Catalyst support for synthesis gas production, and catalyst using same

Abstract

The present invention relates to a catalyst support for synthesis gas production, and a catalyst using same. More specifically, a catalyst support used for supporting an active component in a catalyst that is used in synthesis gas production using a reforming reaction in which various reducing agents are used has specific physical properties. Therefore, the present invention relates to a catalyst support and a catalyst prepared using same, the catalyst support being developed such that, if a specific active component of a catalyst is immersed therein and the catalyst is applied to synthesis gas production using a reforming reaction, an excellent catalytic activity effect can be exhibited.

Description

Catalyst support for synthesis gas production and catalyst using the same

[0001] The present invention relates to a catalyst support for synthesis gas production and a catalyst using the same, and more particularly, to a catalyst support developed to have specific physical properties for carrying an active component of a catalyst used for synthesis gas production by a reforming reaction using various reducing agents, and to a catalyst support developed to exhibit excellent catalytic activity when a specific active component of the catalyst is immersed therein and applied to synthesis gas production, and a catalyst manufactured using the same.

[0002] Unless otherwise indicated herein, the materials described in this section are not prior art to the claims of this application, and their inclusion in this section is not intended to be admitted as prior art.

[0003] The development of the petrochemical industry has resulted in the production of numerous carbon-based environmental pollutants. While it would be desirable to suppress the production of these carbon-based gases, capturing and utilizing the gases inevitably generated during industrialization not only has a positive impact on the atmospheric environment, but also offers economic benefits by expanding resource utilization.

[0004] Among the gases generated from these industrial sites, various studies are being conducted on using biogas as fuel. This generally involves carrying out a reforming reaction to efficiently utilize reducing gases such as carbon dioxide and methane generated during industrialization or other animal activities.

[0005] As a method for producing synthesis gas from such reducing gas, methods such as dry reforming, wet reforming, or composite reforming, which are summarized by the following reaction formula, are known.

[0006] Dry reforming: CO2+ CH4→ 2CO + 2H2O (ΔH=261 kJ / mol)

[0007] Wet reforming: H2O + CH4→ 3H2+ CO (ΔH=226 kJ / mol)

[0008] Complex reforming: CO2+ 3CH4+ 2H2O → 4CO + 8H2 (ΔH=712 kJ / mol)

[0009] Among the reforming reactions using the above-mentioned reducing gas, dry reforming is a synthesis gas production technology that can use the largest amount of CO2 (greenhouse gas) as a raw material among catalytic reforming technologies, and there is great interest worldwide in securing dry reforming technology due to its high greenhouse gas reduction effect.

[0010] In particular, the dry reforming reaction requires a higher proportion of CO2 for chemical product production than other reforming reactions and has a high impact on greenhouse gas reduction, so efforts are being made to secure excellent reaction technology.

[0011] However, in this dry reforming reaction, a catalyst is used to carry out the reaction, and the dry reforming (DRM) technology that can reduce greenhouse gases has fatal shortcomings such as the important catalyst performance and the difficulty in commercializing the catalyst due to carbon deposition and short catalyst life.

[0012] In this way, catalysts for producing synthesis gas, such as catalysts for reforming reactions, have been continuously developed for decades, but they still have the problem of extremely limited lifespan due to deactivation of the catalyst surface and damage to the formulation.

[0013] Therefore, various studies have been proposed to improve the performance and extend the service life of catalysts in the production of synthesis gas through reforming reactions. However, there is a lack of technological approaches other than extending the service life by specifying the composition of the catalyst.

[0014] In particular, although the catalyst components are important, the physicochemical properties of the carrier that supports the catalyst are also important factors. However, research on the catalyst carrier is sluggish due to the focus on the active components of the catalyst.

[0015] Regarding the support of the existing catalyst for producing synthesis gas, Korean Patent Registration No. 10-2035735 proposes a reforming catalyst composition in which a catalyst support is manufactured through a step of forming a catalyst structure having a perovskite crystal structure, a step of forming a catalyst support by extruding the catalyst structure into a predetermined shape, and a step of coating a metal precursor thereon to manufacture a catalyst.

[0016] In addition, Korean Patent Registration No. 10-2056384 discloses a dry reforming catalyst characterized in that an active material is impregnated on the surface of a metal oxide support, and the active material is surrounded by a surfactant, and in this case, the use of a magnesium oxide support as the metal oxide support is proposed. In addition, Korean Patent Registration No. 10-1457098 proposes a homogenous catalyst formed as a single phase by doping yttrium and ruthenium within the perovskite lattice of SrTiO3.

[0017] However, in the case of these conventional supports for synthesis gas production, there was no specific proposal regarding the chemical properties of the support surface based on the fact that they are catalysts for synthesis gas production using waste gases such as hydrocarbon gases, so there were limitations in the effective catalyst composition such as improvement of catalyst activity such as conversion rate or extension of lifespan.

[0018] In addition, Korean Patent Registration No. 10-2194440 proposes a dry reforming catalyst manufactured by supporting an aluminum oxide support powder containing a bayerite and nordstrandite type crystal structure and loading an active ingredient thereon, thereby proposing a technology that applies a powder-type support. However, while this case appears to be an advanced configuration in that the support is provided in powder form, there is room for improvement in that the powder form may present difficulties in processing and may limit its usability.

[0019] Therefore, in the recent situation where environmental issues such as carbon neutrality and ESG are on the rise, there is an urgent need to develop catalyst supports and catalyst compositions utilizing them to improve the performance of catalysts for synthesis gas production using various reducing agents, as well as to solve problems in industries where various types of gas emissions occur, as part of eco-friendly technology development.

[0020] {Prior art literature}

[0021] [Patent Document]

[0022] (Patent Document 1) Korean Patent Registration No. 10-2035735

[0023] (Patent Document 2) Korean Patent Registration No. 10-2056384

[0024] (Patent Document 3) Korean Patent Registration No. 10-1457098

[0025] (Patent Document 4) Korean Patent Registration No. 10-2194440

[0026] The present invention aims to solve the problems of the prior art as described above by improving the support composition of a catalyst for producing synthesis gas through a reforming reaction using various reducing agents.

[0027] Therefore, the purpose of the present invention is to provide a support for a catalyst for producing synthesis gas having excellent physicochemical properties.

[0028] In addition, another object of the present invention is to provide a catalyst for producing synthesis gas by carrying an active ingredient on a catalyst support having such excellent physical properties.

[0029] The purpose of the present invention is not limited to the above-mentioned purpose, and should be understood to include all purposes that can be inferred from the composition of the invention described in the detailed description or claims of the present invention, or all purposes that can be achieved by the description or technical idea of ​​the present invention.

[0030] In order to solve the above-described problem of the present invention, the present invention provides a catalyst support for synthesis gas production, which is a porous molded body including one or more components of cordierite, SiC, Al2O3, SiO2, and MgO, and is characterized by a moisture absorption rate of 15 to 53% and a cell density of 25 to 700 cpsi (cell per square inch).

[0031] According to a preferred embodiment of the present invention, the porous molded body may be made of cordierite having a cell density of 100 to 300 cpsi, or three kinds of oxides of Al2O3, SiO2, and MgO.

[0032] According to a preferred embodiment of the present invention, the porous molded body may have a specific surface area of ​​0.1 to 5 m2 / g and a density of 0.5 to 0.7 g / mL.

[0033] According to a preferred embodiment of the present invention, the porous molded body may be formed of a porous lattice structure having a wall thickness of 0.3 to 0.8 mm.

[0034] In addition, the present invention provides a catalyst for producing synthesis gas, which is a porous molded body including at least one component among cordierite, SiC, Al2O3, SiO2, and MgO as described above, and is coated on a catalyst support for producing synthesis gas having a moisture absorption rate of 15 to 53% and a cell density of 25 to 700 cpsi, by supporting an active component for a reforming reaction with at least one element selected from a group consisting of elements corresponding to groups 1 to 2, 7 to 13, and 16 among elements of three or more periods.

[0035] According to a preferred embodiment of the present invention, the active ingredient may contain Ni:Co in a weight ratio of 1::0.01 to 1.

[0036] The catalyst support for synthesis gas production according to the present invention is a porous molded body having excellent porosity, and by configuring the moisture absorption rate and cell density, etc. within a specific range to improve the surface properties of the support, it is possible to maintain excellent catalytic activity and reactivity, etc.

[0037] In addition, the catalyst support of the present invention has excellent mechanical strength and heat transfer characteristics, and when the internal composition thickness and water absorption rate are controlled, the absorption depth and coating degree of the active ingredient mother liquid immersed in the catalyst support are controlled accordingly, thereby producing a catalyst for reforming reaction with excellent physical properties in which the active ingredient is highly dispersed.

[0038] In particular, the catalyst in which the active ingredient is immersed in the catalyst support according to the present invention is configured to suppress the deactivation of the catalyst and carbon deposition due to deterioration even at a high reaction temperature, and thus has properties with improved thermal durability and can exhibit characteristics that enable long-term use.

[0039] The effects of the present invention are not limited to the effects described above, and should be understood to include all effects that can be inferred from the detailed description of the present invention or the composition of the invention described in the claims.

[0040] Figure 1 is a graph comparing the conversion rates of methane and carbon dioxide in Examples 1 to 4 according to the present invention.

[0041] Figure 2 is a graph showing the conversion rates of methane and carbon dioxide and the ratio of converted hydrogen / carbon monoxide in Example 1 according to the present invention.

[0042] Figure 3 is a graph showing the methane and carbon dioxide conversion rates and the converted hydrogen / carbon monoxide ratio in Comparative Example 1 according to the present invention.

[0043] Figure 4 is a photograph showing an electron scanning microscope image of a support applied to an example or comparative example according to the present invention.

[0044] Hereinafter, the present invention will be described in more detail as an embodiment.

[0045] The present invention relates to a catalyst support configured to have a specific physical property when a porous molded body is configured to have a specific physical property and an active component of a catalyst is supported thereon to form a catalyst, and to a catalyst manufactured using the same so as to exhibit an excellent catalytic activity effect.

[0046] According to a preferred embodiment of the present invention, the catalyst support according to the present invention can be manufactured in the form of a porous molded body using, for example, cordierite, SiC, Al2O3, SiO2, MgO, etc.

[0047] According to a preferred embodiment of the present invention, such a porous molded body can be manufactured to have the characteristics of, for example, a moisture absorption rate of 15 to 53% and a cell density of 25 to 700 cpsi, more preferably 100 to 300 cpsi. If the moisture absorption rate exceeds 53%, the durability of the catalyst is reduced, which makes it difficult to handle during the catalytic reaction process, and in particular, for example, the conversion rate of the gas to be reformed may be significantly reduced. In addition, if the moisture absorption rate is too low, such as less than 15%, it is difficult to expect the effect of producing synthesis gas, and the conversion rate is rapidly reduced. In addition, if the cell density is lower than the above range, when forming a molded body, the mechanical properties are reduced, the moldability is reduced during the production of the molded body, and there are problems in that many defects occur. In addition, if the cell density is too high, the conversion rate is reduced, which is uneconomical.

[0048] According to a preferred embodiment of the present invention, it is more preferable when the porous molded body is composed of, for example, cordierite having a cell density of 100 to 300 cpsi or a mixture of two or more of Al2O3, SiO2 and MgO. Here, the composition of the porous molded body is particularly preferable to be composed of three oxides of Al2O3, SiO2 and MgO in order to have excellent moldability and to effectively support the active ingredient. For example, cordierite composed of a material of 2MgO-2Al2O3-5SiO2 can exhibit desirable physical properties.

[0049] According to a preferred embodiment of the present invention, the porous molded body may have a specific surface area of ​​0.1 to 5 m2 / g and a density of 0.5 to 0.7 g / mL. If the specific surface area is too low, the conversion rate of the catalytic reaction decreases, and if it is too high, the mechanical properties deteriorate rapidly and the moldability is poor.

[0050] According to a preferred embodiment of the present invention, the porous molded body may be formed of a porous lattice structure having a wall thickness of 0.3 to 0.8 mm, such as a honeycomb structure. This honeycomb structure does not mean a structure having a simple hexagonal cross-sectional structure with a large number of pores, but includes a structure in which the cross-sectional shape of the pores forms a polygonal circle, such that the porosity can perform the same function as the honeycomb structure. Most preferably, it is good to form a hexagonal cross-sectional pore structure.

[0051] According to a preferred embodiment of the present invention, the porous molded body of the porous lattice structure of the present invention may have porosity of nanostructures, mesostructures, and macrostructures on the honeycomb side wall surface in addition to the porosity formed by, for example, the honeycomb structure. The porous molded body of the porous lattice structure such as the honeycomb structure of the present invention may typically have a structure such as a cylinder, a polygonal column, a disc, or a polygonal plate.

[0052] According to a preferred embodiment of the present invention, the porous molded body can be applied in the form of particles of an appropriate size in addition to a honeycomb structure as a preferred form, and can be applied to the manufacturing of various types of molded bodies. The use of a porous support is required, and the pore characteristics of the support can be controlled when manufacturing the support or through chemical treatment of the manufactured support. In addition, such a porous support has a channel opening (d h ) can be characterized by size and shape, open frontal area (OFA), cell density (cpsi), etc. Here, the opening (d h ) A support having various size characteristics of 0.5-8 mm can be used, and the size of the opening can be selected and used according to the application field such as automobile catalyst, SCR, etc. For example, a support having an opening size of 0.5-4 mm can be used.

[0053] According to a preferred embodiment of the present invention, in the case of a porous molded body in the form of a porous lattice structure such as the honeycomb structure described above, for example, a support having a front opening area of ​​30-88% can be selected and used depending on the field of application, and preferably, a support having a front opening area of ​​30-80% can be used.

[0054] According to one embodiment of the present invention, the cell density of the porous lattice structure support made of the porous molded body may be, for example, a support having a cell density in the range of 25 to 700 cpsi, preferably a support having a cell density characteristic in the range of 50 to 600 cpsi, and more preferably a support having a cell density characteristic in the range of 100 to 300 cpsi.

[0055] According to the present invention, the porous support of the present invention as described above can be manufactured by, for example, a wash coating method in which all active substances are loaded at once, a method in which active substances are loaded sequentially, or a method in which the surface of the support is given functionality through acid or base treatment before loading the active substance and then loading the active substance, and such a molded body can be manufactured by, for example, 450 to 700 o It can be manufactured by firing at C for 3 to 6 hours.

[0056] According to a preferred embodiment of the present invention, the catalyst support of the present invention having the above-described characteristics may be, for example, a wall-flow monolith, cordierite, silicon carbide, etc. Each channel forming the porous molded body of the present invention may preferably have a square shape, a honeycomb structure, etc., and may have a form in which adjacent channels are alternately blocked.

[0057] According to one embodiment of the present invention, the wall surface of the wall flow monolith may have, for example, a filter porosity of 45 to 50 volume% and a pore size of about 10 to 15 um.

[0058] According to one embodiment of the present invention, cordierite can be suitably used in smoke purification devices when thermal durability is required because it has a high thermal shock parameter. In particular, cordierite has a melting point of 1,450 o C can also be used for high-temperature reactions, in which case it is desirable to maintain the filter removal efficiency by making the pore structure uniform and preventing pore closure.

[0059] According to one embodiment of the present invention, a silicon carbide monolith can be manufactured by extruding SiC powder, and an additive can be added to form pores or control the pore shape during the extrusion process. Here, the extruded monolith is manufactured in a vacuum at 2,000 o Because it is manufactured by calcination at temperatures above C, it can be applied to high-temperature reactions.

[0060] According to a preferred embodiment of the present invention, maintaining the moisture absorption rate within a specific range in the catalyst support composition of the present invention can have a significant effect on the catalyst activity.

[0061] According to one embodiment of the present invention, the monolithic support, as presented as an example in the present invention, has a small specific surface area but has a structure that is elongated in the axial direction, facilitating contact with gaseous reactants. Therefore, due to these structural characteristics, the monolithic support has the advantage of not experiencing a pressure drop due to carbon deposition during the reaction.

[0062] The catalyst support formed of a porous molded body according to the present invention has excellent mechanical properties and, in particular, excellent physicochemical properties such as a moisture absorption rate that maintains a specific range, resulting in excellent catalytic activity and excellent moldability. In particular, the catalyst support of the present invention has excellent thermal stability even in high-temperature reactions, thereby suppressing deactivation due to catalyst deterioration, carbon deposition, etc.

[0063] According to a preferred embodiment of the present invention, the catalyst support of the present invention, when manufactured into a honeycomb structure, has a structure with channels, and thus has excellent mechanical strength and heat transfer characteristics, and has a water absorption rate that varies depending on the thickness of the internal composition, and accordingly, by controlling the absorption depth and coating degree of the active ingredient mother liquid immersed in the catalyst support, it can be manufactured into a catalyst for producing synthesis gas through a reforming reaction with excellent physical properties in which the active ingredient is highly dispersed. In particular, the catalyst support of the present invention can be suitably utilized as a catalyst for producing synthesis gas through a reforming reaction using carbon dioxide and various reducing agents. For example, it can be suitably used as a support for a catalyst for dry reforming or combined reforming reaction using methane and carbon dioxide.

[0064] In the present invention, the reducing agent is defined as a reducing agent that produces synthesis gas by reducing CO2, and mostly refers to a reducing gas that is a gaseous substance. Such reducing gases include, for example, hydrocarbons such as methane, ethane, and propane, or mixtures thereof, or compounds in which these are mixed. Examples of such reducing gases may include mixtures of CH4, CO2, H2, O2, N2, etc. In addition, reducing gases may typically include carbonaceous biogas, industrial gases produced as by-products from industrial activities, carbonaceous mixed gases, greenhouse gases such as methane or carbon dioxide, unreacted products, by-products, and volatile organic compounds generated in factories. Examples of biogas among these may include methane, ethane, propane, butane, alcohols, ketones, and aldehydes.

[0065] Meanwhile, the present invention can manufacture a catalyst for producing synthesis gas by coating the catalyst support for producing synthesis gas of the present invention as described above with at least one element selected from the group consisting of elements corresponding to groups 1 to 2, 7 to 13, and 16 among elements of groups 3 or more as a catalytic active ingredient for reforming reaction.

[0066] According to a preferred embodiment of the present invention, the active component may be a Ni-Co catalyst. For example, the catalyst may be manufactured by supporting the catalyst component so that Ni:Co is contained in a weight ratio of 1:0.01 to 1.

[0067] In addition, according to a preferred embodiment of the present invention, one or more metal components selected from among noble metal components, for example, Zr, Ti, and Ce, may be additionally included as a cocatalyst.

[0068] In this way, the catalyst in which the active ingredient is immersed in the catalyst support according to the present invention is configured to suppress the deactivation of the catalyst and carbon deposition due to deterioration even at a high reaction temperature, and thus has properties with improved thermal durability and can exhibit characteristics that enable long-term use.

[0069] Hereinafter, the present invention will be described based on examples, but the present invention is not limited to the examples.

[0070] [Example 1]

[0071] It is composed of 2MgO-2Al2O3-5SiO2 and has a moisture content of 19% and a specific surface area of ​​0.3 m 2 / g, a honeycomb structure of a cordierite support with a channel wall thickness of 0.32 mm and a cell density of 200 cpsi was used as a support for a catalyst for producing synthesis gas by reforming reaction.

[0072] The catalyst used in this sample was prepared by fixing the total active ingredient content to 1.5 wt%, preparing the main active ingredient, nickel-cobalt, at a 1:1 ratio, and then adding 0.05 wt% of palladium and 0.2 wt% of zirconium as cocatalyst ingredients.

[0073] The cordierite support was immersed in the prepared active ingredient solution so that the active ingredient was absorbed into the support. The cordierite support with the active ingredient absorbed was blown with an air gun to remove excess active ingredient solution, and 100 oC and dried in an oven for more than 12 hours. The prepared catalyst was calcined at 500°C for 4 hours to prepare the catalyst of Example 1.

[0074] [Example 2]

[0075] A cordierite support with a cell density of 200 cpsi composed of 2MgO-2Al2O3-5SiO2 was treated with alumina sol at room temperature to obtain a moisture content of 16.3% and a specific surface area of ​​0.38 m 2 A support of / g was prepared.

[0076] The catalyst of Example 2 was prepared by supporting the active ingredient on the prepared cordierite support in the same manner as in Example 1.

[0077] [Example 3]

[0078] A cordierite support with a cell density of 200 cpsi composed of 2MgO-2Al2O3-5SiO2 was treated with hydrochloric acid at room temperature for 1 hour, and the moisture content was 30% and the specific surface area was 0.52 m 2 A support of / g was prepared.

[0079] The catalyst of Example 3 was prepared by supporting the active ingredient on the prepared cordierite support in the same manner as in Example 1.

[0080] [Example 4]

[0081] A cordierite support having a cell density of 200 cpsi was treated with hydrochloric acid at room temperature for 2 hours to produce a support having a moisture content of 40%, and an active ingredient was loaded thereon in the same manner as in Example 1 to produce a catalyst of Example 4.

[0082] [Example 5]

[0083] A cordierite support having a cell density of 200 cpsi was treated with hydrochloric acid at room temperature for 3 hours to produce a support having a moisture content of 52%, and an active ingredient was loaded thereon in the same manner as in Example 1 to produce a catalyst of Example 5.

[0084] [Example 6]

[0085] A catalyst of Example 6 was prepared in the same manner as in Example 1 using a cordierite support having similar physical properties to the support used in Example 1, but with improved heat capacity by increasing the thickness of the channels from 0.35 mm to 0.42 mm.

[0086] [Example 7]

[0087] A catalyst of Example 7 was prepared in the same manner as Example 1 using a cordierite support with a channel thickness increased to 0.53 mm.

[0088] [Comparative Example 1]

[0089] Manufactured by extruding silicon carbide, it has a moisture content of 53% and a specific surface area of ​​0.45 m 2 / g, a silicon carbide support with a cell density of 200 cpsi was used as a support for the reforming catalyst.

[0090] The modified catalyst was prepared by fixing the total active ingredient content to 1.5 wt%, preparing the main active ingredient, nickel-cobalt, at a 1:1 ratio, and adding 0.05 wt% of palladium and 0.2 wt% of zirconium as cocatalyst ingredients.

[0091] A silicon carbide support was immersed in the prepared active ingredient solution so that the active ingredient was absorbed into the support. The silicon carbide support with the active ingredient absorbed was blown with an air gun to remove excess active ingredient solution, and 100 o C and dried in an oven for more than 12 hours. The manufactured catalyst was calcined at 500°C for 4 hours to manufacture the catalyst of Comparative Example 1.

[0092] [Comparative Example 2]

[0093] Cordierite support with a cell density of 200 cpsi manufactured by extruding silicon carbide was treated with alumina sol to obtain a moisture content of 14.6% and a specific surface area of ​​0.45 m 2A catalyst support having the characteristics of / g was prepared. Using the prepared support, a catalyst of Comparative Example 2 was prepared by processing in the same manner as in Example 1.

[0094] [Comparative Example 3]

[0095] A catalyst of Comparative Example 3 was prepared using a silicon carbide support having similar physical properties to the support used in Comparative Example 1, but with the channel thickness increased from 0.35 mm to 0.53 mm.

[0096] [Comparative Example 4]

[0097] The cordierite support with a cell density of 200 cpsi, composed of 2MgO-2Al2O3-5SiO2, was treated multiple times with alumina sol at room temperature to obtain a moisture content of 11.8% and a specific surface area of ​​0.33 m 2 A support of / g was prepared.

[0098] A catalyst of Comparative Example 4 was prepared by loading the active ingredient onto the prepared cordierite support in the same manner as Comparative Example 1.

[0099] [Experimental Example 1]

[0100] In order to evaluate the performance of the catalysts manufactured by Examples 1 to 6 and Comparative Examples 1 to 3, synthesis gas was manufactured by a dry reforming reaction using methane and carbon dioxide as follows, and the results are shown in Table 1.

[0101] The catalysts prepared in Examples 1 to 6 and Comparative Examples 1 to 3 were subjected to reforming reaction evaluation in a fixed-bed reactor equipped with an external heating system. The reactor was a tubular reactor made of quartz with an outer diameter of 1 / 2 inch. Before the reaction, the catalysts prepared in Examples 1 to 4 and Comparative Examples 1 to 5 were injected into the reactor at a methane / carbon dioxide ratio of 1 and reduced at 1,000°C for 10 minutes. The reforming reaction was performed under the conditions of atmospheric pressure, a reaction temperature of 1,000°C, and a methane / carbon dioxide ratio of 1, and the methane, carbon dioxide, carbon monoxide, and hydrogen gases emitted after the reaction were analyzed using a gas chromatography system equipped with a thermal conductivity detector.

[0102] [Experimental Example 2]

[0103] The weight of 5 cm-sized untreated or hydrochloric acid-treated cordierite or silicon carbide supports was measured, and each support was immersed in deionized water for 5 minutes. Excess water was removed with an air gun, and the weight of the cordierite or silicon carbide support that had absorbed deionized water was measured. The water absorption rate of the cordierite or silicon carbide support was calculated based on the weight increase or decrease before and after deionized water treatment.

[0104] <Confirmation of experimental results>

[0105] The experimental results of Experiments 1 and 2 above are shown in the following table.

[0106] Water absorption rate (%)Channel thickness (mm)Specific surface area (m 2 / g) Methane conversion rate (%) Carbon dioxide conversion rate (%) H2 / CO ratio (%) Example 1 19.00.35 0.319 2.39 5.40.81 Example 2 16.30.34 0.38 9 1.89 4.10.81 Example 3 30.10.33 0.52 87.79 1.10.79 Example 4 41.10.34 0.56 76.27 9.40.78 Example 5 52.50.35 0.74 7 0.17 2.6 0.77 Example 6 19.00.42 0.33 9 0.89 4.10.80 Example 7 19.00.53 0.37 8 8.29 0.30.81 Comparative example 153.20.350.4558.060.10.63Comparative example 214.60.350.4068.169.80.68Comparative example 353.20.530.4565.268.30.66Comparative example 411.80.340.3334.141.20.62

[0107] In addition, the conversion rates of methane and carbon dioxide of the catalysts manufactured in Example 1 and Comparative Example 1 performed under the reaction conditions of Experimental Example 1 are shown in Figures 1 and 2.

[0108] As shown in Figures 1 and 2, the catalyst of Example 1 exhibited a constant conversion of methane and carbon dioxide during 2,000 hours of reforming reaction. The catalysts of Examples 2 to 4, which had increased water absorption rates, exhibited catalytic activity similar to or slightly increased than that of the catalyst of Example 1, and although differences in catalyst stability were observed depending on the water absorption rate, stable reaction activity was observed for 1,200 hours. However, a decrease in the activity of the reforming catalyst was observed after 1,200 hours of reforming reaction.

[0109] In addition, for the catalysts of Examples 5 and 6, which were manufactured from cordierite having the same physical properties as Example 1 but having channel wall thicknesses of 0.42 mm and 0.53 mm, respectively, similar activity behaviors to the catalyst of Example 1 were observed. As the channel wall thickness increased, the methane and carbon dioxide activities of the reforming catalysts each increased by about 1%, and stable catalytic activity was exhibited for 2,000 hours of reaction.

[0110] Meanwhile, in the case of the catalyst of Comparative Example 1, which had the highest water absorption rate, it showed the highest methane and carbon dioxide conversion rate compared to the catalysts of Examples 1 to 4 and had stable catalytic activity for 800 hours of reaction, but it was confirmed that the catalytic activity gradually decreased thereafter.

[0111] The catalyst of Comparative Example 2, in which the water absorption rate was reduced to 14.6% through alumina sol treatment, exhibited similar activity behavior to the catalyst of Comparative Example 1, but exhibited stable activity during 1,200 hours of reaction, after which a decrease in activity was observed.

[0112] In addition, in the case of the comparative example 3 catalyst in which the channel wall thickness of the silicon carbide support having a water absorption rate of 53% was increased, it was confirmed that the catalyst exhibited similar activity behavior to the comparative example 1 catalyst and that the stability of the catalyst was improved.

[0113] In addition, in the case of Comparative Example 4, which has a low moisture absorption rate, it can be confirmed that the conversion rate is significantly reduced compared to the example.

[0114] From the results of Examples 1 to 6 or Comparative Examples 1 to 4, it was confirmed that the activity and stability of the reforming catalyst can be improved by controlling the physical properties of the cordierite or silicon carbide support used in the carbon dioxide-methane dry reforming reaction, such as water absorption and channel wall thickness.

[0115] Therefore, it was confirmed that by controlling the characteristics of the monolithic support proposed in the present invention, it is possible to design an effective catalyst for producing synthesis gas by reforming reaction using various reducing agents such as carbon dioxide-methane, with improved support and stability.

[0116] Although the preferred embodiments of the present invention have been described with reference to the attached drawings, the embodiments described in this specification and the configurations illustrated in the drawings are only the most preferred embodiments of the present invention and do not represent all of the technical ideas of the present invention, and therefore, it should be understood that there may be various equivalents and modified examples that can replace them at the time of filing this application. Therefore, the embodiments described above should be understood as illustrative and not restrictive in all respects, and the scope of the present invention is indicated by the claims described below rather than the detailed description, and all changes or modified forms derived from the meaning and scope of the claims and equivalent concepts should be interpreted as being included in the scope of the present invention.

Claims

1. A catalyst support for producing synthesis gas, characterized by a porous molded body containing one or more of cordierite, SiC, Al2O3, SiO2, and MgO, having a moisture absorption rate of 15 to 53% and a cell density of 25 to 700 cpsi (cell per square inch).

2. A catalyst support for producing synthesis gas, characterized in that in claim 1, the porous molded body is made of cordierite having a cell density of 100 to 300 cpsi, or three types of oxides of Al2O3, SiO2, and MgO.

3. A catalyst support for synthesis gas production according to claim 1, characterized in that the porous molded body has a specific surface area of ​​0.1 to 5 m2 / g and a density of 0.5 to 0.7 g / mL.

4. A catalyst support for producing synthesis gas, characterized in that the porous molded body according to claim 1 is made of a porous lattice structure having a wall thickness of 0.3 to 0.8 mm.

5. A catalyst for producing synthesis gas, which is a porous molded body containing one or more components of cordierite, SiC, Al2O3, SiO2, and MgO, and has a water absorption rate of 15 to 53% and a cell density of 25 to 700 cpsi, and is coated with one or more elements selected from the group consisting of elements corresponding to groups 1 to 2, 7 to 13, and 16 among elements of 3 or more periods to support an active component for a reforming reaction.

6. A catalyst for producing synthesis gas, characterized in that in claim 5, the active ingredient contains Ni:Co in a weight ratio of 1:0.01 to 1.

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