CN108290142B - 含有铜-锰催化剂的用于有害气体去除的复合组合物 - Google Patents
含有铜-锰催化剂的用于有害气体去除的复合组合物 Download PDFInfo
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- CN108290142B CN108290142B CN201680068201.2A CN201680068201A CN108290142B CN 108290142 B CN108290142 B CN 108290142B CN 201680068201 A CN201680068201 A CN 201680068201A CN 108290142 B CN108290142 B CN 108290142B
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- 239000000203 mixture Substances 0.000 title claims abstract description 44
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims abstract description 52
- 150000001875 compounds Chemical class 0.000 claims abstract description 44
- 239000011230 binding agent Substances 0.000 claims abstract description 32
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- 229910003475 inorganic filler Inorganic materials 0.000 claims abstract description 12
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 claims description 16
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 claims description 12
- 239000011148 porous material Substances 0.000 claims description 7
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 claims description 6
- 239000002245 particle Substances 0.000 claims description 6
- 239000007864 aqueous solution Substances 0.000 claims description 5
- 239000008119 colloidal silica Substances 0.000 claims description 5
- OPQARKPSCNTWTJ-UHFFFAOYSA-L copper(ii) acetate Chemical compound [Cu+2].CC([O-])=O.CC([O-])=O OPQARKPSCNTWTJ-UHFFFAOYSA-L 0.000 claims description 5
- 229940071125 manganese acetate Drugs 0.000 claims description 5
- UOGMEBQRZBEZQT-UHFFFAOYSA-L manganese(2+);diacetate Chemical compound [Mn+2].CC([O-])=O.CC([O-])=O UOGMEBQRZBEZQT-UHFFFAOYSA-L 0.000 claims description 5
- 239000012286 potassium permanganate Substances 0.000 claims description 5
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- SHFGJEQAOUMGJM-UHFFFAOYSA-N dialuminum dipotassium disodium dioxosilane iron(3+) oxocalcium oxomagnesium oxygen(2-) Chemical compound [O--].[O--].[O--].[O--].[O--].[O--].[O--].[O--].[Na+].[Na+].[Al+3].[Al+3].[K+].[K+].[Fe+3].[Fe+3].O=[Mg].O=[Ca].O=[Si]=O SHFGJEQAOUMGJM-UHFFFAOYSA-N 0.000 claims description 3
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- UFVKGYZPFZQRLF-UHFFFAOYSA-N hydroxypropyl methyl cellulose Chemical compound OC1C(O)C(OC)OC(CO)C1OC1C(O)C(O)C(OC2C(C(O)C(OC3C(C(O)C(O)C(CO)O3)O)C(CO)O2)O)C(CO)O1 UFVKGYZPFZQRLF-UHFFFAOYSA-N 0.000 claims description 3
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- 239000012855 volatile organic compound Substances 0.000 abstract description 9
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- YXFVVABEGXRONW-UHFFFAOYSA-N Toluene Chemical compound CC1=CC=CC=C1 YXFVVABEGXRONW-UHFFFAOYSA-N 0.000 description 30
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- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 8
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- GUJOJGAPFQRJSV-UHFFFAOYSA-N dialuminum;dioxosilane;oxygen(2-);hydrate Chemical compound O.[O-2].[O-2].[O-2].[Al+3].[Al+3].O=[Si]=O.O=[Si]=O.O=[Si]=O.O=[Si]=O GUJOJGAPFQRJSV-UHFFFAOYSA-N 0.000 description 4
- 239000012153 distilled water Substances 0.000 description 4
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- 238000000034 method Methods 0.000 description 4
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- 229910052757 nitrogen Inorganic materials 0.000 description 4
- KDLHZDBZIXYQEI-UHFFFAOYSA-N palladium Substances [Pd] KDLHZDBZIXYQEI-UHFFFAOYSA-N 0.000 description 4
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Substances [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 description 4
- 239000000126 substance Substances 0.000 description 4
- 238000004458 analytical method Methods 0.000 description 3
- 230000003197 catalytic effect Effects 0.000 description 3
- ZMIGMASIKSOYAM-UHFFFAOYSA-N cerium Chemical compound [Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce] ZMIGMASIKSOYAM-UHFFFAOYSA-N 0.000 description 3
- 239000010949 copper Substances 0.000 description 3
- SYBFKRWZBUQDGU-UHFFFAOYSA-N copper manganese(2+) oxygen(2-) Chemical compound [O--].[O--].[Mn++].[Cu++] SYBFKRWZBUQDGU-UHFFFAOYSA-N 0.000 description 3
- 230000000694 effects Effects 0.000 description 3
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- XCOBTUNSZUJCDH-UHFFFAOYSA-B lithium magnesium sodium silicate Chemical compound [Li+].[Li+].[OH-].[OH-].[OH-].[OH-].[OH-].[OH-].[OH-].[OH-].[OH-].[OH-].[OH-].[OH-].[Na+].[Na+].[Mg+2].[Mg+2].[Mg+2].[Mg+2].[Mg+2].[Mg+2].[Mg+2].[Mg+2].[Mg+2].[Mg+2].[Mg+2].[Mg+2].[Mg+2].[Mg+2].[Mg+2].[Mg+2].O1[Si](O2)([O-])O[Si]3([O-])O[Si]1([O-])O[Si]2([O-])O3.O1[Si](O2)([O-])O[Si]3([O-])O[Si]1([O-])O[Si]2([O-])O3.O1[Si](O2)([O-])O[Si]3([O-])O[Si]1([O-])O[Si]2([O-])O3.O1[Si](O2)([O-])O[Si]3([O-])O[Si]1([O-])O[Si]2([O-])O3.O1[Si](O2)([O-])O[Si]3([O-])O[Si]1([O-])O[Si]2([O-])O3.O1[Si](O2)([O-])O[Si]3([O-])O[Si]1([O-])O[Si]2([O-])O3 XCOBTUNSZUJCDH-UHFFFAOYSA-B 0.000 description 3
- 239000011572 manganese Substances 0.000 description 3
- 238000004519 manufacturing process Methods 0.000 description 3
- 229910052751 metal Inorganic materials 0.000 description 3
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- 238000002336 sorption--desorption measurement Methods 0.000 description 3
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 description 2
- UQSXHKLRYXJYBZ-UHFFFAOYSA-N Iron oxide Chemical compound [Fe]=O UQSXHKLRYXJYBZ-UHFFFAOYSA-N 0.000 description 2
- 229910021380 Manganese Chloride Inorganic materials 0.000 description 2
- GLFNIEUTAYBVOC-UHFFFAOYSA-L Manganese chloride Chemical compound Cl[Mn]Cl GLFNIEUTAYBVOC-UHFFFAOYSA-L 0.000 description 2
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- ODWXUNBKCRECNW-UHFFFAOYSA-M bromocopper(1+) Chemical compound Br[Cu+] ODWXUNBKCRECNW-UHFFFAOYSA-M 0.000 description 2
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- 229910000420 cerium oxide Inorganic materials 0.000 description 2
- 239000011651 chromium Substances 0.000 description 2
- 229910000428 cobalt oxide Inorganic materials 0.000 description 2
- 229910000365 copper sulfate Inorganic materials 0.000 description 2
- ORTQZVOHEJQUHG-UHFFFAOYSA-L copper(II) chloride Chemical compound Cl[Cu]Cl ORTQZVOHEJQUHG-UHFFFAOYSA-L 0.000 description 2
- XTVVROIMIGLXTD-UHFFFAOYSA-N copper(II) nitrate Chemical compound [Cu+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O XTVVROIMIGLXTD-UHFFFAOYSA-N 0.000 description 2
- ARUVKPQLZAKDPS-UHFFFAOYSA-L copper(II) sulfate Chemical compound [Cu+2].[O-][S+2]([O-])([O-])[O-] ARUVKPQLZAKDPS-UHFFFAOYSA-L 0.000 description 2
- GBRBMTNGQBKBQE-UHFFFAOYSA-L copper;diiodide Chemical compound I[Cu]I GBRBMTNGQBKBQE-UHFFFAOYSA-L 0.000 description 2
- RJYMRRJVDRJMJW-UHFFFAOYSA-L dibromomanganese Chemical compound Br[Mn]Br RJYMRRJVDRJMJW-UHFFFAOYSA-L 0.000 description 2
- 238000005516 engineering process Methods 0.000 description 2
- 230000001747 exhibiting effect Effects 0.000 description 2
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- KWLMIXQRALPRBC-UHFFFAOYSA-L hectorite Chemical compound [Li+].[OH-].[OH-].[Na+].[Mg+2].O1[Si]2([O-])O[Si]1([O-])O[Si]([O-])(O1)O[Si]1([O-])O2 KWLMIXQRALPRBC-UHFFFAOYSA-L 0.000 description 2
- 229910000271 hectorite Inorganic materials 0.000 description 2
- 229910010272 inorganic material Inorganic materials 0.000 description 2
- 239000011147 inorganic material Substances 0.000 description 2
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- MIVBAHRSNUNMPP-UHFFFAOYSA-N manganese(2+);dinitrate Chemical compound [Mn+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O MIVBAHRSNUNMPP-UHFFFAOYSA-N 0.000 description 2
- SQQMAOCOWKFBNP-UHFFFAOYSA-L manganese(II) sulfate Chemical compound [Mn+2].[O-]S([O-])(=O)=O SQQMAOCOWKFBNP-UHFFFAOYSA-L 0.000 description 2
- QWYFOIJABGVEFP-UHFFFAOYSA-L manganese(ii) iodide Chemical compound [Mn+2].[I-].[I-] QWYFOIJABGVEFP-UHFFFAOYSA-L 0.000 description 2
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- PWHULOQIROXLJO-UHFFFAOYSA-N Manganese Chemical compound [Mn] PWHULOQIROXLJO-UHFFFAOYSA-N 0.000 description 1
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- 239000003575 carbonaceous material Substances 0.000 description 1
- 239000012018 catalyst precursor Substances 0.000 description 1
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- 239000000919 ceramic Substances 0.000 description 1
- 239000007795 chemical reaction product Substances 0.000 description 1
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- 239000010941 cobalt Substances 0.000 description 1
- GUTLYIVDDKVIGB-UHFFFAOYSA-N cobalt atom Chemical compound [Co] GUTLYIVDDKVIGB-UHFFFAOYSA-N 0.000 description 1
- IVMYJDGYRUAWML-UHFFFAOYSA-N cobalt(ii) oxide Chemical compound [Co]=O IVMYJDGYRUAWML-UHFFFAOYSA-N 0.000 description 1
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- 238000000354 decomposition reaction Methods 0.000 description 1
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- 230000007774 longterm Effects 0.000 description 1
- AMWRITDGCCNYAT-UHFFFAOYSA-L manganese oxide Inorganic materials [Mn].O[Mn]=O.O[Mn]=O AMWRITDGCCNYAT-UHFFFAOYSA-L 0.000 description 1
- WPBNNNQJVZRUHP-UHFFFAOYSA-L manganese(2+);methyl n-[[2-(methoxycarbonylcarbamothioylamino)phenyl]carbamothioyl]carbamate;n-[2-(sulfidocarbothioylamino)ethyl]carbamodithioate Chemical compound [Mn+2].[S-]C(=S)NCCNC([S-])=S.COC(=O)NC(=S)NC1=CC=CC=C1NC(=S)NC(=O)OC WPBNNNQJVZRUHP-UHFFFAOYSA-L 0.000 description 1
- PPNAOCWZXJOHFK-UHFFFAOYSA-N manganese(2+);oxygen(2-) Chemical class [O-2].[Mn+2] PPNAOCWZXJOHFK-UHFFFAOYSA-N 0.000 description 1
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- MHOVAHRLVXNVSD-UHFFFAOYSA-N rhodium atom Chemical compound [Rh] MHOVAHRLVXNVSD-UHFFFAOYSA-N 0.000 description 1
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- 229910001935 vanadium oxide Inorganic materials 0.000 description 1
- 229910052726 zirconium Inorganic materials 0.000 description 1
- 229910001928 zirconium oxide Inorganic materials 0.000 description 1
Images
Classifications
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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
- B01J37/04—Mixing
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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
- B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
- B01J23/70—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper
- B01J23/72—Copper
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/34—Chemical or biological purification of waste gases
- B01D53/74—General processes for purification of waste gases; Apparatus or devices specially adapted therefor
- B01D53/86—Catalytic processes
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/34—Chemical or biological purification of waste gases
- B01D53/74—General processes for purification of waste gases; Apparatus or devices specially adapted therefor
- B01D53/86—Catalytic processes
- B01D53/864—Removing carbon monoxide or hydrocarbons
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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
- B01J21/00—Catalysts comprising the elements, oxides, or hydroxides of magnesium, boron, aluminium, carbon, silicon, titanium, zirconium, or hafnium
- B01J21/16—Clays or other mineral silicates
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Abstract
本发明涉及含有铜‑锰催化剂的用于有害气体去除的复合组合物,所述复合组合物能够去除环境和室内污染物,例如一氧化碳和挥发性有机化合物,所述复合组合物包含与无机层化合物混杂的铜‑锰复合催化剂、无机填料、活性炭和粘合剂。
Description
技术领域
本发明涉及含有铜-锰催化剂的用于有害气体去除的复合组合物,并且更具体地涉及能够去除环境和室内污染物例如一氧化碳和挥发性有机化合物的含有铜-锰催化剂的用于有害气体去除的复合组合物。
背景技术
长期暴露于封闭空间中的有害气体例如一氧化碳会对人体造成致命的损害。
因此需要即使在环境温度下也能够有效地去除这样的有害气体的催化剂。可用作用于在室温下去除一氧化碳的催化剂的Hopcalite(其为锰氧化物、铜氧化物等的混合物)是相对经济的并且在去除一氧化碳方面非常有效,但已知其效果在存在水的情况下急剧降低。
此外,由负载在金属氧化物上的纳米尺寸(5nm)的金(Au)颗粒构成的催化剂具有高的在室温下使一氧化碳氧化的能力。然而,均匀的纳米尺寸金属颗粒的制备和分散需要高技术,这是不期望的。贵金属催化剂例如Au、Pd或Pt表现出优异的催化效率、改善的性能、耐久性和抗中毒性,但由于其高价格而在其分布方面受到限制。此外,一氧化碳去除效率在高温下较高但在低温下降低,并且去除效率不能保持较长的时间。
美国专利第5,283,041号公开了使用包含钒氧化物、锆氧化物以及锰、铈或钴氧化物的三元化合物来处理有机卤化物,韩国专利申请公布第2002-0028791号公开了用铜、锰和稀土金属例如La的混合氧化物来处理挥发性有机化合物。
在上述技术中,基于贵金属的催化剂是有利的,因为在相对低的温度下表现出高活性,但由于相应金属的稀缺及其需求的增加,材料金属是昂贵的并且其价格是波动的。
美国专利第6,458,741号公开了用于挥发性有机化合物分解的催化剂组合物,其基本上含有铈和锆,并且包含诸如Gd、La、Sc、Cr、Ti、V、Mn、Pd或Pt的金属,美国专利第5,851,943号公开了其中钴、铬、铜、铈或铁氧化物负载在铝或二氧化硅上且在其上进一步施加钯、铂、钌或铑的贵金属薄膜的催化剂。
在上述技术中,贵金属和非贵金属一起使用以便解决在单独使用贵金属或非贵金属时的问题,但催化剂组合物中包含的贵金属组分由于废气而中毒,这使催化活性急剧下降。因此,上述技术不能被利用。
以实现在工业领域和多种应用领域中的广泛使用为目标,需要这样的催化剂来代替昂贵的贵金属催化剂:其在室温下具有高的一氧化碳去除效率并且可在室温下有效地去除有气味的气体和挥发性有机化合物。
<专利文献>
美国专利第5283041号(登记日期:1994年2月1日,标题:Catalytic incinerationof organic compounds)
韩国专利申请公布第2002-0028791号(特许公开日期:2002年4月17日,标题:Catalyst for oxidation)
美国专利第6458741号(登记日期:2002年10月1日,标题:Catalysts for low-temperature destruction of volatile organic compounds in air)
美国专利第5851943号(登记日期:1998年12月22日,标题:Ceramic productionprocess)
发明内容
技术问题
因此,考虑到相关技术中遇到的问题而做出了本发明,并且本发明旨在提供含有铜-锰氧化物的用于有害气体去除的复合组合物,与常规昂贵的贵金属催化剂相比,所述复合组合物可在低温(室温)下表现出高的一氧化碳、氮氧化物(NOx)、臭氧、有气味的气体和挥发性有机化合物去除效率。
此外,本发明旨在提供具有高的比表面积和孔体积的含有铜-锰氧化物的用于有害气体去除的复合组合物。
技术方案
因此,本发明提供了含有铜-锰催化剂的用于有害气体去除的复合组合物,其包含与无机层化合物混杂的铜-锰复合催化剂、无机填料、活性炭和粘合剂。
用于有害气体去除的复合组合物优选包含0.5重量%至90重量%的与无机层化合物混杂的铜-锰复合催化剂、5重量%至99重量%的无机填料、0.1重量%至50重量%的活性炭和0.02重量%至10重量%的粘合剂,并且更优选包含1重量%至20重量%的与无机层化合物混杂的铜-锰复合催化剂、45重量%至55重量%的无机填料、30重量%至40重量%的活性炭和4重量%至8重量%的粘合剂。
具体地,无机填料是多孔且重量轻的无机材料,并且其实例可包括无机矿物,例如多孔二氧化硅、氧化铝、二氧化钛、珍珠岩、高岭土等。
粘合剂是选自无机粘合剂和有机粘合剂中的至少一者,并且以基于粘合剂总量的5重量%或更少的量含有有机粘合剂。
无机粘合剂包含选自胶态二氧化硅、二氧化钛、二氧化锆、水玻璃、氧化铝溶胶和无机层化合物中的至少一者。
有机粘合剂包含选自以下中的至少一者:甲基纤维素、羟乙基纤维素、羟丙基甲基纤维素、羟乙基甲基纤维素、甲基乙基纤维素、羧甲基纤维素、羟丙基纤维素、聚乙烯醇、聚乙二醇、聚丙烯酸、聚甲基丙烯酸甲酯和羟丙基。
与无机层化合物混杂的铜-锰复合催化剂具有50nm或更小的粒径,其中铜盐和锰盐以1:2至1:8的摩尔比混合。作为铜盐,选自硝酸铜、氯化铜、碘化铜、溴化铜、硫酸铜和乙酸铜中的至少一者可与锰盐混合,所述锰盐是选自硝酸锰、氯化锰、碘化锰、溴化锰、硫酸锰、高锰酸钾和乙酸锰中的至少一者。
无机层化合物是基于蒙脱石的天然或合成粘土,并且特别地,是选自蒙脱土、膨润土、锂蒙脱石、皂石、贝得石、绿脱石、合成锂皂石(Laponite)、Smecton、白榴岩和可膨胀云母中的至少一者。
作为活性炭,可使用颗粒状或粉末状活性炭而没有特别限制。优选有用的是粉末状活性炭,并且更优选地,使用粒径为约500目或更小的粉末状活性炭。
复合组合物的密度优选为0.3g/cm3至1.0g/cm3,比表面积为300m2/g至800m2/g,并且总孔体积(孔隙率)为0.3cm3/g至1.0cm3/g,并且特别地,密度为0.71g/cm3至0.75g/cm3,比表面积为550m2/g至600m2/g,并且孔隙率为0.85cm3/g至0.9cm3/g。
有益效果
如上所述,本发明在室温下去除对人体有害的一氧化碳、氮氧化物(NOx)、有气味的气体和挥发性有机化合物方面是有效的。
此外,与常规贵金属催化剂相比,本发明可以实现低生产成本并且可以在室温下表现出高的气体去除效率,并且因此可以广泛用于工业领域和多种应用领域。
此外,在本发明中,密度和孔隙率(孔体积)落入适当的范围内,并且比表面积被最大化,由此使有害气体和有气味的物质的物理吸附最大化。
附图说明
图1示出了制备根据本发明的含有铜-锰催化剂的用于有害气体去除的丸粒形式的复合组合物的过程;
图2是示出了根据本发明的含有铜-锰催化剂的用于有害气体去除的丸粒形式的复合组合物的图像;以及
图3是示出了根据本发明的实施例2至5和比较例1的气体去除效率的结果的图。
具体实施方式
在下文中,将参照附图给出本发明的优选实施方案的详细描述。在整个附图中,相应或相同的要素在整个说明书中由相同的附图标记表示。还应注意的是,当相关技术的详细描述使得本发明的主旨不清楚时,将省略相关技术的详细描述。
本发明提出了含有铜-锰催化剂的复合组合物,因此表现出高孔隙率,从而显示出高的有害气体去除效率。根据本发明的含有铜-锰催化剂的用于有害气体去除的复合组合物包含铜-锰催化剂、无机填料、活性炭和粘合剂,并且优选包含0.5重量%至90重量%的与无机层化合物混杂的铜-锰复合催化剂、5重量%至99重量%的无机填料、0.1重量%至50重量%的活性炭和0.02重量%至10重量%的粘合剂,并且更优选包含1重量%至20重量%的与无机层化合物混杂的铜-锰复合催化剂、45重量%至55重量%的无机填料、30重量%至40重量%的活性炭和4重量%至8重量%的粘合剂。
在此,铜-锰催化剂优选包含以1:2至1:8的摩尔比混合的铜盐和锰盐,其粒径为50nm或更小,并且铜盐可为选自硝酸铜、氯化铜、碘化铜、溴化铜、硫酸铜和乙酸铜中的至少一者,锰盐可为选自硝酸锰、氯化锰、碘化锰、溴化锰、硫酸锰、高锰酸钾和乙酸锰中的至少一者。
以下,铜-锰催化剂被称为与无机层化合物混杂的铜-锰复合催化剂。
更优选地,与无机层化合物混杂的铜-锰复合催化剂通过在水溶液相中混合100重量份的无机层化合物与120重量份至180重量份的高锰酸钾、300重量份至400重量份的乙酸锰和100重量份至150重量份的乙酸铜来制备。
在此,无机层化合物为基于蒙脱石的天然或合成粘土,并且为选自蒙脱土、膨润土、锂蒙脱石、皂石、贝得石、绿脱石、合成锂皂石、Smecton、白榴岩和可膨胀云母中的至少一者。
如果与无机层化合物混杂的铜-锰复合催化剂的量小于1重量%,则密度可能降低并且一氧化碳去除效率可能降低。在另一方面,如果其量超过20重量%,则一氧化碳去除效率可能变好,但比表面积和孔隙率可能降低。因此,与无机层化合物混杂的铜-锰复合催化剂可以以实施例1中描述的方式来制备。
无机填料是多孔且重量轻的无机材料,并且其实例可包括无机矿物,例如多孔二氧化硅、氧化铝、二氧化钛、珍珠岩、高岭土等。
活性炭是能够吸附溶液中的溶质或气体的含碳材料,并且活性炭发挥增加孔隙率和比表面积的作用。如果复合组合物中的活性炭的量超过50重量%,则孔隙率和比表面积可能增加,因此可产生良好的粘附性能,但气体去除效率可能降低。
作为活性炭,可使用颗粒状或粉末状活性炭而没有特别限制。在此,优选使用粉末状活性炭,并且更优选使用粒径为约500目或更小的粉末状活性炭。
粘合剂是选自无机粘合剂和有机粘合剂中的至少一者,并且在使用有机粘合剂时,优选地以基于粘合剂总量的5重量%或更小的量含有有机粘合剂。
无机粘合剂包含选自胶态二氧化硅、二氧化钛、二氧化锆、水玻璃、氧化铝溶胶和无机层化合物中的至少一者,有机粘合剂包含选自以下中的至少一者:甲基纤维素、羟乙基纤维素、羟丙基甲基纤维素、羟乙基甲基纤维素、甲基乙基纤维素、羧甲基纤维素、羟丙基纤维素、聚乙烯醇、聚乙二醇、聚丙烯酸、聚甲基丙烯酸甲酯和羟丙基。
复合组合物的密度优选为0.3g/cm3至1.0g/cm3,比表面积为300m2/g至800m2/g,并且总孔体积(孔隙率)为0.3cm3/g至1.0cm3/g。
使含有与无机层化合物混杂的铜-锰复合催化剂的用于有害气体去除的复合组合物形成为丸粒的过程示于图1中。
具体地,将与无机层化合物混杂的浆料型铜-锰复合催化剂、无机填料、活性炭和粘合剂混合(S110)。在此,本发明的实施例2中的与无机层化合物混杂的铜-锰复合催化剂为含水量为80重量%的铜-锰氧化物催化剂浆料,但不仅限于浆料相。
随后,将所得混合物放入模具中并挤出(S120),并且将挤出的产物干燥并进行热处理(S130)。由此,可以以丸粒的形式提供含有铜-锰催化剂的用于有害气体去除的复合组合物。丸粒形式的复合组合物示于图2中。
在实施例2中再次描述了丸粒形式的复合组合物的制备。
[实施例1]与无机层化合物混杂的铜-锰复合催化剂的制备
将无机层化合物和蒸馏水放入反应器中并搅拌,由此制备2kg 2重量%的无机层化合物水溶液。
向所述水溶液中添加0.4mol(63.21g)高锰酸钾(KMnO4),在室温下搅拌1小时,进一步添加通过将0.6mol(147.1g)乙酸锰(Mn(CH3COO)2·4H2O)溶解在2.2mol(40ml)蒸馏水中而获得的水溶液,在室温下搅拌1小时,进一步添加通过将0.25mol(50g)乙酸铜(Cu(CH3COO)2·H2O)溶解在46.6mol(839ml)蒸馏水中而获得的水溶液,并在室温下搅拌2小时。
在搅拌之后,用蒸馏水洗涤反应产物以除去未反应的物质和杂质,最终获得含水量为80重量%的与无机层化合物混杂的铜-锰复合催化剂浆料。即,与无机层化合物混杂的铜-锰复合催化剂的固体含量为20重量%。
[实施例2]丸粒形式的复合组合物的制备
将750g实施例1的与无机层化合物混杂的铜-锰复合催化剂浆料、500g二氧化硅粉末、350g活性炭、200ml 2重量%的无机层化合物水溶液、100ml 1重量%的甲基纤维素水溶液和100ml 50重量%的胶态二氧化硅混合以产生混合物,然后使用混合器对其进行搅拌并使用造粒机挤出成3mm的丸粒。
将由此形成的丸粒在120℃下干燥6小时,然后在300℃下热处理4小时,最终获得丸粒形式的复合组合物。
将以这种方式以丸粒形式产生的复合组合物与通风过滤器一起放置在通过其释放有害物质的通风口处,由此有害物质可以被纯化,然后排出。
[实施例3至5]丸粒形式的复合组合物的制备
以与实施例2中相同的方式制备实施例3至5的丸粒形式的复合组合物,不同之处在于改变其组分的量。
[表1]
<单位g>
实施例2 | 实施例3 | 实施例4 | 实施例5 | |
复合催化剂(20重量%) | 750 | 1250 | 50 | 750 |
气相二氧化硅 | 500 | 500 | 500 | 500 |
活性炭 | 350 | 350 | 500 | 500 |
有机粘合剂(1重量%) | 100 | 100 | 100 | 100 |
胶态二氧化硅(50重量%) | 100 | 100 | 100 | 100 |
无机层化合物(2重量%) | 200 | 200 | 200 | 200 |
[比较例1]非丸粒形式的催化剂的制备
将实施例1的与无机层化合物混杂的铜-锰复合催化剂浆料在120℃下干燥2小时,然后制成粉末状铜-锰催化剂复合物,然后在280℃下热处理2小时,由此获得铜-锰催化剂复合物。
评估如上制备的复合组合物的孔隙率和气体去除性能。
1.孔隙率的评估
通过氮吸附-解吸等温分析评估铜-锰复合催化剂的与孔隙率有关的特性,该铜-锰复合催化剂通过与具有层状结构的无机层化合物混杂的铜-锰复合催化剂前体的热处理制备。
氮吸附-解吸等温分析在氮呈液相的温度(77K)下进行,并且在测量之前在真空中于200℃下将所有样品预处理2小时。
由此测量的氮吸附-解吸等温分析的结果和密度示于下表2中。
[表2]
实施例2 | 实施例3 | 实施例4 | 实施例5 | 比较例1 | |
密度(g/cm<sup>3</sup>) | 0.73 | 0.98 | 0.30 | 0.85 | 1.12 |
比表面积(m<sup>2</sup>/g) | 561 | 350 | 800 | 750 | 336 |
孔隙率(cm<sup>3</sup>/g) | 0.89 | 0.51 | 0.93 | 0.91 | 0.25 |
从表2中可明显看出,其中丸粒的组分的量改变的实施例2至5和比较例1在密度和孔隙率方面不同。
与比较例1相比,实施例2至5的丸粒形式的复合催化剂组合物的密度降低并且与孔隙率有关的特性显著提高。
具体地,与无机层化合物混杂的铜-锰复合催化剂的量在实施例3中比在实施例2中大,并且密度在实施例3中比在实施例2中高,但其比表面积和孔隙率降低。此外,与无机层化合物混杂的铜-锰复合催化剂的量在实施例4中比在实施例2中小,并且活性炭的量在实施例4中比在实施例2中大,因此与实施例2相比,得到高的比表面积和孔隙率但低的密度。
活性炭的量在实施例5中比在实施例2中大,并且当活性炭的量以这种方式增加时,与实施例2相比,密度、比表面积和孔隙率高。
可以确认,密度受与无机层化合物混杂的铜-锰复合催化剂的量和活性炭的量的影响。具体地,为了增加上述影响,当与无机层化合物混杂的铜-锰复合催化剂的量增加时,其他效果降低,并且因此与无机层化合物混杂的铜-锰复合催化剂的量必须在适当的范围内使用。
在根据本发明的实施例2至5中,复合组合物具有落入0.3g/cm3至1.0g/cm3的密度、300m2/g至800m2/g的比表面积和0.3cm3/g至1.0cm3/g的总孔体积(孔隙率)范围内的适当的密度、比表面积和孔隙率,但在比较例1中,密度和孔隙率落在适当的范围以外。与比较例1相比,可以发现根据本发明的实施例2至5的比表面积被最大化。
2.气体去除性能的评估
在评估气体去除性能时,使用实施例2的丸粒形式的复合组合物在室温下测量一氧化碳(CO)、氨(NH3)、硫化氢(H2S)、乙醛(CH3CHO)和甲苯(C6H5CH3)的去除效率。
如下评估实施例2至5和比较例1各自的气体去除性能。
*一氧化碳去除效率的评估
为了评估一氧化碳去除效率,将50g含铜-锰的丸粒型催化剂样品放入5L Tedlar袋中,并向其中注入浓度为50ppm的一氧化碳,之后使用复合气体检测器(Q-RAE Plus)测量浓度随时间的变化。一氧化碳去除效率的测量结果示于下表3中。
30分钟后,在实施例2中除去90%或更大的量的一氧化碳,在实施例3、4和5中分别除去94%、70%和84%的量的一氧化碳,但在比较例1中除去30%的量的一氧化碳。特别地,60分钟后,与实施例相比,在比较例1中去除性能未显著改善。
*氨去除效率的评估
为了评估氨去除效率,将50g含铜-锰的丸粒型催化剂样品放入5LTedlar袋中,并向其中注入浓度为50ppm的氨,之后使用Gastec检测管测量浓度随时间的变化。氨去除效率的测量结果示于下表3中。
30分钟后,在实施例2中除去92%或更大的量的氨,在实施例3、4和5中分别除去60%、86%和70%的量的氨,但在比较例1中去除效率不高,并且不随时间而改善。
*硫化氢去除效率的评估
为了评估硫化氢去除效率,将50g含铜-锰的丸粒型催化剂样品放入5L Tedlar袋中,并向其中注入浓度为50ppm的硫化氢,之后使用Gastec检测管测量浓度随时间的变化。硫化氢去除效率的测量结果示于下表3中。
30分钟后,在实施例2中除去100%的量的硫化氢,在实施例3、4和5中分别除去90%、80%和86%的量的硫化氢,但在比较例1中去除效率不高。
*乙醛去除效率的评估
为了评估乙醛去除效率,将50g含铜-锰的丸粒型催化剂样品放入5LTedlar袋中,并向其中注入浓度为50ppm的乙醛,之后使用Gastec检测管测量浓度随时间的变化。乙醛去除效率的测量结果示于下表3中。
30分钟后,在实施例2中除去80%或更大的量的乙醛,在实施例3、4和5中分别除去50%、50%和70%的量的乙醛,但在比较例1中去除效率不高。
*甲苯去除效率的评估
为了评估甲苯去除效率,将50g含铜-锰的丸粒型催化剂样品放入5LTedlar袋中,并向其中注入浓度为50ppm的甲苯,之后使用Gastec检测管测量浓度随时间的变化。甲苯去除效率的测量结果示于下表3中。
30分钟后,在实施例2中除去66%或更大的量的甲苯,在实施例3、4和5中分别除去50%、40%和76%的量的甲苯,但在比较例1中去除效率不高。
[表3]
<单位ppm>
表3示出了气体去除效率结果,表3中30分钟后的气体去除效率结果绘制在图3中。
从图3和表3中可明显看出,与比较例1相比,实施例2至5的具有优异的与孔隙率有关的特性的复合催化剂组合物在气体去除效率方面显著提高。
更具体地,与无机层化合物混杂的铜-锰复合催化剂的量在实施例3中比在实施例2中大,并且因此一氧化碳去除效率较高,但氨、硫化氢、乙醛和甲苯的去除效率非常低。
此外,与无机层化合物混杂的铜-锰复合催化剂的量在实施例4中比在实施例2中小,并且因此氨、硫化氢、乙醛和甲苯以及一氧化碳的去除效率非常低。
此外,活性炭的量在实施例5中比在实施例2中大,并且因此除甲苯以外的化合物(即一氧化碳、氨、硫化氢和乙醛)的去除效率低。
因此,可以发现本发明在去除多种气体方面非常有效。
因此,本发明能够在室温下有效地去除对人体有害的一氧化碳、有气味的气体和挥发性有机化合物。
此外,与常规贵金属催化剂相比,本发明可以实现低生产成本并且可以在室温下表现出优异的气体去除效率,并且因此可以广泛用于工业领域和多种应用领域中。
此外,在本发明中,密度和孔隙率(孔体积)落入适当的范围内,并且比表面积被最大化,由此使有害气体和有气味的物质的物理吸附最大化。
如上所述的含有铜-锰催化剂的用于有害气体去除的复合组合物不限于上述实施方案的配置和操作方式。上述实施方案可配置成使得所有或一些实施方案可选择性地组合以做出多种修改。
Claims (6)
1.一种含有铜-锰催化剂的用于有害气体去除的复合组合物,包含1重量%至20重量%的与无机层化合物混杂的铜-锰复合催化剂;45重量%至55重量%的无机填料;30重量%至40重量%的活性炭;以及4重量%至8重量%的粘合剂,所述无机层化合物为基于蒙皂石的合成粘土;
与所述无机层化合物混杂的所述铜-锰复合催化剂通过在水溶液相中混合100重量份的所述无机层化合物与120重量份至180重量份的高锰酸钾、300重量份至400重量份的乙酸锰和100重量份至150重量份的乙酸铜来制备。
2.根据权利要求1所述的复合组合物,其中与所述无机层化合物混杂的所述铜-锰复合催化剂的粒径为50nm或更小。
3.根据权利要求1所述的复合组合物,其中所述无机填料为选自多孔二氧化硅、氧化铝、二氧化钛、珍珠岩和高岭土中的至少一者。
4.根据权利要求1所述的复合组合物,其中所述粘合剂为选自无机粘合剂和有机粘合剂中的至少一者,并且以基于所述粘合剂的总量的5重量%或更少的量含有所述有机粘合剂。
5.根据权利要求4所述的复合组合物,其中所述无机粘合剂包含选自胶态二氧化硅、二氧化钛、二氧化锆、水玻璃、氧化铝溶胶和无机层化合物中的至少一者,以及所述有机粘合剂包含选自以下中的至少一者:甲基纤维素、羟乙基纤维素、羟丙基甲基纤维素、羟乙基甲基纤维素、甲基乙基纤维素、羧甲基纤维素、羟丙基纤维素、聚乙烯醇、聚乙二醇、聚丙烯酸、聚甲基丙烯酸甲酯和羟丙基。
6.根据权利要求1所述的复合组合物,其中所述复合组合物的密度为0.3g/cm3至1.0g/cm3,比表面积为300m2/g至800m2/g,以及总孔体积为0.3cm3/g至1.0cm3/g。
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US20180345254A1 (en) | 2018-12-06 |
CN108290142A (zh) | 2018-07-17 |
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EP3381551A1 (en) | 2018-10-03 |
WO2017090836A1 (ko) | 2017-06-01 |
US10556224B2 (en) | 2020-02-11 |
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EP3381551A4 (en) | 2018-11-21 |
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