CN104923215B - Support ordered mesoporous aluminium oxide material and its synthetic method and the application of noble metal - Google Patents
Support ordered mesoporous aluminium oxide material and its synthetic method and the application of noble metal Download PDFInfo
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- CN104923215B CN104923215B CN201510229476.7A CN201510229476A CN104923215B CN 104923215 B CN104923215 B CN 104923215B CN 201510229476 A CN201510229476 A CN 201510229476A CN 104923215 B CN104923215 B CN 104923215B
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Abstract
The invention provides a kind of ordered mesoporous aluminium oxide material for supporting noble metal and its synthetic method and application.The method is comprised the following steps:After acid, alcohol, nonionic surface active agent are well mixed, hydrophobicity precious metal salt and aluminium salt are added, after being well mixed, obtain a mixed solution;Make mixed solution that a period of time is kept at 30 60 DEG C with solvent flashing;Then it is calcined at 300 600 DEG C, obtains supporting the ordered mesoporous aluminium oxide material of noble metal.The ordered mesoporous aluminium oxide material for supporting noble metal can apply to prepare the catalyst of Oxidation of Carbon Monoxide reaction.The present invention uses one-step synthesis method to support the ordered mesoporous aluminium oxide material of noble metal, decentralization of the noble metal nano particles of the material in mesoporous material is high, it is high to support rate, noble metal nano particles size is small, and mesopore orbit structure height is in order, it has catalysis activity and heat endurance high as the catalyst that Oxidation of Carbon Monoxide reacts.
Description
Technical field
The present invention relates to a kind of ordered mesoporous aluminium oxide material for supporting noble metal and its synthetic method and application, belong to expensive
Metal supports porous material technical field.
Background technology
In mesoporous material, mesopore silicon oxide is to study more deep system.Compared to silica, aluminum oxide possesses one
A little properties better than silica, such as hydrolytic stability higher, stronger acidity, be easier to support different metal species etc.
Deng, therefore obtained more being widely applied in fields such as catalysis, absorption.Because aluminum oxide has larger specific surface area, spy
Different pore structure and certain acidity, and heat endurance is higher, specific surface area remains to be maintained at 100m when higher than 800 DEG C2/g
More than, thus be most widely used in catalytic field, have become in chemical industry and petroleum industry most widely used catalyst or
Catalyst carrier, cracking, hydrofinishing, hydrodesulfurization, the reformation hydrogen production of hydrocarbon in petroleum component, gas phase oil product group
Played an important role in the courses of reaction such as purifying, the purification of vehicle exhaust for dividing.Yet with alumina system itself
Feature, the synthetic method of meso-porous alumina is still be not as ripe as mesopore silicon oxide.
Noble metal catalyst has the advantages that high catalytic activity, high temperature resistant, anti-oxidant, and being that a class is wide variety of important urges
Change material, be also one of study hotspot in recent years.With ordered mesoporous material as catalyst carrier material, using mesopore orbit
Confinement is acted on, and can control to support the growth of nano particle;On the other hand, because different molecular has to the diffusion coefficient in duct
Difference, and vestibule is to the transition state Existential Space restriction effect of catalytic reaction, therefore can be according to substrate, product and transition state
Spatial configuration difference etc. realize shape selective catalysis.
It is conventional mainly to have infusion process and grafting to supporting nanoparticle approach in mesopore orbit.Wherein, infusion process is most
It is conventional.But the committed step of the synthetic method of this similar " casting " technique is metal oxide precursor in mesoporous hole
Efficiency is supported in road, and actual conditions are, in dipping process, metal salt solution is more willing to be adsorbed in duct outer surface, together
When capillarity be unique driving force that solution is moved in duct, if mesoporous wall is very weak with the active force of solution, capillary
Effect can also become very little, cause filling rate of the solution in duct low, at the same nano particle be not easy to it is dispersed.It is repeatedly anti-
Multiple dipping is " nanometer casting " general method of method, but the problem so brought is exactly cumbersome time-consuming synthesis step, is really obtained
The yield of ordered structure can not be equal to soft template method, it is impossible to meet extensive synthesis and further practical demand.
Another common method is grafting, although grafting can ensure that nano-particle enters in duct, however it is necessary that finding suitable
Grafting molecule, and supporting needs the multistep to carry out.
The content of the invention
In order to solve the above technical problems, it is an object of the invention to provide a kind of ordered mesoporous aluminium oxide for supporting noble metal
Material and its synthetic method and application.The synthetic method utilizes hydrophobicity noble metal precursor, your gold can be supported with one-step synthesis
The ordered mesoporous aluminium oxide material of category, it is not necessary to first synthesising mesoporous alumina material, then carried noble metal.
To reach above-mentioned purpose, present invention firstly provides a kind of conjunction of the ordered mesoporous aluminium oxide material for supporting noble metal
Into method, it is comprised the following steps:
(1) after being well mixed acid, alcohol, nonionic surface active agent, hydrophobicity precious metal salt is added (as forerunner
Body) and aluminium salt (as presoma), after being well mixed, obtain a mixed solution;
(2) make the mixed solution that a period of time is kept at 30-60 DEG C;
(3) and then at 300-600 DEG C it is calcined, obtains the described ordered mesoporous aluminium oxide material for supporting noble metal.
In above-mentioned synthetic method, it is preferable that the hydrophobicity precious metal salt includes acetylacetone,2,4-pentanedione platinum, acetylacetone,2,4-pentanedione
The combination of one or more in palladium, acetylacetone,2,4-pentanedione silver, acetylacetone,2,4-pentanedione gold, acetylacetone,2,4-pentanedione ruthenium and acetylacetone,2,4-pentanedione rhodium etc.;More preferably
Ground, the hydrophobicity precious metal salt includes the group of one or more in acetylacetone,2,4-pentanedione platinum, palladium acetylacetonate and acetylacetone,2,4-pentanedione silver
Close.
In above-mentioned synthetic method, it is preferable that the aluminium salt includes aluminum chloride sulphate, aluminum nitrate, aluminium isopropoxide and sulphur
The combination of one or more in sour aluminium etc.;It is highly preferred that the aluminium salt includes aluminum nitrate and/or aluminium isopropoxide.
In above-mentioned synthetic method, it is preferable that the alcohol includes methyl alcohol, ethanol, normal propyl alcohol, isopropanol, n-butanol, different
The combination of one or more in butanol and sec-butyl alcohol etc.;It is highly preferred that the alcohol includes ethanol and/or normal propyl alcohol.
In above-mentioned synthetic method, it is preferable that during the acid is including sulfuric acid, nitric acid, hydrochloric acid, acetic acid and citric acid etc.
The combination of one or more;It is highly preferred that the acid includes nitric acid and/or citric acid.Synthetic method of the invention is adjusted using acid
Section alcoholic solution, makes its aobvious acidity, can just make the slow alcoholysis of aluminium presoma, is easy to form mesoporous structure.
In above-mentioned synthetic method, it is preferable that the nonionic surface active agent includes triblock copolymer.It is more excellent
Selection of land, the triblock copolymer for being used including P123, F127, F68 and Brij-56 etc. in the combination of one or more;Especially
For preferably, the triblock copolymer includes P123 and/or F127.Synthetic method of the invention is high using triblock copolymer
Molecular surface active agent as pore structure template.If using the organic molecule of other ionics as template, by
Smaller in itself in organic molecule, the formwork structure of formation is unstable, and induced synthesis hole wall than relatively thin, in roasting
During duct easily cave in, hardly result in the alumina mesoporous material that high-specific surface area and pore distribution are concentrated.
In synthetic method of the invention, the hydrophobicity precious metal salt, aluminium salt, alcohol, acid and non-ionic surfactant
Agent can participate in reaction in the form of pure material or solution, and the concentration of its solution can carry out conventional tune by those skilled in the art
Section.
In above-mentioned synthetic method, it is preferable that with total matter of the ordered mesoporous aluminium oxide material for supporting noble metal
On the basis of amount, the loading of the noble metal is 0.1-5% (with the gauge of precious metal simple substance), more preferably 0.5%-3.5%.
In above-mentioned synthetic method, it is preferable that on the basis of 25mmol aluminium elements, the nonionic surface active agent
Consumption be 5g-15g.
In above-mentioned synthetic method, it is preferable that step (1) is:Acid, alcohol are mixed with nonionic surface active agent
(can suitably stir), then mix with hydrophobicity precious metal salt and aluminium salt under agitation, continue to stir, make the hydrophobicity noble metal
Salt and aluminium salt dissolve, and obtain a mixed solution.It is highly preferred that mix with hydrophobicity precious metal salt and aluminium salt under agitation, then
The time for continuing to stir is 5-12 hours.
In above-mentioned synthetic method, it is preferable that (mixed solution is presoma to the mixed solution in step (1)
Solution after being completely dissolved) pH value be 1-5.
In above-mentioned synthetic method, the consumption of acid and alcohol can be adjusted by those skilled in the art according to actual conditions
Section, as long as making the pH value of the mixed solution obtained in step (1) in the range of 1-5.
In above-mentioned synthetic method, it is preferable that step (1) is carried out at 10-30 DEG C.
In above-mentioned synthetic method, in step (2) at 30-60 DEG C volatilize time, be according to formed gel (or
Dry glue) effect determine, it is preferable that the time kept at 30-60 DEG C in step (2) is 12-72 hours.More preferably
Ground, step (2) is kept for 36-48 hours at 40-50 DEG C.Synthetic method of the invention is using 30-60 DEG C (preferably using 40-
50 DEG C) come the alcohol equal solvent that volatilizees, the formation of meso-hole structure can be easy to.Preferably, mixed solution can be transferred into air blast to do
In dry case, temperature is set as 30-60 DEG C (preferably using 40-50 DEG C), and the volatilization of alcohol equal solvent is carried out with this understanding.
In above-mentioned synthetic method, it is preferable that the time being calcined at 300-600 DEG C in step (3) is 3-10 hours,
To remove nonionic surface active agent template.It is highly preferred that the sintering temperature in step (3) is 400-500 DEG C, roasting time
It is 4-8 hours;Particularly preferably, roasting time is 4-6 hours.
The present invention utilizes sol-gel process, using nonionic surface active agent as template, due to non-ionic surface
Activating agent has the lipophilic group of two ends hydrophilic radical and centre, can be formed in polar solvent with hydrophobic inner core and polarity
The rod-shaped micelle structure of basic unit.A certain amount of hydrophobicity noble metal precursor body is now added, due to the solubilization of micella, this is hydrophobic
Property noble metal precursor body be more likely to enter micella nonpolar hydrophobic kernel in.Aluminium presoma is subsequently added into, then by solvent
Slow volatilization, presoma and surfactant interact to form mesoporous phase.Finally roasting removes template, so that a step is closed
Into the ordered mesoporous aluminium oxide material for supporting noble metal, without first synthesising mesoporous alumina material, then carried noble metal.
On the other hand, present invention also offers a kind of ordered mesoporous aluminium oxide material for supporting noble metal, it is by upper
The synthetic method of that states the support ordered mesoporous aluminium oxide material of noble metal is preparation-obtained.
In the above-mentioned ordered mesoporous aluminium oxide material for supporting noble metal, it is preferable that support having for noble metal with described
On the basis of the gross mass of sequence mesoporous aluminum oxide material, the loading of the noble metal is 0.1-5% (with the amount of precious metal simple substance
Meter), more preferably 0.5%-3.5%.
The meso-hole structure high-sequential of the ordered mesoporous aluminium oxide material for supporting noble metal that the present invention is provided.According to this hair
Bright specific embodiment, it is preferable that the specific surface area for supporting the ordered mesoporous aluminium oxide material of noble metal is 100-
300m2/ g, pore volume is 0.1-0.8cm3/ g, mesoporous pore size is 1-10nm, and the particle diameter of noble metal nano particles is 1-10nm;More
Preferably, the specific surface area is 100-200m2/ g, pore volume is 0.1-0.5cm3/ g, mesoporous pore size is 3-7nm, and noble metal is received
The particle diameter of rice grain is 2-7nm.
The ordered mesoporous aluminium oxide material for supporting noble metal of present invention offer can ensure noble metal in mesoporous material
High degree of dispersion, improve the rate that supports of noble metal, and the mesoporous hole of high-sequential still can be kept under high loadingses
Road structure, while the confinement effect using duct limits the size of noble metal nano particles.
Additionally, preparing an oxygen present invention also offers a kind of above-mentioned ordered mesoporous aluminium oxide material for supporting noble metal
Change the application in the catalyst of oxidation of coal reaction.
The ordered mesoporous aluminium oxide material for supporting noble metal that the present invention is provided, as the catalysis that Oxidation of Carbon Monoxide reacts
Agent, compared with the noble metal prepared with traditional dipping method supports mesoporous aluminum oxide material, the material of the one-step synthesis method
Material has catalysis activity and heat endurance higher, is a kind of catalyst of high thermal stability.
In sum, the present invention uses one-step synthesis method to support the ordered mesoporous aluminium oxide material of noble metal, the material
Decentralization of the noble metal nano particles in mesoporous material it is high, support that rate is high, noble metal nano particles size is small and mesoporous
Pore passage structure high-sequential, it has catalysis activity and heat endurance high as the catalyst that Oxidation of Carbon Monoxide reacts.
Brief description of the drawings
Fig. 1 is the small angle X-ray diffraction figure of the ordered mesoporous aluminium oxide material for supporting platinum of embodiment 1-5.
Fig. 2 is the Wide angle X-ray diffraction figure of the ordered mesoporous aluminium oxide material for supporting platinum of embodiment 1-5.
Fig. 3 is the nitrogen adsorption desorption curve of the ordered mesoporous aluminium oxide material for supporting platinum of embodiment 1-5.
Fig. 4 is the graph of pore diameter distribution of the ordered mesoporous aluminium oxide material for supporting platinum of embodiment 1-5.
Fig. 5 is the transmission electron microscope photo of the ordered mesoporous aluminium oxide material for supporting platinum of embodiment 1.
Fig. 6 is the transmission electron microscope photo of the ordered mesoporous aluminium oxide material for supporting platinum of embodiment 2.
Fig. 7 is the transmission electron microscope photo of the ordered mesoporous aluminium oxide material for supporting platinum of embodiment 3.
Fig. 8 is the transmission electron microscope photo of the ordered mesoporous aluminium oxide material for supporting platinum of embodiment 4.
Fig. 9 is the transmission electron microscope photo of the ordered mesoporous aluminium oxide material for supporting platinum of embodiment 5.
Figure 10 is the small angle X-ray diffraction figure of the ordered mesoporous aluminium oxide material for supporting platinum of embodiment 6.
Figure 11 is the transmission electron microscope photo of the ordered mesoporous aluminium oxide material for supporting platinum of embodiment 6.
Figure 12 is the small angle X-ray diffraction figure of the ordered mesoporous aluminium oxide material for supporting noble metal of embodiment 7 and 8.
Figure 13 is the nitrogen adsorption desorption curve of the ordered mesoporous aluminium oxide material for supporting noble metal of embodiment 7 and 8.
Figure 14 is the graph of pore diameter distribution of the ordered mesoporous aluminium oxide material for supporting noble metal of embodiment 7 and 8.
Figure 15 is the transmission electron microscope photo of the ordered mesoporous aluminium oxide material for supporting silver of embodiment 7.
Figure 16 is the transmission electron microscope photo of the ordered mesoporous aluminium oxide material of the loaded palladium of embodiment 8.
Figure 17 is the transmission electron microscope photo of the mesoporous aluminum oxide material for supporting platinum of infusion process preparation in embodiment 9.
Figure 18 is CO conversion ratios and temperature relation figure in embodiment 10.
Specific embodiment
In order to be more clearly understood to technical characteristic of the invention, purpose and beneficial effect, now to skill of the invention
Art scheme carry out it is described further below, but it is not intended that to it is of the invention can practical range restriction.
Embodiment 1
To 1.0g nonionic surfactant Pluronic P123 and 20mL ethanol is added in 50mL beakers, at room temperature
Stir to Pluronic P123 dissolvings.Add 8.4g citric acids, after stirring and dissolving, add 0.006g acetylacetone,2,4-pentanediones platinum and
3.75g aluminum nitrates, stir 10 hours even for more time at room temperature, until all dissolvings.After dissolving completely, beaker is transferred to
In air dry oven, opening is placed, and temperature is set as 40 DEG C, solvent volatilization is carried out with this understanding.After 48 hours, solvent is waved
Colloid after hair is taken out, and the colloid is transferred in porcelain crucible, is warming up to 400 DEG C, is calcined 4 hours in air atmosphere at a temperature of this
Template agent removing is removed, powder-product is obtained with agate mortar is finely ground, as support the ordered mesoporous aluminium oxide material of platinum, platinum in the material
The mass percent for supporting is 0.6% (amount of the ordered mesoporous aluminium oxide material for supporting platinum with this with the amount of platinum simple substance is calculated).
The small angle XRD of the material is shown in that Fig. 1, wide-angle XRD are shown in Fig. 2;Nitrogen adsorption desorption curve is shown in Fig. 3, and pore-size distribution is shown in Fig. 4, the material
Aperture changes between 4-6nm;Specific surface area and pore volume are shown in Table 1, and transmission electron microscope (TEM) photo is shown in Fig. 5.
Embodiment 2
Identical with the operating method of embodiment 1, difference is that the acetylacetone,2,4-pentanedione platinum for adding is 0.013g, the quality percentage that platinum is supported
Number 1.3%.The small angle XRD of the material is shown in that Fig. 1, wide-angle XRD are shown in Fig. 2;Nitrogen adsorption desorption curve is shown in Fig. 3, and pore-size distribution is shown in Fig. 4,
The aperture of the material changes between 4-6nm;Specific surface area and pore volume are shown in Table 1, and transmission electron microscope (TEM) photo is shown in Fig. 6.
Embodiment 3
Identical with the operating method of embodiment 1, difference is that the acetylacetone,2,4-pentanedione platinum for adding is 0.021g, the quality percentage that platinum is supported
Number 2.1%.The small angle XRD of the material is shown in that Fig. 1, wide-angle XRD are shown in Fig. 2, and nitrogen adsorption desorption curve is shown in Fig. 3, and pore-size distribution is shown in Fig. 4,
The aperture of the material changes between 4-6nm;Specific surface area and pore volume are shown in Table 1, and transmission electron microscope (TEM) photo is shown in Fig. 7.
Embodiment 4
Identical with the operating method of embodiment 1, difference is that the acetylacetone,2,4-pentanedione platinum for adding is 0.03g, the quality percentage that platinum is supported
Number 3.0%.The small angle XRD of the material is shown in that Fig. 1, wide-angle XRD are shown in Fig. 2;Nitrogen adsorption desorption curve is shown in Fig. 3, and pore-size distribution is shown in Fig. 4,
The aperture of the material changes between 4-6nm;Specific surface area and pore volume are shown in Table 1, and transmission electron microscope (TEM) photo is shown in Fig. 8.
Embodiment 5
Identical with the operating method of embodiment 1, difference is that the acetylacetone,2,4-pentanedione platinum for adding is 0.035g, the quality percentage that platinum is supported
Number 3.5%.The small angle XRD of the material is shown in that Fig. 1, wide-angle XRD are shown in Fig. 2;Nitrogen adsorption desorption curve is shown in Fig. 3, and pore-size distribution is shown in Fig. 4,
The aperture of the material changes between 4-6nm;Specific surface area and pore volume are shown in Table 1, and transmission electron microscope (TEM) photo is shown in Fig. 9.
Embodiment 6
Identical with the operating method of embodiment 1, difference is that 8.4g citric acids are changed into 1.5mL concentrated nitric acids, and 3.75g aluminum nitrates change
It is 2.04g aluminium isopropoxides.The small angle XRD of the material is shown in Figure 10, and transmission electron microscope (TEM) photo is shown in Figure 11.
Embodiment 7
Identical with the operating method of embodiment 1, difference is that 0.006g acetylacetone,2,4-pentanedione platinum is changed into 0.011g acetylacetone,2,4-pentanediones silver, silver
The mass percent 1% for supporting.The small angle XRD of the material is shown in Figure 12;Nitrogen adsorption desorption curve is shown in Figure 13, and pore-size distribution is shown in figure
14, the aperture of the material changes between 7-10nm;Specific surface area and pore volume are shown in Table 1, and transmission electron microscope (TEM) photo is shown in figure
15。
Embodiment 8
Identical with the operating method of embodiment 1, difference is that 0.006g acetylacetone,2,4-pentanedione platinum is changed into 0.016g palladium acetylacetonates, palladium
The mass percent 1% for supporting.The small angle XRD of the material is shown in Figure 12, and nitrogen adsorption desorption curve is shown in Figure 13, and pore-size distribution is shown in figure
14, the aperture of the material changes between 7-10nm;Specific surface area and pore volume are shown in Table 1, and transmission electron microscope (TEM) photo is shown in figure
16。
Embodiment 9
The present embodiment is not added with acetylacetone,2,4-pentanedione platinum, and platinum is supported on mesoporous aluminum oxide material, specific method by the method for impregnating
For:Take the H of 7mL 6.0mmol/L2PtCl6Solution adds the water of 4.5mL and the methyl alcohol of 40.5mL as in the flask of 250mL,
And mesoporous aluminum oxide material, after reacting 3 hours, solid absolute ethyl alcohol and deionized water repeatedly to be washed, centrifugation is obtained
Precipitation, then dries in 100 DEG C of baking ovens, and last 300 DEG C are calcined 2 hours.The mass percent 1.4% that platinum is supported.The material
Specific surface area and pore volume be shown in Table 1, transmission electron microscope (TEM) photo is shown in Figure 17.From Figure 17, it is apparent that Jie of the material
Hole is unordered.
Table 1
Embodiment | 1 | 2 | 3 | 4 | 5 | 6 | 7 | 8 | 9 |
113 | 130 | 160 | 165 | 147 | 120 | 142 | 100 | 156 | |
0.208 | 0.213 | 0.324 | 0.410 | 0.301 | 0.240 | 0.296 | 0.193 | 0.310 |
Embodiment 10
CO catalysis oxidations are tested:The material that embodiment 2 and embodiment 9 are prepared respectively 400 DEG C, 500 DEG C, 600
DEG C, 700 DEG C be calcined 1 hour, then respectively take 25mg, uniformly mix with 4g quartz sands respectively, be placed on size for 1 × 60cm not
In rust steel pipe.Reaction gas composition is CO and 20% O that mass fraction is 1%2, with He as Balance Air.Gas composition after reaction
Detected using gas chromatography, the CO conversion ratios for obtaining are shown in Figure 18 with the graph of a relation of temperature.As seen from Figure 18, implement
The material of example 2 as catalyst, the material of its catalysis activity and heat endurance apparently higher than embodiment 9.
As can be seen from the above-described embodiment, the present invention uses one-step synthesis method to support the ordered mesoporous aluminium oxide of noble metal
Material, the decentralization of the noble metal nano particles of the material in mesoporous material is high, high, the noble metal nano particles size that supports rate
It is small, and mesopore orbit structure height in order, its as Oxidation of Carbon Monoxide react catalyst have catalysis activity high and
Heat endurance.
Claims (1)
1. a kind of synthetic method of the ordered mesoporous aluminium oxide material for supporting noble metal, it is comprised the following steps:
(1) to 1.0g nonionic surfactant Pluronic P123 and 20mL ethanol is added in 50mL beakers, stir at room temperature
Mix to Pluronic P123 dissolvings;
(2) 1.5mL concentrated nitric acids are added, after stirring and dissolving, 0.006g acetylacetone,2,4-pentanediones platinum and 2.04g aluminium isopropoxides, room temperature is added
Lower stirring makes the slow alcoholysis of aluminium isopropoxide in 10 hours even for more time, until all dissolvings;
(3) after dissolving completely, beaker is transferred in air dry oven, opening is placed, temperature is set as 40 DEG C, with this understanding
Carry out solvent volatilization;
After (4) 48 hours, the colloid after solvent is volatilized is taken out, and the colloid is transferred in porcelain crucible, is warming up to 400 DEG C, this
At a temperature of in air atmosphere roasting remove template agent removing within 4 hours, with agate mortar it is finely ground powder-product, as described supporting be expensive
The ordered mesoporous aluminium oxide material of metal.
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KR100814812B1 (en) * | 2006-08-23 | 2008-03-19 | 삼성에스디아이 주식회사 | Catalyst for oxidizing carbon monoxide for reformer used in fuel cell, method for preparing the same, and fuel cell system comprising the same |
CN101579635B (en) * | 2009-06-18 | 2011-07-20 | 上海纳米技术及应用国家工程研究中心有限公司 | Room temperature catalytic oxidation carbon monoxide catalyst and preparation method thereof |
CN102424411A (en) * | 2011-09-15 | 2012-04-25 | 暨南大学 | Preparation method for ordered mesoporous gamma-Al2O3 |
CN104588020A (en) * | 2014-12-17 | 2015-05-06 | 中国人民解放军防化学院 | Preparation method of ordered mesoporous alumina supported metal catalyst |
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