Method for preparing ethanolamine platinum solution, and ethanolamine platinum solution prepared using same

Abstract

The present invention provides a method for preparing an ethanolamine platinum solution by using a platinum complex compound and monoethanolamine, and an ethanolamine platinum solution prepared using same.

Description

Method for preparing ethanolamine platinum solution and ethanolamine platinum solution prepared therefrom

[0001] The present invention relates to a method for producing an ethanolamine platinum solution using a platinum complex and monoethanolamine, and to an ethanolamine platinum solution produced thereby.

[0002] In general, chloroplatinic acid has been widely used for a long time as a precursor for manufacturing NOx reduction catalysts for air purification or fuel cell catalysts, and the manufacturing method is also simple: dissolving metal platinum in aqua regia or hydrochloric acid with chlorine gas as an oxidizing agent, filtering out insoluble matter, heating and concentrating the obtained filtrate, and then drying and crystallizing it.

[0003] However, since chloroplatinic acid contains a large amount of chlorine, many problems have occurred, such as corrosion of stainless steel in production facilities, environmental pollution, and human allergies through the chlorine gas and hydrochloric acid gas generated.

[0004] A dinitrodiamine platinum solution was used as an alternative precursor, but this had the problem of dissolving the lanthanum and barium that were loaded as NOx absorbents in the washcoat. In contrast, the ethanolamine platinum solution showed significantly less of the problem of NOx absorbent dissolution, and the platinum loading rate was also higher than when using the dinitrodiamine platinum solution.

[0005] Accordingly, the applicant has completed the present invention by obtaining a method for preparing an ethanolamine platinum solution using a platinum complex and monoethanolamine and an ethanolamine platinum solution prepared therefrom through long-term, painstaking efforts and various studies.

[0006] Accordingly, the purpose of the present invention is to provide a method for preparing an ethanolamine platinum solution using a platinum complex compound and monoethanolamine.

[0007] In addition, an object of the present invention is to provide an ethanolamine platinum solution manufactured by a method for manufacturing an ethanolamine platinum solution using a platinum complex compound and monoethanolamine.

[0008] The problems to be solved by the present invention are not limited to the problems mentioned above, and other problems not mentioned will be clearly understood by those skilled in the art from the description below.

[0009] In order to solve the above problem, according to one aspect of the present invention,

[0010] (a-1) a step of mixing monoethanolamine (a) and ultrapure water (b) and heating them to prepare an ethanolamine aqueous solution at 40 to 65°C; and

[0011] (a-2) A step of preparing an ethanolamine platinum solution by adding at least one platinum complex compound selected from among hydroxide platinum (H2Pt(OH)6), sodium hydroxide platinum (Na2Pt(OH)6), potassium hydroxide platinum (K2Pt(OH)6), and ammonium hydroxide platinum ((NH4)2Pt(OH)6) to the ethanolamine aqueous solution such that the molar ratio of the platinum complex compound (c) and monoethanolamine (a) is c: a = 1: 5.2 to 10, and reacting the mixture at 40 to 65°C.

[0012] A method for preparing an ethanolamine platinum solution is provided.

[0013] According to one embodiment of the present invention, in the step of mixing (a-1) monoethanolamine (a) and ultrapure water (b) and then heating to prepare an ethanolamine aqueous solution at 40 to 65°C,

[0014] The molar ratio of the above monoethanolamine (a) and ultrapure water (b) may be a:b = 1:5 to 50.

[0015] According to one embodiment of the present invention, in the step of preparing an ethanolamine platinum solution by adding at least one platinum complex compound selected from among (a-2) hydroxyplatinic acid (H2Pt(OH)6), sodium hydroxyplatinate (Na2Pt(OH)6), potassium hydroxyplatinate (K2Pt(OH)6), and ammonium hydroxyplatinate ((NH4)2Pt(OH)6) to the ethanolamine aqueous solution such that the molar ratio of the platinum complex compound (c) and monoethanolamine (a) is c: a = 1: 5.2 to 10 and reacting at 40 to 65°C,

[0016] Response time can range from 12 to 64 hours.

[0017] According to one embodiment of the present invention, after step (a-2)

[0018] (a-3) A step of leaving the ethanolamine platinum solution at room temperature for 1 to 24 hours may be further included.

[0019] According to one embodiment of the present invention, after step (a-3)

[0020] (a-4) A step of filtering the above ethanolamine platinum solution may be further included.

[0021] According to one embodiment of the present invention, the platinum content of the ethanolamine platinum solution may be 1 wt% to 20 wt%.

[0022]

[0023] In addition, according to another aspect of the present invention,

[0024] An ethanolamine platinum solution having a platinum content of 1 wt% to 20 wt% prepared by the above method for preparing an ethanolamine platinum solution is provided.

[0025] According to the present invention, a method for producing an ethanolamine platinum solution using a platinum complex and monoethanolamine is provided, so that the process stability is excellent and mass production is possible, making it economical.

[0026] In addition, the present invention provides an ethanolamine platinum solution manufactured by a method for manufacturing an ethanolamine platinum solution using a platinum complex and monoethanolamine, so that the solution has excellent physical properties and can be used for various purposes such as a precursor for a NOx reduction catalyst and / or a fuel cell catalyst.

[0027] 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.

[0028] Figure 1 is a process flow diagram of a method for producing an ethanolamine platinum solution according to one embodiment of the present invention.

[0029] Hereinafter, a preferred embodiment according to the present invention will be described in detail with reference to the attached drawings.

[0030] The advantages and features of the present invention and the method for achieving them will become clear with reference to the embodiments described in detail below together with the attached drawings.

[0031] However, the present invention is not limited to the embodiments disclosed below, but may be implemented in various different forms, and these embodiments are provided only to make the disclosure of the present invention complete and to fully inform a person having ordinary skill in the art to which the present invention pertains of the scope of the invention, and the present invention is defined only by the scope of the claims.

[0032] In addition, when describing the present invention, if it is determined that related known technologies or the like may obscure the gist of the present invention, a detailed description thereof will be omitted.

[0033] Hereinafter, the present invention will be described in detail.

[0034]

[0035] Method for preparing ethanolamine platinum solution

[0036] The present invention provides a method for preparing an ethanolamine platinum solution using a platinum complex compound and monoethanolamine.

[0037] The method for producing the ethanolamine platinum solution of the present invention is as follows:

[0038] (a-1) a step of mixing monoethanolamine (a) and ultrapure water (b) and heating them to prepare an ethanolamine aqueous solution at 40 to 65°C; and

[0039] (a-2) A step of preparing an ethanolamine platinum solution by adding at least one platinum complex compound selected from among hydroxide platinum (H2Pt(OH)6), sodium hydroxide platinum (Na2Pt(OH)6), potassium hydroxide platinum (K2Pt(OH)6), and ammonium hydroxide platinum ((NH4)2Pt(OH)6) to the ethanolamine aqueous solution such that the molar ratio of the platinum complex compound (c) and monoethanolamine (a) is c: a = 1: 5.2 to 10, and reacting the mixture at 40 to 65°C.

[0040] The present invention provides a method for producing an ethanolamine platinum solution using a platinum complex and monoethanolamine, so that the process stability is excellent and mass production is possible, making it economical.

[0041]

[0042] In general, chloroplatinic acid has been widely used for a long time as a precursor for manufacturing NOx reduction catalysts for air purification or fuel cell catalysts, and the manufacturing method is also simple: dissolving metal platinum in aqua regia or hydrochloric acid with chlorine gas as an oxidizing agent, filtering out insoluble matter, heating and concentrating the obtained filtrate, and then drying and crystallizing it.

[0043] However, since chloroplatinic acid contains a large amount of chlorine, many problems have occurred, such as corrosion of stainless steel in production facilities, environmental pollution, and human allergies through the chlorine gas and hydrochloric acid gas generated.

[0044] A dinitrodiamine platinum solution was used as an alternative precursor, but this had the problem of dissolving the lanthanum and barium that were loaded as NOx absorbents in the washcoat. In contrast, the ethanolamine platinum solution showed significantly less of the problem of NOx absorbent dissolution, and the platinum loading rate was also higher than when using the dinitrodiamine platinum solution.

[0045] Accordingly, the applicant has completed the present invention by obtaining a method for preparing an ethanolamine platinum solution using a platinum complex and monoethanolamine and an ethanolamine platinum solution prepared therefrom through long-term, painstaking efforts and various studies.

[0046]

[0047] Here, the present invention may be a method for producing an ethanolamine platinum solution using a platinum complex compound and monoethanolamine (NH2CH2CH2OH).

[0048] At this time, the platinum complex may be at least one selected from among platinum hydroxide (H2Pt(OH)6), sodium hydroxide platinum (Na2Pt(OH)6), potassium hydroxide platinum (K2Pt(OH)6), and ammonium hydroxide platinum ((NH4)2Pt(OH)6).

[0049] In addition, the above ethanolamine platinum solution is represented by the following chemical formula 1, which is indicated by Cas No.: 68133-90-4, which is a unique number given to a chemical substance whose chemical structure or composition is confirmed when using hydroxyplatinic acid (H2Pt(OH)6).

[0050] ------ [Chemical Formula 1]

[0051] It can be a dihydrogen hexahydroxyplatinate(II) in 2-ethanolamine solution, a bis(ethanolammonium)hexahydroxoplatinum(IV) solution, or a platinum ethanolamine solution.

[0052] Here, the above platinum complex (c) and monoethanolamine (a) are added so that the molar ratio is c: a = 1: 5.2 to 10, but in the chemical formula 1, it can be seen that 2 moles of monoethanolamine reacted with 1 mole of hydroxyplatinic acid.

[0053] This may be because the reaction between the platinum complex (c) and monoethanolamine (a) requires an excess of monoethanolamine for the reaction to proceed. In other words, free monoethanolamine may be required.

[0054] And, the above ethanolamine platinum solution may be called disodium hexahydroxyplatinate(II) in 2-ethanolamine solution when sodium hydroxide platinum (Na2Pt(OH)6) is used.

[0055] Additionally, the above ethanolamine platinum solution may be called dipotassium hexahydroxyplatinate(II) in 2-ethanolamine solution when potassium hydroxide platinum (K2Pt(OH)6) is used.

[0056] And, the above ethanolamine platinum solution may be called diammonium hexahydroxyplatinate(II) in 2-ethanolamine solution when ammonium hydroxide platinum ((NH4)2Pt(OH)6) is used.

[0057] First, monoethanolamine and ultrapure water are mixed and then heated to prepare an ethanolamine aqueous solution at 40 to 65°C.

[0058] Here, the ethanolamine aqueous solution can be maintained at a temperature of 40 to 65°C before proceeding with the next step of reaction.

[0059] At this time, if the ethanolamine aqueous solution is maintained within the above temperature range, the synthesis efficiency of the subsequent ethanolamine platinum solution can be significantly improved.

[0060] In addition, the maintenance temperature of the above ethanolamine aqueous solution may preferably be 40 to 62°C, and more preferably 40 to 60°C.

[0061] And, in the step of mixing (a-1) monoethanolamine (a) and ultrapure water (b) and heating to prepare an ethanolamine aqueous solution at 40 to 65°C,

[0062] The molar ratio of the above monoethanolamine (a) and ultrapure water (b) may be a:b = 1:5 to 50.

[0063] Here, when the molar ratio of the monoethanolamine and ultrapure water is within the above range, the synthesis efficiency of the subsequent ethanolamine platinum solution can be significantly improved.

[0064] At this time, the molar ratio of the monoethanolamine (a) and ultrapure water (b) may preferably be a:b = 1:5 to 40, and more preferably a:b = 1:10 to 35.

[0065] In addition, at least one platinum complex compound selected from the above (a-2) platinum hydroxide (H2Pt(OH)6), sodium platinum hydroxide (Na2Pt(OH)6), potassium platinum hydroxide (K2Pt(OH)6), and ammonium platinum hydroxide ((NH4)2Pt(OH)6) is added to the ethanolamine aqueous solution so that the molar ratio of the platinum complex compound (c) and monoethanolamine (a) is c: a = 1: 5.2 to 10, and the mixture is reacted at 40 to 65°C to prepare an ethanolamine platinum solution.

[0066] Here, when the molar ratio of the platinum complex and monoethanolamine is within the above range, the physical properties of the ethanolamine platinum solution can be excellent and the synthesis efficiency can be superior.

[0067] At this time, the molar ratio of the platinum platinum complex (c) and monoethanolamine (a) may preferably be c: a = 1: 5.2 to 9.8, and more preferably c: a = 1: 5.2 to 9.5.

[0068] And, when the platinum complex is added to the ethanolamine aqueous solution at the molar ratio above and reacted within the reaction temperature range above, the physical properties of the ethanolamine platinum solution can be excellent and the synthesis efficiency can be superior.

[0069] At this time, the reaction temperature may preferably be 40 to 62°C, and more preferably 40 to 60°C.

[0070] In addition, in the step of preparing an ethanolamine platinum solution by adding at least one platinum complex compound selected from among the above (a-2) platinum hydroxide (H2Pt(OH)6), sodium platinum hydroxide (Na2Pt(OH)6), potassium platinum hydroxide (K2Pt(OH)6), and ammonium platinum hydroxide ((NH4)2Pt(OH)6) to the ethanolamine aqueous solution such that the molar ratio of the platinum complex compound (c) and monoethanolamine (a) is c: a = 1: 5.2 to 10 and reacting at 40 to 65°C,

[0071] Response time can range from 12 to 64 hours.

[0072] Here, when the platinum complex is added to the ethanolamine aqueous solution at the molar ratio above and reacted within the reaction time range above, the physical properties of the ethanolamine platinum solution can be excellent and the synthesis efficiency can be superior.

[0073] At this time, the reaction time may preferably be 12 to 62 hours, and more preferably 12 to 60 hours.

[0074] And, if the reaction temperature is low, the reaction time may be long, and if the reaction temperature is high, the reaction time may be short.

[0075] Also, after the above step (a-2)

[0076] (a-3) A step of leaving the ethanolamine platinum solution at room temperature for 1 to 24 hours may be further included.

[0077] Here, when the room temperature standing time is within the above range, the physical properties of the ethanolamine platinum solution can be excellent and the synthesis efficiency can be superior.

[0078] At this time, the room temperature standing time may preferably be 1 to 23 hours, and more preferably 1 to 22 hours.

[0079] And, after the above step (a-3)

[0080] (a-4) A step of filtering the above ethanolamine platinum solution may be further included.

[0081] Here, when the above filtration is performed, the physical properties of the ethanolamine platinum solution can be excellent and the synthesis efficiency can be superior.

[0082] Additionally, the platinum content of the ethanolamine platinum solution may be 1 wt% to 20 wt%.

[0083]

[0084] Figure 1 is a process flow diagram of a method for producing an ethanolamine platinum solution according to one embodiment of the present invention.

[0085] Referring to Figure 1, first, monoethanolamine and ultrapure water are mixed and then heated to prepare an ethanolamine aqueous solution at 40 to 65°C (S110).

[0086] After that, the platinum complex compound is added to the ethanolamine aqueous solution so that the molar ratio of the platinum complex compound (c) and monoethanolamine (a) is c: a = 1: 5.2 to 10, and the mixture is reacted at 40 to 65°C to prepare an ethanolamine platinum solution (S120).

[0087]

[0088] Ethanolamine platinum solution

[0089] The present invention provides an ethanolamine platinum solution manufactured by a method for manufacturing an ethanolamine platinum solution using a platinum complex compound and monoethanolamine.

[0090] The present invention provides an ethanolamine platinum solution having a platinum content of 1 wt% to 20 wt%, manufactured by the method for manufacturing the above ethanolamine platinum solution.

[0091] The present invention provides an ethanolamine platinum solution manufactured by a method for manufacturing an ethanolamine platinum solution using a platinum complex and monoethanolamine, and thus has excellent physical properties and can be used for various purposes such as a precursor of a NOx reduction catalyst and / or a fuel cell catalyst.

[0092]

[0093] Hereinafter, the present invention will be described in more detail through examples. However, the following examples are intended to further illustrate the present invention, and the scope of the present invention is not limited by these examples. Those skilled in the art may appropriately modify or alter the following examples within the scope of the present invention.

[0094]

[0095] <Example>

[0096] <Examples 1 and 2> Preparation of ethanolamine platinum solution

[0097] An ethanolamine aqueous solution was prepared by mixing monoethanolamine and ultrapure water and heating to 40 to 65°C.

[0098] After that, the platinum complex compound of Table 1 below was added to the ethanolamine aqueous solution so that the molar ratio of the platinum complex compound and monoethanolamine was the content of Table 1 below, and the mixture was reacted at the reaction temperature and reaction time of Table 1 below, left at room temperature for 12 hours, and then filtered to prepare an ethanolamine platinum solution.

[0099] Then, using the ICP-OES (Inductively coupled plasma - optical emission spectroscopy, PerkinElmer OPTIMA 7300 DV) measurement method, the content of platinum contained in each of the ethanolamine platinum solutions obtained in Examples 1 and 2 was measured and shown in Table 1 below.

[0100] In addition, the yield of platinum contained in each of the ethanolamine platinum solutions in Examples 1 to 2 calculated by the following relational expression 1 is shown in Table 1 below.

[0101]

[0102] [Relationship 1]

[0103]

[0104]

[0105] <Comparative Example> Manufacturing of ethanolamine platinum concentrate

[0106] (1) Platinum hydroxide was prepared as a platinum complex.

[0107] (2) 2.04 g of monoethanolamine and 40.92 g of ultrapure water were added to 5 g of prepared hydroxyplatinic acid (= hydroxyplatinic acid and monoethanolamine were added in an equivalent ratio of 1:2, and hydroxyplatinic acid and ultrapure water were added in an equivalent ratio of 1:27.74), and stirred and reacted at room temperature (25°C) for 3 hours to prepare the first reactant.

[0108] (3) 2.04 g of monoethanolamine was added to the manufactured first reactant (= hydroxyplatinic acid and monoethanolamine were added in an equivalent ratio of 1:2), and stirred and reacted at 80°C for 2 hours to manufacture the second reactant.

[0109] (4) The manufactured second reactant was filtered under reduced pressure to obtain a filtrate containing platinum (Pt).

[0110] (5) The obtained filtrate was concentrated at 80°C to prepare 4.41 g of a concentrate containing platinum (Pt).

[0111] Then, using the ICP-OES (Inductively coupled plasma - optical emission spectroscopy, PerkinElmer OPTIMA 7300 DV) measurement method, the content of platinum contained in the ethanolamine platinum concentrate obtained in the comparative example was measured and shown in Table 1 below.

[0112] In addition, the yield of platinum contained in the ethanolamine platinum concentrate of the comparative example calculated by the following relational expression 2 is shown in Table 1 below.

[0113]

[0114] [Relationship 2]

[0115]

[0116]

[0117] Example 1 Example 2 Comparative example Platinum complex (A) Platinum hydroxide Platinum hydroxide Platinum hydroxide Mass of platinum hydroxide (A) (g) 12.5 7.7 5.0 Monoethanolamine (B) Monoethanolamine Monoethanolamine Step 2 Molar ratio of B / A input 664 Reaction temperature (℃) 40 50 Room temperature, 80 Reaction time (hr) 36 243, 2 Platinum content (weight%) 10.3 16.5 11.2 Yield of platinum (weight%) 94.2 96.9 7 3.9

[0118]

[0119] Referring to Table 1 above, the ethanolamine platinum solutions of Examples 1 and 2 had a platinum content of 10.3 to 16.5 wt%.

[0120] And, referring to Table 1 above, the ethanolamine platinum solutions of Examples 1 and 2 had a platinum yield of 94.2 to 96.9 wt%, which was significantly higher than the platinum yield of 73.9 wt% of the comparative example.

[0121] Therefore, the ethanolamine platinum solutions of Examples 1 and 2 were found to have a high platinum yield.

[0122] In addition, referring to Table 1 above, it was confirmed that the platinum content of the ethanolamine platinum solutions of Examples 1 and 2 was 1 wt% to 20 wt%.

[0123]

[0124] Although specific examples of the method for producing an ethanolamine platinum solution according to the present invention and the ethanolamine platinum solution produced therefrom have been described so far, it is obvious that various modifications are possible within the scope of the present invention.

[0125] Therefore, the scope of the present invention should not be limited to the described embodiments, but should be defined not only by the claims described below but also by equivalents of the claims.

[0126] That is, it should be understood that the above-described embodiments are exemplary in all respects and not restrictive, and the scope of the present invention is indicated by the claims to be described later rather than the detailed description, and all changes or modified forms derived from the meaning and scope of the claims and their equivalent concepts should be interpreted as being included in the scope of the present invention.

[0127] The present invention can be used in a method for producing an ethanolamine platinum solution.

Claims

1. (a-1) A step of mixing monoethanolamine (a) and ultrapure water (b) and heating them to prepare an ethanolamine aqueous solution at 40 to 65°C; and (a-2) a step of preparing an ethanolamine platinum solution by adding at least one platinum complex compound selected from among hydroxide platinum (H2Pt(OH)6), sodium hydroxide platinum (Na2Pt(OH)6), potassium hydroxide platinum (K2Pt(OH)6), and ammonium hydroxide platinum ((NH4)2Pt(OH)6) to the ethanolamine aqueous solution such that the molar ratio of the platinum complex compound (c) and monoethanolamine (a) is c: a = 1: 5.2 to 10 and reacting the mixture at 40 to 65°C. Method for preparing ethanolamine platinum solution.

2. In paragraph 1, In the step of preparing an ethanolamine aqueous solution at 40 to 65°C by mixing and heating the monoethanolamine (a) and ultrapure water (b) above (a-1), The molar ratio of the above monoethanolamine (a) and ultrapure water (b) is characterized by being a:b = 1:5 to 50. Method for preparing ethanolamine platinum solution.

3. In paragraph 1, In the step of preparing an ethanolamine platinum solution by adding at least one platinum complex compound selected from among the above (a-2) platinum hydroxide (H2Pt(OH)6), sodium platinum hydroxide (Na2Pt(OH)6), potassium platinum hydroxide (K2Pt(OH)6), and ammonium platinum hydroxide ((NH4)2Pt(OH)6) to the above ethanolamine aqueous solution such that the molar ratio of the platinum complex compound (c) and monoethanolamine (a) is c: a = 1: 5.2 to 10 and reacting at 40 to 65°C, The reaction time is characterized by 12 to 64 hours. Method for preparing ethanolamine platinum solution.

4. In paragraph 1, After step (a-2) above (a-3) characterized by further including a step of leaving the ethanolamine platinum solution at room temperature for 1 to 24 hours. Method for preparing ethanolamine platinum solution.

5. In paragraph 4, After step (a-3) above (a-4) characterized by further including a step of filtering the ethanolamine platinum solution. Method for preparing ethanolamine platinum solution.

6. In paragraph 1, The platinum content of the above ethanolamine platinum solution is characterized by being 1 wt% to 20 wt%. Method for preparing ethanolamine platinum solution.

7. An ethanolamine platinum solution having a platinum content of 1 wt% to 20 wt%, produced by a method for producing an ethanolamine platinum solution according to any one of claims 1 to 6.

Images