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Catalyst for synthesizing methanol or its precursor, method for preparing the catalyst, and method for producing methanol or its precursor using the catalyst

一种合成甲醇、催化剂的技术，应用在有机化合物/氢化物/配位配合物催化剂、化学仪器和方法、物理/化学过程催化剂等方向，能够解决低选择性等问题，达到良好催化活性、确保长期使用、不易损失和分解的效果

Active Publication Date: 2021-01-05
KOREA INST OF SCI & TECH
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

However, the reaction still requires high temperatures of 600°C or more, and although the catalyst is highly capable of converting methane to methanol, it has very low selectivity

Method used

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  • Catalyst for synthesizing methanol or its precursor, method for preparing the catalyst, and method for producing methanol or its precursor using the catalyst
  • Catalyst for synthesizing methanol or its precursor, method for preparing the catalyst, and method for producing methanol or its precursor using the catalyst
  • Catalyst for synthesizing methanol or its precursor, method for preparing the catalyst, and method for producing methanol or its precursor using the catalyst

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Experimental program
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preparation example Construction

[0054] Another aspect of the present invention relates to a method for the preparation of a catalyst comprising reacting a substituted or unsubstituted aniline with a Pt salt, as shown in the following reaction scheme:

[0055]

[0056] Another aspect of the present invention relates to a method for methane oxidation comprising (a) contacting a catalyst for synthesizing methanol or a precursor thereof according to any embodiment with methane in the presence of an acid.

[0057] As previously mentioned, the catalyst for synthesizing methanol or its precursor represented by one of Formulas 1 to 3 according to the present invention may be used to form methyl ester through esterification to realize methane oxidation. The methyl esters can be used to form functional derivatives by subsequent reaction with nucleophiles.

[0058] Specifically, methyl esters can react with water as a nucleophile to synthesize methanol as a functional derivative. Methyl esters can also be reacted w...

Embodiment 1

[0079] Embodiment 1: the synthesis of catalyst compound

[0080] (1) Synthesis of compound 1-1

[0081] Bis(aniline)dichloroplatinum

[0082]

[0083] Will K 2 PtCl 4 (415 mg, 1.0 mmol) was added to an aqueous solution of aniline (502 mg, 5.4 mmol). After stirring well at room temperature for 18 hours, the precipitate was collected by filtration and washed with water and diethyl ether. The resulting solid was dissolved in dimethylformamide (DMF). The solution was stirred at 80°C for 3 hours. The reaction solution was concentrated under reduced pressure and precipitated with ether. The precipitate was collected by filtration to give the desired product (105 mg, 4.0 mmol) in 23% yield. 1 H NMR (400MHz, DMSO-d 6 )δ7.24-7.20 (m, 8H), 7.12-7.08 (m, 2H), 6.96 (s, 4H) (see image 3 )

[0084] (2) Synthesis of compound 1-2

[0085] Dichlorobis(4-methylaniline)platinum

[0086]

[0087] The desired product was obtained in a yield of 37% in the same manner as compoun...

Embodiment 2

[0132] Example 2: Synthesis of Methanol Precursor and Methanol

[0133] (1) Synthesis of methyl hydrogen sulfate

[0134] 1mg (2.6×10 -3 mmol) catalyst (dichloro-(N,N,N,N-tetramethylethylenediamine) platinum) represented by formula 3-2 and 30g containing 20% ​​by weight SO 3 The oleum was mixed in a glass lined 100ml Inconel autoclave. The reactor was filled with methane gas to a pressure of 20 bar. The methane-filled reactor was heated to 180°C and the reaction was allowed to proceed for 3 hours. The pressure of methane at 180° C. was 35 bar at the initial stage of the reaction and decreased to 30 bar after 3 hours of reaction. After the reaction is complete, use a solution containing methanesulfonic acid (CH 3 SO 3 H) D as internal standard 2 SO 4 pass 1 H-NMR spectroscopy determines the structure of the product (see figure 1 ).

[0135] figure 1 Production of 1.89 g (16.9 mmol) of methyl hydrogensulfate was confirmed. The turnover number (TON) and turnover fr...

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Abstract

Novel catalysts with amine ligands for the synthesis of methanol or its precursors are disclosed. When the catalyst is reacted with an alkane in the presence of an acid, at least one C-H bond of the alkane is catalytically oxidized. Thus, the catalyst is suitable for the formation of alkyl esters from alkanes.

Description

technical field [0001] The present invention relates to a catalyst for synthesizing methanol or its precursor, a method for preparing the catalyst and a method for using the catalyst to produce methanol or methyl hydrogen sulfate as a methanol precursor. More specifically, the present invention relates to diamine-coordinated Pt catalysts, a process for the preparation of said catalysts and a process for the production of methyl bisulphate or even methanol by reacting said catalysts with methane gas in the presence of oleum. Background technique [0002] Methane is one of the most abundant resources on earth and has very high chemical stability. Due to its potential availability and economic benefits, methane is considered an important alternative energy source to fossil fuels. [0003] However, since methane is in a gaseous state at room temperature and has a low boiling point (-161.5° C.), it occupies a large volume at room temperature and is limited in transport and trans...

Claims

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Application Information

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Patent Type & Authority Patents(China)
IPC IPC(8): B01J31/22C07F15/00C07C303/24C07C305/06
CPCB01J31/1805B01J2231/70B01J2531/828C07C303/24C07F15/0013C07C305/06B01J2231/46C07F15/0093B01J31/1815B01J2231/40
Inventor 李炫周秋贤娥李惠正吕丞美朴武圣洪淳赫金在员
Owner KOREA INST OF SCI & TECH
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