JPS6147129B2 - - Google Patents
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- Publication number
- JPS6147129B2 JPS6147129B2 JP57052271A JP5227182A JPS6147129B2 JP S6147129 B2 JPS6147129 B2 JP S6147129B2 JP 57052271 A JP57052271 A JP 57052271A JP 5227182 A JP5227182 A JP 5227182A JP S6147129 B2 JPS6147129 B2 JP S6147129B2
- Authority
- JP
- Japan
- Prior art keywords
- exhaust gas
- reactor
- catalyst
- flow path
- nitrogen
- 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
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Classifications
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J15/00—Chemical processes in general for reacting gaseous media with non-particulate solids, e.g. sheet material; Apparatus specially adapted therefor
Landscapes
- Chemical & Material Sciences (AREA)
- Organic Chemistry (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Exhaust Gas Treatment By Means Of Catalyst (AREA)
- Physical Or Chemical Processes And Apparatus (AREA)
Description
本発明は、窒素酸化物含有燃焼排ガス（以下、
排ガスと称す）から接触還元反応法により窒素酸
化物を除去する方法に関し、特にアスベストペー
パーから形成されたハニカムを担体とする触媒を
効果的に使用して排ガスから窒素酸化物を除去す
る方法に関するものである。
今日、化石燃料の使用量の増大とプラント類の
大型化に伴い、大気中の窒素酸化物（以下、NOX
と称す）の濃度が増大し、光化学スモツグやオキ
シダントの発生要因となつている。そのため、
NOXの排出量が法的に規制され、しかもNOXの除
去あるいは抑制策を講じても上記排出量がその規
制値を下まわらない場合は、燃焼装置等のNOXの
発生源の稼働は許可されない事態となつてきてい
る。
従来、いくつかのNOX低減策が提案されてき
た。該NOXの低減策としては、大別すると抑制法
と除去法があり、この除去法の中でも処理費が安
価であること、排水処理を必要としないこと等の
長所を有する乾式法が注目されている。
前記乾式法の一つとして、アンモニアを還元剤
として用い、無機質繊維からなるハニカム状の触
媒（以下、ハニカム触媒と称す）の存在下におい
て、排ガス中のNOXを選択的に還元し、窒素
（N2）にすることによつてNOXを除去する方法
（以下、排煙脱硝法と称す）が知られているが、
前記排ガス中の硫黄酸化物（以下、SOXと称す）
と前記アンモニアとの化合物が液体または固体と
して析出する場合において該化合物が前記ハニカ
ム触媒に付着し、反応を妨害し、また、排ガス流
路を閉塞する等の欠点を有している。
本発明は、上記欠点を除くためになされたもの
であつて、
(1) 窒素酸化物含有排ガスを触媒物質の存在下、
還元剤としてアンモニアを添加し、窒素酸化物
を選択的に窒素に還元除去する方法において、
アスベストペーパーから形成されたハニカムを
担体とする触媒を配置した反応器を縦置させ、
前記排ガスを地球面に対して垂直に流し、かつ
前記反応器における前記排ガスの空筒速度を
1.5〜５ｍ／秒の範囲内とすることを特徴とす
る排煙脱硝法、
(2) 窒素酸化物含有燃焼排ガスを触媒物質の存在
下、還元剤として、アンモニアを添加し、窒素
酸化物を選択的に窒素に還元除去する方法にお
いて、アスベストペーパーから形成されたハニ
カムを担体とする触媒を配置した反応器を縦置
させ、前記排ガスを地球面に対して垂直に流
し、かつ前記反応器における前記排ガスの空筒
速度を1.5〜５ｍ／秒の範囲内とすると共に、
前記反応器を、前記排ガスの通過方向に対する
垂線と平行な端面を有する円柱状に成形させ、
該円柱状反応器の前記排ガス通過方向の中心軸
を中心に回転可能にし、しかも該反応器の一部
を前記排ガスの流路内に、他の一部を前記排ガ
スの流路外にそれぞれ位置するように設置して
用いることを特徴とする排煙脱硝法、
に関するものである。
以下、本発明方法を実施例に基いて説明する。
第１図は、前記反応器における排ガスの空筒速
度を0.5ｍ／秒と３ｍ／秒の２種類の条件にし、
他の条件は同一にして、空筒速度について比較し
たものである。該図から明らかなように、前者の
場合には1000時間を経過すると触媒層のガス入口
側のダストの付着量がわずかながらも増大して排
ガスのハニカム触媒を通過することに伴う圧力損
失（以下、圧損失と称す）値が増大し始める。一
方、後者の場合には圧損失値の増大は認められな
い。
第２図は、前記反応器における排ガスの空筒速
度を変化させ、他の条件は同一にして、初期にお
ける圧損失値を比較したものであるが、排ガスの
空筒速度が増大するに従つて初期における圧損失
値も増大することが認められる。
第１図と第２図より、反応器における排ガスの
空筒速度にはダストの付着防止と初期の圧損失値
を小さくするという二律背反する目的を達成する
ための最適範囲が存在し、該最適範囲が1.5〜５
ｍ／秒であることが明らかである。
第３図は、前記反応器を縦置として排ガスを地
球面に対して垂直に流した場合(a)と、反応器を横
置として排ガスを地球面に対して平行に流した場
合(b)とについて長期試験を行なつた結果を示した
ものであり、図中のグラフａは前記(a)の場合、グ
ラフｂは前記の(b)の場合にそれぞれ対応してい
る。
第３図より、前記反応器を縦置として排ガスを
地球に対して垂直に流した場合(a)の方がNOXの除
去能力を長期にわたつて高く維持できることが明
らかである。
第４図Ａ，Ｂは、本発明方法に用いられる反応
器の構成の一例を示すものであり、第４図Ａは全
体図、第４図Ｂはハニカム触媒の要部拡大図であ
る。第４図Ａ，Ｂ中の１はハニカム触媒の基材
部、２は該基材部１によつて形成される排ガスの
流路の１つであり、３はこのハニカム触媒を配置
した円柱状の反応器であり、排ガスは上記流路２
群が開口している反応器３の上端面の排ガス流路
６内にある部分（以下、有効部分と称す）４から
流入し、排ガス流路７へ導かれる。ダストやアン
モニアとSOXとの化合物の付着に伴い、上記ハニ
カム触媒の性能が劣化した時に反応器３を回転軸
９を中心に矢印α方向へ回転させ上記有効部４を
排ガスの流路外へ移動させ、ライン１３から導入
される温水または水蒸気によりこのダストやアン
モニアとSOXとの化合物を洗浄排除させハニカム
触媒の性能を回復させる。なお、この時、先に排
ガス流路外に位置していた部分５が排ガス流路内
に移動し、有効部となつて排煙脱硝に供される。
第５図は、本発明方法の一実施態様例を示すフ
ローシートである。図中、第４図と同一符号は第
４図と同一機能部位を示し、６，７は排ガス流
路、８は排ガス発生源、１０は熱交換器、１１，
１２は燃焼用空気の流路、１４はアンモニア注入
管路である。
次に、第４，５図に示す本発明方法で、NOX除
去率が80％を下まわつた時点で水洗し、触媒活性
が回復するまでに使用した水量を測定した。また
比較のために触媒を取り出し、常温の水および
100℃の温水で洗浄した時に要した水の量をも測
定した。
これらの結果を表１に示す。
The present invention provides nitrogen oxide-containing combustion exhaust gas (hereinafter referred to as
This invention relates to a method for removing nitrogen oxides from exhaust gas (referred to as exhaust gas) by a catalytic reduction reaction method, and in particular to a method for effectively removing nitrogen oxides from exhaust gas by effectively using a catalyst using a honeycomb formed from asbestos paper as a carrier. It is. Today, as fossil fuel usage increases and plants become larger, nitrogen oxides (hereinafter referred to as NO
(referred to as oxidants) is increasing, which is a factor in the generation of photochemical smog and oxidants. Therefore,
If NO X emissions are legally regulated and the above emissions do not fall below the regulated value even after NO It has become a situation where this is not allowed. In the past, several NOx reduction measures have been proposed. Measures to reduce NO ing. As one of the dry methods, ammonia is used as a reducing agent to selectively reduce NOx in exhaust gas in the presence of a honeycomb-shaped catalyst made of inorganic fibers (hereinafter referred to as honeycomb catalyst), and nitrogen ( A method of removing NO
Sulfur oxides in the exhaust gas (hereinafter referred to as SOX )
When a compound of ammonia and ammonia precipitates as a liquid or solid, it has disadvantages such as adhering to the honeycomb catalyst, interfering with the reaction, and clogging the exhaust gas flow path. The present invention has been made to eliminate the above-mentioned drawbacks, and includes: (1) treating nitrogen oxide-containing exhaust gas in the presence of a catalyst substance;
In a method of selectively reducing and removing nitrogen oxides to nitrogen by adding ammonia as a reducing agent,
A reactor containing a catalyst using a honeycomb made of asbestos paper as a carrier is placed vertically.
The exhaust gas is caused to flow perpendicularly to the earth surface, and the cylinder velocity of the exhaust gas in the reactor is
A flue gas denitrification method characterized in that the denitrification rate is within the range of 1.5 to 5 m/sec, (2) Ammonia is added as a reducing agent to nitrogen oxide-containing combustion exhaust gas in the presence of a catalyst substance, and nitrogen oxides are selected. In this method, a reactor in which a catalyst having a honeycomb formed from asbestos paper as a carrier is arranged is placed vertically, the exhaust gas is caused to flow perpendicularly to the earth's surface, and the The cylinder velocity of exhaust gas is within the range of 1.5 to 5 m/sec, and
The reactor is formed into a cylindrical shape having an end surface parallel to a perpendicular line to the passing direction of the exhaust gas,
The cylindrical reactor is rotatable about a central axis in the exhaust gas passage direction, and a part of the reactor is located within the exhaust gas flow path and another part is located outside the exhaust gas flow path. The present invention relates to a flue gas denitrification method, which is characterized in that it is installed and used in such a manner as to be used. The method of the present invention will be explained below based on examples. Figure 1 shows two conditions in which the cylinder velocity of the exhaust gas in the reactor is 0.5 m/sec and 3 m/sec.
The other conditions were kept the same, and the cylinder velocity was compared. As is clear from the figure, in the former case, after 1000 hours have elapsed, the amount of dust adhering to the gas inlet side of the catalyst layer increases, albeit slightly, and the pressure loss (hereinafter referred to as , pressure loss) begins to increase. On the other hand, in the latter case, no increase in pressure loss value was observed. Figure 2 compares the initial pressure loss values while changing the cylinder velocity of the exhaust gas in the reactor and keeping other conditions the same.As the cylinder velocity of the exhaust gas increases, It is recognized that the initial pressure loss value also increases. From Figures 1 and 2, there is an optimal range for the cylinder velocity of the exhaust gas in the reactor to achieve the contradictory objectives of preventing dust adhesion and reducing the initial pressure loss value. is 1.5~5
It is clear that m/sec. Figure 3 shows the case where the reactor is placed vertically and the exhaust gas flows perpendicularly to the earth's surface (a), and the case where the reactor is placed horizontally and the exhaust gas flows parallel to the earth's surface (b). Graph a in the figure corresponds to the case (a) above, and graph b corresponds to the case (b) above. From FIG. 3, it is clear that the case (a) in which the reactor is placed vertically and the exhaust gas is flowed perpendicularly to the earth can maintain a high NOx removal ability over a long period of time. FIGS. 4A and 4B show an example of the configuration of a reactor used in the method of the present invention, with FIG. 4A being an overall view and FIG. 4B being an enlarged view of essential parts of a honeycomb catalyst. 4A and B, 1 is the base material part of the honeycomb catalyst, 2 is one of the exhaust gas flow paths formed by the base material part 1, and 3 is the cylindrical shape in which the honeycomb catalyst is arranged. reactor, and the exhaust gas flows through the flow path 2.
The gas flows from a portion (hereinafter referred to as an effective portion) 4 located in the exhaust gas flow path 6 on the upper end surface of the reactor 3 where the group is open, and is guided to the exhaust gas flow path 7 . When the performance of the honeycomb catalyst deteriorates due to adhesion of dust and compounds of ammonia and SOx , the reactor 3 is rotated in the direction of arrow α about the rotating shaft 9 to move the effective part 4 out of the exhaust gas flow path. The dust and the compound of ammonia and SOx are washed away by hot water or steam introduced from the line 13, and the performance of the honeycomb catalyst is restored. At this time, the portion 5 that was previously located outside the exhaust gas flow path moves into the exhaust gas flow path, becomes an effective portion, and is used for exhaust gas denitration. FIG. 5 is a flow sheet showing an embodiment of the method of the present invention. In the figure, the same symbols as in FIG. 4 indicate the same functional parts as in FIG. 4, 6 and 7 are exhaust gas flow paths, 8 is an exhaust gas generation source, 10 is a heat exchanger, 11
12 is a flow path for combustion air, and 14 is an ammonia injection pipe. Next, using the method of the present invention shown in FIGS. 4 and 5, water was washed when the NOx removal rate fell below 80%, and the amount of water used until the catalyst activity was restored was measured. Also, for comparison, we took out the catalyst and added water and water at room temperature.
The amount of water required for washing with 100°C hot water was also measured. These results are shown in Table 1.
【表】
＊ 触媒容量の倍数
表１から明らかなように、本発明方法で温水洗
浄を行なうことが最も優れた効果を示すことが判
る。このように本発明方法によれば、アンモニア
とSOXとの化合物やダストのハニカム触媒への付
着に伴う圧損失値の増大を防止すること、NOXの
除去能力を長期にわたつて高く維持すること等の
効果を奏し得るものである。
なお、本発明方法に係るハニカムとは、第６図
Ａ〜Ｅに例示するように、アスベストペーパーか
ら構成された基材部１の内部に貫通した気体通路
２を有する成形体または成形体の積層したもので
あり、第６図Ｂ中２′で示すように通路２をアス
ベストペーパーで充填することもできる。
また、上記のアスベストペーパーとしては、ア
スベスト繊維を0.05〜0.2mm厚さの紙状物あるい
は不織布としたものが用いられ、該アスベストペ
ーパーを第６図Ａ〜Ｅに示すような成形体あるい
は積層状態に形成させたものとすればよい。フル
ートの寸法としては、径又は高さ及び巾とともに
１〜５mmの寸法が好ましく、アスベスト繊維の太
さについては、アスベストペーパーとして抄紙可
能であれば特に規定しない。
本発明方法では、上記触媒に活性体として硫酸
鉄等通常の乾式脱硝用触媒の活性体を担持させて
用いる。
更に、本発明方法において、上記触媒は、反応
器温度300〜400℃で使用するのが好ましい。これ
は、反応器温度が300℃以下であると、前記した
ように触媒上にSOXとアンモニアとの化合物、例
えば硫酸アンモニウム、重硫酸アンモニウム、重
亜硫酸アンモニウムなどの液体や固体が析出し易
すくなるからであり、また400℃以上になつても
効果が変わらないからである。
以上詳述した本発明方法は、火力発電所等にお
ける大量の排ガス中から有害な窒素酸化物を効率
良く除去する際に多大な利用価値を有するもので
ある。[Table] *Multiples of catalyst capacity As is clear from Table 1, it can be seen that washing with hot water according to the method of the present invention shows the most excellent effect. As described above, according to the method of the present invention, it is possible to prevent an increase in the pressure loss value due to the adhesion of ammonia and SO x compounds and dust to the honeycomb catalyst, and to maintain a high NO x removal ability over a long period of time. This can have the following effects. Note that the honeycomb according to the method of the present invention is a molded body or a stack of molded bodies having a gas passage 2 penetrating inside a base material portion 1 made of asbestos paper, as illustrated in FIGS. 6A to 6E. The passage 2 can also be filled with asbestos paper as shown at 2' in FIG. 6B. In addition, as the above-mentioned asbestos paper, a paper-like material or non-woven fabric made of asbestos fibers with a thickness of 0.05 to 0.2 mm is used, and the asbestos paper is formed into a molded product or a laminated state as shown in Figures 6A to 6E. It is sufficient that the structure is formed as follows. The dimensions of the flute, together with the diameter, height, and width, are preferably 1 to 5 mm, and the thickness of the asbestos fibers is not particularly specified as long as it can be made into asbestos paper. In the method of the present invention, the above-mentioned catalyst is used in such a manner that an active substance of a conventional dry denitrification catalyst, such as iron sulfate, is supported as an active substance. Further, in the method of the present invention, the above catalyst is preferably used at a reactor temperature of 300 to 400°C. This is because, as mentioned above, if the reactor temperature is below 300°C, compounds of SO x and ammonia, such as ammonium sulfate, ammonium bisulfate, and ammonium bisulfite, are likely to precipitate as liquids or solids on the catalyst. This is because the effect does not change even if the temperature exceeds 400°C. The method of the present invention described in detail above has great utility value in efficiently removing harmful nitrogen oxides from a large amount of exhaust gas in a thermal power plant or the like.
第１図は排ガスの空筒速度の圧損失の経時変化
に及ぼす影響を示したものである。第２図は排ガ
スの空筒速度に対する初期の圧損失を示したもの
である。第３図は反応器を縦置した場合と横置し
た場合のNOX除去率の経時変化を示したものであ
る。第４図は本発明方法に用いられる反応器の構
成並びにハニカム触媒の要部拡大図である。第５
図は本発明方法の一実施態様例を示すフローシー
トである。第６図は本発明方法に係るハニカムの
形状の例を示す図である。
１……ハニカム触媒の基材部、２……排ガスの
流路、３……円柱状の反応器、４……有効部、
６，７……排ガス流路、８……排ガス発生源、９
……回転軸、１０……熱交換器、１１，１２……
燃焼用空気の流路、１３……洗浄用水導入ライ
ン、１４……アンモニア注入管路。
FIG. 1 shows the influence of the cylinder velocity of exhaust gas on the change in pressure loss over time. FIG. 2 shows the initial pressure loss versus the cylinder velocity of the exhaust gas. Figure 3 shows the change over time in the NOx removal rate when the reactor was placed vertically and when the reactor was placed horizontally. FIG. 4 is an enlarged view of the structure of the reactor and the main parts of the honeycomb catalyst used in the method of the present invention. Fifth
The figure is a flow sheet showing one embodiment of the method of the present invention. FIG. 6 is a diagram showing an example of the shape of a honeycomb according to the method of the present invention. DESCRIPTION OF SYMBOLS 1... Honeycomb catalyst base material part, 2... Exhaust gas flow path, 3... Cylindrical reactor, 4... Effective part,
6, 7...Exhaust gas flow path, 8...Exhaust gas generation source, 9
... Rotating shaft, 10 ... Heat exchanger, 11, 12 ...
Combustion air flow path, 13...Washing water introduction line, 14...Ammonia injection pipe.
Claims (1)
下、還元剤としてアンモニアを添加し、窒素酸化
物を選択的に窒素に還元除去する方法において、
0.05〜0.2mm厚さのアスベストペーパーから形成
されたハニカムを担体とする触媒を配置した反応
器を縦置させ、前記排ガスを地球面に対して垂直
に流し、かつ反応器における前記排ガスの空筒速
度1.5〜５ｍ／秒の範囲内とすることを特徴とす
る排煙脱硝方法。 ２ 窒素酸化物含有燃焼排ガスを触媒物質の存在
下、還元剤としてアンモニアを添加し、窒素酸化
物を選択的に窒素に還元除去する方法において、
0.05〜0.2mm厚さのアスベストペーパーから形成
されたハニカムを担体とする触媒を配置した反応
器を縦置させ、前記排ガスを地球面に対して垂直
に流し、かつ反応器における前記排ガスの空筒速
度を1.5〜５ｍ／秒の範囲内とすると共に、前記
反応器を、前記排ガスの通過方向に対する垂線と
平行な端面を有する円柱状に成形させ、該円柱状
反応器の前記排ガス通過方向の中心軸を中心に回
転可能に、しかも該反応器の一部を前記排ガスの
流路内に、他の一部を前記排ガスの流路外にそれ
ぞれ位置するように設置して用いることを特徴と
する排煙脱硝方法。[Claims] 1. A method for selectively reducing and removing nitrogen oxides to nitrogen by adding ammonia as a reducing agent to nitrogen oxide-containing combustion exhaust gas in the presence of a catalyst substance,
A reactor in which a catalyst having a honeycomb carrier made of asbestos paper with a thickness of 0.05 to 0.2 mm is arranged is placed vertically, and the exhaust gas is allowed to flow perpendicularly to the earth's surface. A flue gas denitrification method characterized in that the speed is within a range of 1.5 to 5 m/sec. 2. A method for selectively reducing and removing nitrogen oxides to nitrogen by adding ammonia as a reducing agent to nitrogen oxide-containing combustion exhaust gas in the presence of a catalyst substance,
A reactor in which a catalyst having a honeycomb carrier made of asbestos paper with a thickness of 0.05 to 0.2 mm is arranged is placed vertically, and the exhaust gas is allowed to flow perpendicularly to the earth's surface. The speed is within the range of 1.5 to 5 m/sec, and the reactor is formed into a cylindrical shape having an end face parallel to a line perpendicular to the exhaust gas passage direction, and the center of the cylindrical reactor in the exhaust gas passage direction is The reactor is rotatable around an axis and is used by being installed so that a part of the reactor is located inside the exhaust gas flow path and another part is located outside the exhaust gas flow path. Flue gas denitrification method.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP57052271A JPS5840130A (en) | 1982-04-01 | 1982-04-01 | Flue gas denitration method |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP57052271A JPS5840130A (en) | 1982-04-01 | 1982-04-01 | Flue gas denitration method |
Related Parent Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP51124984A Division JPS5827975B2 (en) | 1976-10-20 | 1976-10-20 | Flue gas denitration method |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| JPS5840130A JPS5840130A (en) | 1983-03-09 |
| JPS6147129B2 true JPS6147129B2 (en) | 1986-10-17 |
Family
ID=12910108
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP57052271A Granted JPS5840130A (en) | 1982-04-01 | 1982-04-01 | Flue gas denitration method |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JPS5840130A (en) |
Families Citing this family (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPS60114329A (en) * | 1983-11-28 | 1985-06-20 | Mitsubishi Heavy Ind Ltd | Treating apparatus of exhaust gas |
| JPS60183026A (en) * | 1984-03-01 | 1985-09-18 | Mitsubishi Heavy Ind Ltd | Treatment of exhaust gas |
| JP6051677B2 (en) * | 2012-08-21 | 2016-12-27 | 新東工業株式会社 | Granulator |
Family Cites Families (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| DE2263554A1 (en) * | 1972-01-18 | 1974-07-04 | Feldmuehle Anlagen Prod | CATALYST CARRIER MADE OF SINTERED INORGANIC MATERIAL WITH OUTER SHEATH |
| JPS5739168B2 (en) * | 1975-01-31 | 1982-08-19 |
-
1982
- 1982-04-01 JP JP57052271A patent/JPS5840130A/en active Granted
Also Published As
| Publication number | Publication date |
|---|---|
| JPS5840130A (en) | 1983-03-09 |
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