JP2013173147A - 石炭燃焼公共施設のためのアンモニア酸化触媒 - Google Patents
石炭燃焼公共施設のためのアンモニア酸化触媒 Download PDFInfo
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- JP2013173147A JP2013173147A JP2013124666A JP2013124666A JP2013173147A JP 2013173147 A JP2013173147 A JP 2013173147A JP 2013124666 A JP2013124666 A JP 2013124666A JP 2013124666 A JP2013124666 A JP 2013124666A JP 2013173147 A JP2013173147 A JP 2013173147A
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- Prior art keywords
- ammonia
- catalyst
- flue gas
- titania
- secondary catalyst
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Images
Classifications
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- B01D—SEPARATION
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Abstract
【解決手段】 金属酸化物、たとえばチタニア上貴金属及びバナジアの二次触媒を組み込んで、二酸化硫黄(SO2)量を維持しつつアンモニア及び一酸化炭素(CO)の両方を酸化せしめる。
【選択図】 図1
Description
x放出の主たる原因であることを決定した。これらの規制は、EPAにより、クリーンエアー条例修正1990年の主題IVのもとに確立された。1997年7月、EPAは新原料行動基準において他の変更を提案した。この修正はSCR技術で達成できる成果に基づくものであった。
(1)いくらかのアンモニアは除去されずに処理したガス中に残る;
(2)NOx分解速度は低い;
(3)アンモニアを多量に消費する。
ニアの使用量がSCRを通してNOxを効果的に除去するのに十分である場合、過剰のアンモニアのいくらかが未変化のまま触媒を通り抜けて煙道ガス中にアンモニアスリップとして排出されれば、排出ガス中の有毒反応性ガスという問題が生じる。特に石炭火力発電所の煙道ガスに出る過剰なアンモニアによってもたらされる他の大きな問題は、そのアンモニアがセメントと混合してコンクリートを作るために使用することが意図された飛灰を汚染することである。かくして、一次SCR触媒の下流でアンモニアスリップを最小にする安全で有効な方法が必要とされている。
4NO + 4NH3 + O2 → 4N2 + 6H2O (1)
4NO2 + 4NH3 + O2 → 3N2 + 6H2O (2)
SCR法で用いる触媒は、理想的には高温使用条件、例えば400℃またはそれ以上において、水熱条件下に、及び硫黄化合物の存在下に良好な触媒活性を保持しうるべきである。高温及び水熱条件は、ガスタービンエンジン排気ガスの処理の場合のようにしばしば実際に遭遇する。硫黄または硫黄化合物の存在は、石炭火力発電所の及び含硫黄燃料、例えば燃料油などを用いるタービンまたは他のエンジンの排気ガスを処理する際にしばしば当てはまる。
、未反応のアンモニアの触媒からの放出がそれ自体大気汚染問題を生むから、普通化学量論量以上のかなり過剰なアンモニアを付与しない。そのような未反応アンモニアの放出は、アンモニアが化学量論量または準化学量論量でしか存在しない場合でさえ、不完全な反応及び/またはガス流中でのアンモニアの貧弱な混合の結果として、起こりうる。高アンモニア濃度の通り道は、貧弱な混合でガス流中に形成され、複数の細いガス流路が平行して延びる耐火物を含んでなる一体型ハニカム基材担体を含む触媒を使用する場合には、粒状触媒床の時と異なって流路間のガスの混合機会がないから、特に関心事である。
うな具体例はバナジア及びチタニア及び随時タングステンの混合物を含む押出された均質なハニカム触媒である。そのような触媒は工業ではよく知られており、約5−約10ppmのアンモニアスリップ値を与える。触媒で被覆されたハニカムまたはプレートも使用できる。
4NH3 + 3O2 → 2N2 + 6H2O (3)
2NH3 + 2O2 → 3N2O + 3H2O (4)
4NH3 + 5O2 → 4NO + 6H2O (5)
本明細書に開示される本発明は、非常に有効な二次触媒、すなわちアンモニア酸化触媒をSCRシステムの下流に付加して、望ましくないアンモニアスリップを煙道ガスに存在する残存酸素と反応させることによって除去する。驚くべきことに、ある二次触媒は例え煙道ガス中の残存酸素が少量だけであっても、この目的に使用できることが発見された。約300−450℃で変化する温度において、アンモニアの高転化率はごく少量のNOxを生成するだけで達成できる。
(a)煙道ガス温度、酸素濃度、及び流速においてアンモニアを酸化し得る材料;
(b)硫黄酸化物及び窒素の存在下に機能しうる材料;
(c)アンモニアの酸化の副反応で窒素酸化物を最少でしか生成しないような材料;
(d)アンモニアの出口値が2ppmまたはそれ以下となるようにNOxの低減を向上させるような材料;
(e)CO量を減じるような材料;そして
(f)SO2量を維持するような材料。
の貴金属の化合物及び/または錯体をチタニアバルク担体材料上に分散させることによりチタニア基材上に含ませうる。本明細書で使用するごとき、「化合物」とは、焼成時にまたは触媒の使用時に分解し、またはさもなければ必ずしも必要ないがしばしば酸化物である触媒活性形に転化する触媒的に活性な成分(または「触媒成分」)の塩、錯体などを意味する。1つまたはそれ以上の貴金属触媒化合物の化合物または錯体は、担体材料を湿らすまたはそれにしみこむ、触媒材料の他の成分と悪い反応をしない、そして加熱及び/または真空の適用時に揮発または分解によって触媒から除去できるいずれかの液体に溶解または懸濁させることができる。一般に経済性及び環境面の観点から可溶性化合物または錯体の水溶液は好適である。例えば、適当な水に可溶な白金族金属化合物は、クロロ白金酸、アミン可溶化水酸化白金、塩化ロジウム、硝酸ロジウム、ヘキサミン塩化ロジウム、硝酸パラジウム、または塩化パラジウムなどである。この化合物含有液体を触媒のバルク担体チタニア粒子のポア中に含浸させ、この含浸させた材料を乾燥し、好ましくは焼成して液体を除去し、白金族金属を担体材料中へ結合させる。いくつかの場合には、触媒を使用するまで且つ高温の排気ガスに供するまで、(例えば結晶水として存在しうる)液体の除去は完結してなくてもよい。焼成工程中、または少なくとも触媒使用の初期相中、そのような化合物は白金族金属またはその化合物の触媒活性形に転化される。バナジウム成分をチタニア担体材料に含ませる場合も類似した手法が行われる。例えばバナジウム塩、例えばシュウ酸バナジルはよく知られており、バナジウムのチタニア担体への導入に使用できる。更にチタニア担体材料の代わりにいずれかの有用な金属酸化物担体も使用できる。
本実施例では、約90m2/gの表面積のチタニア担体上に含浸された種々の金属酸化物を含んでなるサンプル触媒を調製した。金属酸化物は、V2O5、MnO、CuO、ZnO、及びMoO3であった。
バナジウム/チタニア触媒は次のように調製した。
1.水中13重量%シュウ酸バナジルの溶液を水7.28gで更に希釈した。
2.ミレニアム(Millenium)からのチタニア193.7gにシュウ酸バナジル溶液142.86gを含浸させた。
3.この含浸させたチタニア粉末を乾燥し、400℃で2時間焼成した。
本実施例では、チタニア上に貴金属及びアルミナ上に貴金属を含んでなる触媒を調製した。
本実施例では、実施例2のPM含浸アルミナ粉末を用いるハニカム触媒の調製を記述する。
た。ついで64cpsiのハニカムを、焼成後1.7g/in3の付加量になるようにスラリーでコーティングした。ついでこのハニカムを乾燥し、500℃で1時間焼成した。
実施例2のPM含浸チタニア粉末を用いるハニカム触媒の調製を記述する。
実施例3及び4に記述したハニカム触媒の、アンモニア転化に対する性能を、CO 25ppm、アンモニア15ppm、酸素15%、水10%、及びNOx 2.5ppmを含むガス流で評価した。アンモニア及びCOの転化率を300℃−500℃で記録した。
転嫁率%=[(NH3 in − NH3 out)/ NH3 in]x100(1)
実施例1で調製したようなチタニア上バナジアの触媒粉末を、実施例4に記述したようなハニカム上にコーティングした。このコーティングしたハニカム上に白金2g/ft3を含浸させた。Pt処理したハニカムを種々の温度でアンモニア転化に関して試験した。試験結果は図3の通りである。図3に示すように、温度が300℃から500℃へ上昇するにつれて、アンモニアの転化率は20%以上から80%以上まで増加し、一方一酸化炭素は二酸化炭素への転化割合が300℃で丁度20%以下及び450℃で50%以上であった。しかしながら温度が上昇するにつれて、生成するNOxの量はかなり増加した。従ってアンモニア酸化の温度を、500℃以下、好ましくは約300−450℃、より好ま
しくは300−400℃に保つことが望ましい。
Claims (19)
- a.アンモニアを石炭の燃焼から得られる煙道ガスに添加しそして一次触媒の存在下に窒素酸化物を還元して、NOx含量が該煙道ガス以下となった未反応のアンモニアを含んでなる、処理した煙道ガスを生成させ;
b.該処理した煙道ガスを二次アンモニア酸化触媒と接触させてアンモニアの量を減じる、但し該二次触媒が貴金属及びバナジアをチタニア、アルミナ、シリカ、アルミナ−シリカ、ジルコニア、酸化マグネシウム、酸化ハフニウム及び酸化ランタンから選ばれる金属酸化物担体上に含んでなる、
工程を含んでなる、アンモニアを選択的触媒還元剤として窒素酸化物を還元するための一次触媒と共に使用する石炭燃焼発電所からの煙道ガス中のアンモニアの除去法。 - 該金属酸化物担体がチタニアである、請求項1の方法。
- 該貴金属が白金、パラジウム、ロジウム及び金からなる群から選択される、請求項1の方法。
- 該貴金属が白金である、請求項1の方法。
- 該二次触媒をハニカム形の基材上に適用する、請求項1の方法。
- 該処理した煙道ガスを300−450℃の温度で二次触媒と接触させる、請求項1の方法。
- 該二次触媒と接触させる前に、酸素源を該処理した煙道ガスに添加する、請求項1の方法。
- 該二次触媒が該基材の立方インチ当り1.0−2.5gの範囲で存在する、請求項5の方法。
- 該一次触媒がチタニア上バナジアである、請求項1の方法。
- 該一次触媒が均質な押出し物である、請求項9の方法。
- 該貴金属が白金である、請求項2の方法。
- 該二次触媒をハニカム形の基材上に適用する、請求項2の方法。
- 該処理した煙道ガスを300−450℃の温度で二次触媒と接触させる、請求項2の方法。
- 該二次触媒と接触させる前に、酸素源を該処理した煙道ガスに添加する、請求項2の方法。
- 該二次触媒が該基材の立方インチ当り1.0−2.5gの範囲で存在する、請求項12の方法。
- 該貴金属が該金属酸化物担体に対して0.1−2.0重量%の量で存在する、請求項1の方法。
- 該バナジアが該金属酸化物担体の1.0−10重量%をなす、請求項1の方法。
- 該貴金属が該チタニアの0.1−2.0重量%の量で存在する、請求項15の方法。
- 該バナジアが該チタニアの1.0−10重量%の量で存在する、請求項18の方法。
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KR20190019930A (ko) * | 2016-06-21 | 2019-02-27 | 할도르 토프쉐 에이/에스 | 오프-가스에서 질소 산화물, voc 및 일산화탄소의 저감을 위한 모노리스 촉매의 제조 방법 |
KR102330444B1 (ko) | 2016-06-21 | 2021-11-26 | 할도르 토프쉐 에이/에스 | 오프-가스에서 질소 산화물, voc 및 일산화탄소의 저감을 위한 모노리스 촉매의 제조 방법 |
Also Published As
Publication number | Publication date |
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CN101160164A (zh) | 2008-04-09 |
WO2006088634A3 (en) | 2006-11-23 |
US20060182676A1 (en) | 2006-08-17 |
US7393511B2 (en) | 2008-07-01 |
EP1874441A2 (en) | 2008-01-09 |
DK1874441T3 (en) | 2014-03-24 |
CN101160164B (zh) | 2011-12-28 |
CA2599114C (en) | 2013-08-20 |
PT1874441E (pt) | 2014-02-12 |
WO2006088634A2 (en) | 2006-08-24 |
EP1874441B1 (en) | 2014-01-01 |
KR20070112201A (ko) | 2007-11-22 |
JP2008529787A (ja) | 2008-08-07 |
ES2448573T3 (es) | 2014-03-14 |
CA2599114A1 (en) | 2006-08-24 |
KR20130085061A (ko) | 2013-07-26 |
PL1874441T3 (pl) | 2014-05-30 |
KR101326359B1 (ko) | 2013-11-11 |
JP5576023B2 (ja) | 2014-08-20 |
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