TW201840361A - 用於voc(揮發性有機物)之低成本氧化催化劑及鹵化voc排放控制 - Google Patents
用於voc(揮發性有機物)之低成本氧化催化劑及鹵化voc排放控制 Download PDFInfo
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- TW201840361A TW201840361A TW107102177A TW107102177A TW201840361A TW 201840361 A TW201840361 A TW 201840361A TW 107102177 A TW107102177 A TW 107102177A TW 107102177 A TW107102177 A TW 107102177A TW 201840361 A TW201840361 A TW 201840361A
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- Prior art keywords
- oxide
- oxidation catalyst
- silicon oxide
- patent application
- ruthenium
- Prior art date
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- 239000003054 catalyst Substances 0.000 title claims abstract description 93
- 238000007254 oxidation reaction Methods 0.000 title claims abstract description 55
- 230000003647 oxidation Effects 0.000 title claims abstract description 49
- KJTLSVCANCCWHF-UHFFFAOYSA-N Ruthenium Chemical compound [Ru] KJTLSVCANCCWHF-UHFFFAOYSA-N 0.000 claims abstract description 31
- 229910052707 ruthenium Inorganic materials 0.000 claims abstract description 31
- 238000000034 method Methods 0.000 claims abstract description 22
- 238000004519 manufacturing process Methods 0.000 claims abstract description 8
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 claims description 47
- 229910052814 silicon oxide Inorganic materials 0.000 claims description 27
- 239000000758 substrate Substances 0.000 claims description 27
- 239000006104 solid solution Substances 0.000 claims description 20
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical group [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 claims description 17
- 239000002002 slurry Substances 0.000 claims description 16
- 239000012855 volatile organic compound Substances 0.000 claims description 16
- 239000000463 material Substances 0.000 claims description 15
- 239000007789 gas Substances 0.000 claims description 14
- 239000000203 mixture Substances 0.000 claims description 14
- 239000000377 silicon dioxide Substances 0.000 claims description 11
- 239000002245 particle Substances 0.000 claims description 10
- MCMNRKCIXSYSNV-UHFFFAOYSA-N ZrO2 Inorganic materials O=[Zr]=O MCMNRKCIXSYSNV-UHFFFAOYSA-N 0.000 claims description 9
- 229910052684 Cerium Inorganic materials 0.000 claims description 8
- 229910000420 cerium oxide Inorganic materials 0.000 claims description 8
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims description 7
- GWXLDORMOJMVQZ-UHFFFAOYSA-N cerium Chemical compound [Ce] GWXLDORMOJMVQZ-UHFFFAOYSA-N 0.000 claims description 7
- 239000001301 oxygen Substances 0.000 claims description 7
- 229910052760 oxygen Inorganic materials 0.000 claims description 7
- XOLBLPGZBRYERU-UHFFFAOYSA-N tin dioxide Chemical compound O=[Sn]=O XOLBLPGZBRYERU-UHFFFAOYSA-N 0.000 claims description 7
- 229910001887 tin oxide Inorganic materials 0.000 claims description 7
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 claims description 6
- 229910052751 metal Inorganic materials 0.000 claims description 6
- 239000002184 metal Substances 0.000 claims description 6
- 229910052697 platinum Inorganic materials 0.000 claims description 6
- 238000000576 coating method Methods 0.000 claims description 5
- 239000011230 binding agent Substances 0.000 claims description 4
- TZIBOXWEBBRIBM-UHFFFAOYSA-N cerium(3+) oxygen(2-) titanium(4+) Chemical compound [O--].[O--].[Ti+4].[Ce+3] TZIBOXWEBBRIBM-UHFFFAOYSA-N 0.000 claims description 4
- OGIDPMRJRNCKJF-UHFFFAOYSA-N titanium oxide Inorganic materials [Ti]=O OGIDPMRJRNCKJF-UHFFFAOYSA-N 0.000 claims description 4
- 229910018072 Al 2 O 3 Inorganic materials 0.000 claims description 3
- 238000002156 mixing Methods 0.000 claims description 3
- 239000002808 molecular sieve Substances 0.000 claims description 3
- URGAHOPLAPQHLN-UHFFFAOYSA-N sodium aluminosilicate Chemical compound [Na+].[Al+3].[O-][Si]([O-])=O.[O-][Si]([O-])=O URGAHOPLAPQHLN-UHFFFAOYSA-N 0.000 claims description 3
- 229910021417 amorphous silicon Inorganic materials 0.000 claims description 2
- 239000011248 coating agent Substances 0.000 claims description 2
- 229910052878 cordierite Inorganic materials 0.000 claims description 2
- 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 claims description 2
- 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 claims description 2
- 229910052746 lanthanum Inorganic materials 0.000 claims description 2
- FZLIPJUXYLNCLC-UHFFFAOYSA-N lanthanum atom Chemical compound [La] FZLIPJUXYLNCLC-UHFFFAOYSA-N 0.000 claims description 2
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- 150000004706 metal oxides Chemical class 0.000 claims description 2
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- 239000002243 precursor Substances 0.000 claims description 2
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- 229910006404 SnO 2 Inorganic materials 0.000 claims 2
- 238000001354 calcination Methods 0.000 claims 2
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- 229910000599 Cr alloy Inorganic materials 0.000 claims 1
- MYMOFIZGZYHOMD-UHFFFAOYSA-N Dioxygen Chemical compound O=O MYMOFIZGZYHOMD-UHFFFAOYSA-N 0.000 claims 1
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- 229910052777 Praseodymium Inorganic materials 0.000 claims 1
- 229910010413 TiO 2 Inorganic materials 0.000 claims 1
- OTUHBRHHGINIPS-UHFFFAOYSA-N cerium(3+);oxygen(2-);tin(4+) Chemical compound [O-2].[Sn+4].[Ce+3] OTUHBRHHGINIPS-UHFFFAOYSA-N 0.000 claims 1
- 239000000788 chromium alloy Substances 0.000 claims 1
- UPHIPHFJVNKLMR-UHFFFAOYSA-N chromium iron Chemical compound [Cr].[Fe] UPHIPHFJVNKLMR-UHFFFAOYSA-N 0.000 claims 1
- 229910001882 dioxygen Inorganic materials 0.000 claims 1
- 239000004744 fabric Substances 0.000 claims 1
- QEFYFXOXNSNQGX-UHFFFAOYSA-N neodymium atom Chemical compound [Nd] QEFYFXOXNSNQGX-UHFFFAOYSA-N 0.000 claims 1
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- 239000000843 powder Substances 0.000 description 5
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 description 4
- 229910002091 carbon monoxide Inorganic materials 0.000 description 4
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- GTCKPGDAPXUISX-UHFFFAOYSA-N ruthenium(3+);trinitrate Chemical compound [Ru+3].[O-][N+]([O-])=O.[O-][N+]([O-])=O.[O-][N+]([O-])=O GTCKPGDAPXUISX-UHFFFAOYSA-N 0.000 description 4
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- KXKVLQRXCPHEJC-UHFFFAOYSA-N acetic acid trimethyl ester Natural products COC(C)=O KXKVLQRXCPHEJC-UHFFFAOYSA-N 0.000 description 3
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- WOCIAKWEIIZHES-UHFFFAOYSA-N ruthenium(iv) oxide Chemical compound O=[Ru]=O WOCIAKWEIIZHES-UHFFFAOYSA-N 0.000 description 2
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- 239000010937 tungsten Substances 0.000 description 2
- SCYULBFZEHDVBN-UHFFFAOYSA-N 1,1-Dichloroethane Chemical compound CC(Cl)Cl SCYULBFZEHDVBN-UHFFFAOYSA-N 0.000 description 1
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- IMQUYRYMPIKEFP-UHFFFAOYSA-N cerium(3+) oxosilicon(2+) oxygen(2-) Chemical compound [O-2].[Ce+3].[Si+2]=O IMQUYRYMPIKEFP-UHFFFAOYSA-N 0.000 description 1
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- 229940117389 dichlorobenzene Drugs 0.000 description 1
- 125000000118 dimethyl group Chemical group [H]C([H])([H])* 0.000 description 1
- FGEKTVAHFDQHBU-UHFFFAOYSA-N dioxoruthenium;hydrate Chemical compound O.O=[Ru]=O FGEKTVAHFDQHBU-UHFFFAOYSA-N 0.000 description 1
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- 238000009826 distribution Methods 0.000 description 1
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- CZMAIROVPAYCMU-UHFFFAOYSA-N lanthanum(3+) Chemical compound [La+3] CZMAIROVPAYCMU-UHFFFAOYSA-N 0.000 description 1
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Classifications
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- 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
- B01J23/54—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals combined with metals, oxides or hydroxides provided for in groups B01J23/02 - B01J23/36
- B01J23/56—Platinum group metals
- B01J23/63—Platinum group metals with rare earths or actinides
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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
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- B—PERFORMING OPERATIONS; TRANSPORTING
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- B01D53/34—Chemical or biological purification of waste gases
- B01D53/74—General processes for purification of waste gases; Apparatus or devices specially adapted therefor
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- B—PERFORMING OPERATIONS; TRANSPORTING
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- B01D53/34—Chemical or biological purification of waste gases
- B01D53/74—General processes for purification of waste gases; Apparatus or devices specially adapted therefor
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- B01D53/8659—Removing halogens or halogen compounds
- B01D53/8662—Organic halogen compounds
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
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- 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
- B01D53/8668—Removing organic compounds not provided for in B01D53/8603 - B01D53/8665
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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
- B01J21/02—Boron or aluminium; Oxides or hydroxides thereof
- B01J21/04—Alumina
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- B—PERFORMING OPERATIONS; TRANSPORTING
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- B01J21/00—Catalysts comprising the elements, oxides, or hydroxides of magnesium, boron, aluminium, carbon, silicon, titanium, zirconium, or hafnium
- B01J21/06—Silicon, titanium, zirconium or hafnium; Oxides or hydroxides thereof
- B01J21/063—Titanium; Oxides or hydroxides thereof
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- B—PERFORMING OPERATIONS; TRANSPORTING
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Abstract
本案之具體實例關於含釕之受載催化劑,該具體實例包括該含釕之受載催化劑之製造和使用之方法,該含釕之受載催化劑透過催化性氧化破壞化學工業排放物所含之有害化合物,要不然就是工業程序製造之有害化合物。
Description
本案之具體實例關於含釕之受載催化劑,該具體實例包括該含釕之受載催化劑之製造和使用之方法,該含釕之受載催化劑透過催化性氧化破壞化學工業排放物所含之有害化合物,要不然就是工業程序製造之有害化合物。
許多有害化合物係於化學、消耗燃料及工業製程之廢氣及/或排氣管排放物中發現到。這些可能源於工業排氣、及來自化學工廠(包括精製對苯二甲酸(PTA)工廠)之廢氣排放物。種種不同排放物中見到之有害化合物可能呈化學副產物及溶劑之形態。同樣地,該有害化合物-包括鹵化VOC及其他毒性高之污染物-給人們及環境帶來許多有害之影響,包括呼吸器官問題、種種癌症、煙霧、及臭氧耗竭。再者,利用焚燒消除某些這些化合物(如某些鹵化化合物)可能隨操作條件而產生其他有毒物質。因為涉及公共健康及環境檢討之種種不同理由,於是地方性、區域性或全球性規範皆要求消除這些有害化合物。
所以,可應用本發明具體實例之催化劑及方法消除的某些排放物所含之有害化合物一般包括揮發性有機化合物(“VOC”)、鹵化揮發性有機化合物(“HVOC”)、及一氧化碳(“CO”)。於許多情形中,儘管不是所有情形,此化合物含有碳及氫,且也可含有其他元素如氧、氮及鹵素。
截至目前,已經有人使用種種方法消除這些有害化合物,例如,吸附於碳或其他吸附劑上、催化性氧化、及熱氧化(焚燒)。然而,吸附僅將危害性污染物集中,而不會破壞它們,且該方法之功效取決於該污染物之濃度波動。此外,熱氧化之特色為高操作溫度及實質操作成本,因為這些反應需要高溫-經常超過750℃。相較之下,催化性氧化使這些有害化合物在氧存在下氧化所需之活化能降低,所以其能於熱氧化所需能量之一部分完成。
為求簡潔,能藉著本文所揭露之本發明催化劑及方法破壞的化合物稱作“有害化合物”。舉幾個例子,這些包括,但是不一定限於一氧化碳;VOC(如苯、甲苯、二甲苯、甲醇、及乙酸甲酯);及HVOC(如氯甲烷、二氯甲烷、二氯乙烷、溴甲烷、二溴甲烷、二溴乙烷、及氯苯、二氯苯、及聚溴苯)。該本發明催化劑係用以使發生這些反應所需之活化能降低,且與其他用於氧化之催化劑相比一般係以低成本方式提供。
一般,已經被利用於與該有害化合物之破壞有關的氧化反應之催化劑包括氧化鋁(Al2
O3
)承載物上鉑、鈀及銠。此催化劑已有多種不同形態被採用,如錠、丸、球、及細粒,以及單片承載物(monolithic supports)。
因為催化性氧化反應係於比熱氧化低之溫度下進行,所以使操作成本降低,且為操作提供其他顯著益處,包括經濟上的節約。但是雖然咸認為催化性氧化是可行之方法,使用昂貴之貴金屬催化劑如鉑及鈀卻限制經濟上的節約,且期望具有類似功效之低成本催化劑。再者,以前為了這些目的使用之催化劑有時候花費更多,所以需要提供更長耐用壽命及較低成本之催化劑。
以前已經有人使用包括貴金屬在內之種種氧化催化劑來破壞各種不同其他種類之有害排放物所含的化學工廠處之有害化合物。然而,據證實大量貴金屬催化劑之高成本有限制。此外,期望成本較低但是同樣能破壞化學工廠排放物之有害化合物(例如於PTA製造工廠)的可供選擇之催化劑。
本文揭露之含釕催化劑提供了與貴金屬催化劑相比之成本優點。於一些具體實例中,該釕催化劑受載於安定化高表面積固體溶液或混合氧化物。不受限制,這些之清單包括氧化鈰-氧化鋯、氧化鈦-氧化鈰、氧化錫-氧化鈰、氧化鋁-氧化鈰、氧化鋯-氧化矽、氧化鈦-氧化矽、氧化錫-氧化矽、及本文所述的其他者。於一些具體實例中,本發明催化劑不含貴金屬催化劑如鉑或鈀。因此,提供與單片承載物結合之有成本效益的氧化催化劑於破壞含有感興趣之有害化合物的排放物。這些有害化合物之破壞(即,消除)因此係於比先前系統較低之溫度下完成。
多個具體實例及替代例包括受載於具有多個經塗佈高表面積混合金屬氧化物或固體溶液之通道或氣室的單片結構上之釕催化劑。該單片承載物可以獨立承載物結構(stand-alone support structures)之形態或以一系列含通道之蜂巢之形態提供,且其可被置於氣流中使該通道大體上與氣體流動方向平行對齊。依此方式,排放物中之有害化合物係藉由觸及這些通道內之催化劑而予以破壞。本發明具體實例之催化性結構顯現使該催化劑暴露於該排放物之高表面積。於一些具體實例中,該受載之催化劑的表面積係至少60 m²/g,較佳地高於100 m²/g。該催化劑材料係塗佈於該單片基材之通道內,且該催化劑本身證實相對於開始該受催化之氧化反應所需的能量之良好熱安定性。
再者,如用於消除包括HVOC在內之某些有害化合物的點火溫度(light-off temperatures)證明的,本發明具體實例之有成本效益的氧化催化劑比用於消除本文所述之有害化合物的更昂貴鉑族催化劑有利。因此,在含有這些有害化合物之某些廢氣以排放物形態排至大氣之前,本發明具體實例使其能使用本文所述之催化劑及方法予以破壞。有益的是,本發明具體實例之催化劑提供改良之效率與低成本應用的平衡。
多個具體實例及替代例包括具有單片承載物之內壁或通道上塗佈釕催化劑者。於一些具體實例中,使用高表面積耐火混合氧化物或固體溶液承載該釕催化劑。除了提供指定形態以外,本文所指之“金屬氧化物”意欲包括此金屬之所有氧化物形態。
於一些具體實例中,該催化劑受載於高表面積固體溶液或耐火混合金屬氧化物上。這些之非限定清單包括氧化鈰-氧化鋯、氧化鈦-氧化鈰、氧化錫-氧化鈰、氧化鋁-氧化鈰、氧化矽-氧化鈰、氧化鋯-氧化矽、氧化鈦-氧化矽、氧化錫-氧化矽,且包括三種組分組合,如氧化鈦-氧化鈰-氧化矽、氧化鋯-氧化鈰-氧化矽;及氧化錫-氧化鈰-氧化矽、氧化鈦-氧化鋯-氧化矽、氧化鋁-氧化鈰-氧化矽。
於一些具體實例中,該高表面積混合氧化物化合物係藉由將該化合物加於包括以下組合之下列一或多者而更進一步安定化:氧化鋁、氧化矽、氧化錫、鎢、氧化鈰、及其他稀土氧化物如鑭(III)或鐠(III)。因此,多個具體實例另包括用於形成這些氧化催化劑之方法,其中該方法之特徵為藉著高表面積固體溶液或混合氧化物將該催化劑安定化。
本發明具體實例也包含一種用於改良含有排放物之流動氣流之方法,其中將帶釕催化劑之單片承載物佈置於該流中使該蜂巢之開口大體上與流動方向平行對齊。適合單片承載物之非限定實例係具有100至400 cpsi(個氣室/平方吋)之氣室密度者。流動氣流之溫度係保持於約200℃上達約500℃,造成排放物中可能發現之有害化合物的消除。
於一些具體實例中,藉由洗塗方法(wash-coating processes)在流過基材(例如,蜂巢、發泡物或其他單片基材)時將該催化劑材料併入。當於形成步驟期間選擇性達成時,該釕裝載在該單片結構上變化於約0.1至5 g/L之範圍,更佳地1至3 g/L。於一些具體實例中,該承載物洗塗材料(support wash-coat materials)介於約30至300 g/L,更佳地80至250 g/L。
咸明白該單片基材本身包含惰性材料,如陶瓷堇青石或鋁莫來石,以及合金材料如鐵鉻鋁合金。儘管一些具體實例中使用單片基材,但是用於催化劑承載物之基材也可使用本文所述之相同類型的塗佈方法而採丸、錠、及球之形態。
於一些具體實例中,應用洗塗方法將催化劑材料沉積於單片承載物上。催化劑組分先與水和黏結劑材料混合且輾壓充分時期以獲得具有適當粒徑之漿料。接著將該單片基材浸入此漿料。必要的話,藉由真空抽引或氣刀等移除過多之漿料材料。其後,將經塗佈之基材料乾燥且於足以將該洗塗材料固定於該基材上之溫度煅燒。
如提及的,該固體溶液或混合氧化物可在結合該釕催化劑之前被洗塗於該單片基材上。關此,該固體溶液或混合氧化物先與水和黏結劑材料混合且輾壓充分時期以獲得具有適當粒徑之漿料。將該單片基材浸入此漿料。必要的話,藉由真空抽引或氣刀等移除過多之漿料材料。其後,將經塗佈之基材料乾燥且煅燒。此刻,透過此技藝已知之技術(例如濕含浸(wetness impregnation)或噴塗)將具有足以達成釕裝載之釕含量的釕溶液沉積於經洗塗之單片基材上。於一些具體實例中,將該釕溶液以釕錯合物(前驅物)形態,於足以達成該承載物上預期釕裝載之濃度下沉積。供適當挑選釕化合物溶液用之來源可獲自,但不限於,烷氧化釕、烷基釕(ruthenium alkyl)、乙脒釕(ruthenium amidinate)、二酮酸釕、及三硝酸根亞硝基釕(trinitratonitrosylruthenium)(II)、乙酸釕、水合氯化釕(III)、五羰基釕、氧化釕(IV)、水合氧化釕(IV)、九羰基二釕、及十二羰基三釕。
於實際應用中,將已經根據本文教旨製備之經催化劑材料洗塗的單片基材置於含排放物之廢氣流裝置,其中該催化性氧化破壞感興趣之有害化合物。含有這些有害化合物之廢氣將會觸及已經沉積於單片基材上之催化劑材料。當這個隨著充分量之氧在標準操作條件之下且於200℃至約500℃之溫度下發生時,該有害化合物係氧化且轉化成二氧化碳及水,伴隨著氫鹵酸/鹵素。“點火溫度”表示對有害化合物或一組有害化合物發生催化性氧化反應之溫度。用於將該有害化合物氧化之本發明催化劑的有利活性之特色為於比熱氧化有利(即,較低)之點火溫度破壞這些化合物。在一些情形中,如實施例中見到的,用於破壞顯著百分比之有害化合物的點火溫度係約250℃或更低。
根據本文所示之多個具體實例及替代例,受載之釕催化劑可另包含氧化鈰-氧化鋯之高表面積固體溶液。此本發明組合包括氧化鈰內5重量%至50重量%氧化鋯之立方晶系氟化物結構作為安定化功能(stabilizing functionality)。必要的話,於一些具體實例中,該固體溶液係藉由重量百分比少於5%之稀土元素如鑭或鐠的添加而進一步安定化。
於一些具體實例中,藉由將5重量%至20重量%氧化鈰加於氧化鈦而藉著氧化鈦-氧化鈰之固體溶液或混合氧化物實現類似安定化特徵。此組合提供金紅石結構或銳鈦礦結構,且係視需要藉由氧化矽或鎢之添加而進一步安定化。於一些具體實例中,藉由將約5重量%至20重量%氧化鈰加於氧化錫而藉著氧化錫-氧化鈰之固體溶液或混合氧化物實現類似安定化特徵。此組合提供金紅石結構,且如所欲藉由氧化矽之添加而進一步安定化。於一些具體實例中,藉由將約5重量%至20重量%氧化鈰加於氧化鋁而藉著氧化鋁-氧化鈰之固體溶液或混合氧化物實現類似安定化特徵。此組合可提供g氧化鋁結構或非晶形結構,且如所欲藉由氧化矽之添加而進一步安定化。
於一些具體實例中,該氧化催化劑之附加組分可為氧化矽。氧化矽可依據該排放流之組成用作替代物。因此,於一些情況中,較佳為氧化矽。也可以,依據該排放流,該氧化催化劑可含有氧化矽或與氧化矽結合。
該氧化矽可為具有表面積大於150 m2
/g、大於100埃之較大孔徑、及粒徑平均0.5至15微米之非晶形相的沉澱氧化矽粉末。其他類型之非晶形氧化矽(如介孔分子篩MCM-41及SBA-15)也可使用。這些分子篩MCM-41及SBA-15也具有大表面積(大於200m2
/g)、較大孔隙體積及大於100埃之均勻孔徑分佈,藉以與習用非晶形氧化矽相比,能獲得活性組分之較高分散度及粒徑之較佳控制。可具有較大表面積之發煙氧化矽由於其低孔隙率而較不適宜作為催化劑承載物。氧化矽具有顯著較低之表面酸度(surface acidity)而導致非常弱之吸附鹵化化合物的能力,其可能造成受毒化之催化劑(poisoned catalysts)。
就利用低成本催化劑之方法的角度來看,於一些具體實例中本發明催化劑係於介於約1,000與100,000 h-1
之間,更佳地介於約5000與50,000 h-1
之間的氣體每小時空間速度(GHSV)下操作。咸明白就特定操作而言,空間速度可藉由增加或減小發生催化性氧化之反應器內的催化劑體積而最佳化。
再者,本發明催化劑或催化劑系統可於寬廣溫度範圍內操作。典型地,操作溫度係見於約200℃至約500℃之範圍,且於一些具體實例中這些操作溫度能介於230℃至400℃,或更特別的是介於240℃至350℃。倘若有足量之氧存於發生氧化反應之處,本發明催化劑便可用以達成來自化學工廠廢氣排放物之化合物的完全或近乎完全催化性氧化。於一些具體實例中,操作溫度可能藉由將足量之輔助燃料(其係更易於揮發之有機化合物)注入廢氣排氣流而進一步受影響。適當輔助燃料之非限定實例包括甲醇、乙醇、乙酸甲酯、合成氣、及其混合物,其皆易於化學工廠獲得。
除於適合GHSV下且於適合溫度範圍內操作之外,本發明催化劑一般於低壓或高壓反應器系統之環境內操作。於一些具體實例中,工作壓力可介於大氣壓力至約300 psi(2.0 MPa)。在高壓操作時,更特別的是介於約100至200 psi之間(0.6至1.4MPa),該催化性氧化反應器可位於廢氣膨脹器(off-gas expander)之上游。也可以,在低壓操作時,廢氣膨脹器之位置下游可能適用於放置催化性氧化反應器。接下來的是關於本發明催化劑及其製造和使用之方法兩者之非限定實施例,其係供進一步例示根據本文之教旨的種種具體實例。
實施例
咸了解這些實施例僅為例示性且不得視為限制本文所述且請求之標的的範疇。實施例1至3關於獲得種種帶催化劑之單片基材,且從破壞有害化合物之角度測試其效能。實施例4使用實施例1之催化劑,但是測試係靠不同混合廢氣樣品進行。圖2A至2D分別提供該混合樣品之圖形。 實施例1
洗塗漿料係藉由於5:1之比率下的氧化鈰-氧化鋯粉末(參見圖1)和氧化矽之固體溶液,偕同足量之去離子水製備。該氧化鈰-氧化鋯粉末具有約85 m²/g之表面積。混合時,將該漿料輾壓成預期之粒徑。將具有400 cpsi之氣室密度的陶瓷單片基材零件浸於該洗塗漿料。過多之漿料係利用氣刀移除。經塗佈之零件係於約150℃下乾燥且於約500℃下煅燒,造成具有約170 g/ L之洗塗裝載的零件。在此經塗佈之零件上,硝酸釕溶液係藉由濕含浸沉積,於150℃下乾燥且於500℃下煅燒,以達成藉由已知技術測量之約2.8 g/L的釕裝載。 實施例2
洗塗漿料係使用具有約85 m²/g之表面積的經氧化矽安定化之氧化鈦粉末、氧化矽膠體及足量之去離子水,之後將該混合物輾壓成預期之粒徑而製備。接著將400 cpsi單片基材零件浸於該洗塗漿料。過多之漿料係利用氣刀移除。經塗佈之零件係於150℃下乾燥且於500℃下煅燒。所得之零件具有約180 g/ L之洗塗裝載。在此經塗佈之零件上,硝酸釕溶液係藉由濕含浸沉積,於150℃下乾燥且於500℃下煅燒,以達成約2.6 g/L之釕裝載。 實施例3
洗塗漿料係使用具有約110 m²/g之表面積的經氧化矽安定化之氧化錫粉末、氧化矽膠體及足量之水,之後將該混合物輾壓成預期之粒徑而製備。接著將400 cpsi單片基材零件浸於該洗塗漿料。過多之漿料係利用真空抽引或氣刀移除。經塗佈之零件係於150℃下乾燥且於500℃下煅燒。這造成具有約180 g/ L之洗塗裝載的零件。在此經塗佈之零件上,硝酸釕溶液係藉由濕含浸或其他適合技術沉積,於150℃下乾燥且於500℃下煅燒,以達成約2.6 g/L之釕裝載。
為以上實施例例示之催化劑評估催化活性。以實驗室級反應器測試以自各個以上實施例之催化劑單片零件切口之催化劑芯部樣品為基礎的反應性。經測試之有害化合物(即,排放物)係50 ppm苯、100 ppm甲基溴、3 vol.%水(即,體積%)、3 vol.%氧、且其餘部分為氮。測試於空間速度25,000 h-1
下進行。 實施例4
獲得實施例1之催化劑之後,將5000 ppm一氧化碳、50 ppm甲基溴、500 ppm乙酸甲酯、10 ppm苯、10 ppm甲苯、10 ppm二甲基、1體積%水及3體積%氧和剩餘部分之氮的混合氣體混合物測試當作模擬PTA工廠廢氣,以測定於20,000 h-1
之空間速度下的催化劑破壞效率。利用熱火焰游離偵檢(heated flame ionization detection)(“HFID”)總烴分析儀、及非色散紅外線(non-dispersive infrared)(“NDIR”)-一氧化碳分析儀監測氧化反應。如圖2D所示之圖形顯示,完全或近乎完全之VOC破壞於約250℃發生。於圖2A至2C中,結果就使溫度要求降低而論類似,於約250℃或更低見到實質之VOC破壞或於300℃或更低見到完全或近乎完全之破壞。
咸了解本文所述之具體實例不限於不限於所述之教指及敘述的細節、或如後附圖形例示之應用。而是,咸了解本文描述且請求之具體實例及替代例能以種種方式實行或進行。而且,咸了解本文使用之單字及片語係為了敘述之目的且理應不得視為限制。如“包括”、“如”、“包含”、“例如”、“含有”、或“具有”之單字或片語及那些單字之變化在本文中的運用意指包含其後列舉之項目、及那些之等效物,以及附加項目。
因此,前述具體實例及替代例之描述意指例示,而非用作本文已經揭露者之範疇的限制。本文之敘述並非意指將具體實例之理解限制於所揭露之精確形態。普通熟悉此技藝者咸了解這些具體實例之修飾及變化根據以上教旨及敘述係合理可行的。
圖1係根據多個具體實例及替代例之氧化鈰-氧化鋯固體溶液的X射線繞射示值讀數。
圖2A至2D分別顯示與實施例1至4討論之受載之釕催化劑相關的催化性氧化試驗結果。
Claims (15)
- 一種用於破壞來自排放流之CO和揮發性有機化合物,特別是鹵化有機化合物,之氧化催化劑,其中該氧化催化劑包含: 至少一種來自鉑族金屬之金屬,其中一者包含釕或鉑, 包含氧化鈰-氧化鋯之固體溶液或混合氧化物的耐火氧化物承載物;及 氧化矽和氧化錫中之一或二者。
- 如申請專利範圍第1項之催化劑,其另包含耐火氧化物承載物,該承載物包含氧化鈦-氧化鈰及氧化矽和氧化錫中之一或二者的固體溶液或混合氧化物;或氧化錫-氧化鈰的固體溶液或混合氧化物;及氧化矽;或氧化鋁-氧化鈰及氧化矽和氧化錫之一或二者的固體溶液或混合氧化物。
- 如申請專利範圍第1項之氧化催化劑,其係沉積於具有蜂巢或單片結構之基材上,其中該基材係由堇青石(cordierite)、莫來石(mullite)、鐵鉻合金及不銹鋼所組成之群組製造。
- 如申請專利範圍第1項之氧化催化劑,其中該鉑族金屬包含釕或鉑。
- 如申請專利範圍第1項之氧化催化劑,其中該鉑族金屬基本上由釕或鉑組成。
- 如申請專利範圍第1項之氧化催化劑,其中該耐火氧化物承載物係藉著氧化矽或一或多種選自由鑭、鈰、釔、鐠、釹、及其混合物所組成之群組的稀土金屬氧化物安定化。
- 如申請專利範圍第1項之氧化催化劑,其中該氧化催化劑包含具有約2m2 /g至200m2 /g之表面積及約1至20微米之粒徑的安定化氧化錫,或其中該氧化催化劑包含具有約2m2 /g至200m2 /g之表面積及約0.2至20微米之粒徑的安定化氧化鈦。
- 如申請專利範圍第3項之氧化催化劑,其中該釕金屬係於包含約0.3g/L至5 g/L之裝載下沉積於該基材上。
- 如申請專利範圍第1項之氧化催化劑,其中該氧化催化劑包含氧化矽,該氧化矽佔該氧化催化劑之約5重量%至約50重量%。
- 如申請專利範圍第1項之氧化催化劑,其中該氧化催化劑包含選自由非晶形氧化矽(amorphous silica)、沉澱氧化矽、分子篩、MCM-41、SBA-15及其組合所組成之群組的氧化矽。
- 如申請專利範圍第1項之氧化催化劑,其中該氧化催化劑包含氧化矽,該氧化矽包含具有高於100 m2 /g之表面積及約0.5至20微米之粒徑的非晶形氧化矽。
- 如申請專利範圍第1項之催化劑,其中該耐火金屬氧化物佔該氧化催化劑之約10重量%至約95重量%。
- 一種沉積於基材上之氧化催化劑之製造方法,該氧化催化劑係用於破壞來自排放流之CO及揮發性有機化合物,特別是鹵化有機化合物,該方法包含: 製備包含CeO2 -ZrO2 、TiO2 -CeO2 、SnO2 -CeO2 、Al2 O3 -CeO2 及氧化矽之固體溶液或混合氧化物之水性混合物漿料以形成混合物; 將該混合物與黏合劑摻和; 用經摻和之混合物洗塗漿料(blended mixture wash-coat slurry)塗佈基材; 將經塗佈之基材乾燥且煅燒; 將至少一種包含至少釕之鉑族金屬前驅物材料沉積於煅燒過之經塗佈之基材上;且 將經釕金屬塗佈之基材乾燥且煅燒。
- 一種氧化催化劑之製造方法,該氧化催化劑係用於破壞來自排放流之CO及揮發性有機化合物,特別是鹵化有機化合物,該方法包含將至少一種貴金屬前驅物沉積於至少一種選自由CeO2 -ZrO2 、TiO2 -CeO2 、SnO2 -CeO2 、Al2 O3 -CeO2 及氧化矽之固體溶液或混合氧化物所組成之群組的組分上以與摻合混合物之黏合劑形成混合物;用經摻和之混合物塗佈基材;且將經塗佈之基材乾燥且煅燒。
- 一種含有CO及VOC之氣流之處理方法,該VOC包括鹵化VOC、及其混合物,該方法包含將含有CO及包括鹵化VOC在內之VOC之氣流與氧合併;且使經合併之氧-氣流與如申請專利範圍第1項之催化劑於約200℃至500℃之溫度下接觸。
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CN109174094A (zh) * | 2018-09-18 | 2019-01-11 | 贵州大学 | 一种金红石相固溶体材料的制备方法及应用 |
CN110404534B (zh) * | 2019-07-03 | 2021-03-30 | 浙江大学 | 一种高效抗氯中毒的挥发性有机物催化氧化催化剂及其制备方法 |
CN110479317B (zh) * | 2019-08-29 | 2020-08-11 | 昆明理工大学 | 一种VOCs催化燃烧催化剂及其制备方法和应用 |
CN110917872B (zh) * | 2019-11-05 | 2021-08-10 | 河北科技大学 | 一种液态合金吸收及催化氧化卤代烃的方法 |
CN113209984B (zh) * | 2020-01-21 | 2023-05-23 | 中国石油化工股份有限公司 | 用于微波强化催化氧化处理VOCs的催化剂及其制备方法和应用 |
CN113209996B (zh) * | 2020-01-21 | 2023-05-16 | 中国石油化工股份有限公司 | 用于微波强化催化氧化处理VOCs的催化剂及其制备方法和应用 |
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CN113101925B (zh) * | 2021-04-16 | 2022-05-06 | 河北工业大学 | 一种木质素基吸附-催化材料的制备方法及应用 |
CN114669296A (zh) * | 2022-04-28 | 2022-06-28 | 杭州森发环保科技有限公司 | 一种块状Ru-Pt有机废气净化催化剂及其制备方法 |
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