JP6653715B2 - 合成ガスから高品質の灯油留分を選択的に合成するための担体、その触媒、およびその調製方法 - Google Patents
合成ガスから高品質の灯油留分を選択的に合成するための担体、その触媒、およびその調製方法 Download PDFInfo
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- 239000003054 catalyst Substances 0.000 title claims description 55
- 238000003786 synthesis reaction Methods 0.000 title claims description 48
- 230000015572 biosynthetic process Effects 0.000 title claims description 44
- 239000003350 kerosene Substances 0.000 title claims description 28
- 230000002194 synthesizing effect Effects 0.000 title claims description 21
- 238000000034 method Methods 0.000 title claims description 19
- 238000002360 preparation method Methods 0.000 title description 12
- VLKZOEOYAKHREP-UHFFFAOYSA-N n-Hexane Chemical compound CCCCCC VLKZOEOYAKHREP-UHFFFAOYSA-N 0.000 claims description 96
- 239000012065 filter cake Substances 0.000 claims description 32
- 239000002808 molecular sieve Substances 0.000 claims description 25
- 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 25
- MCMNRKCIXSYSNV-UHFFFAOYSA-N Zirconium dioxide Chemical compound O=[Zr]=O MCMNRKCIXSYSNV-UHFFFAOYSA-N 0.000 claims description 24
- 239000000203 mixture Substances 0.000 claims description 22
- 239000011148 porous material Substances 0.000 claims description 18
- JPUHCPXFQIXLMW-UHFFFAOYSA-N aluminium triethoxide Chemical compound CCO[Al](OCC)OCC JPUHCPXFQIXLMW-UHFFFAOYSA-N 0.000 claims description 16
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 claims description 14
- 150000001868 cobalt Chemical class 0.000 claims description 14
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 claims description 12
- 229910052782 aluminium Inorganic materials 0.000 claims description 12
- 229910052710 silicon Inorganic materials 0.000 claims description 12
- 239000010703 silicon Substances 0.000 claims description 12
- 238000003756 stirring Methods 0.000 claims description 11
- 239000000843 powder Substances 0.000 claims description 10
- 239000002994 raw material Substances 0.000 claims description 10
- 239000000243 solution Substances 0.000 claims description 10
- 241000219782 Sesbania Species 0.000 claims description 9
- GRYLNZFGIOXLOG-UHFFFAOYSA-N Nitric acid Chemical compound O[N+]([O-])=O GRYLNZFGIOXLOG-UHFFFAOYSA-N 0.000 claims description 5
- 229910017052 cobalt Inorganic materials 0.000 claims description 5
- 239000010941 cobalt Substances 0.000 claims description 5
- 229910017604 nitric acid Inorganic materials 0.000 claims description 5
- 241000736305 Marsilea quadrifolia Species 0.000 claims description 4
- 241000219793 Trifolium Species 0.000 claims description 4
- 239000002253 acid Substances 0.000 claims description 4
- 238000001816 cooling Methods 0.000 claims description 4
- 239000011259 mixed solution Substances 0.000 claims description 4
- 239000012488 sample solution Substances 0.000 claims description 4
- 239000007864 aqueous solution Substances 0.000 claims description 3
- 238000001035 drying Methods 0.000 claims description 3
- 238000001914 filtration Methods 0.000 claims description 3
- 238000005470 impregnation Methods 0.000 claims description 3
- 238000012546 transfer Methods 0.000 claims description 3
- 238000005303 weighing Methods 0.000 claims description 3
- 239000007848 Bronsted acid Substances 0.000 claims description 2
- 239000002841 Lewis acid Substances 0.000 claims description 2
- 229910019142 PO4 Inorganic materials 0.000 claims description 2
- 238000001354 calcination Methods 0.000 claims description 2
- 229940011182 cobalt acetate Drugs 0.000 claims description 2
- UFMZWBIQTDUYBN-UHFFFAOYSA-N cobalt dinitrate Chemical group [Co+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O UFMZWBIQTDUYBN-UHFFFAOYSA-N 0.000 claims description 2
- 229910001981 cobalt nitrate Inorganic materials 0.000 claims description 2
- QAHREYKOYSIQPH-UHFFFAOYSA-L cobalt(II) acetate Chemical compound [Co+2].CC([O-])=O.CC([O-])=O QAHREYKOYSIQPH-UHFFFAOYSA-L 0.000 claims description 2
- 238000004898 kneading Methods 0.000 claims description 2
- 150000007517 lewis acids Chemical class 0.000 claims description 2
- 238000002156 mixing Methods 0.000 claims description 2
- 238000012986 modification Methods 0.000 claims description 2
- 230000004048 modification Effects 0.000 claims description 2
- 239000002245 particle Substances 0.000 claims description 2
- NBIIXXVUZAFLBC-UHFFFAOYSA-K phosphate Chemical compound [O-]P([O-])([O-])=O NBIIXXVUZAFLBC-UHFFFAOYSA-K 0.000 claims description 2
- 239000010452 phosphate Substances 0.000 claims description 2
- 238000005406 washing Methods 0.000 claims description 2
- 239000000047 product Substances 0.000 description 19
- 239000007789 gas Substances 0.000 description 16
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 10
- 238000006317 isomerization reaction Methods 0.000 description 9
- 238000006243 chemical reaction Methods 0.000 description 8
- 150000002430 hydrocarbons Chemical class 0.000 description 8
- 150000001335 aliphatic alkanes Chemical class 0.000 description 7
- 239000003502 gasoline Substances 0.000 description 7
- 229930195733 hydrocarbon Natural products 0.000 description 6
- 239000000523 sample Substances 0.000 description 6
- 239000011734 sodium Substances 0.000 description 6
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 5
- 239000003921 oil Substances 0.000 description 5
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 4
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 4
- 239000004480 active ingredient Substances 0.000 description 4
- GUTLYIVDDKVIGB-UHFFFAOYSA-N cobalt atom Chemical compound [Co] GUTLYIVDDKVIGB-UHFFFAOYSA-N 0.000 description 4
- 230000000694 effects Effects 0.000 description 4
- 239000001257 hydrogen Substances 0.000 description 4
- 229910052739 hydrogen Inorganic materials 0.000 description 4
- 230000009467 reduction Effects 0.000 description 4
- HEMHJVSKTPXQMS-UHFFFAOYSA-M Sodium hydroxide Chemical compound [OH-].[Na+] HEMHJVSKTPXQMS-UHFFFAOYSA-M 0.000 description 3
- 239000000969 carrier Substances 0.000 description 3
- 238000009826 distribution Methods 0.000 description 3
- 230000003993 interaction Effects 0.000 description 3
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 description 2
- 230000002378 acidificating effect Effects 0.000 description 2
- 238000009472 formulation Methods 0.000 description 2
- 238000007710 freezing Methods 0.000 description 2
- 230000008014 freezing Effects 0.000 description 2
- 239000000446 fuel Substances 0.000 description 2
- 239000000295 fuel oil Substances 0.000 description 2
- 238000005984 hydrogenation reaction Methods 0.000 description 2
- 238000011065 in-situ storage Methods 0.000 description 2
- 238000009776 industrial production Methods 0.000 description 2
- 238000004519 manufacturing process Methods 0.000 description 2
- 229910052757 nitrogen Inorganic materials 0.000 description 2
- 230000008569 process Effects 0.000 description 2
- 241001175904 Labeo bata Species 0.000 description 1
- KJTLSVCANCCWHF-UHFFFAOYSA-N Ruthenium Chemical compound [Ru] KJTLSVCANCCWHF-UHFFFAOYSA-N 0.000 description 1
- 229910004298 SiO 2 Inorganic materials 0.000 description 1
- NINIDFKCEFEMDL-UHFFFAOYSA-N Sulfur Chemical compound [S] NINIDFKCEFEMDL-UHFFFAOYSA-N 0.000 description 1
- 229910021536 Zeolite Inorganic materials 0.000 description 1
- 230000032683 aging Effects 0.000 description 1
- 150000001336 alkenes Chemical class 0.000 description 1
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 1
- 239000011230 binding agent Substances 0.000 description 1
- 229910021393 carbon nanotube Inorganic materials 0.000 description 1
- 239000002041 carbon nanotube Substances 0.000 description 1
- 239000003575 carbonaceous material Substances 0.000 description 1
- 230000003197 catalytic effect Effects 0.000 description 1
- 238000004517 catalytic hydrocracking Methods 0.000 description 1
- 238000003776 cleavage reaction Methods 0.000 description 1
- UMYVESYOFCWRIW-UHFFFAOYSA-N cobalt;methanone Chemical compound O=C=[Co] UMYVESYOFCWRIW-UHFFFAOYSA-N 0.000 description 1
- 239000002131 composite material Substances 0.000 description 1
- 150000001875 compounds Chemical class 0.000 description 1
- 238000011161 development Methods 0.000 description 1
- 230000018109 developmental process Effects 0.000 description 1
- 238000009792 diffusion process Methods 0.000 description 1
- HNPSIPDUKPIQMN-UHFFFAOYSA-N dioxosilane;oxo(oxoalumanyloxy)alumane Chemical compound O=[Si]=O.O=[Al]O[Al]=O HNPSIPDUKPIQMN-UHFFFAOYSA-N 0.000 description 1
- 238000011156 evaluation Methods 0.000 description 1
- 238000010438 heat treatment Methods 0.000 description 1
- 239000007788 liquid Substances 0.000 description 1
- 239000012263 liquid product Substances 0.000 description 1
- 238000011068 loading method Methods 0.000 description 1
- 239000002048 multi walled nanotube Substances 0.000 description 1
- 229910052759 nickel Inorganic materials 0.000 description 1
- TVMXDCGIABBOFY-UHFFFAOYSA-N octane Chemical compound CCCCCCCC TVMXDCGIABBOFY-UHFFFAOYSA-N 0.000 description 1
- 238000005457 optimization Methods 0.000 description 1
- 229910052760 oxygen Inorganic materials 0.000 description 1
- 239000001301 oxygen Substances 0.000 description 1
- 238000006116 polymerization reaction Methods 0.000 description 1
- 238000012545 processing Methods 0.000 description 1
- 230000009257 reactivity Effects 0.000 description 1
- 238000011160 research Methods 0.000 description 1
- 229910052707 ruthenium Inorganic materials 0.000 description 1
- 230000007017 scission Effects 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
- 239000011593 sulfur Substances 0.000 description 1
- 229910052717 sulfur Inorganic materials 0.000 description 1
- 238000001308 synthesis method Methods 0.000 description 1
- 238000012360 testing method Methods 0.000 description 1
- 239000010457 zeolite Substances 0.000 description 1
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
- B01J29/00—Catalysts comprising molecular sieves
- B01J29/82—Phosphates
- B01J29/84—Aluminophosphates containing other elements, e.g. metals, boron
- B01J29/85—Silicoaluminophosphates (SAPO compounds)
-
- 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
-
- 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
-
- 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
- B01J21/06—Silicon, titanium, zirconium or hafnium; Oxides or hydroxides thereof
- B01J21/066—Zirconium or hafnium; Oxides or hydroxides thereof
-
- 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
- B01J23/16—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of arsenic, antimony, bismuth, vanadium, niobium, tantalum, polonium, chromium, molybdenum, tungsten, manganese, technetium or rhenium
- B01J23/24—Chromium, molybdenum or tungsten
- B01J23/28—Molybdenum
-
- 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
- B01J27/00—Catalysts comprising the elements or compounds of halogens, sulfur, selenium, tellurium, phosphorus or nitrogen; Catalysts comprising carbon compounds
- B01J27/14—Phosphorus; Compounds thereof
- B01J27/185—Phosphorus; Compounds thereof with iron group metals or platinum group metals
- B01J27/1853—Phosphorus; Compounds thereof with iron group metals or platinum group metals with iron, cobalt or nickel
-
- 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
- B01J29/041—Mesoporous materials having base exchange properties, e.g. Si/Al-MCM-41
-
- B01J35/50—
-
- B01J35/60—
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B39/00—Compounds having molecular sieve and base-exchange properties, e.g. crystalline zeolites; Their preparation; After-treatment, e.g. ion-exchange or dealumination
- C01B39/02—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof; Direct preparation thereof; Preparation thereof starting from a reaction mixture containing a crystalline zeolite of another type, or from preformed reactants; After-treatment thereof
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B39/00—Compounds having molecular sieve and base-exchange properties, e.g. crystalline zeolites; Their preparation; After-treatment, e.g. ion-exchange or dealumination
- C01B39/54—Phosphates, e.g. APO or SAPO compounds
-
- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10G—CRACKING HYDROCARBON OILS; PRODUCTION OF LIQUID HYDROCARBON MIXTURES, e.g. BY DESTRUCTIVE HYDROGENATION, OLIGOMERISATION, POLYMERISATION; RECOVERY OF HYDROCARBON OILS FROM OIL-SHALE, OIL-SAND, OR GASES; REFINING MIXTURES MAINLY CONSISTING OF HYDROCARBONS; REFORMING OF NAPHTHA; MINERAL WAXES
- C10G2/00—Production of liquid hydrocarbon mixtures of undefined composition from oxides of carbon
-
- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10G—CRACKING HYDROCARBON OILS; PRODUCTION OF LIQUID HYDROCARBON MIXTURES, e.g. BY DESTRUCTIVE HYDROGENATION, OLIGOMERISATION, POLYMERISATION; RECOVERY OF HYDROCARBON OILS FROM OIL-SHALE, OIL-SAND, OR GASES; REFINING MIXTURES MAINLY CONSISTING OF HYDROCARBONS; REFORMING OF NAPHTHA; MINERAL WAXES
- C10G47/00—Cracking of hydrocarbon oils, in the presence of hydrogen or hydrogen- generating compounds, to obtain lower boiling fractions
- C10G47/02—Cracking of hydrocarbon oils, in the presence of hydrogen or hydrogen- generating compounds, to obtain lower boiling fractions characterised by the catalyst used
- C10G47/10—Cracking of hydrocarbon oils, in the presence of hydrogen or hydrogen- generating compounds, to obtain lower boiling fractions characterised by the catalyst used with catalysts deposited on a carrier
- C10G47/12—Inorganic carriers
- C10G47/16—Crystalline alumino-silicate carriers
- C10G47/20—Crystalline alumino-silicate carriers the catalyst containing other metals or compounds thereof
-
- 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
- B01J2229/00—Aspects of molecular sieve catalysts not covered by B01J29/00
- B01J2229/60—Synthesis on support
- B01J2229/62—Synthesis on support in or on other molecular sieves
-
- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10G—CRACKING HYDROCARBON OILS; PRODUCTION OF LIQUID HYDROCARBON MIXTURES, e.g. BY DESTRUCTIVE HYDROGENATION, OLIGOMERISATION, POLYMERISATION; RECOVERY OF HYDROCARBON OILS FROM OIL-SHALE, OIL-SAND, OR GASES; REFINING MIXTURES MAINLY CONSISTING OF HYDROCARBONS; REFORMING OF NAPHTHA; MINERAL WAXES
- C10G2400/00—Products obtained by processes covered by groups C10G9/00 - C10G69/14
- C10G2400/04—Diesel oil
Description
Claims (15)
- 合成ガスから高品質の灯油留分を選択的に合成するための担体であって、前記担体の原料の組成は重量部で、5〜50部のメソポーラスジルコニア、10〜55部のシリコアルミノホスフェート分子ふるい、5〜50部の修飾Al-SBA-16、1〜3部のセスバニアガム粉末、および10〜70部のアルミナを含むことを特徴とする合成ガスから高品質の灯油留分を選択的に合成するための担体。
- 前記担体の原料の組成は重量部で、10〜30部のメソポーラスジルコニア、25〜45部のシリコアルミノホスフェート分子ふるい、10〜30部の修飾Al-SBA-16、1〜3部のセスバニアガム粉末、および30〜55部のアルミナを含む、請求項1に記載の合成ガスから高品質の灯油留分を選択的に合成するための担体。
- 前記担体の原料の組成は重量部で、20部のメソポーラスジルコニア、30部のシリコアルミノホスフェート分子ふるい、25部の修飾Al-SBA-16、1部のセスバニアガム粉末、および30部のアルミナを含む、請求項2に記載の合成ガスから高品質の灯油留分を選択的に合成するための担体。
- 前記修飾Al-SBA-16は、SBA-16とアルミニウムトリエトキシドとを含み、SBA-16とアルミニウムトリエトキシドの重量比が1:3.0〜4.5である、請求項1ないし3のいずれか一項に記載の合成ガスから高品質の灯油留分を選択的に合成するための担体。
- 前記修飾Al-SBA-16中のケイ素とアルミニウムのモル比nが5〜55であり、ブレンステッド酸含有量が39〜92μmol・g-1であり、ルイス酸含有量が71〜105μmol・g-1であり、Na2O含有量≦0.1wt%である、請求項1ないし3のいずれか一項に記載の合成ガスから高品質の灯油留分を選択的に合成するための担体。
- 前記修飾Al-SBA-16中のケイ素とアルミニウムのモル比nが10〜55であり、比表面積が550〜930m2・g-1であり、平均細孔径が4.0〜7.5nmであり、全細孔容積は0.45〜0.70cm3・g-1である、請求項5に記載の合成ガスから高品質の灯油留分を選択的に合成するための担体。
- 前記メソポーラスジルコニアの比表面積が190〜350m2・g-1、平均細孔径が5.0〜8.5nm、全細孔容積が0.40〜0.55cm3・g-1である、請求項1ないし3のいずれか一項に記載の合成ガスから高品質の灯油留分を選択的に合成するための担体。
- 前記シリコアルミノホスフェート分子ふるいは、全酸含有量が0.1〜0.35mmolNH3・g-1、ケイ素とアルミニウムのモル比が0〜1.0、比表面積≧150m2・g-1、Na2O含有量≦0.2wt%、全細孔容積が0.10〜0.30cm3・g-1である、請求項1ないし3のいずれか一項に記載の合成ガスから高品質の灯油留分を選択的に合成するための担体。
- 前記シリコアルミノホスフェート分子ふるいは、ケイ素とアルミニウムのモル比が0.21〜0.38、比表面積≧180m2・g-1以上、Na2O含有量≦0.2wt%、全細孔容積が0.10〜0.30cm3・g-1であり、或いは前記シリコアルミノホスフェート分子ふるいは、ケイ素とアルミニウムのモル比が0〜1.0、比表面積≧150m2・g-1、Na2O含有量≦0.2wt%、全細孔容積が0.13〜0.26cm3・g-1である、請求項8に記載の合成ガスから高品質の灯油留分を選択的に合成するための担体。
- 合成ガスから高品質の灯油留分を選択的に合成するための担体の調製方法であって、
1)SBA-16とアルミニウムトリエトキシドを1:3.0〜4.5の重量比で計量し、アルミニウムトリエトキシドを2等分する工程と、
2)SBA-16をn-ヘキサンに加え、室温で均一に撹拌して混合溶液を得、アルミニウムトリエトキシドの一部をn-ヘキサンに加え、アルミニウムトリエトキシドが溶解するまで室温で撹拌し、アルミニウムトリエトキシドが溶解したn-ヘキサンを混合溶液に加え、室温で一晩攪拌して試料溶液を得る工程と、
3)2)で得られた試料溶液をブフナー漏斗に移し、n-ヘキサンで洗浄し、吸引濾過し、前記工程を2〜4回繰り返すことにより一次フィルタケーキを得る工程と、
4)前記フィルタケーキをn-ヘキサンに加え、室温で撹拌し、別の部分のアルミニウムトリエトキシドを加え、室温で一晩攪拌し、ブフナー漏斗に移し、n-ヘキサンで洗浄し、吸引濾過し、前記工程を2〜4回繰り返すことにより二次フィルタケーキを得る工程と、
5)前記二次フィルタケーキを500〜650℃で6〜10時間焼成することにより修飾Al-SBA-16を得る工程と、
6)ミクロ多孔質アルミナと濃度が5〜20wt%である希硝酸溶液を1:0.5〜1.5の重量比で均一に混練し、粘性ペーストを調製する工程と、
7)重量部で、5〜50部のメソポーラスジルコニア、10〜55部のシリコアルミノホスフェート分子ふるい、5〜50部の修飾Al-SBA-16、1〜3部のセスバニアガム粉末、10〜70部のアルミナをベースとする粘性ペーストとなるように計量し、それらを均一に混合し、ローラ圧縮し、押出成形し、90〜120℃で6〜12時間乾燥させた後、500〜600℃の空気中で4〜10時間焼成し、室温まで冷却して担体を得る工程と
を含むことを特徴とする方法。 - 前記担体は、円筒形細片、クローバーまたは四葉クローバーの形状であり、円筒形細片形状の担体は、1.2〜1.6mmの粒度および5〜10mmの長さを有し、クローバーまたは四葉クローバーの形状の担体は、2枚の葉の間の距離が1.1〜1.8mmであり、長さが5〜10mmである、請求項10に記載の合成ガスから高品質の灯油留分を選択的に合成するための担体の調製方法。
- 合成ガスから高品質の灯油留分を選択的に合成するための触媒であって、前記触媒は可溶性コバルト塩および請求項1に記載の担体を含み、前記可溶性コバルト塩が担体の表面に担持されることを特徴とする触媒。
- 前記可溶性コバルト塩が触媒の5〜20重量%を占める、請求項12に記載の合成ガスから高品質の灯油留分を選択的に合成するための触媒。
- 前記可溶性コバルト塩が硝酸コバルト、酢酸コバルトまたはコバルトカルボニルである、請求項12または13に記載の合成ガスから高品質の灯油留分を選択的に合成するための触媒。
- 請求項12に記載の触媒の調製方法であって、等容積含浸により可溶性コバルト塩を含む水溶液に担体を含浸させ、室温で一晩熟成させ、次いで90〜120℃の常圧下で4〜12時間乾燥させ、500〜600℃の空気中で4〜10時間焼成し、そして室温まで冷却して触媒を得る工程を含む方法。
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