KR101322136B1 - Catalyst compositions and support-type catalysts comrising the same - Google Patents
Catalyst compositions and support-type catalysts comrising the same Download PDFInfo
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- KR101322136B1 KR101322136B1 KR1020080133453A KR20080133453A KR101322136B1 KR 101322136 B1 KR101322136 B1 KR 101322136B1 KR 1020080133453 A KR1020080133453 A KR 1020080133453A KR 20080133453 A KR20080133453 A KR 20080133453A KR 101322136 B1 KR101322136 B1 KR 101322136B1
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- 239000003054 catalyst Substances 0.000 title claims abstract description 59
- 239000000203 mixture Substances 0.000 title claims abstract description 45
- 239000010457 zeolite Substances 0.000 claims abstract description 44
- 229910021536 Zeolite Inorganic materials 0.000 claims abstract description 38
- HNPSIPDUKPIQMN-UHFFFAOYSA-N dioxosilane;oxo(oxoalumanyloxy)alumane Chemical compound O=[Si]=O.O=[Al]O[Al]=O HNPSIPDUKPIQMN-UHFFFAOYSA-N 0.000 claims abstract description 31
- 239000000463 material Substances 0.000 claims abstract description 16
- 239000010970 precious metal Substances 0.000 claims abstract description 16
- 229910052751 metal Inorganic materials 0.000 claims abstract description 14
- 239000002184 metal Substances 0.000 claims abstract description 14
- WSFSSNUMVMOOMR-NJFSPNSNSA-N methanone Chemical compound O=[14CH2] WSFSSNUMVMOOMR-NJFSPNSNSA-N 0.000 claims abstract description 6
- 150000002739 metals Chemical class 0.000 claims abstract 2
- 239000000919 ceramic Substances 0.000 claims description 39
- KDLHZDBZIXYQEI-UHFFFAOYSA-N Palladium Chemical compound [Pd] KDLHZDBZIXYQEI-UHFFFAOYSA-N 0.000 claims description 19
- 238000000034 method Methods 0.000 claims description 19
- 229910052763 palladium Inorganic materials 0.000 claims description 9
- 239000011572 manganese Substances 0.000 claims description 8
- 229910000510 noble metal Inorganic materials 0.000 claims description 7
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical compound [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 claims description 6
- PWHULOQIROXLJO-UHFFFAOYSA-N Manganese Chemical compound [Mn] PWHULOQIROXLJO-UHFFFAOYSA-N 0.000 claims description 5
- 229910052748 manganese Inorganic materials 0.000 claims description 5
- 239000007769 metal material Substances 0.000 claims description 5
- 239000010931 gold Substances 0.000 claims description 3
- 229910052697 platinum Inorganic materials 0.000 claims description 3
- 239000010948 rhodium Substances 0.000 claims description 3
- 229910052709 silver Inorganic materials 0.000 claims description 3
- 229910052684 Cerium Inorganic materials 0.000 claims description 2
- KJTLSVCANCCWHF-UHFFFAOYSA-N Ruthenium Chemical compound [Ru] KJTLSVCANCCWHF-UHFFFAOYSA-N 0.000 claims description 2
- BQCADISMDOOEFD-UHFFFAOYSA-N Silver Chemical compound [Ag] BQCADISMDOOEFD-UHFFFAOYSA-N 0.000 claims description 2
- GWXLDORMOJMVQZ-UHFFFAOYSA-N cerium Chemical compound [Ce] GWXLDORMOJMVQZ-UHFFFAOYSA-N 0.000 claims description 2
- 229910001657 ferrierite group Inorganic materials 0.000 claims description 2
- PCHJSUWPFVWCPO-UHFFFAOYSA-N gold Chemical compound [Au] PCHJSUWPFVWCPO-UHFFFAOYSA-N 0.000 claims description 2
- 229910052737 gold Inorganic materials 0.000 claims description 2
- 229910052741 iridium Inorganic materials 0.000 claims description 2
- GKOZUEZYRPOHIO-UHFFFAOYSA-N iridium atom Chemical compound [Ir] GKOZUEZYRPOHIO-UHFFFAOYSA-N 0.000 claims description 2
- 229910052680 mordenite Inorganic materials 0.000 claims description 2
- 229910052762 osmium Inorganic materials 0.000 claims description 2
- SYQBFIAQOQZEGI-UHFFFAOYSA-N osmium atom Chemical compound [Os] SYQBFIAQOQZEGI-UHFFFAOYSA-N 0.000 claims description 2
- 229910052703 rhodium Inorganic materials 0.000 claims description 2
- MHOVAHRLVXNVSD-UHFFFAOYSA-N rhodium atom Chemical compound [Rh] MHOVAHRLVXNVSD-UHFFFAOYSA-N 0.000 claims description 2
- 229910052707 ruthenium Inorganic materials 0.000 claims description 2
- 239000004332 silver Substances 0.000 claims description 2
- 230000000694 effects Effects 0.000 abstract description 5
- 230000001747 exhibiting effect Effects 0.000 abstract description 5
- 239000000383 hazardous chemical Substances 0.000 abstract 1
- 230000003197 catalytic effect Effects 0.000 description 9
- WSFSSNUMVMOOMR-UHFFFAOYSA-N Formaldehyde Chemical compound O=C WSFSSNUMVMOOMR-UHFFFAOYSA-N 0.000 description 8
- 230000000052 comparative effect Effects 0.000 description 8
- -1 aldehyde compounds Chemical class 0.000 description 6
- 239000011230 binding agent Substances 0.000 description 6
- 239000000835 fiber Substances 0.000 description 6
- 238000006243 chemical reaction Methods 0.000 description 5
- 239000011149 active material Substances 0.000 description 4
- 239000000126 substance Substances 0.000 description 4
- 229910052878 cordierite Inorganic materials 0.000 description 3
- JSKIRARMQDRGJZ-UHFFFAOYSA-N dimagnesium dioxido-bis[(1-oxido-3-oxo-2,4,6,8,9-pentaoxa-1,3-disila-5,7-dialuminabicyclo[3.3.1]nonan-7-yl)oxy]silane Chemical compound [Mg++].[Mg++].[O-][Si]([O-])(O[Al]1O[Al]2O[Si](=O)O[Si]([O-])(O1)O2)O[Al]1O[Al]2O[Si](=O)O[Si]([O-])(O1)O2 JSKIRARMQDRGJZ-UHFFFAOYSA-N 0.000 description 3
- 239000007789 gas Substances 0.000 description 3
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 2
- 239000004698 Polyethylene Substances 0.000 description 2
- 239000002202 Polyethylene glycol Substances 0.000 description 2
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 2
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 description 2
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 description 2
- 229910000323 aluminium silicate Inorganic materials 0.000 description 2
- 239000001768 carboxy methyl cellulose Substances 0.000 description 2
- 238000005516 engineering process Methods 0.000 description 2
- 238000004519 manufacturing process Methods 0.000 description 2
- 229910044991 metal oxide Inorganic materials 0.000 description 2
- 150000004706 metal oxides Chemical class 0.000 description 2
- 229920002401 polyacrylamide Polymers 0.000 description 2
- 229920000573 polyethylene Polymers 0.000 description 2
- 239000011148 porous material Substances 0.000 description 2
- 239000010944 silver (metal) Substances 0.000 description 2
- 239000002002 slurry Substances 0.000 description 2
- 244000025254 Cannabis sativa Species 0.000 description 1
- 235000012766 Cannabis sativa ssp. sativa var. sativa Nutrition 0.000 description 1
- 235000012765 Cannabis sativa ssp. sativa var. spontanea Nutrition 0.000 description 1
- 229920002134 Carboxymethyl cellulose Polymers 0.000 description 1
- 229920001353 Dextrin Polymers 0.000 description 1
- 239000004375 Dextrin Substances 0.000 description 1
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- 238000005033 Fourier transform infrared spectroscopy Methods 0.000 description 1
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- 238000004566 IR spectroscopy Methods 0.000 description 1
- 229910018380 Mn(NO3)2.6H2 O Inorganic materials 0.000 description 1
- 239000004677 Nylon Substances 0.000 description 1
- 239000004743 Polypropylene Substances 0.000 description 1
- 239000004372 Polyvinyl alcohol Substances 0.000 description 1
- 229920000297 Rayon Polymers 0.000 description 1
- 229920002472 Starch Polymers 0.000 description 1
- MCMNRKCIXSYSNV-UHFFFAOYSA-N ZrO2 Inorganic materials O=[Zr]=O MCMNRKCIXSYSNV-UHFFFAOYSA-N 0.000 description 1
- DPXJVFZANSGRMM-UHFFFAOYSA-N acetic acid;2,3,4,5,6-pentahydroxyhexanal;sodium Chemical compound [Na].CC(O)=O.OCC(O)C(O)C(O)C(O)C=O DPXJVFZANSGRMM-UHFFFAOYSA-N 0.000 description 1
- NIXOWILDQLNWCW-UHFFFAOYSA-N acrylic acid group Chemical group C(C=C)(=O)O NIXOWILDQLNWCW-UHFFFAOYSA-N 0.000 description 1
- 239000003463 adsorbent Substances 0.000 description 1
- 239000004760 aramid Substances 0.000 description 1
- 229920003235 aromatic polyamide Polymers 0.000 description 1
- 235000009120 camo Nutrition 0.000 description 1
- 235000010948 carboxy methyl cellulose Nutrition 0.000 description 1
- 239000008112 carboxymethyl-cellulose Substances 0.000 description 1
- CETPSERCERDGAM-UHFFFAOYSA-N ceric oxide Chemical compound O=[Ce]=O CETPSERCERDGAM-UHFFFAOYSA-N 0.000 description 1
- 229910000422 cerium(IV) oxide Inorganic materials 0.000 description 1
- 235000005607 chanvre indien Nutrition 0.000 description 1
- 239000011248 coating agent Substances 0.000 description 1
- 238000000576 coating method Methods 0.000 description 1
- 229910017052 cobalt Inorganic materials 0.000 description 1
- 239000010941 cobalt Substances 0.000 description 1
- GUTLYIVDDKVIGB-UHFFFAOYSA-N cobalt atom Chemical compound [Co] GUTLYIVDDKVIGB-UHFFFAOYSA-N 0.000 description 1
- 150000001875 compounds Chemical class 0.000 description 1
- 239000000356 contaminant Substances 0.000 description 1
- 235000019425 dextrin Nutrition 0.000 description 1
- KZHJGOXRZJKJNY-UHFFFAOYSA-N dioxosilane;oxo(oxoalumanyloxy)alumane Chemical compound O=[Si]=O.O=[Si]=O.O=[Al]O[Al]=O.O=[Al]O[Al]=O.O=[Al]O[Al]=O KZHJGOXRZJKJNY-UHFFFAOYSA-N 0.000 description 1
- 239000000839 emulsion Substances 0.000 description 1
- 238000001125 extrusion Methods 0.000 description 1
- 238000009408 flooring Methods 0.000 description 1
- 239000006260 foam Substances 0.000 description 1
- 235000019447 hydroxyethyl cellulose Nutrition 0.000 description 1
- 238000005470 impregnation Methods 0.000 description 1
- 229920000609 methyl cellulose Polymers 0.000 description 1
- 239000001923 methylcellulose Substances 0.000 description 1
- 235000010981 methylcellulose Nutrition 0.000 description 1
- 239000004200 microcrystalline wax Substances 0.000 description 1
- 235000019808 microcrystalline wax Nutrition 0.000 description 1
- 229910052863 mullite Inorganic materials 0.000 description 1
- 229920001778 nylon Polymers 0.000 description 1
- 230000003647 oxidation Effects 0.000 description 1
- 238000007254 oxidation reaction Methods 0.000 description 1
- RVTZCBVAJQQJTK-UHFFFAOYSA-N oxygen(2-);zirconium(4+) Chemical compound [O-2].[O-2].[Zr+4] RVTZCBVAJQQJTK-UHFFFAOYSA-N 0.000 description 1
- 239000003973 paint Substances 0.000 description 1
- 239000012188 paraffin wax Substances 0.000 description 1
- 229920003023 plastic Polymers 0.000 description 1
- 239000004033 plastic Substances 0.000 description 1
- 229920003229 poly(methyl methacrylate) Polymers 0.000 description 1
- 229920002037 poly(vinyl butyral) polymer Polymers 0.000 description 1
- 229920000728 polyester Polymers 0.000 description 1
- 229920001223 polyethylene glycol Polymers 0.000 description 1
- 229920001155 polypropylene Polymers 0.000 description 1
- 229920002451 polyvinyl alcohol Polymers 0.000 description 1
- 235000019422 polyvinyl alcohol Nutrition 0.000 description 1
- 238000001556 precipitation Methods 0.000 description 1
- 239000002243 precursor Substances 0.000 description 1
- 239000002964 rayon Substances 0.000 description 1
- 239000000377 silicon dioxide Substances 0.000 description 1
- 235000019812 sodium carboxymethyl cellulose Nutrition 0.000 description 1
- 229920001027 sodium carboxymethylcellulose Polymers 0.000 description 1
- 239000011122 softwood Substances 0.000 description 1
- 238000003980 solgel method Methods 0.000 description 1
- 239000008107 starch Substances 0.000 description 1
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- 239000000725 suspension Substances 0.000 description 1
- 229920002994 synthetic fiber Polymers 0.000 description 1
- 239000012209 synthetic fiber Substances 0.000 description 1
- 239000004408 titanium dioxide Substances 0.000 description 1
- 239000001993 wax Substances 0.000 description 1
- 238000004804 winding Methods 0.000 description 1
- 239000002023 wood Substances 0.000 description 1
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- 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
- B01J29/00—Catalysts comprising molecular sieves
- B01J29/04—Catalysts comprising molecular sieves having base-exchange properties, e.g. crystalline zeolites
- B01J29/06—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof
- B01J29/70—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof of types characterised by their specific structure not provided for in groups B01J29/08 - B01J29/65
- B01J29/72—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof of types characterised by their specific structure not provided for in groups B01J29/08 - B01J29/65 containing iron group metals, noble metals or copper
- B01J29/74—Noble metals
- B01J29/7415—Zeolite Beta
-
- 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
- B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
- B01J23/38—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals
- B01J23/40—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals of the platinum group metals
- B01J23/46—Ruthenium, rhodium, osmium or iridium
-
- 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
- B01J35/00—Catalysts, in general, characterised by their form or physical properties
- B01J35/60—Catalysts, in general, characterised by their form or physical properties characterised by their surface properties or porosity
- B01J35/61—Surface area
- B01J35/617—500-1000 m2/g
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- 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
- B01J37/00—Processes, in general, for preparing catalysts; Processes, in general, for activation of catalysts
- B01J37/02—Impregnation, coating or precipitation
- B01J37/0201—Impregnation
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- 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
- B01J2523/00—Constitutive chemical elements of heterogeneous catalysts
- B01J2523/30—Constitutive chemical elements of heterogeneous catalysts of Group III (IIIA or IIIB) of the Periodic Table
- B01J2523/37—Lanthanides
- B01J2523/3712—Cerium
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- 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
- B01J2523/00—Constitutive chemical elements of heterogeneous catalysts
- B01J2523/70—Constitutive chemical elements of heterogeneous catalysts of Group VII (VIIB) of the Periodic Table
- B01J2523/72—Manganese
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Abstract
본 발명은 제올라이트, 상기 제올라이트에 담지된 귀금속 물질; 및 활성 금속을 포함하는 촉매 조성물 및 그를 포함하는 담지형 촉매에 관한 것이다. 본 발명에서는 귀금속 물질을 담지하는 담체로서, 제올라이트를 사용함과 동시에, 촉매 조성물에 활성 금속을 적절히 포함시킴으로써, 적은 양의 귀금속을 사용하여도 우수한 활성을 나타낼 수 있는 촉매 조성물 및 그를 포함하는 담지형 촉매를 제공할 수 있다.The present invention is a zeolite, a precious metal material supported on the zeolite; And a catalyst composition comprising an active metal and a supported catalyst comprising the same. In the present invention, a catalyst composition capable of exhibiting excellent activity even when a small amount of precious metal is used by appropriately including an active metal in the catalyst composition as well as using a zeolite as a carrier supporting the precious metal material, and a supported catalyst comprising the same Can be provided.
유해 화학 물질, 포름알데히드, 제올라이트, 귀금속 물질, 활성 금속 Hazardous Chemicals, Formaldehyde, Zeolites, Precious Metals, Active Metals
Description
본 발명은 포름알데히드 등의 유해 가스를 효율적으로 제거할 수 있는 촉매 조성물 및 상기 조성물을 포함하는 담지형 촉매에 관한 것이다.The present invention relates to a catalyst composition capable of efficiently removing harmful gases such as formaldehyde, and a supported catalyst comprising the composition.
아파트, 빌딩, 주택, 학교, 병원 또는 사무실 등과 같은 주거 환경 내에 부설된 벽재 또는 바닥재 등으로부터 방출되는 화학 물질은 인체에 매우 큰 악영향을 미칠 수 있고, 이에 따라 상기와 같은 화학 물질을 효율적으로 제거하기 위한 기술에 대한 연구가 진행되고 있다.Chemicals emitted from walls or floors installed in residential environments such as apartments, buildings, houses, schools, hospitals, or offices can have a very bad effect on the human body, thereby effectively removing such chemicals. Research on the technology for this is in progress.
이와 같은 유해 화학 물질의 대표적인 예로는 포름알데히드 등의 알데히드 화합물을 들 수 있는데, 이와 같은 화합물은 페인트, 벽지, 플라스틱 또는 합성 수지제 바닥재, 카페트, 창 또는 도어 등의 내장재에 주로 함유되어 있다.Representative examples of such harmful chemicals include aldehyde compounds such as formaldehyde, and such compounds are mainly contained in interior materials such as paints, wallpaper, plastic or synthetic floorings, carpets, windows or doors.
현재까지 알려진 방법으로서, 이와 같은 화학 물질의 제거를 위한 대표적인 방법은 활성탄 등과 같은 흡착성이 강한 물질을 사용하여, 오염 물질을 흡착 제거하는 방법이다.As known to date, a representative method for removing such chemicals is a method of adsorbing and removing contaminants by using a strongly adsorbent material such as activated carbon.
또 다른 방법으로는 귀금속 등의 촉매 활성 물질을 금속 산화물 담체에 담지 시켜 사용하는 방법이 알려져 있는데, 예를 들면, 일본특허공개공보 제2006-187760호는 포름알데히드 가스 산화용 촉매로서, 귀금속(ex. Pt, Au, Rh, Pd 또는 Ag 등)이 담지된 금속 산화물 담체(ex. 이산화 세륨, 이산화 지르코늄, 이산화 티탄 등)를 포함하는 촉매 조성물을 개시하고 있다.As another method, a method is known in which a catalytically active material such as a noble metal is supported on a metal oxide carrier. For example, Japanese Patent Laid-Open No. 2006-187760 is a catalyst for formaldehyde gas oxidation. Disclosed is a catalyst composition comprising a metal oxide carrier (eg, cerium dioxide, zirconium dioxide, titanium dioxide, etc.) supported with Pt, Au, Rh, Pd or Ag.
그러나, 상술한 종래 기술, 특히 귀금속 촉매를 사용한 방법의 경우, 그 제거 효율은 어느 정도 우수하나, 만족스러운 제거 효율을 달성하기 위해서는 다량의 귀금속 물질이 사용되어아 한다. 즉, 현재까지 알려진 기술에서는 고가의 귀금속 물질을 많은 양으로 사용하여야 하기 때문에, 그 가격이 높아져 경제성이 현저히 떨어진다는 단점을 가지고 있다.However, in the above-described prior art, in particular the method using the noble metal catalyst, the removal efficiency is somewhat superior, but a large amount of precious metal material should be used to achieve satisfactory removal efficiency. In other words, the technology known to date has a disadvantage in that the expensive noble metal material must be used in a large amount, so that the price is high and economic efficiency is significantly reduced.
본 발명은 전술한 종래 기술의 문제점을 고려하여 이루어진 것으로, 종래에 비해 적은 양의 귀금속을 사용하면서도 우수한 촉매 활성을 나타낼 수 있는 촉매 조성물 및 이를 포함하는 담지형 촉매를 제공하는 것을 목적으로 한다.SUMMARY OF THE INVENTION The present invention has been made in view of the above-described problems of the prior art, and an object thereof is to provide a catalyst composition capable of exhibiting excellent catalytic activity while using a smaller amount of precious metals than in the prior art, and a supported catalyst comprising the same.
본 발명은 상기 과제를 해결하기 위한 수단으로서, 제올라이트; 상기 제올라이트에 담지된 귀금속 물질; 및 활성 금속을 포함하는 촉매 조성물을 제공한다.The present invention as a means for solving the above problems, zeolite; Precious metal materials supported on the zeolite; And it provides a catalyst composition comprising an active metal.
본 발명은 상기 과제를 해결하기 위한 다른 수단으로서, 다공성 세라믹 구조체; 및 상기 다공성 세라믹 구조체에 담지된 본 발명에 따른 촉매 조성물을 포함하는 담지형 촉매를 제공한다.The present invention as another means for solving the above problems, a porous ceramic structure; And it provides a supported catalyst comprising the catalyst composition according to the invention supported on the porous ceramic structure.
본 발명에서는 귀금속 물질을 담지하는 담체로서, 제올라이트를 사용함과 동시에, 촉매 조성물에 활성 금속을 적절히 포함시킴으로써, 적은 양의 귀금속을 사용하여도 우수한 활성을 나타낼 수 있는 촉매 조성물 및 그를 포함하는 담지형 촉매를 제공할 수 있다.In the present invention, a catalyst composition capable of exhibiting excellent activity even when a small amount of precious metal is used by appropriately including an active metal in the catalyst composition as well as using a zeolite as a carrier supporting the precious metal material, and a supported catalyst comprising the same Can be provided.
본 발명은, 제올라이트; 상기 제올라이트에 담지된 귀금속 물질; 및 활성 금속을 포함하는 촉매 조성물에 관한 것이다.The present invention, zeolite; Precious metal materials supported on the zeolite; And a catalyst composition comprising an active metal.
이하, 본 발명의 촉매 조성물을 보다 상세히 설명한다.Hereinafter, the catalyst composition of the present invention will be described in more detail.
본 발명에서는 촉매 활성을 나타내는 귀금속 물질을 담지하는 담체로서 제올라이트를 사용한다. 본 발명에서 사용하는 용어 「제올라이트」는 결정성 알루미노 규산염을 총칭하는 용어로서, 천연적으로 생산되는 제올라이트 및 인공적으로 합성된 제올라이트를 포함하는 개념으로 사용된다.In the present invention, zeolite is used as a carrier for supporting a noble metal material exhibiting catalytic activity. The term "zeolite" used in the present invention is a generic term for crystalline aluminosilicate, and is used as a concept including a naturally produced zeolite and an artificially synthesized zeolite.
본 발명에서는 이와 같이 제올라이트를 촉매 활성 물질의 담체로 사용함으로 해서, 적은 양의 촉매 활성 물질을 사용하면서도 우수한 촉매 활성을 나타내는 촉매 조성물을 제공할 수 있다.In the present invention, by using the zeolite as a carrier of the catalytically active material in this way, it is possible to provide a catalyst composition exhibiting excellent catalytic activity while using a small amount of catalytically active material.
본 발명에서 사용하는 상기 제올라이트는 비표면적이 400m2/g 이상인 것이 바람직하며, 보다 바람직하게는 600m2/g 이상인 것이 바람직하다. 본 발명에서 사용하는 용어 「비표면적」은 담체인 제올라이트의 단위 질량 당 표면적을 의미한다. 상기 비표면적이 400m2/g 미만이면, 흡착될 수 있는 촉매 활성 물질의 양이 줄어들게 되므로 촉매 활성이 저하될 우려가 있다..The zeolite used in the present invention preferably has a specific surface area of 400 m 2 / g or more, and more preferably 600 m 2 / g or more. The term "specific surface area" used in the present invention means the surface area per unit mass of zeolite serving as a carrier. If the specific surface area is less than 400 m 2 / g, the amount of catalytically active material that can be adsorbed is reduced, so that the catalytic activity may be lowered.
본 발명에서 사용할 수 있는 제올라이트의 종류는 특별히 한정되지 않으며, 이 분야에서 공지된 각종 제올라이트를 모두 사용할 수 있다. 이와 같은 제올라이트의 예로는 모르데나이트(mordenite), 페리에라이트(ferrierite), ZSM-5, β-제올라이트, Ga-실리케이트, Ti-실리케이트, Fe-실리케이트 또는 Mn-실리케이트 등의 일종 또는 이종 이상을 들 수 있다. The kind of zeolite which can be used in this invention is not specifically limited, Various zeolites known in this field can be used. Examples of such zeolites include one or more types of mordenite, ferrierite, ZSM-5, β-zeolite, Ga-silicate, Ti-silicate, Fe-silicate or Mn-silicate. Can be mentioned.
본 발명에서는 특히 상기 중 β-제올라이트를 사용하는 것이 보다 바람직하다. β-제올라이트는 다른 종류의 제올라이트에 비하여 기공률 및 비표면적 등의 특성이 우수하며, 특히, 비표면적의 경우, ZSM-5 제올라이트와 같은 다른 제올라이트에 비하여 1.5배나 높기 때문에 본 발명의 촉매 조성물에 사용되는 제올라이트로써 보다 바람직한 효과를 나타낼 수 있다.In this invention, it is especially preferable to use the said (beta) -zeolite among these. β-zeolite has excellent properties such as porosity and specific surface area compared to other types of zeolites, and in particular, the specific surface area is 1.5 times higher than other zeolites such as ZSM-5 zeolites. As a zeolite, a more preferable effect can be exhibited.
본 발명의 촉매 조성물에서 상기 제올라이트에 담지되어 사용되는 귀금속 물질은 포름알데히드 등의 유해 가스를 분해, 제거하는 촉매 활성을 나타내는 것으로서, 그 구체적인 종류는 특별히 제한되지 않는다.The precious metal material supported on the zeolite in the catalyst composition of the present invention exhibits catalytic activity for decomposing and removing harmful gases such as formaldehyde, and the specific kind thereof is not particularly limited.
예를 들어, 본 발명에서는 상기 귀금속 물질로서, 루테늄(Ru), 로듐(Rh), 팔라듐(Pd), 은(Ag), 오스뮴(Os), 이리듐(Ir), 백금(Pt) 또는 금(Au) 등의 일종 또는 이종 이상을 사용할 수 있으나, 이에 제한되는 것은 아니다. 본 발명에서는 특히 가격 대비 촉매 활성이 우수하다는 점에서 팔라듐을 사용할 수 있다.For example, in the present invention, as the precious metal material, ruthenium (Ru), rhodium (Rh), palladium (Pd), silver (Ag), osmium (Os), iridium (Ir), platinum (Pt) or gold (Au) Or the like, or a combination of two or more, but is not limited thereto. In the present invention, palladium may be used, in particular, in terms of excellent catalytic activity compared to price.
본 발명에서는 상기 귀금속 물질은 담체로 사용되는 제올라이트 100 중량부에 대하여 0.25 중량부 내지 1 중량부의 양으로 포함될 수 있다. 상기 함량이 0.25 중량부 미만이면, 촉매 활성이 저하될 우려가 있고, 1 중량부를 초과하면, 제올라이트 담체의 상대적인 유효 면적이 줄어들어 역시 촉매 활성이 저하되거나, 최종 조성물의 가격이 지나치게 고가가 될 우려가 있다.In the present invention, the noble metal material may be included in an amount of 0.25 parts by weight to 1 part by weight based on 100 parts by weight of zeolite used as a carrier. If the content is less than 0.25 parts by weight, there is a fear that the catalytic activity is lowered, if it exceeds 1 parts by weight, the relative effective area of the zeolite carrier is reduced, and also the catalyst activity is lowered, or the price of the final composition may be too expensive have.
본 발명의 촉매 조성물은 또한 전술한 성분에 추가로 활성 금속을 포함할 수 있다. 이와 같이 활성 금속이 포함됨으로 해서, 촉매 조성물에 적은 양의 귀금속이 포함될 경우에도 우수한 촉매 활성을 나타낼 수 있게 된다.The catalyst composition of the present invention may also comprise an active metal in addition to the aforementioned components. As such, since the active metal is included, even when a small amount of precious metal is included in the catalyst composition, excellent catalytic activity can be exhibited.
본 발명에서 사용될 수 있는 활성 금속의 종류는, 전술한 특성을 나타낼 수 있는 것이라면 특별히 한정되지 않으며, 예를 들면 망간(Mn), 세륨(Ce) 및 코발트(Co)로 이루어진 군으로부터 선택된 일종 또는 이종 이상을 사용할 수 있다.The type of active metal that can be used in the present invention is not particularly limited as long as it can exhibit the above-described properties, and is selected from the group consisting of manganese (Mn), cerium (Ce), and cobalt (Co), for example. The above can be used.
상기와 같은 활성 금속은 귀금속 물질과 함께 담체인 제올라이트에 담지된 상태로 촉매 조성물에 포함되어 있을 수 있으며, 이 때 그 함량은 제올라이트 100 중량부에 대하여 5 중량부 내지 20 중량부일 수 있다. 상기 함량이 5 중량부 미만이면, 활성 금속이 촉매 활성에 기여하는 정도가 작아질 우려가 있고, 20 중량부를 초과하면, 귀금속 물질 등 촉매 활성 성분의 상대적 함량이 작아져서, 촉매 조성물의 성능이 저하될 우려가 있다.The active metal as described above may be included in the catalyst composition in a state supported on the zeolite, which is a carrier together with the precious metal material, and the content thereof may be 5 parts by weight to 20 parts by weight based on 100 parts by weight of the zeolite. If the content is less than 5 parts by weight, the degree of contribution of the active metal to the catalytic activity may be reduced. If the content is more than 20 parts by weight, the relative content of the catalytically active component such as a noble metal material is reduced, and the performance of the catalyst composition is lowered. There is a concern.
본 발명에서 상기 각각의 성분을 포함하는 촉매 조성물을 제조하는 방법은 특별히 제한되지 않는다. 예를 들면, 상기 촉매 조성물은 상술한 각각의 성분 또는 그 전구체를 사용하여, 일반적인 함침법, 침전법 또는 솔겔(sol-gel)법 등의 과정을 거쳐 제조될 수 있다.In the present invention, the method for preparing the catalyst composition including the respective components is not particularly limited. For example, the catalyst composition may be prepared by a process such as a general impregnation method, precipitation method or sol-gel method using each of the above-described components or precursors thereof.
본 발명은 또한, 다공성 세라믹 구조체; 및The present invention also provides a porous ceramic structure; And
상기 다공성 세라믹 구조체에 담지된 전술한 본 발명에 따른 촉매 조성물을 포함하는 담지형 촉매에 관한 것이다.It relates to a supported catalyst comprising the catalyst composition according to the present invention described above supported on the porous ceramic structure.
상기 본 발명의 담지형 촉매에서 본 발명의 촉매 조성물이 담지되는 세라믹 구조체의 종류는 특별히 한정되지 않는다. 예를 들면, 본 발명에서는 상기 다공성 세라믹 페이퍼로서, 코디어라이트 계열의 세라믹 구조체, 세라믹 페이퍼를 사용하여 제조된 세라믹 구조체 및 세라믹 폼 등의 일반적인 구조체를 사용할 수 있다.The kind of ceramic structure in which the catalyst composition of the present invention is supported in the supported catalyst of the present invention is not particularly limited. For example, in the present invention, as the porous ceramic paper, general structures such as cordierite-based ceramic structures, ceramic structures manufactured using ceramic papers, and ceramic foams may be used.
특별히 한정되는 것은 아니나, 본 발명에서는 특히 상기 세라믹 구조체로서 세라믹 페이퍼를 사용하여 제조되는 세라믹 구조체를 사용하는 것이 바람직하다.Although it does not specifically limit, In this invention, it is especially preferable to use the ceramic structure manufactured using ceramic paper as said ceramic structure.
이와 같이 세라믹 페이퍼로 제조되는 세라믹 구조체는 압출 방식으로 제조되는 코디어라이트 계열의 구조체에 비해 생산성이 우수하고, 그 기공 특성(ex. 기공 크기 및 기공률 등)도 용이하게 제어할 수 있는 이점이 있다. 또한, 상기 세라믹 페이퍼를 사용한 구조체의 경우, 코디어라이트계 구조체에 비하여, 사용되는 촉매 성분 및 반응 물질의 유효 접촉 면적을 극대화시킬 수 있다.As such, the ceramic structure made of ceramic paper has advantages in that the productivity is superior to that of the cordierite-based structure manufactured by the extrusion method, and the pore characteristics (eg pore size and porosity) can be easily controlled. . In addition, in the case of the structure using the ceramic paper, compared to the cordierite-based structure, it is possible to maximize the effective contact area of the catalyst component and the reaction material used.
보다 구체적으로 상기 본 발명의 세라믹 구조체는 예를 들면, 세라믹 파형 페이퍼 및 상기 파형 페이퍼에 부착된 세라믹 판형 페이퍼를 포함하는 구조를 가질 수 있다. 세라믹 구조체가 위와 같이 3차원 망목 구조를 가짐으로 해서, 포함되는 촉매 성분의 반응 영역을 보다 극대화시킬 수 있다. More specifically, the ceramic structure of the present invention may have a structure including, for example, ceramic corrugated paper and ceramic plate paper attached to the corrugated paper. Since the ceramic structure has a three-dimensional network structure as described above, it is possible to further maximize the reaction region of the catalyst component included.
상기에서 사용되는 세라믹 판형 및 파형 페이퍼 등은 예를 들면, 세라믹 섬유, 유기 섬유 및/또는 바인더 등을 포함하는 슬러리 등을 사용하여 일반적인 제지 공법으로 제조될 수 있다.The ceramic plate and corrugated paper used in the above can be produced by a general papermaking process using, for example, a slurry containing ceramic fibers, organic fibers and / or binders, and the like.
이 때 사용될 수 있는 세라믹 섬유의 종류로는 실리카, 알루미나, 실리카-알루미나, 알루미노 실리케이트, 알루미노 보로실리케이트 및 뮬라이트로 이루어진 군으로부터 선택된 하나 이상을 들 수 있고, 유기 섬유의 예로는 침엽수 펄프, 우드 섬유 또는 헴프(hemp) 등의 천연 섬유; 및 나일론, 레이욘, 폴리에스테르, 폴리프로필렌, 폴리에틸렌, 아라미드 또는 아크릴 등의 합성 섬유를 들 수 있으며, 바인더의 예로는 에폭시계 바인더, 소듐 카복시메틸 셀룰로오스(CMC), 폴리아크릴아미드(PAM), 폴리에틸렌옥시드(PEO), 메틸 셀룰로오스, 히드록시에틸 셀룰로오스, 정제 녹말, 덱스트린, 폴리비닐알코올, 폴리비닐부티랄, 폴리메틸(메타)아크릴레이트, 폴리에틸렌글리콜, 파라핀, 왁스 에멀션 및 미결정 왁스(microcrystalline wax)의 일종 또는 이종 이상의 혼합을 들 수 있으나, 이에 제한되는 것은 아니다. At this time, the type of ceramic fibers that can be used include one or more selected from the group consisting of silica, alumina, silica-alumina, aluminosilicate, alumino borosilicate, and mullite, and examples of organic fibers include softwood pulp and wood. Natural fibers such as fibers or hemps; And synthetic fibers such as nylon, rayon, polyester, polypropylene, polyethylene, aramid or acrylic, and examples of the binder include an epoxy-based binder, sodium carboxymethyl cellulose (CMC), polyacrylamide (PAM), and polyethylene. Oxide (PEO), methyl cellulose, hydroxyethyl cellulose, refined starch, dextrin, polyvinyl alcohol, polyvinyl butyral, polymethyl (meth) acrylate, polyethylene glycol, paraffin, wax emulsion and microcrystalline wax It may be one kind or a mixture of two or more, but is not limited thereto.
상기와 같은 성분을 포함하는 세라믹 페이퍼로 다공성 세라믹 구조체를 제조하는 방법은 특별히 한정되지 않으며, 예를 들면, 상기 성분을 포함하는 세라믹 그린 페이퍼를 파형화하여 세라믹 파형 페이퍼를 제조하고, 제조된 파형 페이퍼를 세라믹 판형 페이퍼와 부착시킨 후, 경우에 따라서는 권취 공정 등을 거쳐 제조된 세라믹 성형체를 바인더 물질로 코팅한 다음 소성시키는 과정을 거쳐 제조할 수 있다.The method for producing the porous ceramic structure from the ceramic paper including the above components is not particularly limited. For example, the ceramic green paper including the above components is corrugated to produce ceramic corrugated paper, and the manufactured corrugated paper is manufactured. After adhering to the ceramic plate-shaped paper, in some cases, the ceramic molded body produced through a winding process or the like may be coated with a binder material and then fired.
상기 다공성 세라믹 구조체를 제조하는 방법에서 각 단계의 구체적인 조건 또는 사용되는 바인더의 종류 등은 특별히 한정되지 않으며, 이 분야의 평균적 기술자는 목적하는 세라믹 구조체에 따라서 적절한 조건을 용이하게 선택할 수 있다.In the method of manufacturing the porous ceramic structure, the specific conditions of each step or the kind of the binder to be used are not particularly limited, and an average person skilled in the art may easily select appropriate conditions according to the desired ceramic structure.
또한, 상기와 같은 방식으로 제조된 다공성 세라믹 구조체에 전술한 본 발명의 촉매 조성물을 담지시키는 방법 역시 특별히 한정되지 않는다. 예를 들면, 본 발명에서는 상기 촉매 조성물을 포함하는 슬러리 또는 현탁액에 세라믹 구조체를 침지시키거나, 또는 촉매 성분을 구조체 표면에 도포, 코팅하는 방법 등을 통해 담지시킬 수 있으며, 경우에 따라서는 적절한 바인더 물질을 사용하여 촉매 성분을 다공성 세라믹 구조체에 담지시킬 수 있다.In addition, the method of supporting the catalyst composition of the present invention described above on the porous ceramic structure prepared in the above manner is not particularly limited. For example, in the present invention, the ceramic structure may be immersed in a slurry or suspension containing the catalyst composition, or the catalyst component may be supported by a method of applying or coating the surface of the structure, and in some cases, a suitable binder. The material may be used to support the catalyst component in the porous ceramic structure.
이하, 하기 실시예를 통하여 본 발명을 보다 상세하게 설명하도록 한다. 다만, 본 발명이 이에 제한되는 것은 아니다.Hereinafter, the present invention will be described in more detail with reference to the following examples. However, the present invention is not limited thereto.
[실시예 1]Example 1
β-제올라이트 5g에 Mn(NO3)2·6H2O 5.061g 및 Pd(NO3)2·XH2O 0.027g을 각각 함침 시키고, 건조한 후 400℃에서 3시간 동안 소성하였다. 5 g of β-zeolite was impregnated with 5.061 g of Mn (NO 3 ) 2 .6H 2 O and 0.027 g of Pd (NO 3 ) 2 .XH 2 O, respectively, and dried and calcined at 400 ° C. for 3 hours.
그 결과, 하기 표 1에 나타난 바와 같이, β-제올라이트 전체 100 중량부에 대하여 망간 20 중량부 및 팔라듐 0.25 중량부를 포함하는 촉매 조성물을 제조하였다.As a result, as shown in Table 1 below, a catalyst composition including 20 parts by weight of manganese and 0.25 parts by weight of palladium was prepared based on 100 parts by weight of the total β-zeolite.
[실시예 2][Example 2]
β-제올라이트 전체 100 중량부에 대하여 팔라듐이 0.1 중량부로 함유된다는 점을 제외하고는 상기 실시예 1과 동일한 방법으로 촉매 조성물을 제조하였다.A catalyst composition was prepared in the same manner as in Example 1, except that 0.1 part by weight of palladium was contained based on 100 parts by weight of the total β-zeolite.
[비교예 1]Comparative Example 1
팔라듐을 포함하지 않았다는 점을 제외하고는 상기 실시예 2와 동일한 방법 으로 촉매 조성물을 제조하였다.A catalyst composition was prepared in the same manner as in Example 2, except that it did not contain palladium.
[비교예 2]Comparative Example 2
망간을 포함하지 않았다는 점을 제외하고는 상기 실시예 2와 동일한 방법으로 촉매 조성물을 제조하였다.A catalyst composition was prepared in the same manner as in Example 2, except that no manganese was included.
이와 같이 실시예 1, 2 및 비교예 1, 2를 통하여 제조된 촉매 조성물의 조성 및 함량을 하기 표 1에 나타내었다.Thus, the compositions and contents of the catalyst compositions prepared through Examples 1 and 2 and Comparative Examples 1 and 2 are shown in Table 1 below.
[시험예][Test Example]
제조 된 촉매 조성물들을 상대습도가 80%인 분위기 (40ppm HCHO, 20%O2, 3%H2O) 조건에서 온도에 따라 HCHO 전환율을 적외선 분광법(FTIR)을 이용하여 측정하고, 이를 도 1에 나타내었다.The prepared catalyst compositions were measured for HCHO conversion using infrared spectroscopy (FTIR) according to the temperature in an atmosphere of 40% relative humidity (40 ppm HCHO, 20% O 2 , 3% H 2 O) and shown in FIG. 1. .
도 1에 나타난 바와 같이, 40℃ 근처의 낮은 온도에서는 실시예 1 및 2에 비하여 비교예 1 및 비교예 2의 HCHO 전환율이 현저하게 떨어지는 것으로 나타났으며, 특히, 100℃를 넘는 경우에도 귀금속인 팔라듐을 전혀 포함하지 않는 비교예 1의 경우, HCHO 전환율이 현저하게 떨어진다는 것을 확인할 수 있다.As shown in FIG. 1, the HCHO conversion rates of Comparative Examples 1 and 2 were significantly lower than those of Examples 1 and 2 at low temperatures of about 40 ° C., and in particular, even when the temperature was above 100 ° C., In the case of Comparative Example 1 containing no palladium, it can be seen that the HCHO conversion rate is significantly lower.
도 1은 본 발명의 일 실시예에 따른 촉매 조성물과 비교예로 사용된 촉매 조성물의 온도에 따른 HCHO 제거율을 비교한 그래프이다.1 is a graph comparing HCHO removal rate with temperature of a catalyst composition according to one embodiment of the present invention and a catalyst composition used as a comparative example.
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