CN109395727A - Condensed-nuclei aromatics lightening catalyst - Google Patents
Condensed-nuclei aromatics lightening catalyst Download PDFInfo
- Publication number
- CN109395727A CN109395727A CN201710709584.3A CN201710709584A CN109395727A CN 109395727 A CN109395727 A CN 109395727A CN 201710709584 A CN201710709584 A CN 201710709584A CN 109395727 A CN109395727 A CN 109395727A
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- CN
- China
- Prior art keywords
- catalyst
- condensed
- compound
- nuclei aromatics
- hours
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
- Granted
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- 239000003054 catalyst Substances 0.000 title claims abstract description 135
- 229910052751 metal Inorganic materials 0.000 claims abstract description 65
- 150000001875 compounds Chemical class 0.000 claims abstract description 26
- 239000002253 acid Substances 0.000 claims abstract description 11
- 229910000765 intermetallic Inorganic materials 0.000 claims abstract description 7
- 238000009826 distribution Methods 0.000 claims abstract description 3
- 238000006243 chemical reaction Methods 0.000 claims description 100
- 229910052739 hydrogen Inorganic materials 0.000 claims description 73
- 239000001257 hydrogen Substances 0.000 claims description 73
- 239000002184 metal Substances 0.000 claims description 59
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Substances [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 claims description 37
- KDLHZDBZIXYQEI-UHFFFAOYSA-N palladium Substances [Pd] KDLHZDBZIXYQEI-UHFFFAOYSA-N 0.000 claims description 34
- -1 alcohol compound Chemical class 0.000 claims description 32
- PNEYBMLMFCGWSK-UHFFFAOYSA-N Alumina Chemical compound [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 claims description 29
- 229910052733 gallium Inorganic materials 0.000 claims description 29
- 239000004215 Carbon black (E152) Substances 0.000 claims description 24
- 229930195733 hydrocarbon Natural products 0.000 claims description 24
- GYHNNYVSQQEPJS-UHFFFAOYSA-N Gallium Chemical compound [Ga] GYHNNYVSQQEPJS-UHFFFAOYSA-N 0.000 claims description 23
- 239000000969 carrier Substances 0.000 claims description 22
- 229910052763 palladium Inorganic materials 0.000 claims description 21
- 229910052697 platinum Inorganic materials 0.000 claims description 20
- 229910052703 rhodium Inorganic materials 0.000 claims description 19
- 239000010948 rhodium Substances 0.000 claims description 19
- MHOVAHRLVXNVSD-UHFFFAOYSA-N rhodium atom Chemical compound [Rh] MHOVAHRLVXNVSD-UHFFFAOYSA-N 0.000 claims description 12
- RTZKZFJDLAIYFH-UHFFFAOYSA-N Diethyl ether Chemical compound CCOCC RTZKZFJDLAIYFH-UHFFFAOYSA-N 0.000 claims description 8
- 239000007864 aqueous solution Substances 0.000 claims description 8
- 229910052732 germanium Inorganic materials 0.000 claims description 8
- 229910052741 iridium Inorganic materials 0.000 claims description 8
- 150000003839 salts Chemical class 0.000 claims description 8
- 238000000034 method Methods 0.000 claims description 7
- 229910052718 tin Inorganic materials 0.000 claims description 7
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 5
- WURBVZBTWMNKQT-UHFFFAOYSA-N 1-(4-chlorophenoxy)-3,3-dimethyl-1-(1,2,4-triazol-1-yl)butan-2-one Chemical compound C1=NC=NN1C(C(=O)C(C)(C)C)OC1=CC=C(Cl)C=C1 WURBVZBTWMNKQT-UHFFFAOYSA-N 0.000 claims description 4
- GNPVGFCGXDBREM-UHFFFAOYSA-N germanium atom Chemical compound [Ge] GNPVGFCGXDBREM-UHFFFAOYSA-N 0.000 claims description 4
- 229910052745 lead Inorganic materials 0.000 claims description 4
- 239000003208 petroleum Substances 0.000 claims description 4
- 230000001376 precipitating effect Effects 0.000 claims description 4
- 239000011959 amorphous silica alumina Substances 0.000 claims description 3
- 238000007598 dipping method Methods 0.000 claims description 3
- 238000002360 preparation method Methods 0.000 claims description 3
- 239000005995 Aluminium silicate Substances 0.000 claims description 2
- 238000010521 absorption reaction Methods 0.000 claims description 2
- 235000012211 aluminium silicate Nutrition 0.000 claims description 2
- 238000000576 coating method Methods 0.000 claims description 2
- HNPSIPDUKPIQMN-UHFFFAOYSA-N dioxosilane;oxo(oxoalumanyloxy)alumane Chemical compound O=[Si]=O.O=[Al]O[Al]=O HNPSIPDUKPIQMN-UHFFFAOYSA-N 0.000 claims description 2
- NLYAJNPCOHFWQQ-UHFFFAOYSA-N kaolin Chemical compound O.O.O=[Al]O[Si](=O)O[Si](=O)O[Al]=O NLYAJNPCOHFWQQ-UHFFFAOYSA-N 0.000 claims description 2
- 150000002941 palladium compounds Chemical class 0.000 claims description 2
- 229910052789 astatine Inorganic materials 0.000 claims 3
- 229910000323 aluminium silicate Inorganic materials 0.000 claims 1
- 238000005984 hydrogenation reaction Methods 0.000 abstract description 16
- YXFVVABEGXRONW-UHFFFAOYSA-N Toluene Chemical compound CC1=CC=CC=C1 YXFVVABEGXRONW-UHFFFAOYSA-N 0.000 description 108
- UFWIBTONFRDIAS-UHFFFAOYSA-N Naphthalene Chemical compound C1=CC=CC2=CC=CC=C21 UFWIBTONFRDIAS-UHFFFAOYSA-N 0.000 description 90
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 49
- 230000009257 reactivity Effects 0.000 description 44
- 238000005470 impregnation Methods 0.000 description 41
- 239000000243 solution Substances 0.000 description 41
- UHOVQNZJYSORNB-UHFFFAOYSA-N Benzene Chemical compound C1=CC=CC=C1 UHOVQNZJYSORNB-UHFFFAOYSA-N 0.000 description 33
- 239000000463 material Substances 0.000 description 25
- 239000002994 raw material Substances 0.000 description 23
- 238000011835 investigation Methods 0.000 description 22
- 238000001035 drying Methods 0.000 description 20
- UPWPDUACHOATKO-UHFFFAOYSA-K gallium trichloride Chemical compound Cl[Ga](Cl)Cl UPWPDUACHOATKO-UHFFFAOYSA-K 0.000 description 13
- TXUICONDJPYNPY-UHFFFAOYSA-N (1,10,13-trimethyl-3-oxo-4,5,6,7,8,9,11,12,14,15,16,17-dodecahydrocyclopenta[a]phenanthren-17-yl) heptanoate Chemical compound C1CC2CC(=O)C=C(C)C2(C)C2C1C1CCC(OC(=O)CCCCCC)C1(C)CC2 TXUICONDJPYNPY-UHFFFAOYSA-N 0.000 description 12
- 229910021626 Tin(II) chloride Inorganic materials 0.000 description 12
- PIBWKRNGBLPSSY-UHFFFAOYSA-L palladium(II) chloride Chemical compound Cl[Pd]Cl PIBWKRNGBLPSSY-UHFFFAOYSA-L 0.000 description 12
- 239000001119 stannous chloride Substances 0.000 description 12
- 235000011150 stannous chloride Nutrition 0.000 description 12
- 125000005575 polycyclic aromatic hydrocarbon group Chemical group 0.000 description 9
- SONJTKJMTWTJCT-UHFFFAOYSA-K rhodium(iii) chloride Chemical compound [Cl-].[Cl-].[Cl-].[Rh+3] SONJTKJMTWTJCT-UHFFFAOYSA-K 0.000 description 9
- 238000005660 chlorination reaction Methods 0.000 description 6
- NGNBDVOYPDDBFK-UHFFFAOYSA-N 2-[2,4-di(pentan-2-yl)phenoxy]acetyl chloride Chemical compound CCCC(C)C1=CC=C(OCC(Cl)=O)C(C(C)CCC)=C1 NGNBDVOYPDDBFK-UHFFFAOYSA-N 0.000 description 5
- 239000000203 mixture Substances 0.000 description 5
- 150000004945 aromatic hydrocarbons Chemical class 0.000 description 4
- 230000008901 benefit Effects 0.000 description 3
- 239000003795 chemical substances by application Substances 0.000 description 3
- 230000000052 comparative effect Effects 0.000 description 3
- 230000000694 effects Effects 0.000 description 3
- GKOZUEZYRPOHIO-UHFFFAOYSA-N iridium atom Chemical compound [Ir] GKOZUEZYRPOHIO-UHFFFAOYSA-N 0.000 description 3
- 239000002808 molecular sieve Substances 0.000 description 3
- 239000003921 oil Substances 0.000 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 description 3
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 description 2
- XUIMIQQOPSSXEZ-UHFFFAOYSA-N Silicon Chemical compound [Si] XUIMIQQOPSSXEZ-UHFFFAOYSA-N 0.000 description 2
- 239000006227 byproduct Substances 0.000 description 2
- 238000004523 catalytic cracking Methods 0.000 description 2
- PCHJSUWPFVWCPO-UHFFFAOYSA-N gold Chemical compound [Au] PCHJSUWPFVWCPO-UHFFFAOYSA-N 0.000 description 2
- 229910052737 gold Inorganic materials 0.000 description 2
- 239000010931 gold Substances 0.000 description 2
- RLJMLMKIBZAXJO-UHFFFAOYSA-N lead nitrate Chemical compound [O-][N+](=O)O[Pb]O[N+]([O-])=O RLJMLMKIBZAXJO-UHFFFAOYSA-N 0.000 description 2
- 229910000510 noble metal Inorganic materials 0.000 description 2
- 238000012913 prioritisation Methods 0.000 description 2
- 239000010703 silicon Substances 0.000 description 2
- 229910052710 silicon Inorganic materials 0.000 description 2
- 230000002195 synergetic effect Effects 0.000 description 2
- 241001120493 Arene Species 0.000 description 1
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 1
- 206010013786 Dry skin Diseases 0.000 description 1
- VGGSQFUCUMXWEO-UHFFFAOYSA-N Ethene Chemical compound C=C VGGSQFUCUMXWEO-UHFFFAOYSA-N 0.000 description 1
- 239000005977 Ethylene Substances 0.000 description 1
- ZOKXTWBITQBERF-UHFFFAOYSA-N Molybdenum Chemical compound [Mo] ZOKXTWBITQBERF-UHFFFAOYSA-N 0.000 description 1
- NINIDFKCEFEMDL-UHFFFAOYSA-N Sulfur Chemical compound [S] NINIDFKCEFEMDL-UHFFFAOYSA-N 0.000 description 1
- UCKMPCXJQFINFW-UHFFFAOYSA-N Sulphide Chemical compound [S-2] UCKMPCXJQFINFW-UHFFFAOYSA-N 0.000 description 1
- 229910021536 Zeolite Inorganic materials 0.000 description 1
- 230000002378 acidificating effect Effects 0.000 description 1
- 239000000654 additive Substances 0.000 description 1
- 230000000996 additive effect Effects 0.000 description 1
- 150000004645 aluminates Chemical class 0.000 description 1
- 125000003118 aryl group Chemical group 0.000 description 1
- 239000010953 base metal Substances 0.000 description 1
- 125000002619 bicyclic group Chemical group 0.000 description 1
- 229910052799 carbon Inorganic materials 0.000 description 1
- 238000004517 catalytic hydrocracking Methods 0.000 description 1
- 238000006555 catalytic reaction Methods 0.000 description 1
- 239000002283 diesel fuel Substances 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- 125000004435 hydrogen atom Chemical group [H]* 0.000 description 1
- 230000003993 interaction Effects 0.000 description 1
- 239000007788 liquid Substances 0.000 description 1
- 238000004519 manufacturing process Methods 0.000 description 1
- 229910044991 metal oxide Inorganic materials 0.000 description 1
- 150000004706 metal oxides Chemical class 0.000 description 1
- 150000002739 metals Chemical class 0.000 description 1
- 238000002156 mixing Methods 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 229910052750 molybdenum Inorganic materials 0.000 description 1
- 239000011733 molybdenum Substances 0.000 description 1
- 229910052759 nickel Inorganic materials 0.000 description 1
- 230000008569 process Effects 0.000 description 1
- 239000000047 product Substances 0.000 description 1
- RWRDJVNMSZYMDV-UHFFFAOYSA-L radium chloride Chemical compound [Cl-].[Cl-].[Ra+2] RWRDJVNMSZYMDV-UHFFFAOYSA-L 0.000 description 1
- 229910001630 radium chloride Inorganic materials 0.000 description 1
- 238000007670 refining Methods 0.000 description 1
- 238000007142 ring opening reaction Methods 0.000 description 1
- 229920006395 saturated elastomer Polymers 0.000 description 1
- 238000007493 shaping process Methods 0.000 description 1
- 229910052717 sulfur Inorganic materials 0.000 description 1
- 239000011593 sulfur Substances 0.000 description 1
- 229910052723 transition metal Inorganic materials 0.000 description 1
- 150000003624 transition metals Chemical class 0.000 description 1
- 239000010457 zeolite Substances 0.000 description 1
Classifications
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Abstract
The present invention relates to a kind of condensed-nuclei aromatics lightening catalyst, mainly solve to exist in the prior art that condensed-nuclei aromatics hydrogenation selectivity is not high, the high problem of mononuclear aromatics loss late.The present invention passes through a kind of condensed-nuclei aromatics selective hydrocatalyst, it include: containing nonacid or faintly acid porous carrier, and at least two metallic elements or compound selected from VIII, III A, IV A of load thereon, the metallic element or compound are in the technical solution of nuclear shell distribution on the surface of the carrier, condensed-nuclei aromatics hydrogenation selectivity is significantly improved, mononuclear aromatics loss is reduced.
Description
Technical field
The present invention relates to a kind of condensed-nuclei aromatics lightening catalysts and preparation method thereof.
Background technique
Condensed-nuclei aromatics refers to bicyclic and multiring structure aromatic component, be largely present in catalytic cracking, ethylene bottom oil and
PX production process, it is most of by as diesel oil blending component if catalytic cracking light cycle oil annual output is more than 10,000,000 tons.Closely
With the continuous increase of China's PX demand over year, the situation that supply falls short of demand is presented in PX.Realize Aromatic Hydrocarbon United Plant enlargement and
Raw material diversification is to solve one of the key factor of present problems.Therefore, make full use of Aromatic Hydrocarbon United Plant by-product condensed-nuclei aromatics,
The condensed-nuclei aromatics of research and utilization oil refining apparatus by-product is of great significance to produce light aromatics.From the point of view of reaction process, realize
Condensed-nuclei aromatics to mononuclear aromatics conversion most critical the step of first is that realize condensed-nuclei aromatics selective hydrogenation, by polycyclic aromatic hydrocarbon
Partial hydrogenation generates mononuclear aromatics component.It is coexisted in system in monocycle and polycyclic aromatic hydrocarbon, realizes that arenes selectivity adds hydrogen to be to improve
The significant process of mononuclear aromatics yield.The mononuclear aromatics such as benzene, toluene are controlled while producing mononuclear aromatics adds hydrogen saturation, gold
Belong to the metals such as platinum, palladium and base metal molybdenum, nickel have been reported for polycyclic aromatic hydrocarbon plus hydrogen saturation.
CN104117386A discloses a kind of condensed-nuclei aromatics and adds hydrogen ring opening catalyst, and catalyst is containing 5%-100%'s
Beta molecular sieve component, and the noble metal for selecting Pt, Ir, Pd of the 0.1%-3% of load thereon.
CN102688770A discloses a kind of aromatic hydrocarbon hydrogenation catalyst, is to form with mesoporous zeolite and noble metal, improves
The hydrogenation aromatics-removing activity and sulfur resistance of catalyst.
CN103301874B discloses the method and carbon monoxide-olefin polymeric of a kind of polycyclic aromatic hydrocarbon selective hydrogenation open loop, including
Acidic molecular sieve loads VIII family metal oxide and catalyst containing Mo, and catalyst containing Mo is Mo and the bimetallic of transition metal composition
Sulfide significantly improves the yield of selective opening product using combination catalyst and water additive.
CN103666553 discloses a kind of method of hydro-conversion polycyclic aromatic hydrocarbon, and polycyclic aromatic hydrocarbon is first in hydroconversion reaction zone
It is at least partially saturated, 40% or more polycyclic aromatic hydrocarbon conversion ratio of acquisition, mononuclear aromatics yield 4-80%,；Pass through hydrocracking again
Reaction zone reaction, obtains 85% or more polycyclic aromatic hydrocarbon conversion ratio, mononuclear aromatics yield advantage 4-30%, to reduce polycyclic aromatic hydrocarbon
Convert hydrogen consumption.
Above patent document is not directed to that monocycle, condensed-nuclei aromatics coexists under system, realizes that condensed-nuclei aromatics is highly selective
Partial hydrogenation technology.
Summary of the invention
The technical problem to be solved by the present invention is to the prior art, that there are condensed-nuclei aromatics hydrogenation selectivities is low, mononuclear aromatics is received
The low problem of rate, provides a kind of new condensed-nuclei aromatics selective hydrocatalyst, the catalyst for handle containing mononuclear aromatics with
When condensed-nuclei aromatics material, have condensed-nuclei aromatics selective hydrogenation rate high, mononuclear aromatics loses small advantage.
In order to solve the above technical problems, the present invention is as follows using technical solution: a kind of condensed-nuclei aromatics lightening catalyst packet
It includes: being selected from VIII, III A, the metallic element of IV A or compound wherein containing nonacid or faintly acid porous carrier, at least two, institute
Stating metallic element or compound on the surface of the carrier is in nuclear shell distribution.
In above-mentioned technical proposal, nonacid or faintly acid porous carrier is selected from aluminium oxide, amorphous silica-alumina, kaolin, silicon
At least one of aluminate.The metal in Pt, Pd, Ir, Rh, Ga, Ge, Sn, Pb at least two.The nuclear phase layer
Metal is selected from least one of metal and its compound of Ga, Ge, Sn, Pb.The shell phase layer metal is selected from Pt, Pd, Ir, Rh
At least one of metal and its compound.
In more optimized scheme, nuclear phase layer metal be selected from Ga and Sn mixture, wherein the weight ratio of Ga and Sn be (0.1~
10): 1；The mixture of Ga and Sn has synergistic effect in terms of the selective hydrogenation for improving fused ring compound.
In more optimized scheme, shell phase layer metal includes the mixture of Pd and Rh simultaneously, and wherein the weight ratio of Pd and Rh is
(0.1~10): 1；Pd and Rh mixture has synergistic effect in terms of the selective hydrogenation activity for improving fused ring compound.
The condensed-nuclei aromatics lightening catalyst, based on parts by weight, nuclear phase layer tenor are 0.01-15 parts,
Prioritization scheme is 0.05-5 parts；Shell phase layer tenor is 0.01-5 parts, and prioritization scheme is 0.03-3 parts.A kind of condensed-nuclei aromatics is light
The preparation method of matter catalyst, comprising:
A) salt of containing nuclear phase layer metal is dissolved in water or non-aqueous solution, then is existed by the method for precipitating, physics bonding, dipping
One layer of metallic compound of supported on carriers roasts in 400-600 DEG C after dry, the catalyst I with nuclear phase layer structure is made.
B) salt containing shell phase layer metal is dissolved in water or non-aqueous solution, then negative by dipping, precipitating or coating process
It is loaded on catalyst I, is roasted after dry in 400-600 DEG C, condensed-nuclei aromatics lightening catalyst is made；
Wherein, a) metal salt in step is selected from germanium-containing compound, gallium-containing compound, sn-containing compound, lead-containing compounds
At least one of, the non-aqueous solution is selected from one kind of alcohol compound, ketone compounds, petroleum ether；B) gold in step
Belong to salt to be selected from compound containing platinum, containing palladium compound, contain at least one of iridic compound, rhodium-containing compound, the non-aqueous solution
Selected from one of alcohol compound, ketone compounds, petroleum ether.
The catalyst is 100-500 DEG C, reaction pressure 0.5-5MPa in reaction temperature, and hydrogen hydrocarbon molar ratio is 1-8, into
Material weight space velocity is reacted under the conditions of being 0.5-20.
In the present invention, based on the interaction between nuclear shell carried metal, the electronic characteristic of shell metallic can be effectively adjusted,
To which modulation shell metallic is to aromatics absorption intensity, the selective hydrogenation activity to condensed-nuclei aromatics is improved.The catalyst treatment contains
When mononuclear aromatics and condensed-nuclei aromatics material, have condensed-nuclei aromatics selective hydrogenation rate high, mononuclear aromatics loses small advantage.
Below by the description to embodiment, further illustrates but does not limit the present invention:
Specific embodiment
[embodiment 1]
Take 20 grams of alumina balls carriers, the certain chlorination Gallium solution of incipient impregnation, 120 DEG C drying 4 hours, 550 DEG C of roastings 4
Hour, the modified catalyst A1 that gallium content is 2% (wt) is made and obtains the certain platinum acid chloride solution of catalyst A1 incipient impregnation
Platinum content is the nucleocapsid metal layer catalyst B1 of 0.2% (wt).
5 grams of nucleocapsid metal layer catalyst B1 are placed in reactor, logical hydrogen restores 3 hours at 450 DEG C, then is cooled to
It 350 DEG C, is passed through hydrogen and containing toluene and naphthalene material contacts with catalyst and carries out reactivity investigation.Reaction condition are as follows: total
Weight space velocity is 10 hours-1, 350 DEG C of reaction temperature, reaction pressure 3.0MPa, hydrogen hydrocarbon molecule is than 3.0.Reaction raw materials are toluene:
Naphthalene=90:10 (weight), reactivity worth is as shown in table 1.Wherein, R2/R1 indicates that the weight hydrogenation rate of naphthalene and toluene by weight add hydrogen
The ratio between rate has reacted catalyst to the hydrogenation selectivity of condensed-nuclei aromatics.
[embodiment 2]
Take 20 grams of alumina balls carriers, the certain chlorination germanium solution of incipient impregnation, 120 DEG C drying 4 hours, 550 DEG C of roastings 4
Hour, the modified catalyst A2 that Ge content is 2% (wt) is made and obtains the certain platinum acid chloride solution of catalyst A2 incipient impregnation
The nucleocapsid metal layer that platinum content is 0.2% (wt) is catalyzed B2.
5 grams of nucleocapsid metal layer catalyst B2 are placed in reactor, logical hydrogen restores 3 hours at 450 DEG C, then is cooled to
It 350 DEG C, is passed through hydrogen and containing toluene and naphthalene material contacts with catalyst and carries out reactivity investigation.Reaction condition are as follows: total
Weight space velocity is 10 hours-1, 350 DEG C of reaction temperature, reaction pressure 3.0MPa, hydrogen hydrocarbon molecule is than 3.0.Reaction raw materials are toluene:
Naphthalene=90:10 (weight), reactivity worth is as shown in table 1.
[embodiment 3]
Take 20 grams of alumina balls carriers, the certain stannous chloride solution of incipient impregnation, 120 DEG C drying 4 hours, 550 DEG C of roastings
It burns 4 hours, the modified catalyst A3 that Theil indices are 2% (wt) is made, by the certain platinum acid chloride solution of catalyst A3 incipient impregnation,
Obtain the nucleocapsid metal layer catalyst B3 that platinum content is 0.5% (wt).
5 grams of nucleocapsid metal layer catalyst B3 are placed in reactor, logical hydrogen restores 3 hours at 450 DEG C, then is cooled to
It 350 DEG C, is passed through hydrogen and containing toluene and naphthalene material contacts with catalyst and carries out reactivity investigation.Reaction condition are as follows: total
Weight space velocity is 10 hours-1, 350 DEG C of reaction temperature, reaction pressure 3.0MPa, hydrogen hydrocarbon molecule is than 3.0.Reaction raw materials are toluene:
Naphthalene=90:10 (weight), reactivity worth is as shown in table 1.
[embodiment 4]
Take 20 grams of alumina balls carriers, the certain lead nitrate solution of incipient impregnation, 120 DEG C drying 4 hours, 550 DEG C of roastings 4
Hour, the modified catalyst A4 that lead content is 2% (wt) is made and obtains the certain platinum acid chloride solution of catalyst A4 incipient impregnation
Platinum content is the nucleocapsid metal layer catalyst B4 of 0.2% (wt).
5 grams of nucleocapsid metal layer catalyst B4 are placed in reactor, logical hydrogen restores 3 hours at 450 DEG C, then is cooled to
It 350 DEG C, is passed through hydrogen and containing toluene and naphthalene material contacts with catalyst and carries out reactivity investigation.Reaction condition are as follows: total
Weight space velocity is 10 hours-1, 350 DEG C of reaction temperature, reaction pressure 3.0MPa, hydrogen hydrocarbon molecule is than 3.0.Reaction raw materials are toluene:
Naphthalene=90:10 (weight), reactivity worth is as shown in table 1.
[embodiment 5]
Take 20 grams of alumina balls carriers, the certain chlorination Gallium solution of incipient impregnation, 120 DEG C drying 4 hours, 550 DEG C of roastings 4
Hour, the modified catalyst A5 that gallium content is 2% (wt) is made and obtains the certain palladium chloride solution of catalyst A5 incipient impregnation
Palladium content is the nucleocapsid metal layer catalyst B5 of 0.2% (wt).
5 grams of nucleocapsid metal layer catalyst B5 are placed in reactor, logical hydrogen restores 3 hours at 450 DEG C, then is cooled to
It 350 DEG C, is passed through hydrogen and containing toluene and naphthalene material contacts with catalyst and carries out reactivity investigation.Reaction condition are as follows: total
Weight space velocity is 10 hours-1, 350 DEG C of reaction temperature, reaction pressure 3.0MPa, hydrogen hydrocarbon molecule is than 3.0.Reaction raw materials are toluene:
Naphthalene=90:10 (weight), reactivity worth is as shown in table 1.
[embodiment 6]
Take 20 grams of alumina balls carriers, the certain chlorination Gallium solution of incipient impregnation, 120 DEG C drying 4 hours, 550 DEG C of roastings 4
Hour, the modified catalyst A6 that gallium content is 2% (wt) is made and obtains the certain Chloroiridic Acid solution of catalyst A6 incipient impregnation
Iridium content is the nucleocapsid metal layer catalyst B6 of 0.2% (wt).
5 grams of nucleocapsid metal layer catalyst B6 are placed in reactor, logical hydrogen restores 3 hours at 450 DEG C, then is cooled to
It 350 DEG C, is passed through hydrogen and containing toluene and naphthalene material contacts with catalyst and carries out reactivity investigation.Reaction condition are as follows: total
Weight space velocity is 10 hours-1, 350 DEG C of reaction temperature, reaction pressure 3.0MPa, hydrogen hydrocarbon molecule is than 3.0.Reaction raw materials are toluene:
Naphthalene=90:10 (weight), reactivity worth is as shown in table 1.
[embodiment 7]
Take 20 grams of alumina balls carriers, the certain chlorination Gallium solution of incipient impregnation, 120 DEG C drying 4 hours, 550 DEG C of roastings 4
Hour, the modified catalyst A7 that gallium content is 2% (wt) is made and obtains the certain rhodium chloride solution of catalyst A7 incipient impregnation
Rhodium content is the nucleocapsid metal layer catalyst B7 of 0.2% (wt).
5 grams of nucleocapsid metal layer catalyst B7 are placed in reactor, logical hydrogen restores 3 hours at 450 DEG C, then is cooled to
It 350 DEG C, is passed through hydrogen and containing toluene and naphthalene material contacts with catalyst and carries out reactivity investigation.Reaction condition are as follows: total
Weight space velocity is 10 hours-1, 350 DEG C of reaction temperature, reaction pressure 3.0MPa, hydrogen hydrocarbon molecule is than 3.0.Reaction raw materials are toluene:
Naphthalene=90:10 (weight), reactivity worth is as shown in table 1.
[embodiment 8]
Take 20 grams of alumina balls carriers, the certain gallium chloride of incipient impregnation and stannous chloride solution, 120 DEG C drying 4 hours,
550 DEG C roast 4 hours, the modified catalyst A8 that gallium content is 1% (wt), Theil indices are 1% (wt) are made, by catalyst A8 etc.
The certain platinum acid chloride solution of volume impregnation obtains the nucleocapsid metal layer catalyst B8 that platinum content is 0.2% (wt).
5 grams of nucleocapsid metal layer catalyst B8 are placed in reactor, logical hydrogen restores 3 hours at 450 DEG C, then is cooled to
It 350 DEG C, is passed through hydrogen and containing toluene and naphthalene material contacts with catalyst and carries out reactivity investigation.Reaction condition are as follows: total
Weight space velocity is 10 hours-1, 350 DEG C of reaction temperature, reaction pressure 3.0MPa, hydrogen hydrocarbon molecule is than 3.0.Reaction raw materials are toluene:
Naphthalene=90:10 (weight), reactivity worth is as shown in table 1.
[embodiment 9]
Take 20 grams of alumina balls carriers, the certain gallium chloride of incipient impregnation and stannous chloride solution, 120 DEG C drying 4 hours,
550 DEG C roast 4 hours, the modified catalyst A9 that gallium content is 1% (wt), Theil indices are 1% (wt) are made, by catalyst A9 etc.
The certain radium chloride of volume impregnation and palladium chloride solution obtain the nucleocapsid metal layer that rhodium content is 0.1% (wt), palladium content is 0.1%
Catalyst B9.
5 grams of nucleocapsid metal layer catalyst B9 are placed in reactor, logical hydrogen restores 3 hours at 450 DEG C, then is cooled to
It 350 DEG C, is passed through hydrogen and containing toluene and naphthalene material contacts with catalyst and carries out reactivity investigation.Reaction condition are as follows: total
Weight space velocity is 10 hours-1, 350 DEG C of reaction temperature, reaction pressure 3.0MPa, hydrogen hydrocarbon molecule is than 3.0.Reaction raw materials are toluene:
Naphthalene=90:10 (weight), reactivity worth is as shown in table 1.
[embodiment 10]
Take 20 grams of alumina balls carriers, the certain gallium chloride of incipient impregnation and stannous chloride solution, 120 DEG C drying 4 hours,
550 DEG C roast 4 hours, the modified catalyst A10 that gallium content is 1% (wt), Theil indices are 1% (wt) are made, by catalyst A10
The certain chloroplatinic acid of incipient impregnation and palladium chloride solution obtain the nucleocapsid metal that platinum content is 0.1% (wt), palladium content is 0.1%
Layer catalyst B10.
5 grams of nucleocapsid metal layer catalyst B10 are placed in reactor, logical hydrogen restores 3 hours at 450 DEG C, then cools down
To 350 DEG C, it is passed through hydrogen and containing toluene and naphthalene material contacts with catalyst and carries out reactivity investigation.Reaction condition are as follows:
Total weight air speed is 10 hours-1, 350 DEG C of reaction temperature, reaction pressure 3.0MPa, hydrogen hydrocarbon molecule is than 3.0.Reaction raw materials are first
Benzene: naphthalene=90:10 (weight), reactivity worth is as shown in table 1.
[embodiment 11]
Take 20 grams of alumina balls carriers, the certain gallium chloride of incipient impregnation and stannous chloride solution, 120 DEG C drying 4 hours,
550 DEG C roast 4 hours, the modified catalyst A11 that gallium content is 1% (wt), Theil indices are 1% (wt) are made, by catalyst A11
The certain chloro-iridic acid of incipient impregnation and palladium chloride solution obtain the nucleocapsid metal that iridium content is 0.1% (wt), palladium content is 0.1%
Layer catalyst B11.
5 grams of nucleocapsid metal layer catalyst B11 are placed in reactor, logical hydrogen restores 3 hours at 450 DEG C, then cools down
To 350 DEG C, it is passed through hydrogen and containing toluene and naphthalene material contacts with catalyst and carries out reactivity investigation.Reaction condition are as follows:
Total weight air speed is 10 hours-1, 350 DEG C of reaction temperature, reaction pressure 3.0MPa, hydrogen hydrocarbon molecule is than 3.0.Reaction raw materials are first
Benzene: naphthalene=90:10 (weight), reactivity worth is as shown in table 1.
[embodiment 12]
Take 20 grams of alumina balls carriers, the certain gallium chloride of incipient impregnation and stannous chloride solution, 120 DEG C drying 4 hours,
550 DEG C roast 4 hours, the modified catalyst A12 that gallium content is 1% (wt), Theil indices are 1% (wt) are made, by catalyst A12
The certain chloroplatinic acid of incipient impregnation and Chloroiridic Acid solution obtain the nucleocapsid metal that platinum content is 0.1% (wt), iridium content is 0.1%
Layer catalyst B12.
5 grams of nucleocapsid metal layer catalyst B12 are placed in reactor, logical hydrogen restores 3 hours at 450 DEG C, then cools down
To 350 DEG C, it is passed through hydrogen and containing toluene and naphthalene material contacts with catalyst and carries out reactivity investigation.Reaction condition are as follows:
Total weight air speed is 10 hours-1, 350 DEG C of reaction temperature, reaction pressure 3.0MPa, hydrogen hydrocarbon molecule is than 3.0.Reaction raw materials are first
Benzene: naphthalene=90:10 (weight), reactivity worth is as shown in table 1.
[embodiment 13]
Take 20 grams of alumina balls carriers, the certain gallium chloride of incipient impregnation and stannous chloride solution, 120 DEG C drying 4 hours,
550 DEG C roast 4 hours, the modified catalyst A13 that gallium content is 1% (wt), Theil indices are 1% (wt) are made, by catalyst A13
The certain chloroplatinic acid of incipient impregnation and rhodium chloride solution obtain the nucleocapsid that platinum content is 0.1% (wt), rhodium content is 0.1% (wt)
Metal layer catalyst B13.
5 grams of nucleocapsid metal layer catalyst B13 are placed in reactor, logical hydrogen restores 3 hours at 450 DEG C, then cools down
To 350 DEG C, it is passed through hydrogen and containing toluene and naphthalene material contacts with catalyst and carries out reactivity investigation.Reaction condition are as follows:
Total weight air speed is 10 hours-1, 350 DEG C of reaction temperature, reaction pressure 3.0MPa, hydrogen hydrocarbon molecule is than 3.0.Reaction raw materials are first
Benzene: naphthalene=90:10 (weight), reactivity worth is as shown in table 1.
[embodiment 14]
Take 20 grams of alumina balls carriers, the certain gallium chloride of incipient impregnation and stannous chloride solution, 120 DEG C drying 4 hours,
550 DEG C roast 4 hours, the modified catalyst A14 that gallium content is 1% (wt), Theil indices are 1% (wt) are made, by catalyst A14
The certain palladium chloride of incipient impregnation and rhodium chloride solution obtain the core that palladium content is 0.05% (wt), rhodium content is 0.15% (wt)
Shell metal layer catalyst B14.
5 grams of nucleocapsid metal layer catalyst B14 are placed in reactor, logical hydrogen restores 3 hours at 450 DEG C, then cools down
To 350 DEG C, it is passed through hydrogen and containing toluene and naphthalene material contacts with catalyst and carries out reactivity investigation.Reaction condition are as follows:
Total weight air speed is 10 hours-1, 350 DEG C of reaction temperature, reaction pressure 3.0MPa, hydrogen hydrocarbon molecule is than 3.0.Reaction raw materials are first
Benzene: naphthalene=90:10 (weight), reactivity worth is as shown in table 1.
[embodiment 15]
Take 20 grams of alumina balls carriers, the certain gallium chloride of incipient impregnation and stannous chloride solution, 120 DEG C drying 4 hours,
550 DEG C roast 4 hours, the modified catalyst A15 that gallium content is 1% (wt), Theil indices are 1% (wt) are made, by catalyst A15
The certain palladium chloride of incipient impregnation and rhodium chloride solution obtain the core that palladium content is 0.15% (wt), rhodium content is 0.05% (wt)
Shell metal layer catalyst B15.
5 grams of nucleocapsid metal layer catalyst B15 are placed in reactor, logical hydrogen restores 3 hours at 450 DEG C, then cools down
To 350 DEG C, it is passed through hydrogen and containing toluene and naphthalene material contacts with catalyst and carries out reactivity investigation.Reaction condition are as follows:
Total weight air speed is 10 hours-1, 350 DEG C of reaction temperature, reaction pressure 3.0MPa, hydrogen hydrocarbon molecule is than 3.0.Reaction raw materials are first
Benzene: naphthalene=90:10 (weight), reactivity worth is as shown in table 1.
[embodiment 16]
Take 20 grams of alumina balls carriers, the certain gallium chloride of incipient impregnation and chlorination germanium solution, 120 DEG C drying 4 hours,
550 DEG C roast 4 hours, the modified catalyst A16 that gallium content is 1% (wt), Ge content is 1% (wt) are made, by catalyst A16
The certain palladium chloride of incipient impregnation and rhodium chloride solution obtain the core that palladium content is 0.15% (wt), rhodium content is 0.05% (wt)
Shell metal layer catalyst B16.
5 grams of nucleocapsid metal layer catalyst B16 are placed in reactor, logical hydrogen restores 3 hours at 450 DEG C, then cools down
To 350 DEG C, it is passed through hydrogen and containing toluene and naphthalene material contacts with catalyst and carries out reactivity investigation.Reaction condition are as follows:
Total weight air speed is 10 hours-1, 350 DEG C of reaction temperature, reaction pressure 3.0MPa, hydrogen hydrocarbon molecule is than 3.0.Reaction raw materials are first
Benzene: naphthalene=90:10 (weight), reactivity worth is as shown in table 1.
[embodiment 17]
Take 20 grams of alumina balls carriers, the certain gallium chloride of incipient impregnation and lead nitrate solution, 120 DEG C drying 4 hours,
550 DEG C roast 4 hours, the modified catalyst A17 that gallium content is 1% (wt), lead content is 1% (wt) are made, by catalyst A17
The certain palladium chloride of incipient impregnation and rhodium chloride solution obtain the core that palladium content is 0.15% (wt), rhodium content is 0.05% (wt)
Shell metal layer catalyst B17.
5 grams of nucleocapsid metal layer catalyst B17 are placed in reactor, logical hydrogen restores 3 hours at 450 DEG C, then cools down
To 350 DEG C, it is passed through hydrogen and containing toluene and naphthalene material contacts with catalyst and carries out reactivity investigation.Reaction condition are as follows:
Total weight air speed is 10 hours-1, 350 DEG C of reaction temperature, reaction pressure 3.0MPa, hydrogen hydrocarbon molecule is than 3.0.Reaction raw materials are first
Benzene: naphthalene=90:10 (weight), reactivity worth is as shown in table 1.
[embodiment 18]
Take 20 grams of balloon borne bodies of amorphous silica-alumina, the certain gallium chloride of incipient impregnation and stannous chloride solution, 120 DEG C of dryings 4
Hour, 550 DEG C roast 4 hours, and the modified catalyst A18 that gallium content is 1% (wt), Theil indices are 1% (wt) is made, will be catalyzed
The certain palladium chloride of agent A18 incipient impregnation and rhodium chloride solution, obtain that palladium content is 0.15% (wt), rhodium content is 0.05% (wt)
Nucleocapsid metal layer catalyst B18.
5 grams of nucleocapsid metal layer catalyst B18 are placed in reactor, logical hydrogen restores 3 hours at 450 DEG C, then cools down
To 350 DEG C, it is passed through hydrogen and containing toluene and naphthalene material contacts with catalyst and carries out reactivity investigation.Reaction condition are as follows:
Total weight air speed is 10 hours-1, 350 DEG C of reaction temperature, reaction pressure 3.0MPa, hydrogen hydrocarbon molecule is than 3.0.Reaction raw materials are first
Benzene: naphthalene=90:10 (weight), reactivity worth is as shown in table 1.
[embodiment 19]
The shaping carrier of 20 grams high silicon Y molecular sieve and aluminium oxide is taken, the certain gallium chloride of incipient impregnation and stannous chloride are molten
Liquid, 120 DEG C drying 4 hours, 550 DEG C roast 4 hours, and gallium content is 1% (wt), Theil indices are 1% (wt) modification is made and urges
The certain palladium chloride of catalyst A19 incipient impregnation and rhodium chloride solution are obtained palladium content and contained for 0.15% (wt), rhodium by agent A19
Amount is the nucleocapsid metal layer catalyst B19 of 0.05% (wt).
5 grams of nucleocapsid metal layer catalyst B19 are placed in reactor, logical hydrogen restores 3 hours at 450 DEG C, then cools down
To 350 DEG C, it is passed through hydrogen and containing toluene and naphthalene material contacts with catalyst and carries out reactivity investigation.Reaction condition are as follows:
Total weight air speed is 10 hours-1, 350 DEG C of reaction temperature, reaction pressure 3.0MPa, hydrogen hydrocarbon molecule is than 3.0.Reaction raw materials are first
Benzene: naphthalene=90:10 (weight), reactivity worth is as shown in table 1.
[comparative example 1]
20 grams of alumina balls carriers are taken, the certain palladium chloride solution of incipient impregnation obtains the catalysis that palladium content is 0.2% (wt)
Agent B20.
5 grams of catalyst B20 are placed in reactor, logical hydrogen restores 3 hours at 450 DEG C, then is cooled to 350 DEG C, leads to
Enter hydrogen and containing toluene and naphthalene material contacts with catalyst and carries out reactivity investigation.Reaction condition are as follows: total weight air speed
It is 10 hours-1, 350 DEG C of reaction temperature, reaction pressure 3.0MPa, hydrogen hydrocarbon molecule is than 3.0.Reaction raw materials are toluene: naphthalene=90:10
(weight), reactivity worth is as shown in table 1.
[comparative example 2]
20 grams of alumina balls carriers, the certain palladium chloride of incipient impregnation and rhodium chloride solution are taken, obtaining palladium content is 0.05%
(wt), rhodium content is the catalyst B21 of 0.15% (wt).
5 grams of catalyst B21 are placed in reactor, logical hydrogen restores 3 hours at 450 DEG C, then is cooled to 350 DEG C, leads to
Enter hydrogen and containing toluene and naphthalene material contacts with catalyst and carries out reactivity investigation.Reaction condition are as follows: total weight air speed
It is 10 hours-1, 350 DEG C of reaction temperature, reaction pressure 3.0MPa, hydrogen hydrocarbon molecule is than 3.0.Reaction raw materials are toluene: naphthalene=90:10
(weight), reactivity worth is as shown in table 1.
[comparative example 3]
Take 20 grams of alumina balls carriers, the certain gallium chloride of incipient impregnation and stannous chloride solution, 120 DEG C drying 4 hours,
550 DEG C roast 4 hours, and the modified catalyst B22 that gallium content is 1% (wt), Theil indices are 1% (wt) is made.
5 grams of catalyst B22 are placed in reactor, logical hydrogen restores 3 hours at 450 DEG C, then is cooled to 350 DEG C, leads to
Enter hydrogen and containing toluene and naphthalene material contacts with catalyst and carries out reactivity investigation.Reaction condition are as follows: total weight air speed
It is 10 hours-1, 350 DEG C of reaction temperature, reaction pressure 3.0MPa, hydrogen hydrocarbon molecule is than 3.0.Reaction raw materials are toluene: naphthalene=90:10
(weight), reactivity worth is as shown in table 1.
Table 1
Claims (9)
1. a kind of condensed-nuclei aromatics lightening catalyst, which is characterized in that catalyst includes:
A) contain nonacid or faintly acid porous carrier, and load thereon
B) at least two metallic element or compound selected from VIII, III A, IV A
Wherein, the metallic element or compound are in nuclear shell distribution on the surface of the carrier.
2. condensed-nuclei aromatics lightening catalyst according to claim 1, it is characterised in that the porous load of nonacid or faintly acid
Body is selected from least one of aluminium oxide, amorphous silica-alumina, kaolin, alumino-silicate.
3. condensed-nuclei aromatics lightening catalyst according to claim 1, it is characterised in that the metal be selected from Pt, Pd, Ir,
At least two in Rh, Ga, Ge, Sn, Pb.
4. condensed-nuclei aromatics lightening catalyst according to claim 1, it is characterised in that the nuclear phase layer metal be selected from Ga,
At least one of metal and its compound of Ge, Sn, Pb.
5. condensed-nuclei aromatics lightening catalyst according to claim 1, it is characterised in that the shell phase layer metal be selected from Pt,
At least one of Pd, Ir, Rh metal and its compound.
6. condensed-nuclei aromatics lightening catalyst according to claim 1, which is characterized in that based on parts by weight, nuclear phase layer
Tenor is 0.01-15 part of overall catalyst weight.
7. condensed-nuclei aromatics lightening catalyst according to claim 1, which is characterized in that based on parts by weight, shell phase layer
Tenor is 0.01-5 part of overall catalyst weight.
8. a kind of preparation method using any one condensed-nuclei aromatics lightening catalyst described in claim 1~7, feature
It is, comprising:
A) salt of containing nuclear phase layer metal is dissolved in water or non-aqueous solution, then passes through precipitating, exchange, method physics bonding, impregnated
In one layer of metallic compound of supported on carriers, is roasted after dry in 400-600 DEG C, the catalyst I with nuclear phase layer structure is made；
B) salt containing shell phase layer metal is dissolved in water or non-aqueous solution, then negative by dipping, absorption, precipitating or coating process
It is loaded on the catalyst I with nuclear phase layer structure, is roasted after dry in 400-600 DEG C, condensed-nuclei aromatics lightening catalyst is made；
Wherein, a) metal salt in step in germanium-containing compound, gallium-containing compound, sn-containing compound, lead-containing compounds
At least one, the non-aqueous solution are selected from one of alcohol compound, ketone compounds, petroleum ether；B) metal in step
Salt is selected from compound containing platinum, containing palladium compound, contains at least one of iridic compound, rhodium-containing compound, the non-aqueous solution choosing
From one of alcohol compound, ketone compounds, petroleum ether.
9. a kind of condensed-nuclei aromatics lightening method, which is characterized in that reaction temperature is 100-500 DEG C, reaction pressure 0.5-
5MPa, hydrogen hydrocarbon molar ratio are 1-8, and feed weight air speed is 0.5-20.
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| CN201710709584.3A CN109395727B (en) | 2017-08-18 | 2017-08-18 | Catalyst for conversion of polycyclic aromatic hydrocarbon into light aromatic hydrocarbon |
| JP2018153138A JP7158953B2 (en) | 2017-08-18 | 2018-08-16 | Catalyst for producing light aromatic hydrocarbons from heavy aromatic hydrocarbons, production method and application thereof |
| KR1020180095695A KR102504661B1 (en) | 2017-08-18 | 2018-08-16 | Catalyst for producing light aromatics with heavy aromatics, method for preparing the catalyst, and use thereof |
| ES201830831A ES2700899B2 (en) | 2017-08-18 | 2018-08-17 | Catalyst for producing light aromatics with heavy aromatics, method of preparing the catalyst and use thereof |
| DE102018213896.6A DE102018213896A1 (en) | 2017-08-18 | 2018-08-17 | Catalyst for the production of light aromatic substances with heavy aromatic substances, process for the preparation of the catalyst and use thereof |
| BE2018/5572A BE1025972B1 (en) | 2017-08-18 | 2018-08-17 | CATALYST FOR PRODUCING LIGHT AROMATICS WITH HEAVY AROMATICS, PROCESS FOR PREPARING THE CATALYST AND USE THEREOF |
| FR1800885A FR3070130B1 (en) | 2017-08-18 | 2018-08-20 | CATALYST FOR PRODUCING LIGHT AROMATICS WITH HEAVY AROMATICS, METHOD FOR PREPARING THE CATALYST AND USE THEREOF |
| US16/105,293 US11065604B2 (en) | 2017-08-18 | 2018-08-20 | Catalyst for producing light aromatics with heavy aromatics, method for preparing the catalyst, and use thereof |
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| CN1117404A (en) * | 1994-08-22 | 1996-02-28 | 中国石油化工总公司 | Catalyst and method for converting heavy arene into light one |
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