KR101834486B1 - Metal complex oxide composite of core shell structure, manufacturing method thereof, and catalyst complex comprising the same - Google Patents
Metal complex oxide composite of core shell structure, manufacturing method thereof, and catalyst complex comprising the same Download PDFInfo
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- KR101834486B1 KR101834486B1 KR1020150096171A KR20150096171A KR101834486B1 KR 101834486 B1 KR101834486 B1 KR 101834486B1 KR 1020150096171 A KR1020150096171 A KR 1020150096171A KR 20150096171 A KR20150096171 A KR 20150096171A KR 101834486 B1 KR101834486 B1 KR 101834486B1
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- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J19/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
- B01J19/32—Packing elements in the form of grids or built-up elements for forming a unit or module inside the apparatus for mass or heat transfer
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J21/00—Catalysts comprising the elements, oxides, or hydroxides of magnesium, boron, aluminium, carbon, silicon, titanium, zirconium, or hafnium
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- 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
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- B01J2231/00—Catalytic reactions performed with catalysts classified in B01J31/00
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- B01J2231/00—Catalytic reactions performed with catalysts classified in B01J31/00
- B01J2231/70—Oxidation reactions, e.g. epoxidation, (di)hydroxylation, dehydrogenation and analogues
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Abstract
TECHNICAL FIELD The present invention relates to a metal composite oxide composite having a core shell structure, a method for producing the same, and a catalyst composite on which the catalyst is supported. More particularly, the present invention includes a metal aluminum core and a shell composed of a composite metal oxide surrounding the core A metal complex oxide composite having a core shell structure, a method for producing the same, and a catalyst composite on which the catalyst is supported on the composite.
The metal composite oxide composite particles of the core shell structure according to the present invention can be produced by a simple method and include a composite oxide shell containing pores while surrounding the aluminum core, And mass transfer efficiency.
Description
The present invention relates to a metal composite oxide composite having a core shell structure, a method for producing the composite metal oxide complex, and a catalyst composite on which the catalyst is supported on the metal composite oxide composite, and more particularly to a catalyst composite comprising a metal aluminum core and a composite metal oxide A metal complex oxide composite having a core shell structure and improved heat and mass transfer characteristics including a shell, a method for producing the same, and a catalyst composite on which a catalyst is supported on the composite.
A catalyst is a third substance that does not change itself but promotes or inhibits a chemical reaction, and can be divided into an inorganic catalyst and an organic catalyst.
Inorganic catalysts are often used in the form of an inorganic metal fixed to a carrier. Catalyst carrier has a great influence on catalytic activity and selectivity. This is because the catalytic activity and selectivity are different due to the structural characteristics (pore structure, surface area, pore size, pore volume, etc.) of the catalyst support and the unique interaction between the active metal and the catalyst support.
The heat and mass transfer characteristics in the catalyst carrier are also important characteristics affecting the catalytic activity and the reaction activity. The heterogeneous reaction caused by the supported catalyst is additionally required for the mass transfer process in which the reactant moves to the catalyst side because the catalyst is fixed to the carrier, that is, the catalyst is held in the carrier. According to Reactor Analysis and Design and Elements of Chemical Reaction Engineering (author: HS Fogler), the reaction steps in the heterogeneous catalysis are i) the transfer of the reactants in the bulk mixture to the catalyst particles, ii) V) adsorption of the reactants to the active surface, iv) product formation due to the reaction of the reactants, v) product desorption from the active surface, vi) product transfer from the catalyst voids, and vii) It is known that 7 stages of product transfer to the mixture are required.
In other words, surface reaction rate, heat transfer and mass transfer are important factors for the heterogeneous catalytic reaction using the supported catalyst. In particular, heat and mass transfer are very important factors in heterogeneous catalytic reactions used for high endothermic and exothermic reactions. At present, energy loss due to high endothermic and exothermic reaction and inactivation of catalysts are problematic in the process of catalytic reaction (steam reforming of hydrocarbons and oxygenated hydrocarbons, FT synthesis, etc.). Recently, the development of fuel cells and microreactors The heat and mass transfer characteristics of the catalyst are becoming more important as the size of the catalytic reactor and the number of chemical reactors requiring high operating characteristics are increased.
However, the catalytic materials in the conventional chemical reaction and reaction engineering fields are mostly based on ceramics having low thermal conductivity, and there is a great restriction in terms of heat and mass transfer.
Accordingly, in order to improve the low heat and mass transfer rate of the supported catalyst, a catalyst module and wash coat prepared by attaching a porous carrier layer and an active catalyst component on the surface of a metal structure such as a metal plate or a metal net have been used. Such a catalyst composite has a higher thermal conductivity than conventional catalyst carriers, has a faster temperature response characteristic, has a higher surface area per unit volume, can be easily manufactured, and has a high mechanical strength.
However, when the porous structure layer is coated on the metal structure, the adhesion strength of the porous structure layer is weak and a large amount of binder is used.
In order to solve this problem, Korean Patent Application No. 2002-0068210 discloses a method of depositing a catalytically active component after coating a porous metal particle-metal oxide layered particle layer on the surface of a metal structure. In this method, metal particles are first coated on the metal structure, and the metal structure coated with the metal particles is oxidized at 400 to 1200 ° C to form a metal oxide, which is called a metal-metal oxide layered particle coating layer for a catalyst carrier.
Korean Patent Application No. 2005-0005816 discloses a metal-metal oxide for a catalyst carrier in which an aluminum oxide shell is synthesized on the surface by hydrothermal synthesis of metal particles. In this method, an aluminum oxide shell was synthesized by hydrothermal reaction of aluminum metal particles, and a metal-metal oxide structure for a catalyst support was synthesized.
However, in the case of the catalyst module manufactured by the above methods, it is advantageous to increase the adhesion strength of the catalyst particles, but it is difficult to control the morphology of the surface of the structure, and the physical and chemical properties There is a disadvantage that the utilization rate thereof is lowered.
It is an object of the present invention to provide a metal complex oxide composite structure having a core shell structure having a novel structure having excellent heat and mass transfer characteristics and a method of manufacturing the same, in order to solve the problems of the prior art.
The present invention also aims to provide a catalyst composite in which a catalyst is supported on a composite metal oxide composite structure having a core shell structure according to the present invention.
In order to solve the above-described problems, the present invention provides an aluminum core having the following general formula (1): And a composite oxide shell surrounding the aluminum core; The present invention also provides a metal composite oxide composite structure having a core shell structure including the core-shell structure.
Me1 x1 Me2 x2 Me3 x3 Al y O z @ Al
Mn, Zn, Cu, and Fe in the formula (1), 0 < x1, 0 x2, 0 x3, 0 y3, 0 z2, Me1, Selected from the group consisting of
The above formula (1) shows a structure in which aluminum is used as a core and a shell made of a metal oxide consisting of Al and / or metals Me1, Me2, and Me3 surrounds the aluminum core.
In the metal composite oxide structure of the core shell structure according to the present invention, the shape of the core portion is not particularly limited and may be any of a particle shape, a metal plate, a metal rod, a metal fill, a felt, a mat, a mesh, a foam, a foil or a monolith And the metal composite oxide structure of the core shell structure according to the present invention includes all the structures including the composite metal oxide surrounding the core portions of the various shapes.
In the metal composite oxide composite structure of the core shell structure according to the present invention, the shell portion is characterized by being a secondary particle shape in which primary particles of a plurality of metal composite oxides are aggregated. The metal composite oxide composite structure of the core shell structure according to the present invention is characterized in that the shell portion is composed of a composite metal oxide consisting of a core metal and a shell portion composed of secondary particles in which primary particles of a plurality of metal composite oxides grown from the metal core portion are aggregated, The adhesion strength between the two layers can be increased. In the present invention, the size of the primary particles is not particularly limited, and can range from several nanometers to centimeters.
The composite metal oxide composite structure of the core shell structure according to the present invention includes pores formed between the primary particles and has a structure in which the primary particles are dense from the shell portion toward the core portion, And an average pore size of 1.0 to 40.0 nm is preferable because it can prevent the decrease of the reaction selectivity of the catalyst.
In the metal composite oxide composite structure of the core shell structure according to the present invention, the shell portion is a metal complex oxide, which is a bimetal or multimetal structure as shown in
In the metal composite oxide composite structure of the core shell structure according to the present invention, the thickness of the shell portion is 0.1 to 500 탆.
The present invention also relates to
An aluminum powder or metal plate for forming an aluminum core portion, an aluminum structure in the form of a metal rod, a metal fill, a felt, a mat, a mesh, a foam, a foil or a monolith; And dissolving a metal precursor compound for forming a composite oxide shell part surrounding the aluminum core part in distilled water;
Applying heat to the mixed solution to form a composite metal oxide shell on the outer periphery of the core;
Drying the metal composite oxide composite structure of the core shell structure; And
Heat-treating the dried composite metal oxide composite structure having a core shell structure; The present invention provides a method of manufacturing a composite metal oxide composite structure having a core shell structure according to the present invention.
FIG. 1 schematically shows a method of manufacturing a composite structure of a metal-oxide-oxide composite having a core-shell structure according to the present invention in a particle structure.
In the method for producing a composite metal oxide composite body having a core shell structure according to the present invention, a method of applying heat in the step of applying heat is not particularly limited, and a heating method in an autoclave, A heating method in which a microwave is irradiated, and the like can also be used.
In the method for producing a metal complex oxide composite structure having a core shell structure according to the present invention, the metal precursor may be at least one selected from the group consisting of nitrate, acetate, sulfonate, chloride, hydroxide, A carbonate, and a hydrogen carbonate salt.
In the method for manufacturing a composite metal oxide composite body having a core shell structure according to the present invention, the concentration of the metal precursor is 0.1M to 10.0M.
In the method of manufacturing a composite metal oxide composite structure having a core shell structure according to the present invention, heat is applied to 300K to 600K in the step of applying heat to the aqueous solution, and the applied heat is determined according to the produced composite metal oxide .
In the method for manufacturing a composite metal oxide composite structure having a core shell structure according to the present invention, the dried composite structure is subjected to heat treatment at a temperature of 600K to 900K for 0.5 hours to 5 hours.
The present invention also relates to a metal complex oxide composite structure having a core shell structure according to the present invention; And a catalyst supported on the metal composite oxide composite structure of the core shell structure; ≪ / RTI >
In the catalyst composite according to the invention, the catalyst may comprise non-noble metals, noble metals and / or mixtures or alloys thereof. Suitable non-noble metals may be selected from transition metal groups of the element cycle system (PSE) Select. Examples include aluminum (Al), titanium (Ti), vanadium (V), chromium (Cr), manganese (Mn), iron (Fe), cobalt (Co), nickel (Ni), copper ), Zirconium (Zr), niobium (Nb), molybdenum (Mo), tantalum (Ta), tin (Sn), tungsten (W) and rhenium (Re) ), Rhodium (Rh), iridium (Ir), palladium (Pd), platinum (Pt), silver (Ag) and gold (Au).
In the catalyst composite according to the present invention, the catalyst is more preferably Rh (rhodium), Ru, Pt, Ir, Pd, Ni, Co, , Iron (Fe), and the like.
The catalyst composite according to the present invention is not limited to hydrogenation, dehydrogenation reaction, epoxidation reaction, isomerization reaction, alkylation reaction, cracking reaction, reforming reaction, hydrogenation desulfurization reaction, polymerization reaction and the like depending on the supported catalyst And the reforming reaction for generating the hydrogen gas may include a steam reforming reaction, a partial oxidation reaction, etc. The catalyst complex according to the present invention may include steam reforming of hydrocarbons and oxygenated hydrocarbons, FT synthesis, etc. Endothermic reaction, CO oxidation, VOC oxidation reaction, and the like.
The metal complex oxide composite structure of the core shell structure according to the present invention can be manufactured by a simpler synthesis method than the metal ceramic composite material used in the prior art, and includes a composite oxide shell surrounding the aluminum core and containing pores, The catalyst composite having the catalyst supported thereon is excellent in heat and mass transfer efficiency and is thus applicable to various applications such as a multilayer ceramic capacitor, a secondary battery, a medical device and a catalyst. It is possible.
FIG. 1 schematically shows a method for producing a composite metal oxide composite structure having a core shell structure according to the present invention.
Fig. 2 shows SEM photographs of the particles produced in the examples of the present invention.
3 shows the results of measuring the shell thickness, surface area, pore size and pore volume of the particles prepared in the examples of the present invention.
FIG. 4 shows the results of measurement of XRD characteristics of the particles produced in the examples of the present invention.
5 shows the results of measurement of the TEM characteristics of the particles produced in the examples of the present invention.
6 shows the results of measuring the XPS characteristics of the particles produced in the examples of the present invention.
Fig. 7 shows TEM photographs of the catalyst composite for glycerol reforming prepared in Examples and Comparative Examples of the present invention before and after the reforming reaction.
8 shows SEM photographs and XRD measurements of the glycerol reforming catalyst composite prepared in Examples and Comparative Examples of the present invention before and after the reforming reaction.
FIG. 9 shows the results of measuring the turnover frequency (TOF) of the catalyst composite for glycerol reforming prepared in Examples and Comparative Examples of the present invention.
Hereinafter, the present invention will be described in more detail by way of examples. However, the present invention is not limited by the following examples.
< Example >
(NO 3 ) 2 .6H 2 O, Co (NO 3 ) 2 .6H 2 O and Zn (NO 3 ) 2 as a metal precursor compound for forming a shell part surrounding the core, · 6H 2 O dissolved in water was prepared, and the aqueous solution and the aluminum powder were mixed in an autoclave.
The Mg (NO 3) 2 · 6H 2 O to perform for three hours the hydrothermal synthesis and that the temperature is maintained at 473K as a PID control to the metallic core when used - producing the particles of the shell structure, and the Co (NO 3) 2 In the case of 6H 2 O and Zn (NO 3 ) 2 .6H 2 O, the reaction was performed for 3 hours while maintaining the temperature by applying heat to 423K to prepare a composite structure having an aluminum core.
The prepared particles were washed several times with distilled water, dried at 393K for 12 hours, and then heat-treated at 823K for 4 hours to prepare composite particles of a metal core-ceramic shell structure.
< Comparative Example >
As Comparative Example 1, an Al powder was placed in distilled water and r-Al 2 O 3 Al .
As Comparative Example 2, without adding a separate core portion, the aluminum precursor Al (NO 3) 2 · 9H 2 O, and a metallic precursor compound Mg (NO 3) 2 · 6H 2 O, Co (NO 3) 2 · 6H 2 O , and Zn (NO 3 ) 2 · 6H 2 O were mixed and the pH was maintained at 9.5.
The compounds and synthesis conditions used in Examples and Comparative Examples are shown in Table 1 below.
compound
Compound concentration
Temperature
< Experimental Example > SEM Photo measurement
SEM photographs of S1 to S4 particles of Comparative Example 1 and Example were measured and the results are shown in Fig.
In FIG. 2, it can be seen that the thickness of MgAl 2 O 4 @ Al (S1) is 2 to 3 μm in the cross-sectional SEM photograph.
It can also be seen that the structure of the surface primary particles varies depending on the type of the metal precursor added for forming the shell part in the S1 to S4 particles.
< Experimental Example > Measurement of particle properties
The shell thickness, surface area, pore size, and pore volume of the particles prepared in the above Examples and Comparative Examples were measured and the results are shown in Table 2 and FIG.
The shell thickness in Table 2 is a calculated result for an average diameter of 10 占 퐉 using XRD measurement results, and the numerical values in parentheses are the surface area and the pore volume, both represents the measured results by considering, brackets in front of a number to the exception of the core and represents a value in terms of only the value of the shell, MgAl 2 O 4 (cop) , ZnAl 2 O 4 (cop), CoAl 2 O 4 ( cop) shows a comparative example prepared by coprecipitation.
In Table 2 and FIG. 3, the average particle size of the aluminum core-composite oxide shell particles prepared according to the embodiment of the present invention is distributed in the range of 3.0 nm to 4.0 nm, and the average pore size , And the pore volume is large.
< Experimental Example > XRD Measure
The XRD characteristics of the particles prepared in the above examples were measured and the results are shown in FIG.
In FIG. 4, the portion indicated by blue is the portion indicated by the aluminum core, and the portion indicated by red indicates the peak due to the compound forming the shell. In Fig. 4, it can be seen that each particle shows both the peak due to the aluminum core and the peak due to the compound forming the shell.
< Experimental Example > TEM Measure
The TEM characteristics of the particles prepared in the above examples were measured and the results are shown in FIG. In FIG. 5, it can be seen that the shapes of the primary particles constituting the secondary particles vary depending on the metal used for forming the shell portion.
< Experimental Example > XPS Measure
The XPS characteristics of the particles prepared in the above examples were measured and the results are shown in FIG. From the XPS results in FIG. 6, the binding energy of the particles prepared according to the embodiment of the present invention can be confirmed, and it can be confirmed that the particles are spinel bimetal crystallites.
< Example 2> Rh The catalyst Supported Particle manufacturing of metallic core-ceramic shell structures and CO chemisorption Experiment
Rh precursor of RhCl 3 · xH MgAl 2 O of the prepared particles to the aqueous solution 2 O 4 @Al And MgAl 2 O 4 prepared in the above Comparative Example were supported by incipient wetness impregnation to synthesize a catalyst composite.
The synthesized catalyst was dried at 393K for 12 hours and heat treated at 873K for 4 hours to prepare Rh catalyst supported core - shell structure particles.
< Experimental Example > Measurement of catalytic activity for glycerol liquid phase reforming reaction
The dispersion degree and the particle size of the Rh catalyst supported in the particles of the aluminum core-shell structure impregnated with Rh catalyst prepared in Example 2 were measured using Co adsorption, and the results are shown in Table 3 below.
In Table 3, in the case of the particles of the aluminum core-shell structure supported with Rh catalyst prepared according to the example of the present invention, the dispersibility of the supported Rh catalyst particles was increased and the size of the catalyst particles was decreased as compared with the comparative example, It can be confirmed that the deterioration of the catalyst properties due to the increase of the particle size is improved.
< Experimental Example > TEM Photo measurement
TEM photographs of the particles before and after the glycerol liquid phase reforming reaction of the aluminum core-shell structure particles supported on the Rh catalyst prepared in the above Examples and Comparative Examples were measured and the results are shown in FIG.
< Experimental Example > Particle stability evaluation - SEM And XRD Measure
SEM photographs and XRD of the particles before and after the glycerol liquid phase reforming reaction of the aluminum core-ceramic shell structure particles loaded with Rh catalyst prepared in the above example were measured and the results are shown in FIG.
8, the particle size and morphology of the aluminum core-shell structure supported on Rh catalyst prepared in the example of the present invention did not change before and after the catalytic reaction. From this, the Rh catalyst prepared in the example of the present invention It can be seen that the particles of the supported metal core-ceramic shell structure are thermally chemically stable.
< Experimental Example > Glycerol conversion rate measurement
The reforming reaction of glycerol was carried out in a fixed-bed reactor under a high-pressure atmosphere under the following conditions.
A fixed bed quartz reactor (
The liquid and unreacted products at the end of the reactor were separated by using a condenser at -4 ° C. The gas products were analyzed in real time at constant intervals using a gas chromatograph equipped with a thermal conductivity sensor.
The glycerol reforming reaction turnover frequency (TOF) at each catalyst was measured at three space velocities (WHSV = 17000, 34000, 68000 mL / g.h and the results are shown in FIG.
FIG. 9 shows that the catalyst activity of Rh was significantly increased when supported on the aluminum core-shell particles prepared in the example of the present invention.
Claims (15)
Aluminum core; And
A composite oxide shell surrounding the aluminum core;
A metal complex oxide composite structure having a core shell structure
???????? Me x Al y O z @ Al
(Wherein 0 <x, 0 <y? 3, 0 <z? 6 in Formula 1, Me is selected from the group consisting of Mg, Co, Ni, Mn, Zn, Cu and Fe).
Wherein the core is in the form of a particle or a metal plate, a metal rod, a metal fill, a felt, a mat, a mesh, a foam, a foil or a monolith.
Wherein the shell portion is a secondary particle shape in which primary particles are aggregated.
Wherein the pores are formed between the primary particles and the average pore size is 1.0 to 40.0 nm.
Wherein the shell portion is a bimetal or multimetal structure.
And the shell portion has a thickness of 0.1 to 500 탆.
Applying heat to the mixed solution to form a composite metal oxide shell on the outer periphery of the core;
Drying the metal composite oxide composite structure of the core shell structure; And
Heat-treating the dried composite metal oxide composite structure having a core shell structure; Wherein the metal-composite oxide composite structure has a core-shell structure according to claim 1.
Wherein the metal precursor is acetate, nitrate, sulfonate, or chloride. The method of claim 1, wherein the metal precursor is selected from the group consisting of acetate, nitrate, sulfonate, and chloride.
Wherein the concentration of the metal precursor is 0.1M to 10.0M.
Wherein the heat is applied to the mixed solution at a temperature of 300K to 600K in the step of applying heat to the mixed solution.
In the step of applying heat to the mixed solution, heat is applied by a method of heating the mixed solution with an autoclave, a method of applying microwave, a method of heating by hot wire, or a method of heating by radiant heat. A method for producing a composite oxide composite structure.
Wherein the dried particles are heat-treated at a temperature of 600K to 900K for 0.5 hours to 5 hours in the step of heat-treating the dried particles.
A catalyst supported on the metal composite oxide composite structure of the core shell structure; ≪ / RTI >
The catalyst supported on the metal-composite oxide composite structure of the core-shell structure includes at least one of aluminum (Al), titanium (Ti), vanadium (V), chromium (Cr), manganese (Mn), iron (Fe), cobalt (Ni), copper (Cu), zinc (Zn), zirconium (Zr), niobium Nb, molybdenum Mo, tantalum Ta, tin Sn, tungsten W and rhenium Re, (Au) selected from the group consisting of Rh (rhodium), ruthenium (Ru), osmium (Os), rhodium (Rh), iridium (Ir), palladium (Pd), platinum Lt; RTI ID = 0.0 > 1 < / RTI >
Wherein the catalyst composite is used for hydrogenation, dehydrogenation, epoxidation, isomerization, alkylation, cracking, reforming, hydrodesulfurization, and polymerization.
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| KR20230048675A (en) | 2021-10-05 | 2023-04-12 | 포항공과대학교 산학협력단 | Catalyst For Ammoxidation Having Core Shell Structure and Making Process Thereof |
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| KR102349759B1 (en) * | 2017-08-14 | 2022-01-11 | 한국전기연구원 | Method of manufacturing piezo-electric ceramic element using internal electrode |
| WO2020106013A1 (en) * | 2018-11-19 | 2020-05-28 | 주식회사 엘지화학 | Catalyst for oxidative dehydrogenation reaction, and method for producing same |
| KR102436310B1 (en) * | 2018-11-19 | 2022-08-25 | 주식회사 엘지화학 | Catalyst for oxidative dehydrogenation and method for manufacturing the catalyst |
| CN111422926B (en) * | 2020-04-10 | 2021-06-29 | 浙江帕瓦新能源股份有限公司 | Core-shell structure Al/La co-doped high-nickel ternary precursor and preparation method thereof, and anode material |
| CN116550326A (en) * | 2022-01-28 | 2023-08-08 | 中国科学院大连化学物理研究所 | Pretreatment method of cobalt-based Fischer-Tropsch synthesis catalyst before being used for Fischer-Tropsch synthesis reaction |
| CN115385436B (en) * | 2022-08-27 | 2023-12-29 | 西南石油大学 | Method for treating sewage by uniformly loading zero-valent iron catalytic particles of core-shell graphene oxide |
| CN115779927B (en) * | 2022-12-08 | 2024-05-03 | 万华化学集团股份有限公司 | Cobalt-aluminum shell-core composite oxide loaded monoatomic iridium catalyst and preparation method and application thereof |
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| Xiaohong Wang 외 4, Current advances in precious metal core-shell catalyst design, Sci. Technol. Adv. Mater. Vol.15(2014.08.05.) |
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| KR20230048675A (en) | 2021-10-05 | 2023-04-12 | 포항공과대학교 산학협력단 | Catalyst For Ammoxidation Having Core Shell Structure and Making Process Thereof |
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