
え、更にCOを10000ppm添加した後に、80℃で電
子線を1.8Mrad照射した（日本原子力研究所の１
号加速器を使用）。Example 1 After adding 585 ppm of NH 3 to the exhaust gas containing 200 ppm of SO 2 , 185 ppm of NO x and 185 ppm of CO and a flow rate of 15/min and further adding 10,000 ppm of CO, it was irradiated with an electron beam of 1.8 Mrad at 80°C (Japan Atomic Energy Research Institute 1
(using a No. 1 accelerator).
照射後の排ガスを電気集塵機に通し、生成した
生成物を捕集して分析した結果によると、スルフ
アミン酸系化合物は検出限界以下（0.001％以下）
であつた。 According to the results of passing the exhaust gas after irradiation through an electrostatic precipitator and collecting and analyzing the generated products, sulfamic acid compounds were below the detection limit (0.001% or less).
It was hot.
また、その際の脱硫率は93％、脱硝率は99％で
あつた。 Furthermore, the desulfurization rate at that time was 93% and the denitrification rate was 99%.
比較例 １
COを添加することなく、他は実施例１と同じ
条件で実施した。その生成物を分析した結果、ス
ルフアミン酸系化合物は1.7％存在した。Comparative Example 1 The experiment was carried out under the same conditions as in Example 1 except that CO was not added. Analysis of the product revealed that 1.7% of sulfamic acid compounds were present.
その際の脱硫率は76％、脱硝率は80％であつ
た。 At that time, the desulfurization rate was 76% and the denitrification rate was 80%.
７ 発明の効果
本発明においては、アンモニア添加と放射線照
射による排ガスの脱硫・脱硝方法において、放射
線照射の際にOHラジカルの捕捉剤を添加するこ
とによつて、スルフアミン酸系化合物の生成を抑
制し、植物に有害なスルフアミン酸系化合物が含
有されない硝安および／または硫安が得られるも
のである。7 Effects of the Invention In the present invention, in a method for desulfurizing and denitrating exhaust gas by adding ammonia and irradiating radiation, the generation of sulfamic acid compounds is suppressed by adding an OH radical scavenger during radiation irradiation. , ammonium nitrate and/or ammonium sulfate that does not contain sulfamic acid compounds harmful to plants can be obtained.
また前記捕捉剤を添加することによつて、排ガ
スの脱硝率および脱硫率を高く保持することがで
きるという顕著な効果も生じる。 Further, by adding the scavenger, a remarkable effect is produced in that the denitrification rate and desulfurization rate of the exhaust gas can be maintained high.
第１図は、本発明を実施する際のフローシート
を表わすものである。
１……燃焼用空気供給ブロアー、２……ボイラ
ー、３……捕捉剤の添加位置、４……CO分析計
またはH2分析計、５……SOx分析計、６……
NOx分析計、７……NH3添加位置、８……反応
器、９……電子ビーム発生装置、１０……集塵
機、１１……排ガス誘引フアン。
FIG. 1 represents a flow sheet for implementing the present invention. 1...Combustion air supply blower, 2...Boiler, 3...Scavenger addition position, 4...CO analyzer or H2 analyzer, 5...SO x analyzer, 6...
NO x analyzer, 7... NH 3 addition position, 8... Reactor, 9... Electron beam generator, 10... Dust collector, 11... Exhaust gas induction fan.
Claims (1)
を脱硫・脱硝処理する方法において、OHラジカ
ルの捕捉剤の存在下で放射線を照射し、生成する
副生成物中のスルフアミン酸系化合物を低減する
ことを特徴とする放射線照射排ガス処理方法。 ２ 前記OHラジカルの捕捉剤が一酸化炭素
（CO）または水素（H2）であることを特徴とす
る特許請求の範囲第１項に記載の方法。[Claims] 1. In a method for desulfurizing and denitrating exhaust gas by adding ammonia and irradiating radiation, radiation is irradiated in the presence of an OH radical scavenger, and sulfamic acid compounds in the generated by-products are removed. A radiation irradiation exhaust gas treatment method characterized by reducing radiation irradiation. 2. The method according to claim 1, wherein the OH radical scavenger is carbon monoxide (CO) or hydrogen ( H2 ).
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP61249889A JPS63104635A (en) | 1986-10-21 | 1986-10-21 | Exhaust gas treatment by addition of ammonia and irradiation of radiant ray |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP61249889A JPS63104635A (en) | 1986-10-21 | 1986-10-21 | Exhaust gas treatment by addition of ammonia and irradiation of radiant ray |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| JPS63104635A JPS63104635A (en) | 1988-05-10 |
| JPH0521608B2 true JPH0521608B2 (en) | 1993-03-25 |
Family
ID=17199716
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP61249889A Granted JPS63104635A (en) | 1986-10-21 | 1986-10-21 | Exhaust gas treatment by addition of ammonia and irradiation of radiant ray |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JPS63104635A (en) |
Families Citing this family (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| EP0269060B1 (en) * | 1986-11-26 | 1991-05-08 | Ebara Corporation | Process for treating by-product of radiation treatment of ammonia-added effluent gas |
| JPH0640945B2 (en) * | 1987-12-10 | 1994-06-01 | 株式会社荏原製作所 | Radiation irradiation exhaust gas treatment method |
| WO1998023557A1 (en) * | 1996-11-25 | 1998-06-04 | Ebara Corporation | Process and apparatus for producing fertilizer from sulfur oxide-containing gas |
| KR19990018051A (en) * | 1997-08-26 | 1999-03-15 | 김징완 | Flue gas treatment method by electron beam irradiation |
Citations (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPS59222213A (en) * | 1983-05-30 | 1984-12-13 | Japan Atom Energy Res Inst | Treatment of waste gas |
-
1986
- 1986-10-21 JP JP61249889A patent/JPS63104635A/en active Granted
Patent Citations (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPS59222213A (en) * | 1983-05-30 | 1984-12-13 | Japan Atom Energy Res Inst | Treatment of waste gas |
Also Published As
| Publication number | Publication date |
|---|---|
| JPS63104635A (en) | 1988-05-10 |
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