JPS5915690B2 - Desulfurization and denitrification methods - Google Patents
Desulfurization and denitrification methodsInfo
- Publication number
- JPS5915690B2 JPS5915690B2 JP52005826A JP582677A JPS5915690B2 JP S5915690 B2 JPS5915690 B2 JP S5915690B2 JP 52005826 A JP52005826 A JP 52005826A JP 582677 A JP582677 A JP 582677A JP S5915690 B2 JPS5915690 B2 JP S5915690B2
- Authority
- JP
- Japan
- Prior art keywords
- denitrification
- desulfurization
- exhaust gas
- activated carbon
- reduction
- 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
Links
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】
本発明は排ガス中の硫黄酸化物と窒素酸化物を除去する
脱硫、脱硝プロセスに係り、長時間にわたり、高い脱硫
、脱硝率を維持するための湿式脱硫、脱硝プロセスに関
するものである。Detailed Description of the Invention The present invention relates to a desulfurization and denitrification process for removing sulfur oxides and nitrogen oxides from exhaust gas, and relates to a wet desulfurization and denitrification process for maintaining high desulfurization and denitrification rates over a long period of time. It is something.
ボイラ排ガスなどに混入する硫黄酸化物や窒素酸化物は
人体に有害であるため、これらを除去する脱硫、脱硝の
プロセスの研究開発が進められている。Sulfur oxides and nitrogen oxides mixed in boiler exhaust gas are harmful to the human body, so research and development is underway on desulfurization and denitrification processes to remove them.
脱硝技術の分野では乾式法のアンモニア選択触媒還元法
がすでに実用化の段階に達している。In the field of denitrification technology, the dry method of ammonia selective catalytic reduction has already reached the stage of practical application.
一方湿式法においては還元吸収法、酸化吸収法、錯体吸
収還元法、アルカリ吸収法、など多くのプロセスが研究
開発されている。On the other hand, in the wet method, many processes such as reduction absorption method, oxidation absorption method, complex absorption reduction method, and alkali absorption method are being researched and developed.
発明者らは錯体吸収還元法の鉄ＥＤＴＡ錯体溶液による
プロセス化の開発段階において、排ガス中に含まれてい
る数パーセントの０２ により第一鉄ＥＤＴＡ錯体（Ｆ
ｅ（ｉｌ）Ｙ２）が酸化して脱硝性能のない第二ＥＤＴ
Ａ錯体（Ｆｅ（１１□）Ｙ ）に変化するため、脱硝
率は急激に低下してしまうことが判明した。In the development stage of the complex absorption reduction process using an iron EDTA complex solution, the inventors discovered that ferrous EDTA complex (F
e(il)Y2) is oxidized and the second EDT has no denitrification performance.
It was found that the denitrification rate rapidly decreased due to the change to A complex (Fe(11□)Y).
このため高い脱硝率を維持するためには
Ｆｅ （１□）Ｙ２−の酸化を防止するか、あるいは酸
化により生成したＦｅ（１□１）Ｙ−を還元する手段が
必要である。Therefore, in order to maintain a high denitration rate, it is necessary to either prevent the oxidation of Fe(1□)Y2- or to reduce the Fe(1□1)Y- produced by oxidation.
発明者らは酸化防止法と還元法について検討し、Ｆ ｅ
（１□）Ｙ２−に活性炭が共存することにより、Ｆｅ
（１１）Ｙ２−の酸化を著しく抑制し、しかも酸化に
より生成したＦｅ（１□１）Ｙ−は活性炭の共存により
Ｓ０２による還元速度が向上し、
Ｆｅ（、□＞ｙ２−゛を再生することを見い出した。The inventors studied antioxidant methods and reduction methods, and found that F e
(1□) Due to the coexistence of activated carbon in Y2-, Fe
(11) The oxidation of Y2− is significantly suppressed, and the reduction rate of Fe(1□1)Y− produced by oxidation by S02 is improved due to the coexistence of activated carbon, regenerating Fe(,□>y2−゛). I found out.
このため活性炭共存のＦｅ（１□）Ｙ２− を利用する
ことによりすぐれた脱硫、脱硝プロセスの開発が期待さ
れている。Therefore, it is expected that an excellent desulfurization and denitrification process will be developed by utilizing Fe(1□)Y2- coexisting with activated carbon.
本発明はＦｅ（１□＞ｙ２−に活性炭を共存させること
により、Ｆｅ （１□）Ｙ２−の酸化を抑制し、Ｆｅ（
１１）Ｙ２− でＮＯを吸収すると同時に酸化生成物の
Ｆｅ （１□１）Ｙ−を排ガス中のＳＯ３により還元し
、Ｆ ｅ （１□）Ｙ２−を再生して高い脱硫、脱硝率
を長時間にわたり維持する脱硫、脱硝プロセスの提供に
ある。The present invention suppresses the oxidation of Fe(1□)Y2- by coexisting activated carbon with Fe(1□>y2-,
11) At the same time as NO is absorbed by Y2-, the oxidation product Fe (1□1)Y- is reduced by SO3 in the exhaust gas, and Fe (1□)Y2- is regenerated to maintain high desulfurization and denitrification rates. Our aim is to provide desulfurization and denitrification processes that can be maintained over time.
Ｆｅ（ｔ□）Ｙ２−に活性炭を共存させることにより、
活性炭はＦｅ（１□）Ｙ２−の酸化を著しく抑制する一
方、酸化生成物のＦｅ（１□１）Ｙ−を８０２で還元す
る際に触媒作用をし、還元速度を向上させることは実験
により確認されており、脱硫、脱硝プロセスへの適用が
考えられている。By coexisting activated carbon with Fe(t□)Y2-,
Experiments have shown that while activated carbon significantly suppresses the oxidation of Fe(1□)Y2-, it acts as a catalyst when reducing the oxidized product Fe(1□1)Y- with 802, improving the reduction rate. This has been confirmed, and its application to desulfurization and denitrification processes is being considered.
さらに活性炭共存のＦｅ（ｏ）Ｙ２−が排ガス中の０２
によりＦｅ（１□１）Ｙ−になる酸化速度と活性炭共
存のＦｅ（□１１）Ｙ−が排ガス中のＳＯ２による還元
速度について検討し、ｐＨ２以下の低ｐＨ領域でＳＯ２
濃度が高い場合にはＦｅ（１□１）Ｙ−の還元速度が著
しく向上し、この傾向はｐＨの低いほど急速であること
が判明した。Furthermore, Fe(o)Y2- coexisting with activated carbon is 02 in the exhaust gas.
We investigated the oxidation rate of Fe(1□1)Y- to Fe(1□1)Y- and the reduction rate of Fe(□11)Y- coexisting with activated carbon by SO2 in the exhaust gas.
It was found that the reduction rate of Fe(1□1)Y- was significantly improved when the concentration was high, and this tendency was more rapid as the pH was lowered.
Ｆｅ（１□１）Ｙ−の還元にはｐＨが低いほど還元が進
むため有利であるがｐＨが低い程ＮＯを吸収するＦｅ（
１、）Ｙ２− の解離が進行するため、液中のＦｅ（１
１）Ｙ２− が減少し、ＮＯ吸収量は減少して脱硝率は
低下して終うため、ｐＨと脱硝率の関係を検討してｐＨ
２が最適条件であることを見い出した。For the reduction of Fe(1□1)Y-, the lower the pH, the more the reduction progresses, which is advantageous.
1.) As the dissociation of Y2− progresses, Fe(1
1) Y2- decreases, the amount of NO absorbed decreases, and the denitration rate ends up decreasing, so consider the relationship between pH and denitrification rate and adjust the pH.
It was found that 2 is the optimal condition.
これらの実験結果から、ＳＯ□濃度の高い排ガスを活性
炭共存のＦｅ（１□）Ｙ２− と反応させることにより
、Ｆ ｅ （１１） Ｙ２−でＮＯを吸収する脱硝と、
排ガス中の０２による酸化生成物のＦｅ （１□１）Ｙ
−を排ガス中のＳ０２で還元する脱硫を同時に行ない、
Ｆｅ（１１）Ｙ２−濃度を一定に保つため高い脱硫、脱
硝率を長時間維持できるのが本発明の要点である。From these experimental results, we found that by reacting exhaust gas with a high SO□ concentration with Fe(1□)Y2- coexisting with activated carbon, denitrification can be achieved by absorbing NO with Fe(11)Y2-.
Fe (1□1)Y of oxidation products due to 02 in exhaust gas
At the same time, desulfurization is carried out to reduce - with S02 in the exhaust gas,
The key point of the present invention is that high desulfurization and denitrification rates can be maintained for a long time because the Fe(11)Y2− concentration is kept constant.
すなわちＳ０２濃度の高い排ガスに対して、活性炭共存
のＦｅ（１□）Ｙ２− はＮＯを吸収する一方、酸化生
成物のＦｅ（１□１）Ｙ−を排ガス中のＳＯ２で還元し
Ｎｏ吸収力のあるＦｅ（１、）Ｙ２− を再生して高い
脱硫、脱硝性能を得るため、−石工長の効果がある。In other words, for exhaust gas with a high S02 concentration, Fe(1□)Y2- coexisting with activated carbon absorbs NO, while reducing the oxidation product Fe(1□1)Y- with SO2 in the exhaust gas, increasing the NO absorption capacity. In order to obtain high desulfurization and denitrification performance by regenerating some Fe(1,)Y2-, there is a - masonry effect.
このようにしてＮＯを吸収した活性炭共存のＦｅ（１□
）Ｙ２−は加熱あるいはｐＨを低下させることにより、
ＮＯを放出してＮｏ吸収力のあるＦｅ（ｔ□）Ｙ２−が
再生される。In this way, Fe (1□
) Y2- is heated or lowered by lowering the pH,
Fe(t□)Y2-, which has NO absorption ability, is regenerated by releasing NO.
このため活性炭共存のＦｅ（１、）Ｙ２−は脱硫（Ｆｅ
（、ｔｔ）Ｙ−の還元）と脱硝、さらに吸収したＮＯの
放出により、Ｆｅ（１□）ｙ２−の再生を繰返して循環
するた１め、長時間にわたり高い脱硫、脱硝率を維持す
ることが可能となる。Therefore, Fe(1,)Y2− coexisting with activated carbon is desulfurized (Fe
(, tt) Y- reduction) and denitrification, and the regeneration of Fe (1 becomes possible.
第１図に示した本発明のフローシートにより説明する。This will be explained with reference to the flow sheet of the present invention shown in FIG.
Ｓ０２濃度の高い排ガス１１は脱硫脱硝塔１に導かれ、
活性炭共存のＦｅ（１□）Ｙ２− にヨリ下記反応で排
ガス中のＮＯを吸収する。The exhaust gas 11 with a high S02 concentration is led to the desulfurization and denitrification tower 1,
Fe(1□)Y2- coexisting with activated carbon absorbs NO in the exhaust gas through the following reaction.
Ｆｅ（１１）Ｙ２−＋ＮＯ−→Ｆｅ（１１）Ｙ２−・Ｎ
Ｏしかしながら排ガス中には数パーセントの０２が含ま
れており、この０２でＦｅ（１１）Ｙ２− は酸化し、
Ｎｏ吸収力のないＦｅ（□１１）Ｙ−に変化するがＮＯ
の吸収と同時に排ガス中のＳ０２により、Ｆｅ（１□１
）Ｙ−の還元は次式のように進み、Ｆｅ（１□）Ｙ２−
が再生される。Fe(11)Y2-+NO-→Fe(11)Y2-・N
However, the exhaust gas contains several percent of 02, and this 02 oxidizes Fe(11)Y2-.
No.Fe without absorption ability (□11) changes to Y-, but NO
Fe(1□1
)Y- reduction proceeds as shown in the following equation, resulting in Fe(1□)Y2-
is played.
このため脱硫脱硝塔１ではＮＯの吸収とＳＯ２によるＦ
ｅ（１，１）Ｙ−の還元が行なわれる。For this reason, in the desulfurization and denitrification tower 1, NO absorption and SO2
Reduction of e(1,1)Y- takes place.
本発明プロセスでは排ガス中のＳＯ２はＦｅ（１，１）
Ｙ−の還元に有効活用して脱硫、脱硝の同時処理が行な
われる。In the process of the present invention, SO2 in the exhaust gas is Fe(1,1)
Simultaneous desulfurization and denitrification treatments are carried out by effectively utilizing the reduction of Y-.
ＮＯを吸収した活性炭共存のＦｅ（１□）Ｙ２−は循環
ポンプ２により、ＮＯ放出塔３に送られ、ここで、スチ
ーム１２などにより加熱して（支）を放出して、Ｎｏ吸
収力のある活性炭共存の
Ｆｅ（１１）Ｙ２− となる。The Fe(1□)Y2- coexisting with activated carbon that has absorbed NO is sent to the NO release tower 3 by the circulation pump 2, where it is heated with steam 12 etc. to release (support) and reduce the NO absorption capacity. Fe(11)Y2- coexists with a certain activated carbon.
Ｎｏ放出塔３ではｐＨの低い方がＮｏの放出に有利であ
るが、９０℃に加熱する場合にはｐＨ２で吸収したＮＯ
に対してほぼ１００％のＮＯを放出する。In the No release tower 3, lower pH is more advantageous for releasing No, but when heating to 90°C, NO absorbed at pH 2
It releases almost 100% NO.
ここで放出したＮｏはＮｕ（３１３により接触還元して
人体に無害なＮ２１５として大気中に放出できる。The No released here can be catalytically reduced by Nu(313) and released into the atmosphere as N215, which is harmless to the human body.
一方ＮＯ放出塔３で再生された活性炭共存のＦｅ（１□
）Ｙ２−は活性炭分離槽４で活性炭とＦｅ（Ｈ）Ｙ２−
液に分別するがＦｅ（１、）Ｙ２−液には、Ｆｅ（１□
、）Ｙ−を還元した時に生成した５０１−が含まれてい
るため、石膏回収槽５にＣａＳＯ４１９として回収し、
ＣＯ３Ｏ４とＦｅ（１□）Ｙ２−液に分別する。On the other hand, Fe (1□
)Y2- is separated from activated carbon and Fe(H)Y2- in activated carbon separation tank 4.
Fe(1,)Y2− liquid contains Fe(1□
,) Since it contains 501- generated when reducing Y-, it is collected as CaSO419 in the gypsum recovery tank 5,
Separate into CO3O4 and Fe(1□)Y2- liquid.
このＦｅ（１□）Ｙ２−液に活性炭分離槽４に回収した
活苛炭２１を加え、活性炭共存のＦｅ（１、）Ｙ２−
としてｐＨ調整槽６で適正ｐＨに調整し、ＮＯの吸収力
のある活性炭共存のＦｅ（ｏ）Ｙ２−にして、脱硫、脱
硝塔に戻すサイクルの繰返しにより高い脱硫、脱硝率の
維持が可能である。Activated caustic carbon 21 collected in the activated carbon separation tank 4 was added to this Fe(1□)Y2- liquid, and Fe(1,)Y2- with activated carbon coexisted was added.
It is possible to maintain a high desulfurization and denitrification rate by repeating the cycle of adjusting the pH to an appropriate pH in the pH adjustment tank 6, converting it to Fe(o)Y2-, which coexists with activated carbon that has NO absorption ability, and returning it to the desulfurization and denitrification tower. be.
第２図は第１図に示した本発明プロセスのフローシート
に従いベンチスケールテストを行った結果である。FIG. 2 shows the results of a bench scale test conducted according to the flow sheet of the process of the present invention shown in FIG.
脱硫、脱硝塔はテラレットを充填した充填塔とし、Ｆｅ
（１１）Ｙ２ ０．２モル、活性炭１０ｗｔ％からなる
ｐＨ２の活性炭共存のＦｅ（１□）Ｙ２ ２Ｎｉを０．
２ Ｎ ｍ／ｍ１ｙｒで循環し、Ｎｏ ３００ ｐｐｍ
、 ５Ｏ２１０００ｐｐｍ、 ０２ ５％、Ｎ２残から
なるボイラ排ガスと前記排ガスにＳＯ７を付加しＮｏ
３００ｐｐｍ、 、５Ｏ２１５００ｐｐｍ、０２５％、
Ｎ２残からなるガスを２０ Ｎ ｍ３／ ｈで脱硫、脱
硝塔に流入した。The desulfurization and denitrification tower is a packed tower filled with Terraret.
(11) Fe(1□)Y2 2Ni coexisting with activated carbon at pH 2 consisting of 0.2 mol of Y2 and 10 wt% activated carbon.
Circulated at 2 N m/mlyr, No 300 ppm
, 5O2 1000ppm, 02 5%, boiler exhaust gas consisting of N2 remainder and SO7 added to the exhaust gas.
300ppm, 5O21500ppm, 025%,
The gas consisting of N2 residue was flowed into the desulfurization and denitrification tower at 20 N m3/h.
ＳＯ□濃度１１０００ｐｐを含む排ガスの脱硝率Ａは初
期脱硝率が９２％であるが１時間で７５％低下し、その
後もゆるやかに脱硝率は低下して４時間後に６０％にな
るがその後は脱硝率の変化はなく１０時間後も６０％を
維持している。The initial denitrification rate A of exhaust gas containing SO□ concentration 11000 pp is 92%, but it decreases by 75% in 1 hour, and after that, the denitrification rate gradually decreases to 60% after 4 hours, but after that, denitrification continues. There was no change in the rate and it remained at 60% even after 10 hours.
一方ＳＯ７濃度１５００ｐｐｍを含む排ガスの脱硝率Ｂ
は初期脱硝率が９７％であり、Ａとほとんど差がなく、
その後の脱硝率の低下は小さく３時間後は８０％で、そ
の後は変化なく１０時間後にも８０％の高脱硝率を維持
している。On the other hand, denitrification rate B of exhaust gas containing SO7 concentration 1500 ppm
The initial denitrification rate was 97%, and there was almost no difference from A.
Thereafter, the denitrification rate decreased only slightly, reaching 80% after 3 hours, and maintained a high denitrification rate of 80% even after 10 hours.
ＳＯ□については、Ａ、 Ｂの両者とも脱硫率がほぼ１
００％であり、排ガス中のＳＯ２はすべてＦｅ（１，１
）Ｙ２− の還元に作用している。Regarding SO□, the desulfurization rate is almost 1 for both A and B.
00%, and all SO2 in the exhaust gas is Fe(1,1
) acts on the reduction of Y2-.
以上のテスト結果から本発明プロセスはＳＯａ度の高い
排ガスの脱硫、脱硝の同時処理にきわめて有効であるこ
とが確められた。From the above test results, it was confirmed that the process of the present invention is extremely effective for simultaneous desulfurization and denitration treatment of exhaust gas with a high SOa content.
本発明によれば活性炭共存のＦｅ（Ｈ）Ｙ２− による
脱硝１と排ガス中のＳｏ ２によりＦｅ（ｔｌ、）Ｙ−
の還元を同時に行なうためＦｅ（ｕ）Ｙ−濃度を一定に
保つことができ高い脱硫、脱硝率を長時間維持する効果
があり、ＳＯ２濃度の高いガスの処理に最適である。According to the present invention, denitration 1 using Fe(H)Y2- in the presence of activated carbon and Fe(tl,)Y-
Since the reduction of Fe(u)Y- is carried out at the same time, the Fe(u)Y- concentration can be kept constant, which has the effect of maintaining high desulfurization and denitrification rates for a long time, making it ideal for processing gas with a high SO2 concentration.
第１図は本発明による脱硫、脱硝プロセスのフローシー
ト、第２図は本発明プロセスによるベンチスケールテス
トの結果である。
符号の説明、１・・・・・・脱硫脱硝塔、３・・・・・
・Ｎｏ放出塔、４・・・・・・活性炭分離槽、５・・・
・・・石膏回収槽、６・・・・・・ｐＨ調整槽。FIG. 1 is a flow sheet of the desulfurization and denitrification process according to the present invention, and FIG. 2 is the result of a bench scale test using the process according to the present invention. Explanation of symbols, 1... Desulfurization and denitrification tower, 3...
・No. release tower, 4...Activated carbon separation tank, 5...
...Gypsum recovery tank, 6...pH adjustment tank.
Claims (1)
て、吸収塔内で第一鉄ＥＤＴＡ錯体と活性炭の混合液に
排ガスを通過させてＮＯを吸収し、且つ酸化した第二鉄
ＥＤＴＡを排ガス中のＳＯ２で還元し、ＮＯの吸収能力
の持つ第一鉄ＥＤＴＡ錯体に再生することにより、脱硫
、脱硝を同時に行ないＮＯを吸収した混合液を吸収塔外
で加熱し、濃縮したＮＯとして回収してＮＯの吸収能力
を持つ混合液を再生させ、循環、再使用することを特徴
とする脱硫、脱硝方法。1 In a method for removing SO2 and NO in exhaust gas, the exhaust gas is passed through a mixture of a ferrous EDTA complex and activated carbon in an absorption tower to absorb NO, and the oxidized ferric EDTA is removed from SO2 in the exhaust gas. The mixed solution that has absorbed NO through simultaneous desulfurization and denitrification is heated outside the absorption tower, and is recovered as concentrated NO to recover NO. A desulfurization and denitrification method characterized by regenerating, circulating, and reusing a mixed liquid with absorption capacity.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP52005826A JPS5915690B2 (en) | 1977-01-24 | 1977-01-24 | Desulfurization and denitrification methods |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP52005826A JPS5915690B2 (en) | 1977-01-24 | 1977-01-24 | Desulfurization and denitrification methods |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| JPS5391074A JPS5391074A (en) | 1978-08-10 |
| JPS5915690B2 true JPS5915690B2 (en) | 1984-04-11 |
Family
ID=11621855
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP52005826A Expired JPS5915690B2 (en) | 1977-01-24 | 1977-01-24 | Desulfurization and denitrification methods |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JPS5915690B2 (en) |
Families Citing this family (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN109821381A (en) * | 2019-01-16 | 2019-05-31 | 北京清新环境技术股份有限公司 | A method for enhancing wet complex desulfurization and denitrification with modified activated carbon |
| CN117125681A (en) * | 2022-05-20 | 2023-11-28 | 浙江锘兴技术有限公司 | Portable Nitric Oxide Generator |
-
1977
- 1977-01-24 JP JP52005826A patent/JPS5915690B2/en not_active Expired
Also Published As
| Publication number | Publication date |
|---|---|
| JPS5391074A (en) | 1978-08-10 |
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