KR20170128220A - 촉매화된 세라믹 캔들 필터 및 오프가스 또는 배기가스의 정화 방법 - Google Patents
촉매화된 세라믹 캔들 필터 및 오프가스 또는 배기가스의 정화 방법 Download PDFInfo
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- KR20170128220A KR20170128220A KR1020177021030A KR20177021030A KR20170128220A KR 20170128220 A KR20170128220 A KR 20170128220A KR 1020177021030 A KR1020177021030 A KR 1020177021030A KR 20177021030 A KR20177021030 A KR 20177021030A KR 20170128220 A KR20170128220 A KR 20170128220A
- Authority
- KR
- South Korea
- Prior art keywords
- filter
- exhaust gas
- calcium
- offgas
- particulate matter
- Prior art date
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- 238000000034 method Methods 0.000 title claims abstract description 20
- 239000000919 ceramic Substances 0.000 title claims description 18
- KDLHZDBZIXYQEI-UHFFFAOYSA-N Palladium Chemical compound [Pd] KDLHZDBZIXYQEI-UHFFFAOYSA-N 0.000 claims abstract description 36
- 239000003054 catalyst Substances 0.000 claims abstract description 28
- MWUXSHHQAYIFBG-UHFFFAOYSA-N nitrogen oxide Inorganic materials O=[N] MWUXSHHQAYIFBG-UHFFFAOYSA-N 0.000 claims abstract description 27
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 claims abstract description 17
- 229910052763 palladium Inorganic materials 0.000 claims abstract description 15
- 238000007254 oxidation reaction Methods 0.000 claims abstract description 14
- XHCLAFWTIXFWPH-UHFFFAOYSA-N [O-2].[O-2].[O-2].[O-2].[O-2].[V+5].[V+5] Chemical compound [O-2].[O-2].[O-2].[O-2].[O-2].[V+5].[V+5] XHCLAFWTIXFWPH-UHFFFAOYSA-N 0.000 claims abstract description 13
- 230000003647 oxidation Effects 0.000 claims abstract description 13
- 239000013618 particulate matter Substances 0.000 claims abstract description 13
- 229910001935 vanadium oxide Inorganic materials 0.000 claims abstract description 13
- 229930195733 hydrocarbon Natural products 0.000 claims abstract description 11
- 150000002430 hydrocarbons Chemical class 0.000 claims abstract description 11
- 239000004071 soot Substances 0.000 claims abstract description 10
- 229910052751 metal Inorganic materials 0.000 claims abstract description 6
- 239000002184 metal Substances 0.000 claims abstract description 6
- 239000002956 ash Substances 0.000 claims abstract description 5
- 150000002736 metal compounds Chemical class 0.000 claims abstract description 5
- 239000007789 gas Substances 0.000 claims description 26
- 239000000835 fiber Substances 0.000 claims description 9
- 239000003638 chemical reducing agent Substances 0.000 claims description 6
- FGZBFIYFJUAETR-UHFFFAOYSA-N calcium;magnesium;silicate Chemical compound [Mg+2].[Ca+2].[O-][Si]([O-])([O-])[O-] FGZBFIYFJUAETR-UHFFFAOYSA-N 0.000 claims description 5
- 229910010293 ceramic material Inorganic materials 0.000 claims description 5
- 239000000203 mixture Substances 0.000 claims description 5
- 239000006185 dispersion Substances 0.000 claims description 4
- QJGQUHMNIGDVPM-UHFFFAOYSA-N nitrogen group Chemical group [N] QJGQUHMNIGDVPM-UHFFFAOYSA-N 0.000 claims description 4
- 239000000378 calcium silicate Substances 0.000 claims description 3
- 229910052918 calcium silicate Inorganic materials 0.000 claims description 3
- 229960003340 calcium silicate Drugs 0.000 claims description 3
- 235000012241 calcium silicate Nutrition 0.000 claims description 3
- OYACROKNLOSFPA-UHFFFAOYSA-N calcium;dioxido(oxo)silane Chemical compound [Ca+2].[O-][Si]([O-])=O OYACROKNLOSFPA-UHFFFAOYSA-N 0.000 claims description 3
- 238000010531 catalytic reduction reaction Methods 0.000 claims description 3
- GNTDGMZSJNCJKK-UHFFFAOYSA-N divanadium pentaoxide Chemical compound O=[V](=O)O[V](=O)=O GNTDGMZSJNCJKK-UHFFFAOYSA-N 0.000 description 10
- 239000010936 titanium Substances 0.000 description 5
- 239000012855 volatile organic compound Substances 0.000 description 5
- 239000000428 dust Substances 0.000 description 4
- 239000011149 active material Substances 0.000 description 3
- 238000004519 manufacturing process Methods 0.000 description 3
- 238000006722 reduction reaction Methods 0.000 description 3
- -1 waste incineration Substances 0.000 description 3
- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 description 2
- 230000010718 Oxidation Activity Effects 0.000 description 2
- NINIDFKCEFEMDL-UHFFFAOYSA-N Sulfur Chemical compound [S] NINIDFKCEFEMDL-UHFFFAOYSA-N 0.000 description 2
- 229910021541 Vanadium(III) oxide Inorganic materials 0.000 description 2
- 229910021542 Vanadium(IV) oxide Inorganic materials 0.000 description 2
- 229910002091 carbon monoxide Inorganic materials 0.000 description 2
- 238000006243 chemical reaction Methods 0.000 description 2
- 150000002013 dioxins Chemical class 0.000 description 2
- 239000003344 environmental pollutant Substances 0.000 description 2
- 150000002240 furans Chemical class 0.000 description 2
- 231100000719 pollutant Toxicity 0.000 description 2
- 239000002243 precursor Substances 0.000 description 2
- 229910052717 sulfur Inorganic materials 0.000 description 2
- 239000011593 sulfur Substances 0.000 description 2
- IBYSTTGVDIFUAY-UHFFFAOYSA-N vanadium monoxide Chemical compound [V]=O IBYSTTGVDIFUAY-UHFFFAOYSA-N 0.000 description 2
- 239000004215 Carbon black (E152) Substances 0.000 description 1
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 description 1
- 239000011865 Pt-based catalyst Substances 0.000 description 1
- 230000004913 activation Effects 0.000 description 1
- 239000003513 alkali Substances 0.000 description 1
- 229910000323 aluminium silicate Inorganic materials 0.000 description 1
- 229910021529 ammonia Inorganic materials 0.000 description 1
- 230000015572 biosynthetic process Effects 0.000 description 1
- 239000004568 cement Substances 0.000 description 1
- 239000003245 coal Substances 0.000 description 1
- 238000002485 combustion reaction Methods 0.000 description 1
- 238000007796 conventional method Methods 0.000 description 1
- 230000009849 deactivation Effects 0.000 description 1
- 238000000354 decomposition reaction Methods 0.000 description 1
- 230000009977 dual effect Effects 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 238000001914 filtration Methods 0.000 description 1
- 239000000446 fuel Substances 0.000 description 1
- 239000011521 glass Substances 0.000 description 1
- 230000008595 infiltration Effects 0.000 description 1
- 238000001764 infiltration Methods 0.000 description 1
- 229910052500 inorganic mineral Inorganic materials 0.000 description 1
- 239000002923 metal particle Substances 0.000 description 1
- 239000011859 microparticle Substances 0.000 description 1
- 239000011707 mineral Substances 0.000 description 1
- 229910000510 noble metal Inorganic materials 0.000 description 1
- KFAFTZQGYMGWLU-UHFFFAOYSA-N oxo(oxovanadiooxy)vanadium Chemical compound O=[V]O[V]=O KFAFTZQGYMGWLU-UHFFFAOYSA-N 0.000 description 1
- DUSYNUCUMASASA-UHFFFAOYSA-N oxygen(2-);vanadium(4+) Chemical compound [O-2].[O-2].[V+4] DUSYNUCUMASASA-UHFFFAOYSA-N 0.000 description 1
- 239000002245 particle Substances 0.000 description 1
- 238000000746 purification Methods 0.000 description 1
- 239000000376 reactant Substances 0.000 description 1
- 150000003839 salts Chemical class 0.000 description 1
- 150000004760 silicates Chemical class 0.000 description 1
- 239000002002 slurry Substances 0.000 description 1
- 229910052720 vanadium Inorganic materials 0.000 description 1
- LEONUFNNVUYDNQ-UHFFFAOYSA-N vanadium atom Chemical class [V] LEONUFNNVUYDNQ-UHFFFAOYSA-N 0.000 description 1
- GRUMUEUJTSXQOI-UHFFFAOYSA-N vanadium dioxide Chemical compound O=[V]=O GRUMUEUJTSXQOI-UHFFFAOYSA-N 0.000 description 1
- 238000004056 waste incineration Methods 0.000 description 1
Classifications
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- B01J23/38—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals
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- B01D53/34—Chemical or biological purification of waste gases
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- F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
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- F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
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Abstract
세라믹 캔들 필터, 및 공정 오프가스 또는 엔진 배기가스에 존재하는 탄화수소 및 질소 산화물과 함께, 그을음, 애시, 금속 및 금속 화합물의 형태의 미립자 물질의 제거에서 필터의 사용으로서, 이 필터는 적어도 분산 측 상에 및/또는 필터의 벽 내부에 배열된 조합된 SCR 및 산화 촉매를 포함하며, 조합된 SCR 및 산화 촉매는 팔라듐, 바나듐 산화물 및 티타니아를 포함한다.
Description
본 발명은 세라믹 캔들 필터 및 오프가스 또는 배기가스의 정화 방법에 관한 것이다. 더 구체적으로, 본 발명은 공정 가스 중의 분진 및 미립자 물질과 공정 가스에 함유된 유해 성분들의 제거를 위한 촉매화된 세라믹 캔들 필터를 제공한다. 촉매화된 세라믹 캔들 필터는 특히 미네랄, 유리, 시멘트의 생산, 폐기물 소각, 또는 석탄 연료 보일러 및 엔진과 같은 연소를 수반하는 산업 공정으로부터의 공정 가스 또는 생 가스(raw gas)의 정화에 유용하다.
필터 캔들 형태의 세라믹 필터는 공정 가스로부터 미립자 물질의 제거를 위해 많은 산업분야에서 사용된다. 이들은 이용가능한 집진기의 가장 효과적인 종류 중 하나이며, 미립자에 대해 99%를 초과하는 집진 효율을 달성할 수 있다. 이 필터는 알칼리 및 알칼리 토류 실리케이트, 또는 알루미노 실리케이트로 이루어진 세라믹 섬유를 포함하는 다양한 세라믹 재료로 제조될 수 있다.
세라믹 캔들 필터의 높은 미립자 제거 효율은 일부는 캔들 필터의 표면 상에 형성된 분진 케이크로 인한 것이고, 일부는 캔들 필터 조성 및 기공도로 인한 것이다. 필터 전체에서 충분한 여과 활성 및 허용되는 낮은 압력 강하를 제공하기 위하여 종래의 세라믹 캔들 필터는 70 내지 90%의 기공도를 가진다. 이들 필터의 벽 두께는 충분한 안정성 및 기계 강도를 위해 10-20mm의 범위 내여야 한다.
입자-함유 공정 오프가스 및 엔진 배기가스는 매우 자주 복수의 오염물질, 예를 들어 NOx, 휘발성 유기 화합물(VOC), SO2, CO, NH3, 다이옥신 및 푸란을, 지역 규제에 따라서는 감소되어야 하는 농도로 함유한다. 이 목적을 위해 몇 가지 종래의 방법이 이용될 수 있다.
NOx, VOC, 다이옥신 및 푸란과 같은 가스상 오염물질의 경감은 촉매와의 접촉에 의해 효과적으로 수행될 수 있다. 특히, 바나듐 산화물-기재 촉매는 고정적 용도 및 자동차 용도에서 NH3를 사용한 NOx의 선택적 환원에 의한 NOx 환원에서 흔히 사용되는 촉매이다.
이 촉매는 탄화수소의 산화 제거 및 NH3와의 반응에 의한 NOx의 선택적 촉매 환원에서 모두 활성이다.
Pd 촉매와 같은 귀금속 촉매와 비교하여 바나듐 산화물 촉매는 CO2의 형성에서 덜 선택적이고, 어느 정도의 CO가 산화 반응 동안 생성된다. CO는 바나듐 산화물 촉매와의 접촉에 의해서 의미있는 반응 속도로 CO2로 산화될 수 없다.
우리는 바나듐 산화물과 팔라듐을 둘 다 포함하는 촉매를 가진 캔들 필터를 제공할 때 NOx의 암모니아-SCR 및 필터로부터 암모니아 및 일산화탄소의 더 적은 슬립과 함께 탄화수소 및 그을음의 효과적인 산화를 가져온다는 것을 발견했다.
이 발견에 따라서, 본 발명은 공정 오프가스 또는 엔진 배기가스에 존재하는 탄화수소 및 질소 산화물과 함께, 그을음, 애시, 금속 및 금속 화합물의 형태의 미립자 물질의 제거에 적합한 세라믹 캔들 필터를 제공하며, 이 필터는 적어도 분산 측 상에 및/또는 필터의 벽 내부에 배열된 조합된 SCR 및 산화 촉매를 포함하고, 조합된 SCR 및 산화 촉매는 팔라듐, 바나듐 산화물 및 티타니아를 포함한다.
여기 사용된 용어 "분산 측" 및 "침투 측"은 각각 필터되지 않은 배기가스와 마주한 필터의 유동 측 및 필터된 오프가스 또는 배기가스와 마주한 유동 측을 말한다.
추가로, 본 발명은 공정 오프가스 또는 엔진 배기가스에 존재하는 탄화수소 및 질소 산화물과 함께, 그을음, 애시, 금속 및 금속 화합물의 형태의 미립자 물질의 제거 방법을 제공하며, 이 방법은
질소성 환원제를 함유하는 공정 오프가스 또는 엔진 배기가스를 제공하거나 오프가스 또는 배기가스에 질소성 환원제를 첨가하는 단계;
오프가스 또는 배기가스를 세라믹 캔들 필터를 통과시키고 미립자 물질을 포착하는 단계; 및
적어도 하나의 미립자 필터 상에 포착된 미립자 물질에서 그을음의 양을 감소시키고, 탄화수소의 산화에 의해 그리고 분산 측 상에 및/또는 필터의 벽 내부에 배열된 조합된 SCR 및 산화 촉매와 접촉한 질소성 환원제에 의한 질소 산화물의 선택적 촉매 환원(SCR)에 의해 오프가스 또는 배기가스에서 질소 산화물 및 탄화수소의 양을 감소시키는 단계
를 포함하며, 조합된 SCR 및 산화 촉매는 팔라듐, 바나듐 산화물 및 티타니아를 포함한다.
용어 "한 바나듐 산화물" 또는 "바나듐 산화물"은 바나듐(II)산화물(바나듐 모노옥사이드), VO; 또는 바나듐(III)산화물(바나듐 세스퀴옥사이드 또는 트리옥사이드), V2O3; 또는 바나듐(IV)산화물(바나듐 디옥사이드), VO2; 또는 바나듐(V)산화물(바나듐펜톡사이드), V2O5를 말한다.
바람직하게, 본 발명에서 사용하기 위한 바나듐 산화물은 바나듐(V)산화물(바나듐펜톡사이드), V2O5를 포함하거나 그것으로 구성된다.
용어 "티타니아"는 이산화티타늄(TiO2)을 말한다.
팔라듐의 촉매 활성 형태는 금속 및/또는 산화 형태의 팔라듐이다.
단축된 Pd/V/Ti는 팔라듐, 바나듐 산화물 및 티타니아로 구성된 촉매를 의미한다.
Pd/V/Ti 촉매는 i) 이중 기능성(NOx의 제거 및 VOC, 휘발성 유기 화합물의 제거); ii) S-관용성; 및 iii) 다른 촉매 조성물, 예를 들어 Pt-기재 촉매와 비교하여 낮은 SO2 산화 활성을 가진다.
Pd/V/Ti 촉매를 이용할 때, 촉매화된 필터 캔들은 황 내성이며, 즉 황 불활성화를 겪지 않는다. Pd/V/Ti 촉매는 추가로 SO2의 산화에 의해 형성된 SO3의 양을 감소시킨다. H2S가 또한 필터로 들어가는 공정 가스에 존재한다면, 그것은 또한 Pd/V/Ti 촉매 상에서 SO2로 산화될 것이다.
촉매 활성 재료는 티타니아 마이크로-입자의 형태의 촉매 활성 재료 및 활성 재료의 전구체, 즉 바나듐 및 팔라듐의 염을 함유하는 슬러리로 함침시킴으로써 세라믹 필터 상에 적용될 수 있다. 일단 함침되면, 필터는 이어서 건조되고 모든 전구체의 분해 및 촉매의 활성화에 필요한 온도로 가열된다.
모노리스로 형성된 필터 또는 벽 유동형 필터와 비교하여, 팔라듐 금속 입자와 가스 중 반응물 간의 효과적인 가스 접촉이 훨씬 더 높고, 이것은 합당한 산화 활성을 얻기 위해 필요한 팔라듐의 양을 훨씬 감소시키는 결과를 가져온다.
전형적으로, 본 발명에서 이용된 촉매는 20 내지 1000ppm/필터 중량, 바람직하게 200ppm/중량 미만의 양으로 팔라듐을 함유한다.
고온 세라믹 필터의 경우, 몇 가지 종류의 섬유가 그것의 생산에 사용될 수 있다. 이들은, 예를 들어 실리카-알루미네이트 및 칼슘-실리케이트 섬유, 또는 이들의 혼합물에 의해 구성될 수 있다.
다른 바람직한 세라믹 섬유는 칼슘-마그네슘-실리케이트의 군으로부터 선택된 생체용해성(bio-soluble) 섬유를 포함한다.
Claims (8)
- 공정 오프가스 또는 엔진 배기가스에 존재하는 탄화수소 및 질소 산화물과 함께, 그을음, 애시, 금속 및 금속 화합물의 형태의 미립자 물질의 제거에 적합한 세라믹 캔들 필터로서, 상기 필터는 적어도 분산 측 상에 및/또는 필터의 벽 내부에 배열된 조합된 SCR 및 산화 촉매를 포함하며, 조합된 SCR 및 산화 촉매는 팔라듐, 바나듐 산화물 및 티타니아를 포함하는 세라믹 캔들 필터.
- 제 1 항에 있어서, 촉매는 20 내지 1000ppm/필터의 중량, 바람직하게 20 내지 200ppm의 양으로 팔라듐을 함유하는 것을 특징으로 하는 세라믹 캔들 필터.
- 제 1 항 또는 제 2 항에 있어서, 필터의 세라믹 재료는 실리카-알루미네이트, 칼슘-마그네슘-실리케이트, 칼슘-실리케이트 섬유, 또는 이들의 혼합물의 군으로부터 선택되는 것을 특징으로 하는 세라믹 캔들 필터.
- 제 1 항 내지 제 3 항 중 어느 한 항에 있어서, 필터의 세라믹 재료는 칼슘-마그네슘-실리케이트의 군으로부터 선택된 생체용해성(bio-soluble) 섬유로 구성되는 것을 특징으로 하는 세라믹 캔들 필터.
- 공정 오프가스 또는 엔진 배기가스에 존재하는 탄화수소 및 질소 산화물과 함께, 그을음, 애시, 금속 및 금속 화합물의 형태의 미립자 물질의 제거 방법으로서,
질소성 환원제를 함유하는 공정 오프가스 또는 엔진 배기가스를 제공하거나 오프가스 또는 배기가스에 질소성 환원제를 첨가하는 단계;
오프가스 또는 배기가스를 세라믹 캔들 필터를 통해 통과시키고, 미립자 물질을 포착하는 단계; 및
적어도 하나의 미립자 필터 상에 포착된 미립자 물질에서 그을음의 양을 감소시키고, 탄화수소의 산화에 의해 그리고 분산 측 상에 및/또는 필터의 벽 내부에 배열된 조합된 SCR 및 산화 촉매와 접촉한 질소성 환원제에 의한 질소 산화물의 선택적 촉매 환원(SCR)에 의해 오프가스 또는 배기가스에서 질소 산화물 및 탄화수소의 양을 감소시키는 단계
를 포함하며, 조합된 SCR 및 산화 촉매는 팔라듐, 바나듐 산화물 및 티타니아를 포함하는 방법. - 제 5 항에 있어서, 조합된 산화 및 SCR 촉매는 20 내지 1000ppm/필터의 중량, 바람직하게 20 내지 200ppm의 양으로 팔라듐을 함유하는 것을 특징으로 하는 방법.
- 제 5 항 또는 제 6 항에 있어서, 필터의 세라믹 재료는 실리카-알루미네이트, 칼슘-마그네슘-실리케이트, 칼슘-실리케이트 섬유, 또는 이들의 혼합물로부터 선택되는 것을 특징으로 하는 방법.
- 제 5 항 또는 제 6 항에 있어서, 필터의 세라믹 재료는 칼슘-마그네슘-실리케이트의 군으로부터 선택된 생체용해성 섬유를 포함하는 것을 특징으로 하는 방법.
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PCT/EP2015/055952 WO2016150465A1 (en) | 2015-03-20 | 2015-03-20 | Catalyzed ceramic candle filter and method for cleaning of off- or exhaust gases |
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JP (1) | JP6571788B2 (ko) |
KR (1) | KR102424112B1 (ko) |
CN (1) | CN107427771B (ko) |
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US10076743B2 (en) * | 2015-03-20 | 2018-09-18 | Haldor Topsøe A/S | Catalyzed ceramic candle filter and method of cleaning process off- or exhaust gases |
US10105682B2 (en) * | 2015-03-20 | 2018-10-23 | Haldor Topsøe A/S | Catalyzed ceramic candle filter and method for cleaning of off- or exhaust gases |
CN107427772B (zh) | 2015-03-20 | 2021-02-05 | 托普索公司 | 催化的陶瓷烛式过滤器和清洁工艺尾气或废气的方法 |
CN107636271B (zh) * | 2015-05-19 | 2019-12-27 | 优米科尔股份公司及两合公司 | 用于除去来自发动机废气的颗粒物质和有害化合物的方法、多功能过滤器和*** |
JP7202051B2 (ja) | 2017-06-09 | 2023-01-11 | ビーエーエスエフ コーポレーション | 触媒物品および排気ガス処理システム |
WO2018224651A2 (en) * | 2017-06-09 | 2018-12-13 | Basf Se | Catalytic article and exhaust gas treatment systems |
CN107803113A (zh) * | 2017-12-15 | 2018-03-16 | 江苏龙净科杰催化剂再生有限公司 | 烟气除尘脱硝脱二噁英一体化陶瓷过滤器的制备方法 |
EP3533511A1 (en) | 2018-02-28 | 2019-09-04 | Xpuris GmbH | An exhaust gas treatment method and system arranged for treating exhaust gases collected from at least one foundry process |
EP3533510A1 (en) | 2018-02-28 | 2019-09-04 | Infuser IP ApS | An exhaust gas treatment method and system arranged for treating exhaust gases |
CA3094306C (en) | 2018-04-04 | 2024-05-14 | Unifrax I Llc | Activated porous fibers and products including same |
EP3730210A1 (en) | 2019-04-26 | 2020-10-28 | Umicore Ag & Co. Kg | Catalyst ceramic candle filter for combined particulate removal and the selective catalytic reduction (scr) of nitrogen-oxides |
TWI835948B (zh) | 2018-12-19 | 2024-03-21 | 丹麥商愛利Ip有限公司 | 空氣處理方法及在無塵室中之空氣處理系統 |
TW202103768A (zh) | 2019-03-27 | 2021-02-01 | 英商強生麥特公司 | 用於處理來自固定排放源之含微粒排氣的催化過濾系統 |
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AR103898A1 (es) | 2017-06-14 |
EP3271050A1 (en) | 2018-01-24 |
CN107427771B (zh) | 2021-07-02 |
US10105682B2 (en) | 2018-10-23 |
KR102424112B1 (ko) | 2022-07-25 |
US20180008964A1 (en) | 2018-01-11 |
CN107427771A (zh) | 2017-12-01 |
CA2976131A1 (en) | 2016-09-29 |
JP6571788B2 (ja) | 2019-09-04 |
CA2976131C (en) | 2021-07-06 |
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