JP2781518B2 - NO remover - Google Patents
NO removerInfo
- Publication number
- JP2781518B2 JP2781518B2 JP6094182A JP9418294A JP2781518B2 JP 2781518 B2 JP2781518 B2 JP 2781518B2 JP 6094182 A JP6094182 A JP 6094182A JP 9418294 A JP9418294 A JP 9418294A JP 2781518 B2 JP2781518 B2 JP 2781518B2
- Authority
- JP
- Japan
- Prior art keywords
- activated carbon
- nox
- nitric acid
- removal
- oxygen
- 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 - Fee Related
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- Carbon And Carbon Compounds (AREA)
- Treating Waste Gases (AREA)
- Solid-Sorbent Or Filter-Aiding Compositions (AREA)
Description
【０００１】[0001]
【産業上の利用分野】本発明は、空気中に含まれる二酸
化窒素（ＮＯ2）・一酸化窒素（ＮＯ）（以下ＮＯ2、Ｎ
Ｏを総称してＮＯｘという）を除去するＮＯ除去剤およ
びＮＯｘ除去ユニットおよびＮＯｘ除去装置に関するも
のである。The present invention relates to nitrogen dioxide contained in the air (NO 2) · nitric oxide (NO) (hereinafter NO 2, N
The present invention relates to a NO removal agent, a NOx removal unit, and a NOx removal device that remove NO (collectively referred to as NOx).
【０００２】[0002]
【従来の技術】近年、自動車などの増加によりＮＯｘの
濃度が上昇し、しばしば環境基準値を上回るようになっ
てきており、ＮＯｘを除去する材料開発が要望されてい
る。2. Description of the Related Art In recent years, the concentration of NOx has increased due to an increase in automobiles and the like, and has often exceeded an environmental standard value. Therefore, development of a material for removing NOx has been demanded.
【０００３】従来、この種のＮＯｘ除去技術は大別する
と、前処理技術としての燃料からの含窒素化合物の除
去、燃料燃焼中のサーマルＮＯｘの低減、ＮＯｘの
後処理技術がある。[0003] Conventionally, this type of NOx removal technology can be roughly classified into removal of nitrogen-containing compounds from fuel, reduction of thermal NOx during fuel combustion, and NOx post-treatment technology as pretreatment technologies.
【０００４】は石油化学関連技術としては重要である
が、これを成因とするＮＯｘの発生量はわずかである。
に関してガスタービン、ボイラー内でのサーマルＮＯ
ｘの燃焼に触媒燃焼が提案されている。の方法を大別
すると、乾式法と湿式法があり、乾式法としては分解
法、接触還元法、吸着法、吸収法があり、湿式法として
は酸化吸収法、酸化還元吸収法、錯塩吸収法がある。特
に簡易的にＮＯｘを除去するＮＯｘ除去剤としては、水
酸化カルシウムを主成分とする乾式の吸収剤がある（特
開昭５３−１３１２７２号公報）。またＮＯの分解触媒
に関しては金属イオン担持ゼオライトがある（特開平２
−２５１２４７、２５１２４８公報）。[0004] Although is important as a petrochemical-related technology, the amount of NOx generated due to this is small.
Thermal NO in gas turbines and boilers
Catalytic combustion has been proposed for the combustion of x. The methods are roughly divided into dry method and wet method.The dry method includes decomposition method, catalytic reduction method, adsorption method and absorption method, and the wet method includes oxidation absorption method, redox absorption method and complex salt absorption method. There is. As a NOx removing agent for removing NOx in a simple manner, there is a dry absorbent mainly composed of calcium hydroxide (JP-A-53-131272). As for the NO decomposition catalyst, there is a zeolite supporting metal ions (Japanese Patent Laid-Open No.
251247, 251248).
【０００５】[0005]
【発明が解決しようとする課題】このような従来の方法
は開発中であり、実用化されているものはほとんどない
か、実用化されているものであっても、空気中（酸素濃
度が高い場合）のＮＯｘを除去することは酸化雰囲気と
なるため、酸素による被毒がおこり触媒を利用してＮＯ
ｘを窒素まで還元することは非常に困難である。他の方
法についても、高温度が必要か、あるいはコストが非常
に高いという課題があった。また、ＮＯｘの中でもＮＯ
は特に除去することが困難であるという課題があり、こ
のＮＯの除去触媒に関して有効であるとされている金属
イオン担持ゼオライトは活性が低く、また３００℃〜８
００℃の高温が必要であり、ＮＯｘ除去剤のほかに加熱
手段が必要となるため、コストがかり、また応用できる
民生用品が限られる。また、通常の活性炭にＮＯｘガス
を通風した場合、ＮＯについてはほとんど除去されない
が、ＮＯ2はある程度除去される。しかし、除去された
ＮＯ2の一部が活性炭でＮＯに還元されるという課題が
あった。Such conventional methods are under development, and few of them have been put into practical use, or even if they have been put into practical use, they have been used in the air (at high oxygen concentrations). In this case, the removal of NOx becomes an oxidizing atmosphere, so that poisoning by oxygen occurs and NO is removed by using a catalyst.
It is very difficult to reduce x to nitrogen. Other methods also have a problem that a high temperature is required or the cost is very high. Also, among NOx, NO
Has a problem that it is particularly difficult to remove the metal ion-supported zeolite, which is said to be effective for this NO removal catalyst, and has a low activity.
Since a high temperature of 00 ° C. is required, and a heating means is required in addition to the NOx removing agent, cost is high and applicable consumer goods are limited. When NOx gas is passed through ordinary activated carbon, NO is hardly removed, but NO 2 is removed to some extent. However, there was a problem that a part of the removed NO 2 was reduced to NO by activated carbon.
【０００６】また、本発明者らが発見したＮＯ2の除去
性能がすぐれたＮＯｘ除去剤でも、ＮＯ2濃度がＮＯ濃
度に比べ非常に高い場合のガスを通風した場合には、平
衡関係から微量ではあるがＮＯへ還元するという課題が
あった（特出平５−１６４３４５号公報）。Further, in case the NOx removing agent present inventors have superior has discovered NO 2 removal performance, the NO 2 concentration was ventilated very high when gas compared to NO concentration, trace from equilibrium However, there was a problem of reduction to NO (Japanese Patent Publication No. 5-164345).
【０００７】本発明は、上記課題を解決するもので、常
温にて活性のあるＮＯ除去剤を提供することを第１の目
的とする。[0007] The present invention has been made to solve the above problems, and has as its first object to provide a NO remover which is active at ordinary temperature.
【０００８】第２の目的は、ＮＯの再放出を防止したＮ
Ｏ除去剤を提供することである。A second object is to prevent N from being re-released.
It is to provide an O remover.
【０００９】[0009]
【課題を解決するための手段】本発明の第１の目的を達
成するための第１の手段は、活性炭の表面を酸化表面に
し、かつ酸素とともに窒素でも前記活性炭の表面を覆う
処理を行なったものである。A first means for achieving the first object of the present invention is to make the surface of the activated carbon an oxidized surface, and to cover the surface of the activated carbon with nitrogen together with oxygen. Things.
【００１０】また、第２の目的を達成するための第２の
手段は、活性炭の表面を酸化表面にし、かつ前記活性炭
の表面を酸素とともに窒素でも覆う処理をした後、ＰＨ
値を７〜９に調整処理したものである。A second means for achieving the second object is to make the surface of the activated carbon an oxidized surface and to cover the surface of the activated carbon with nitrogen together with oxygen,
The value is adjusted to 7 to 9.
【００１１】[0011]
【作用】本発明は上記した第１の手段の構成により、活
性炭の表面を酸素で覆い、酸化表面にするとともに、酸
素だけでなく窒素も覆うこととなり、窒素の持つ非共有
電子対により活性点が増加しＮＯ除去性能が向上するも
のである。According to the first aspect of the present invention, the surface of the activated carbon is covered with oxygen to form an oxidized surface and also covers not only oxygen but also nitrogen. And the NO removal performance is improved.
【００１２】また、第２の手段の構成により、処理後の
ｐＨ値を７〜９にすることで活性炭表面に酸化吸着され
たＮＯを塩の形で保持でき、ＮＯの再放出を防止するこ
とができる。Further, by the constitution of the second means, the NO value oxidized and adsorbed on the activated carbon surface can be held in the form of a salt by setting the pH value after the treatment to 7 to 9, thereby preventing the re-release of NO. Can be.
【００１３】[0013]
【実施例】以下本発明の第１実施例について説明する。The first embodiment of the present invention will be described below.
【００１４】活性炭を硝酸で処理することにより、活性
炭の表面を酸素で覆うとともに、酸素だけでなく窒素も
覆うこととなり、窒素の持つ非共有電子対により活性点
が増加しＮＯ除去性能が向上する。[0014] By treating the activated carbon with nitric acid, the surface of the activated carbon is covered with oxygen and not only oxygen but also nitrogen, and the active sites are increased by the lone pair of electrons possessed by nitrogen, so that the NO removal performance is improved. .
【００１５】この活性炭を硝酸で処理したＮＯ除去剤の
ＮＯ除去性能を説明する。やしがら活性炭１２０ｇを６
１％の硝酸５０ｃｃに４８時間浸積した。これをろ過
し、炭酸ナトリウムで中和後１１０℃で３時間乾燥し
た。この硝酸処理した活性炭を横型の内径２０ｍｍのガ
ラスカラムに２ｇ充填し、片側から、空気希釈の一酸化
窒素ガス１ｐｐｍを２リットル／分で通風した。一酸化
窒素の入口濃度と出口濃度度を化学発光式のＮＯｘ計で
測定し、式Ｉによって除去率を求めた。The NO removal performance of the NO remover obtained by treating the activated carbon with nitric acid will be described. 6 g of activated charcoal 120g
It was immersed in 50 cc of 1% nitric acid for 48 hours. This was filtered, neutralized with sodium carbonate, and dried at 110 ° C. for 3 hours. 2 g of the activated carbon treated with nitric acid was packed in a horizontal glass column having an inner diameter of 20 mm, and 1 ppm of an air-diluted nitric oxide gas was blown from one side at 2 liter / min. The inlet concentration and outlet concentration of nitric oxide were measured with a chemiluminescent NOx meter, and the removal rate was determined by the formula I.
【００１６】 除去率％＝［１−（出口濃度／入口濃度）］×１００ （Ｉ） その結果を図２に示す。図１に無処理の活性炭の性能を
示すが、ＮＯ処理を行なうと、図２に示すようにＮＯ除
去性能が高性能となる。このように硝酸で活性炭を処理
することでＮＯ除去性能を向上させることができる。Removal rate% = [1- (outlet concentration / inlet concentration)] × 100 (I) The results are shown in FIG. FIG. 1 shows the performance of the untreated activated carbon. When the NO treatment is performed, the NO removal performance becomes high as shown in FIG. By treating the activated carbon with nitric acid in this way, the NO removal performance can be improved.
【００１７】次に本発明の第２実施例について説明す
る。活性炭を硝酸処理する場合に最適な硝酸濃度は少な
くとも、活性炭１ｇに対して硝酸そのものの重量は０．
０１ｇ、すなわち１％の硝酸を含浸させることが必要で
ある。また、硝酸の量が多くても活性炭の活性点を減少
させることになる。Next, a second embodiment of the present invention will be described. When the activated carbon is treated with nitric acid, the optimum nitric acid concentration is at least 0.1 g per 1 g of activated carbon.
It is necessary to impregnate 01 g, ie 1% nitric acid. Further, even if the amount of nitric acid is large, the active point of activated carbon is reduced.
【００１８】やしがら活性炭１２０ｇを６１％硝酸２５
ｃｃ、５０ｃｃ、７１ｃｃ、１２０ｃｃを純水希釈し１
６５ｃｃとしたものおよび６１％硝酸１６５ｃｃに４８
時間浸積した。これはやしがら活性炭１ｇに対して硝酸
の重量でそれぞれ０．１８、０．３５、０．５０、０．
８０、１．２０ｇに相当し、重量比で示すと１８、３
５、５０、８０、１２０％である。Yashigara 120 g of activated carbon is mixed with 61% nitric acid 25
cc, 50cc, 71cc, 120cc diluted with pure water
48 to 65cc and 165cc of 61% nitric acid
Time immersion. These are 0.18, 0.35, 0.50, and 0.18, 0.35, 0.50, and 0.
80, 1.20 g.
5, 50, 80, and 120%.
【００１９】これらの各硝酸濃度で処理した活性炭を横
型の内径２０ｍｍのガラスカラムに５ｇ充填し、片側か
ら、空気希釈の一酸化窒素ガス２００ｐｐｍを２リット
ル／分で通風した。（第１実施例と違って、加速試験を
実施）一酸化窒素の入口濃度と出口濃度をガス検知管
（北川式）で測定し、式Ｉによって除去率を求めた。そ
の結果を図３に示す。5 g of the activated carbon treated with each of these nitric acid concentrations was filled in a horizontal glass column having an inner diameter of 20 mm, and from one side, 200 ppm of an air-diluted nitric oxide gas was blown at 2 liter / min. (According to the first embodiment, an accelerated test was performed.) The inlet concentration and the outlet concentration of nitric oxide were measured with a gas detector tube (Kitakawa formula), and the removal rate was determined by formula I. The result is shown in FIG.
【００２０】このように活性炭の重量に対する硝酸の重
量％は１〜１００％でＮＯ除去活性を持つが、５０〜８
０％が最も好ましく１００％以上含浸するとＮＯ除去性
能が低下し、製造時にＮＯ2ガスが発生する。したがっ
て、活性炭に対する硝酸の重量％を１〜１００％とする
ことでＮＯ除去性能を向上させることができる。As described above, the weight percentage of nitric acid based on the weight of activated carbon is 1 to 100% and has NO removal activity, but 50 to 8%.
If 0% is the most preferable and if 100% or more is impregnated, the NO removal performance is reduced, and NO 2 gas is generated during the production. Therefore, NO removal performance can be improved by setting the weight percentage of nitric acid to activated carbon to 1 to 100%.
【００２１】次に、本発明の第３実施例について説明す
る。活性炭に硝酸を含浸させ、酸化表面にした時点で活
性炭のＰＨ値は１以下である。硝酸処理を行った後、こ
の活性炭のＰＨ値を１〜１２まで炭酸ナトリウムの様な
弱塩基性物質を用いてコントロールした。硝酸処理を行
ったやしがら活性炭３０ｇを２５０ｃｃの純水で洗浄
し、５％（ｗｔ／ｗｔ）炭酸ナトリウム水溶液８０ｃ
ｃ、１６０ｃｃ、２４０ｃｃ、２８０ｃｃ、３２０ｃ
ｃ、および４００ｃｃに浸積し、１時間振とうした。そ
の後活性炭をろ過し、さらに８０ｃｃの純水で３回洗浄
した。その後１１０℃で３時間乾燥した。この中和処理
を行った硝酸処理活性炭のＰＨ値はそれぞれ２、４．
５、７、９、９．５および１２である。これらのＰＨ値
をコントロールした活性炭を横型の内径２０ｍｍのガラ
スカラムに５ｇ充填し、片側から空気希釈の一酸化窒素
ガス１０ｐｐｍを２リットル／分で通風した。一酸化窒
素の入口濃度と出口濃度を化学発光式ＮＯｘ計で測定
し、式Ｉによって除去率を求めた。その結果を図４に示
す。Next, a third embodiment of the present invention will be described. When activated carbon is impregnated with nitric acid to form an oxidized surface, the PH value of the activated carbon is 1 or less. After the nitric acid treatment, the pH value of the activated carbon was controlled from 1 to 12 using a weakly basic substance such as sodium carbonate. 30 g of activated carbon treated with nitric acid is washed with 250 cc of pure water, and a 5% (wt / wt) aqueous sodium carbonate solution 80 c
c, 160cc, 240cc, 280cc, 320c
c and 400 cc and shaken for 1 hour. Thereafter, the activated carbon was filtered and further washed three times with 80 cc of pure water. Thereafter, it was dried at 110 ° C. for 3 hours. The pH values of the neutralized nitric acid-treated activated carbon were 2, 4 and 4, respectively.
5, 7, 9, 9.5 and 12. 5 g of the activated carbon having a controlled PH value was filled in a horizontal glass column having an inner diameter of 20 mm, and 10 ppm of air-diluted nitric oxide gas was blown from one side at 2 liter / min. The inlet concentration and outlet concentration of nitric oxide were measured with a chemiluminescent NOx meter, and the removal rate was determined by Formula I. FIG. 4 shows the results.
【００２２】このように硝酸処理を行った後、中和を行
い、活性炭のＰＨ値をコントロールする際、ＰＨ値は７
〜９でＮＯに対する除去活性を得ることができるが、Ｐ
Ｈ８〜９が最も好ましく、ＰＨ値がこの範囲内であれば
ＮＯがＮＯ→ＮＯ2→ＮＯ3となり酸化吸着されたあと塩
を形成し、安定化する。ＰＨ値が７未満ではＮＯ除去性
能は低下し、ＰＨ値１０以上にするには非常に時間がか
かり不経済である。したがって、活性炭のＰＨ値を７〜
９にすることでＮＯ除去後の脱離を効率よく防止するこ
とができる。After the nitric acid treatment, neutralization is performed to control the PH value of the activated carbon.
-9, the removal activity against NO can be obtained.
H8 to 9 are most preferable. If the PH value is within this range, NO becomes NO → NO 2 → NO 3 , and after oxidatively adsorbed, a salt is formed and stabilized. If the PH value is less than 7, the NO removal performance is reduced, and it takes a very long time to achieve a PH value of 10 or more, which is uneconomical. Therefore, the pH value of activated carbon is 7 ~
By setting it to 9, desorption after NO removal can be efficiently prevented.
【００２３】[0023]
【発明の効果】以上の実施例から明らかなように、活性
炭の表面を酸化表面にし、かつ酸素とともに窒素でも前
記活性炭の表面を覆う処理をすることで、空気中に含ま
れる低濃度のＮＯに対して除去性能が高いＮＯ除去剤を
提供できるという実用上大きな効果が得られる。As is apparent from the above embodiments, the surface of the activated carbon is made to be an oxidized surface, and the surface of the activated carbon is also covered with nitrogen together with oxygen, so that low-concentration NO contained in the air can be reduced. On the other hand, a practically great effect of providing a NO removing agent having a high removal performance can be obtained.
【００２４】また、活性炭の表面を酸化表面にし、かつ
前記活性炭の表面を酸素とともに窒素でも覆う処理した
後、ＰＨを７〜９に調整することでＮＯの再放出を防止
したＮＯ除去剤を提供することができる。Further, the present invention provides a NO remover which prevents the re-release of NO by adjusting the pH to 7 to 9 after treating the surface of the activated carbon with an oxidized surface and covering the surface of the activated carbon with nitrogen together with oxygen. can do.
【図１】本発明の第１実施例の一酸化窒素除去性能図FIG. 1 is a diagram showing the performance of removing nitric oxide according to a first embodiment of the present invention.
【図２】同第２実施例の一酸化窒素除去性能図FIG. 2 is a graph showing the performance of removing nitric oxide according to the second embodiment.
【図３】同第３実施例の一酸化窒素除去性能図FIG. 3 is a graph showing the performance of removing nitric oxide according to the third embodiment.
【図４】同第４実施例の一酸化窒素除去性能図FIG. 4 is a diagram showing the performance of removing nitric oxide according to the fourth embodiment.
───────────────────────────────────────────────────── フロントページの続き (72)発明者 田代 義和 大阪府大阪市城東区今福西６丁目２番61 号 松下精工株式会社内 (56)参考文献 特開 平５−253435（ＪＰ，Ａ) 特開 平４−293542（ＪＰ，Ａ) 特開 平４−90849（ＪＰ，Ａ) 特開 昭64−85137（ＪＰ，Ａ) 特開 平６−126161（ＪＰ，Ａ) (58)調査した分野(Int.Cl.6，ＤＢ名) B01J 20/00 - 20/34────────────────────────────────────────────────── ─── Continuation of the front page (72) Inventor Yoshikazu Tashiro, Matsushita Seiko Co., Ltd., 6-2-61 Imafukunishi, Joto-ku, Osaka-shi, Osaka (56) JP-A-4-293542 (JP, A) JP-A-4-90849 (JP, A) JP-A-64-85137 (JP, A) JP-A-6-126161 (JP, A) (58) Int.Cl. 6 , DB name) B01J 20/00-20/34
Claims (2)
ともに窒素でも前記活性炭の表面を覆う処理をしてなる
ＮＯ除去剤。1. A NO remover obtained by treating the surface of activated carbon with an oxidized surface and covering the surface of the activated carbon with nitrogen together with oxygen.
性炭の表面を酸素とともに窒素でも覆う処理をした後、
ｐＨを７〜９に調整した請求項１記載のＮＯ除去剤。2. After the surface of the activated carbon is oxidized and the surface of the activated carbon is covered with nitrogen together with oxygen,
The NO remover according to claim 1, wherein the pH is adjusted to 7 to 9.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP6094182A JP2781518B2 (en) | 1993-12-24 | 1994-05-06 | NO remover |
Applications Claiming Priority (3)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP5-329067 | 1993-12-24 | ||
| JP32906793 | 1993-12-24 | ||
| JP6094182A JP2781518B2 (en) | 1993-12-24 | 1994-05-06 | NO remover |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| JPH07227538A JPH07227538A (en) | 1995-08-29 |
| JP2781518B2 true JP2781518B2 (en) | 1998-07-30 |
Family
ID=26435463
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP6094182A Expired - Fee Related JP2781518B2 (en) | 1993-12-24 | 1994-05-06 | NO remover |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JP2781518B2 (en) |
Families Citing this family (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| EP1545305B1 (en) * | 2002-09-16 | 2006-07-19 | Aerocrine AB | Scrubber |
| KR100669490B1 (en) * | 2005-11-30 | 2007-01-16 | 주식회사 케이티앤지 | Process for surface modification of activated carbon |
Family Cites Families (5)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPS6485137A (en) * | 1987-09-26 | 1989-03-30 | Osaka Gas Co Ltd | Active carbon fiber capable of adsorbing nitric oxide and manufacture thereof |
| JPH0490849A (en) * | 1990-08-03 | 1992-03-24 | Sakai Chem Ind Co Ltd | Nitrogen oxide adsorbing agent |
| JP3068231B2 (en) * | 1991-03-22 | 2000-07-24 | 株式会社神戸製鋼所 | NO adsorbent |
| JPH05253435A (en) * | 1991-12-12 | 1993-10-05 | Kobe Steel Ltd | Nitrogen monoxide adsorbent and production thereof |
| JPH06126161A (en) * | 1992-10-13 | 1994-05-10 | Meidensha Corp | Denitration agent, method for manufacturing denitration agent and denitration method |
-
1994
- 1994-05-06 JP JP6094182A patent/JP2781518B2/en not_active Expired - Fee Related
Also Published As
| Publication number | Publication date |
|---|---|
| JPH07227538A (en) | 1995-08-29 |
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