High-temperature desulfurizer, synthetic method thereof, high-temperature desulfurizer composition and application

By developing high-temperature desulfurization agents with specific hydrocarbon groups and alkylene substituted groups, the problems of poor high-temperature desulfurization capability and easy scaling of desulfurization products in the prior art are solved, and efficient and stable high-temperature desulfurization effect is achieved.

CN119874629APending Publication Date: 2025-04-25CHINA PETROLEUM & CHEMICAL CORP +1
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Patent Information

Application Number
CN202311391808.2
Authority / Receiving Office
CN · China
Patent Type
Applications(China)
Current Assignee / Owner
Filing Date
2023-10-25
Publication Date
2025-04-25

AI Technical Summary

Technical Problem

The existing desulfurizer has poor desulfurization ability at high temperatures, and the desulfurization products are prone to scale and blockage of pipelines, resulting in low treatment efficiency and equipment damage.

Method used

A high-temperature desulfurization agent has been developed, whose molecular structure includes specific hydrocarbon groups and alkylene substituted groups, which are prepared by specific synthetic methods, and has the advantages of high sulfur capacity and desulfurization products being not prone to scaling.

Benefits of technology

It realizes the maintenance of high desulfurization activity at high temperatures, avoids the scaling problem of desulfurization products, improves the treatment efficiency and reduces the risk of equipment damage.

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Abstract

The invention belongs to the technical field of oil field chemicals, and relates to a high-temperature desulfurizer, a synthesis method thereof, a high-temperature desulfurizer composition and application. The invention relates to a synthesis method of a high-temperature desulfurizing agent, which comprises the following steps in parts by mole: (1) reacting a compound # imgabs 0 # with a structure shown in a formula (Y) and a compound # imgabs 1 # with a structure shown in a formula (Z) with a first catalyst at 0-300 DEG C for 5-30 hours to generate an amide reaction product; and (2) putting a compound # imgabs2 # with a structure as shown in a formula (X) into the amide reaction product obtained in the step (1), and then reacting at 50-300 DEG C for 5-24 hours to generate the high-temperature desulfurizer. The invention has the following beneficial effects: (1) the raw material source is wide, and the preparation process is simple; and (2) high desulfurization activity is maintained at high temperature. And (3) the dispersing performance is good, and scaling substances cannot be generated due to sulfur absorption in the use process.
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Description

Technical Field

[0001] The invention belongs to the technical field of oilfield chemicals and relates to a high-temperature desulfurizer and a synthesis method thereof, a high-temperature desulfurizer composition and application. Background Art

[0002] In the development process of oil and gas fields, hydrogen sulfide is often generated. The sources of hydrogen sulfide are mainly three aspects:

[0003] (1) Sulfur-containing organic compounds, such as mercaptans, sulfides, thiophenes, etc., exist in the reservoirs of oil and gas fields, which crack to produce hydrogen sulfide at high temperatures;

[0004] (2) Under high temperature conditions, sulfate ions in formation water react with hydrocarbons to reduce sulfate to hydrogen sulfide and carbon dioxide;

[0005] (3) The reservoir environment of oil and gas fields is suitable for the growth of sulfate-reducing bacteria. Sulfate ions in water are reduced to hydrogen sulfide by sulfate-reducing bacteria in an anaerobic environment with the participation of organic matter.

[0006] Due to the presence of hydrogen sulfide, corrosion and damage to oil and gas pipelines and instruments and equipment often occur. In addition, hydrogen sulfide is a colorless, flammable, and highly toxic gas that poses a serious threat to human safety.

[0007] At present, there are many methods for treating hydrogen sulfide in the process of oil and gas field development at home and abroad, which are mainly divided into dry desulfurization and wet desulfurization. Dry desulfurization uses the reducibility and flammability of hydrogen sulfide to desulfurize or directly burn it with solid oxidants and adsorbents. Dry desulfurization is mostly used for the treatment of external gas at joint stations. Wet desulfurization is to add liquid desulfurizers to the system for desulfurization. Wet desulfurization is mostly used at the wellhead and gathering and transportation process of oil and gas fields. At present, the most widely used liquid desulfurizers are alcoholamine desulfurizers and triazine desulfurizers.

[0008] Chinese patent application CN106552478A (application number: 201510639670.2) discloses a composite desulfurizer, which is composed of N-methyldiethanolamine, sterically hindered amine, stabilizer, corrosion inhibitor, defoamer 2,4,6-tris(dimethylaminomethyl)phenol and dimethyltin mercaptan. Alcoholamine desulfurizers are mainly used for natural gas and refinery gas desulfurization, using the principle of physical adsorption, but they may desorb. In addition, alcoholamine desulfurizers have low sulfur capacity and poor processing capacity.

[0009] Chinese patent application CN105056710A (application number: 201510516647.4) discloses a liquid absorbent for removing hydrogen sulfide from oil and gas, which is composed of hexahydrotriazine compounds and oxazolidine compounds, which have a synergistic effect on hydrogen sulfide absorption. However, after absorbing hydrogen sulfide, triazine desulfurizers are prone to produce dithiazine and trithiazine precipitation, which block pipelines, and have low sulfur capacity at high temperatures. Summary of the invention

[0010] Purpose of the invention: In view of the problems that the above-mentioned desulfurizer has poor high-temperature desulfurization ability and the desulfurization products are easy to scale and clog pipelines, the present invention discloses a high-temperature desulfurizer and its synthesis method, a high-temperature desulfurizer composition and application. The high-temperature desulfurizer of the present invention has the advantages of high sulfur capacity (especially strong desulfurization ability at high temperature) and the desulfurization products are not easy to scale.

[0011] Technical solution: A high-temperature desulfurizer, whose molecular structure is shown in formula (1):

[0012] R'-ML

[0013] Formula (1), where

[0014] R' is a structure shown in formula (2):

[0015] in:

[0016] R1 is one of H, C1-C8 hydrocarbon group, and C1-C8 hydrocarbon group containing a substituent, wherein the substituent of the C1-C8 hydrocarbon group containing a substituent is one or more of hydroxyl group, carboxyl group, and amine group; R1 is preferably H, C1-C6 hydrocarbon group, and C1-C6 hydrocarbon group containing a substituent, wherein the substituent of the C1-C6 hydrocarbon group containing a substituent is one or more of hydroxyl group, carboxyl group, and amine group;

[0017] R2 is one of H, C1-C8 hydrocarbon group, and C1-C8 hydrocarbon group containing a substituent, wherein the substituent of the C1-C8 hydrocarbon group containing a substituent is one or more of hydroxyl, carboxyl, and amine; R2 is preferably H, C1-C6 hydrocarbon group, and C1-C6 hydrocarbon group containing a substituent, wherein the substituent of the C1-C6 hydrocarbon group containing a substituent is one or more of hydroxyl, carboxyl, and amine;

[0018] R3 is a C1-C8 alkylene group, preferably a C1-C6 alkylene group, more preferably a C1-C3 alkylene group;

[0019] M is a structure shown in formula (3):

[0020] in:

[0021] R4 is C1-C 10 An alkylene group, preferably a C1-C6 alkylene group, more preferably a C1-C4 alkylene group;

[0022] R5 is C1-C 10 An alkylene group, preferably a C1-C6 alkylene group, more preferably a C1-C4 alkylene group;

[0023] L is a structure shown in formula (4):

[0024]

[0025] In the formula, B is C1-C 20 Hydrocarbon groups, C1-C 20 One of the hydrocarbon groups, wherein: a C1-C 20 The substituent of the hydrocarbon group is one or more of hydroxyl, carboxyl, and amine; B is preferably C1-C 10 Hydrocarbon groups, C1-C 10 One of the hydrocarbon groups, wherein: a C1-C 10 The substituent of the hydrocarbon group is one or more of hydroxyl, carboxyl and amine groups, and B is more preferably a C1-C5 hydrocarbon group or a C1-C5 hydrocarbon group containing a substituent, wherein the substituent of the C1-C5 hydrocarbon group containing a substituent is one or more of hydroxyl, carboxyl and amine groups.

[0026] Furthermore, the high-temperature desulfurizing agent is one of the compounds having the structure shown in formula (5), the compounds having the structure shown in formula (6), and the compounds having the structure shown in formula (7):

[0027]

[0028]

[0029] A high-temperature desulfurizer, whose molecular structure is shown in formula (8):

[0030] in:

[0031] R1 is one of H, C1-C8 hydrocarbon group, and C1-C8 hydrocarbon group containing a substituent, wherein the substituent of the C1-C8 hydrocarbon group containing a substituent is one or more of hydroxyl group, carboxyl group, and amine group; R1 is preferably H, C1-C6 hydrocarbon group, and C1-C6 hydrocarbon group containing a substituent, wherein the substituent of the C1-C6 hydrocarbon group containing a substituent is one or more of hydroxyl group, carboxyl group, and amine group;

[0032] R2 is one of H, C1-C8 hydrocarbon group, and C1-C8 hydrocarbon group containing a substituent, wherein the substituent of the C1-C8 hydrocarbon group containing a substituent is one or more of hydroxyl, carboxyl, and amine; R2 is preferably H, C1-C6 hydrocarbon group, and C1-C6 hydrocarbon group containing a substituent, wherein the substituent of the C1-C6 hydrocarbon group containing a substituent is one or more of hydroxyl, carboxyl, and amine;

[0033] R3 is a C1-C8 alkylene group, preferably a C1-C6 alkylene group, more preferably a C1-C3 alkylene group;

[0034] R4 is C1-C 10 An alkylene group, preferably a C1-C6 alkylene group, more preferably a C1-C4 alkylene group;

[0035] R5 is C1-C 10 The alkylene group is preferably a C1-C6 alkylene group, and more preferably a C1-C4 alkylene group.

[0036] A high-temperature desulfurizer, whose molecular structure is shown in formula (9):

[0037] in:

[0038] B is C1-C 20 Hydrocarbon groups, C1-C 20 One of the hydrocarbon groups, wherein: a C1-C 20 The substituent of the hydrocarbon group is one or more of hydroxyl, carboxyl, and amine; B is preferably C1-C 10 Hydrocarbon groups, C1-C 10 One of the hydrocarbon groups, wherein: a C1-C 10 The substituent of the hydrocarbon group is one or more of hydroxyl, carboxyl, and amine. B is more preferably a C1-C5 hydrocarbon group or a C1-C5 hydrocarbon group containing a substituent, wherein the substituent of the C1-C5 hydrocarbon group containing a substituent is one or more of hydroxyl, carboxyl, and amine.

[0039] R3 is a C1-C8 alkylene group, preferably a C1-C6 alkylene group, more preferably a C1-C3 alkylene group;

[0040] R4 is C1-C 10 An alkylene group, preferably a C1-C6 alkylene group, more preferably a C1-C4 alkylene group;

[0041] R5 is C1-C 10 An alkylene group, preferably a C1-C6 alkylene group, more preferably a C1-C4 alkylene group;

[0042] R6 is a C1-C8 alkylene group, preferably a C1-C6 alkylene group, and more preferably a C1-C3 alkylene group;

[0043] R7 is a C1-C8 alkylene group, preferably a C1-C6 alkylene group, and more preferably a C1-C3 alkylene group.

[0044] A method for synthesizing the above-mentioned high-temperature desulfurizer, in terms of molar parts, comprises the following steps:

[0045] (1) 0.8-1.3 parts of a compound having a structure represented by formula (Y), 0.8-1.0 parts of a compound having a structure represented by formula (Z) and 0.5-2 parts of a first catalyst are reacted at 0-300° C. for 5-30 hours to generate an amide reaction product, wherein:

[0046] The compound represented by the structure of formula (Y):

[0047]

[0048] R4 is C1-C 10 An alkylene group, preferably a C1-C6 alkylene group, more preferably a C1-C4 alkylene group;

[0049] A' is OR a , F, Cl, Br, I, where R a It is one of H and C1-C4 alkyl;

[0050] A″ is OR a , F, Cl, Br, I, where R a It is one of H and C1-C4 alkyl;

[0051] The compound represented by the structure of formula (Z):

[0052] in:

[0053] R5 is C1-C 10 An alkylene group, preferably a C1-C6 alkylene group, more preferably a C1-C4 alkylene group;

[0054] B is C1-C 20 Hydrocarbon groups, C1-C 20 One of the hydrocarbon groups, wherein: a C1-C 20 The substituent of the hydrocarbon group is one or more of hydroxyl, carboxyl, and amine; B is preferably C1-C 10 Hydrocarbon groups, C1-C 10 One of the hydrocarbon groups, wherein: a C1-C 10The substituent of the hydrocarbon group is one or more of hydroxyl, carboxyl, and amine. B is more preferably a C1-C5 hydrocarbon group or a C1-C5 hydrocarbon group containing a substituent, wherein the substituent of the C1-C5 hydrocarbon group containing a substituent is one or more of hydroxyl, carboxyl, and amine.

[0055] (2) placing 0.8-1.3 parts of the compound having the structure represented by formula (X) into the amide reaction product obtained in step (1), and then reacting at 50-300° C. for 5-24 hours to generate a high-temperature desulfurization agent, wherein:

[0056] The compound represented by the structure of formula (X):

[0057] in:

[0058] R3 is a C1-C8 alkylene group, preferably a C1-C6 alkylene group, more preferably a C1-C3 alkylene group;

[0059] R8 is one of H, C1-C8 hydrocarbon group, and C1-C8 hydrocarbon group containing a substituent, wherein the substituent of the C1-C8 hydrocarbon group containing a substituent is one or more of hydroxyl, carboxyl, and amine; R8 is preferably one of H, C1-C6 hydrocarbon group, and C1-C6 hydrocarbon group containing a substituent, wherein the substituent of the C1-C6 hydrocarbon group containing a substituent is one or more of hydroxyl, carboxyl, and amine;

[0060] R9 is one of H, C1-C8 hydrocarbon group, and C1-C8 hydrocarbon group containing substituents, wherein the substituents of the C1-C8 hydrocarbon group containing substituents are one or more of hydroxyl, carboxyl, and amine groups; R9 is preferably one of H, C1-C6 hydrocarbon group, and C1-C6 hydrocarbon group containing substituents, wherein the substituents of the C1-C6 hydrocarbon group containing substituents are one or more of hydroxyl, carboxyl, and amine groups.

[0061] Furthermore, the first catalyst is one or more of HBTU, DMC, HOBT, HATU, DCC, CDI and propyl chloroformate.

[0062] Furthermore, the reaction temperature of step (1) is 0-200°C, and the reaction time is 5-20h. More preferably, the reaction temperature of step (1) is 0-110°C, and the reaction time is 5-12h.

[0063] Furthermore, the reaction temperature of step (2) is 0-200° C., and the reaction time is 5-12 h.

[0064] Furthermore, 0.05-0.12 parts of a second catalyst are added in step (2).

[0065] Furthermore, the second catalyst is one or more of an inorganic acid, an organic acid, a metal salt of an organic acid, and an acidic resin.

[0066] Furthermore, the inorganic acid is one or more of sulfuric acid, hydrochloric acid, nitric acid, phosphoric acid, boric acid and heteropoly acid.

[0067] Furthermore, the organic acid is one or more of benzenesulfonic acid, cyclohexanesulfonic acid and methanesulfonic acid.

[0068] Furthermore, the metal salt of the organic acid is one or more of a zinc salt of the organic acid, a potassium salt of the organic acid and a sodium salt of the organic acid.

[0069] A method for synthesizing the above-mentioned high-temperature desulfurizer, in terms of molar parts, comprises the following steps:

[0070] (1) reacting 0.8-1.3 parts of an anhydride of a compound of formula (Y') with 0.8-1.0 parts of a compound of formula (Z) at 0-300° C. for 5-30 hours to generate an amide reaction product, wherein:

[0071] The structure of the acid anhydride of the compound represented by the structure of formula (Y') is as follows:

[0072]

[0073] Where: R a H, C 1~ One of the C4 alkyl groups;

[0074] The compound represented by the structure of formula (Z):

[0075] in:

[0076] R5 is C1-C 10 An alkylene group, preferably a C1-C6 alkylene group, more preferably a C1-C4 alkylene group;

[0077] B is C1-C 20 Hydrocarbon groups, C1-C 20 One of the hydrocarbon groups, wherein: a C1-C 20 The substituent of the hydrocarbon group is one or more of hydroxyl, carboxyl, and amine; B is preferably C1-C 10 Hydrocarbon groups, C1-C 10 One of the hydrocarbon groups, wherein: a C1-C 10The substituent of the hydrocarbon group is one or more of hydroxyl, carboxyl, and amine. B is more preferably a C1-C5 hydrocarbon group or a C1-C5 hydrocarbon group containing a substituent, wherein the substituent of the C1-C5 hydrocarbon group containing a substituent is one or more of hydroxyl, carboxyl, and amine.

[0078] (2) adding 0.8-1.3 parts of the compound having the structure represented by formula (X) to the amide reaction product obtained in step (1), and reacting at 50-300° C. for 5-24 hours to generate a high-temperature desulfurization agent, wherein:

[0079] The compound represented by the structure of formula (X):

[0080] in:

[0081] R3 is a C1-C8 alkylene group, preferably a C1-C6 alkylene group, more preferably a C1-C3 alkylene group;

[0082] R8 is one of H, C1-C8 hydrocarbon group, and C1-C8 hydrocarbon group containing a substituent, wherein the substituent of the C1-C8 hydrocarbon group containing a substituent is one or more of hydroxyl, carboxyl, and amine; R8 is preferably one of H, C1-C6 hydrocarbon group, and C1-C6 hydrocarbon group containing a substituent, wherein the substituent of the C1-C6 hydrocarbon group containing a substituent is one or more of hydroxyl, carboxyl, and amine;

[0083] R9 is one of H, C1-C8 hydrocarbon group, and C1-C8 hydrocarbon group containing substituents, wherein the substituents of the C1-C8 hydrocarbon group containing substituents are one or more of hydroxyl, carboxyl, and amine groups; R9 is preferably one of H, C1-C6 hydrocarbon group, and C1-C6 hydrocarbon group containing substituents, wherein the substituents of the C1-C6 hydrocarbon group containing substituents are one or more of hydroxyl, carboxyl, and amine groups.

[0084] Furthermore, the reaction temperature in step (1) is 0-200° C., and the reaction time is 5-20 h. Preferably, the reaction temperature in step (1) is 0-110° C., and the reaction time is 5-12 h.

[0085] Furthermore, the reaction temperature of step (2) is 0-200° C., and the reaction time is 5-12 h.

[0086] Furthermore, 0.08-0.12 parts of a second catalyst are added in step (2).

[0087] Furthermore, the second catalyst is one or more of an inorganic acid, an organic acid, a metal salt of an organic acid, and an acidic resin.

[0088] Furthermore, the inorganic acid is one or more of sulfuric acid, hydrochloric acid, nitric acid, phosphoric acid, boric acid and heteropoly acid.

[0089] Furthermore, the organic acid is one or more of benzenesulfonic acid, cyclohexanesulfonic acid and methanesulfonic acid.

[0090] Furthermore, the metal salt of the organic acid is one or more of a zinc salt of the organic acid, a potassium salt of the organic acid and a sodium salt of the organic acid.

[0091] A method for synthesizing a high-temperature desulfurizer, in terms of molar parts, comprises the following steps:

[0092] (1) 0.8-1.3 parts of a compound having a structure represented by formula (X), 0.8-1.0 parts of a compound having a structure represented by formula (Y), and 0.05-0.12 parts of a second catalyst are reacted at 50-300° C. for 5-24 hours to generate an ester reaction product, wherein:

[0093] The compound represented by the structure of formula (X):

[0094] in:

[0095] R3 is a C1-C8 alkylene group, preferably a C1-C6 alkylene group, more preferably a C1-C3 alkylene group;

[0096] R8 is one of H, C1-C8 hydrocarbon group, and C1-C8 hydrocarbon group containing a substituent, wherein the substituent of the C1-C8 hydrocarbon group containing a substituent is one or more of hydroxyl, carboxyl, and amine; R8 is preferably one of H, C1-C6 hydrocarbon group, and C1-C6 hydrocarbon group containing a substituent, wherein the substituent of the C1-C6 hydrocarbon group containing a substituent is one or more of hydroxyl, carboxyl, and amine;

[0097] R9 is one of H, C1-C8 hydrocarbon group, and C1-C8 hydrocarbon group containing a substituent, wherein the substituent of the C1-C8 hydrocarbon group containing a substituent is one or more of hydroxyl group, carboxyl group, and amine group; R9 is preferably one of H, C1-C6 hydrocarbon group, and C1-C6 hydrocarbon group containing a substituent, wherein the substituent of the C1-C6 hydrocarbon group containing a substituent is one or more of hydroxyl group, carboxyl group, and amine group;

[0098] The compound represented by the structure of formula (Y):

[0099]

[0100] R4 is C1-C 10 An alkylene group, preferably a C1-C6 alkylene group, more preferably a C1-C4 alkylene group;

[0101] A' is OR a , F, Cl, Br, I, where R a H, C 1~ One of the C4 alkyl groups;

[0102] A″ is OR a , F, Cl, Br, I, where R a H, C 1~ One of the C4 alkyl groups;

[0103] (2) Add 0.8-1.3 parts of the compound having the structure represented by formula (Z) to the ester reaction product obtained in step (1), and react at 0-300° C. for 5-30 hours to generate a high-temperature desulfurization agent, wherein:

[0104] The compound represented by the structure of formula (Z):

[0105] in:

[0106] R5 is C1-C 10 An alkylene group, preferably a C1-C6 alkylene group, more preferably a C1-C4 alkylene group;

[0107] B is C1-C 20 Hydrocarbon groups, C1-C 20 One of the hydrocarbon groups, wherein: a C1-C 20 The substituent of the hydrocarbon group is one or more of hydroxyl, carboxyl, and amine; B is preferably C1-C 10 Hydrocarbon groups, C1-C 10 One of the hydrocarbon groups, wherein: a C1-C 10 The substituent of the hydrocarbon group is one or more of hydroxyl, carboxyl and amine groups, and B is more preferably a C1-C5 hydrocarbon group or a C1-C5 hydrocarbon group containing a substituent, wherein the substituent of the C1-C5 hydrocarbon group containing a substituent is one or more of hydroxyl, carboxyl and amine groups.

[0108] Furthermore, the reaction temperature of step (1) is 0-200°C, and the reaction time is 5-12h.

[0109] Furthermore, in step (1), the second catalyst is one or more of an inorganic acid, an organic acid, a metal salt of an organic acid and an acidic resin.

[0110] Furthermore, the inorganic acid is selected from one or more of sulfuric acid, hydrochloric acid, nitric acid, phosphoric acid, boric acid and heteropoly acid.

[0111] Furthermore, the organic acid is selected from one or more of benzenesulfonic acid, cyclohexanesulfonic acid and methanesulfonic acid.

[0112] Furthermore, the metal salt of the organic acid is selected from one or more of the zinc salt of the organic acid, the potassium salt of the organic acid and the sodium salt of the organic acid.

[0113] Furthermore, the reaction temperature of step (2) is 0-200° C., and the reaction time is 5-20 h. Preferably, the reaction temperature is 0-110° C., and the reaction time is 5-12 h.

[0114] Furthermore, in step (2), 0.5-2 parts of a first catalyst are added, wherein the first catalyst is one or more of HBTU, DMC, HOBT, HATU, DCC, CDI and propyl chloroformate.

[0115] A method for synthesizing a high-temperature desulfurizer, in terms of molar parts, comprises the following steps:

[0116] (1) reacting 0.8-1.3 parts of a compound of formula (X) with 0.8-1.0 parts of an anhydride of a compound of formula (Y') at 50-300° C. for 5-24 hours to produce an ester reaction product, wherein:

[0117] The compound represented by the structure of formula (X):

[0118] in:

[0119] R3 is a C1-C8 alkylene group, preferably a C1-C6 alkylene group, more preferably a C1-C3 alkylene group;

[0120] R8 is one of H, C1-C8 hydrocarbon group, and C1-C8 hydrocarbon group containing a substituent, wherein the substituent of the C1-C8 hydrocarbon group containing a substituent is one or more of hydroxyl, carboxyl, and amine; R8 is preferably one of H, C1-C6 hydrocarbon group, and C1-C6 hydrocarbon group containing a substituent, wherein the substituent of the C1-C6 hydrocarbon group containing a substituent is one or more of hydroxyl, carboxyl, and amine;

[0121] R9 is one of H, C1-C8 hydrocarbon group, and C1-C8 hydrocarbon group containing a substituent, wherein the substituent of the C1-C8 hydrocarbon group containing a substituent is one or more of hydroxyl group, carboxyl group, and amine group; R9 is preferably one of H, C1-C6 hydrocarbon group, and C1-C6 hydrocarbon group containing a substituent, wherein the substituent of the C1-C6 hydrocarbon group containing a substituent is one or more of hydroxyl group, carboxyl group, and amine group;

[0122] The structure of the acid anhydride of the compound represented by the structure of formula (Y') is as follows:

[0123]

[0124] Where: Ra H, C 1~ One of the C4 alkyl groups;

[0125] (2) adding 0.8-1.3 parts of the compound having the structure represented by formula (Z) to the ester reaction product obtained in step (1) and reacting at 0-300° C. for 5-30 hours to generate a high-temperature desulfurization agent, wherein:

[0126] The compound represented by the structure of formula (Z):

[0127] in:

[0128] R5 is C1-C 10 An alkylene group, preferably a C1-C6 alkylene group, more preferably a C1-C4 alkylene group;

[0129] B is C1-C 20 Hydrocarbon groups, C1-C 20 One of the hydrocarbon groups, wherein: a C1-C 20 The substituent of the hydrocarbon group is one or more of hydroxyl, carboxyl, and amine; B is preferably C1-C 10 Hydrocarbon groups, C1-C 10 One of the hydrocarbon groups, wherein: a C1-C 10 The substituent of the hydrocarbon group is one or more of hydroxyl, carboxyl and amine groups, and B is more preferably a C1-C5 hydrocarbon group or a C1-C5 hydrocarbon group containing a substituent, wherein the substituent of the C1-C5 hydrocarbon group containing a substituent is one or more of hydroxyl, carboxyl and amine groups.

[0130] Furthermore, the reaction temperature of step (1) is 0-200° C., and the reaction time is 5-12 h.

[0131] Furthermore, the reaction temperature of step (2) is 0-200° C., and the reaction time is 5-20 h. Preferably, the reaction temperature is 0-110° C., and the reaction time is 5-12 h.

[0132] Furthermore, in step (2), 0.5-2 parts of a first catalyst are added, wherein the first catalyst is one or more of HBTU, DMC, HOBT, HATU, DCC, CDI and propyl chloroformate.

[0133] The high-temperature desulfurization agent composition is composed of the above-mentioned high-temperature desulfurization agent, water and an auxiliary agent, wherein:

[0134] The mass ratio of the high-temperature desulfurizer, water and auxiliary agent is (30-40): (30-50): (1-10).

[0135] Furthermore, the auxiliary agent is one or more of an antioxidant, a corrosion inhibitor, a pH regulator, a defoaming agent, and a dispersant.

[0136] Furthermore, the antioxidant is one of a hindered phenol antioxidant and an amine antioxidant.

[0137] Furthermore, the corrosion inhibitor is one of nitrite, silicate, phosphoric acid and phosphate.

[0138] Furthermore, the pH adjuster is one of sodium hydroxide, sodium carbonate, hydrochloric acid and phosphoric acid.

[0139] Furthermore, the defoaming agent is one of polysiloxane defoaming agent and polyether modified silicone oil.

[0140] Furthermore, the dispersant is one of sodium tripolyphosphate, sodium hexametaphosphate, triethylhexyl phosphate, and sodium dodecyl sulfate.

[0141] The use of any of the above-mentioned high-temperature desulfurizers, the high-temperature desulfurizers prepared by any of the above-mentioned preparation methods, and the high-temperature desulfurizer compositions as desulfurizers.

[0142] The desulfurizer of the present invention can effectively remove hydrogen sulfide generated during the exploitation of oil and gas wells, and can effectively remove hydrogen sulfide in tail gas during the production process of oil refineries and chemical plants.

[0143] The invention greatly improves the temperature resistance of triazine desulfurizer by introducing piperazine into the triazine structure. In addition, the desulfurization product has a stable structure, which prevents it from further reacting with hydrogen sulfide to form precipitation. The desulfurization product also has partial dispersibility, which can inhibit the formation of scale in the collection and transportation process.

[0144] The high-temperature desulfurizer can be used in oil and gas field exploitation, refinery tail gas treatment, and natural gas purification, and can effectively remove sulfur-containing compounds such as hydrogen sulfide.

[0145] The present invention has the following beneficial effects:

[0146] (1) The raw materials are widely available and the preparation process is simple;

[0147] (2) Maintain high desulfurization activity at high temperature (150°C).

[0148] (3) The desulfurization product is stable in scaling and does not scale during use.

[0149] (4) Desulfurization products can inhibit the formation of scale during the gathering and transportation process. Specific implementation method:

[0150] The specific embodiments of the present invention are described in detail below.

[0151] The endpoints and any values ​​of the ranges disclosed in this article are not limited to the precise ranges or values, and these ranges or values ​​should be understood to include values ​​close to these ranges or values. For numerical ranges, the endpoint values ​​of each range, the endpoint values ​​of each range and the individual point values, and the individual point values ​​can be combined with each other to obtain one or more new numerical ranges, which should be considered as specifically disclosed in this article.

[0152] Characterization methods:

[0153] Preparation method of desulfurizer: add 40g of the sample to be tested, 0.1g of defoaming agent, and 0.8g of pH adjuster into 100g of water, and stir at 60℃ for 2h to mix the solution evenly.

[0154] Desulfurization effect method: Weigh 3g of chemically pure Na2S·9H2O, add it into a 1000mL wide-mouth bottle, then add about 200g of desalted water, cover it with a rubber stopper connected to the detection tube and the constant pressure dropping funnel, and keep the detection tube of the pump suction hydrogen sulfide detector above the reaction liquid level.

[0155] Add a stirring magnet, place the wide-mouth bottle in a 95°C water bath, turn on the magnetic stirring, then drop a certain amount of H2SO4 solution into the constant pressure dropping funnel, add a certain amount of solution, and after 5 minutes, use a hydrogen sulfide detector to detect the concentration of hydrogen sulfide in the wide-mouth bottle at this time as the initial concentration.

[0156] Quickly add 3 g of the sample to be tested after aging in an oven at 150°C for 24 hours. At regular intervals, turn on the hydrogen sulfide detector to detect the concentration of hydrogen sulfide in the wide-mouth bottle. End the test after 30 minutes and record the hydrogen sulfide concentration.

[0157] Scaling evaluation method:

[0158] Prepare 1500ml of 1% desulfurization agent solution, add 500ml to the reaction bottle and 500ml to each of the two absorption bottles. Slowly pass 500ppm hydrogen sulfide standard gas into the reaction bottle, and observe whether there is precipitation in the reaction bottle after 30 minutes. (Triazine has precipitation, but this patent has no precipitation)

[0159] In the present invention, the devices or equipment used are all conventional devices or equipment known in the art and are commercially available.

[0160] In the following examples and comparative examples, unless otherwise specified, all reagents used were commercially available chemically pure reagents.

[0161] In this application document: the high temperature desulfurization agent prepared in Example 47 is named as "HDSF47". The high temperature desulfurization composition prepared in Example 47 is referred to as "HDSF47 group" for short, and the following examples are similar.

[0162] Example 1

[0163] A high-temperature desulfurizer, whose molecular structure is shown in formula (1):

[0164] R'-ML

[0165] Formula (1), where

[0166] R' is a structure shown in formula (2):

[0167] in:

[0168] R1 is n-octyl;

[0169] R2 is n-octyl;

[0170] R3 is a C8 alkylene group;

[0171] M is a structure shown in formula (3):

[0172] in:

[0173] R4 is C 10 of alkylene;

[0174] R5 is C 10 of alkylene;

[0175] L is a structure shown in formula (4):

[0176]

[0177] In the formula, B is C 20 of hydrocarbon groups.

[0178] Example 2

[0179] A high-temperature desulfurizer, whose molecular structure is shown in formula (1):

[0180] R'-ML

[0181] Formula (1), where

[0182] R' is a structure shown in formula (2):

[0183] in:

[0184] R1 is a methyl group;

[0185] R2 is methyl;

[0186] R3 is a C1 alkylene group;

[0187] M is a structure shown in formula (3):

[0188] in:

[0189] R4 is a C1 alkylene group;

[0190] R5 is C 10 of alkylene;

[0191] L is a structure shown in formula (4):

[0192]

[0193] In the formula, B is a methyl group.

[0194] Example 3

[0195] A high-temperature desulfurizer, whose molecular structure is shown in formula (1):

[0196] R'-ML

[0197] Formula (1), where

[0198] R' is a structure shown in formula (2):

[0199] in:

[0200] R1 is n-butyl;

[0201] R2 is n-butyl;

[0202] R3 is a C6 alkylene group; in another embodiment, R3 is a C3 alkylene group;

[0203] M is a structure shown in formula (3):

[0204] in:

[0205] R4 is a C6 alkylene group; in another embodiment, R4 is a C4 alkylene group;

[0206] R5 is a C6 alkylene group; in another embodiment, R5 is a C4 alkylene group;

[0207] L is a structure shown in formula (4):

[0208]

[0209] In the formula, B is n-butyl.

[0210] Embodiment 4-7

[0211] It is substantially the same as Example 1, except that the substituents R1 and R2 are different:

[0212] <![CDATA[R1]]> <![CDATA[R2]]> Example 4 H Ethylamino Example 5 <![CDATA[CH2-OH]]> <![CDATA[C8H 17 -COOH]]> Example 6 <![CDATA[C8H 17 -COOH]]> <![CDATA[CH2-OH]]> Example 7 Ethylamino H

[0213] Embodiment 8-15

[0214] The same as Example 1, the only difference is that the substituent B in formula (4) is different:

[0215] B Example 8 <![CDATA[CH2-OH]]> Example 9 Ethylamino Example 10 <![CDATA[C 20 H 41 -COOH]]> Embodiment 11 n-Decyl Example 12 <![CDATA[C 10 H 21 -COOH]]> Embodiment 13 <![CDATA[C5H 11 -OH]]> Embodiment 14 <![CDATA[C5H 11 -COOH]]> Embodiment 15 <![CDATA[C3H7-OH]]>

[0216] Example 16

[0217] A high-temperature desulfurizer, whose molecular structure is shown in formula (5):

[0218]

[0219] Embodiment 17

[0220] A high-temperature desulfurizer, whose molecular structure is shown in formula (6):

[0221]

[0222] Embodiment 18

[0223] A high-temperature desulfurizer, whose molecular structure is shown in formula (7):

[0224]

[0225] Embodiment 19

[0226] A high-temperature desulfurizer, whose molecular structure is shown in formula (8):

[0227] Wherein: R1 is H;

[0228] R2 is H;

[0229] R3 is a C8 alkylene group;

[0230] R4 is C 10 of alkylene;

[0231] R5 is C 10 of alkylene.

[0232] Examples 20-26

[0233] The same as Example 19, the only difference is that the substituents R1 and R2 are different

[0234]

[0235]

[0236] Examples 27-30

[0237] The same as Example 19, the only difference is that the substituents R3, R4, and R5 are different

[0238] <![CDATA[R3]]> <![CDATA[R4]]> <![CDATA[R5]]> Embodiment 27 <![CDATA[C6 alkylene]]> <![CDATA[C6 alkylene]]> <![CDATA[C6 alkylene]]> Embodiment 28 <![CDATA[The alkylene group of C3]]> <![CDATA[C4 alkylene]]> <![CDATA[C4 alkylene]]> Embodiment 29 <![CDATA[The alkylene group of C2]]> <![CDATA[The alkylene group of C3]]> <![CDATA[The alkylene group of C3]]> Embodiment 30 <![CDATA[The alkylene group of C1]]> <![CDATA[The alkylene of C1]]> <![CDATA[The alkylene of C1]]>

[0239] Embodiment 31

[0240] A high-temperature desulfurizer, whose molecular structure is shown in formula (9):

[0241] in:

[0242] B is a methyl group;

[0243] R3 is a C8 alkylene group;

[0244] R4 is C 10 of alkylene;

[0245] R5 is C 10 of alkylene;

[0246] R6 is a C8 alkylene group;

[0247] R7 is a C8 alkylene group.

[0248] Examples 32-38

[0249] The same as Example 31, the only difference is that the substituents B, R3 and R4 are different:

[0250] B <![CDATA[R3]]> <![CDATA[R4]]> Embodiment 32 <![CDATA[C 20 Hydrocarbon]]> <![CDATA[C6 alkylene]]> <![CDATA[C6 alkylene]]> Embodiment 33 <![CDATA[C 10 Hydrocarbon]]> <![CDATA[The alkylene group of C3]]> <![CDATA[C4 alkylene]]> Embodiment 34 n-pentyl <![CDATA[The alkylene of C2]]> <![CDATA[The alkylene group of C3]]> Embodiment 35 n-propyl <![CDATA[The alkylene of C1]]> <![CDATA[The alkylene group of C1 <!-- 14 -->]]> Embodiment 36 <![CDATA[C 20 H 41 -OH]]> <![CDATA[C4 alkylene]]> <![CDATA[C4 alkylene]]> Embodiment 37 <![CDATA[C 10 H 21 -COOH]]> <![CDATA[C5 alkylene]]> <![CDATA[C5 alkylene]]> Embodiment 38 Ethylamino <![CDATA[C7 alkylene]]> <![CDATA[C9 alkylene group]]>

[0251] Examples 39-43

[0252] The same as Example 31, the only difference is that the substituents R5, R6 and R7 are different:

[0253] <![CDATA[R5]]> <![CDATA[R6]]> <![CDATA[R7]]> Embodiment 39 <![CDATA[C6 alkylene]]> <![CDATA[C6 alkylene]]> <![CDATA[C6 alkylene]]> Embodiment 40 <![CDATA[C4 alkylene]]> <![CDATA[The alkylene group of C3]]> <![CDATA[The alkylene group of C3]]> Embodiment 41 <![CDATA[The alkylene of C2]]> <![CDATA[The alkylene of C2]]> <![CDATA[The alkylene group of C2]]> Embodiment 42 <![CDATA[The alkylene group of C1]]> <![CDATA[The alkylene of C1]]> <![CDATA[The alkylene group of C1]]> Embodiment 43 <![CDATA[C4 alkylene]]> <![CDATA[The alkylene group of C3]]> <![CDATA[The alkylene of C1]]>

[0254] Embodiment 44

[0255] A method for synthesizing a high-temperature desulfurizer, in terms of molar parts, comprises the following steps:

[0256] (1) 0.8 parts of the compound represented by the structure of formula (Y), 0.8 parts of the compound represented by the structure of formula (Z) and 0.5 parts of the first catalyst are reacted at 200° C. for 6 hours to generate an amide reaction product, wherein:

[0257] The compound represented by the structure of formula (Y):

[0258]

[0259] R4 is a C1 alkylene group;

[0260] A' is OR a , where R a is H;

[0261] A″ is OR a , where R a is H;

[0262] The compound represented by the structure of formula (Z):

[0263] in:

[0264] R5 is C1 alkylene;

[0265] B is a methyl group;

[0266] (2) 0.8 parts of the compound having the structure represented by formula (X) is placed in the amide reaction product obtained in step (1), and then reacted at 100° C. for 10 hours to generate a high-temperature desulfurization agent, referred to as “HDSF44”, wherein:

[0267] The compound represented by the structure of formula (X):

[0268] in:

[0269] R3 is a C1 alkylene group;

[0270] R8 is H;

[0271] R9 is H.

[0272] Furthermore, the first catalyst is a mixture of HBTU, DMC, HOBT, HATU, DCC, CDI and propyl chloroformate in equal mass ratios.

[0273] In another embodiment, the reaction temperature of step (1) is 0°C and the reaction time is 20 hours. In yet another embodiment, the reaction temperature of step (1) is 0°C and the reaction time is 12 hours.

[0274] In another embodiment, the reaction temperature of step (2) is 0°C and the reaction time is 12h.

[0275] Furthermore, 0.05 parts of a second catalyst is added in step (2).

[0276] Furthermore, the second catalyst is a mixture of equal masses of inorganic acid, organic acid, metal salt of organic acid and acidic resin.

[0277] Further, the inorganic acid is sulfuric acid. In another embodiment, the inorganic acid is hydrochloric acid. In another embodiment, the inorganic acid is nitric acid. In another embodiment, the inorganic acid is phosphoric acid. In another embodiment, the inorganic acid is boric acid. In another embodiment, the inorganic acid is a heteropolyacid.

[0278] In yet another embodiment, the organic acid is benzenesulfonic acid. In another embodiment, the organic acid is cyclohexane acid. In another embodiment, the organic acid is methanesulfonic acid.

[0279] Further, the metal salt of the organic acid is a zinc salt of the organic acid. In another embodiment, the metal salt of the organic acid is a potassium salt of the organic acid. In another embodiment, the metal salt of the organic acid is a sodium salt of the organic acid.

[0280] The high-temperature desulfurization agent composition is composed of the above-mentioned high-temperature desulfurization agent, water and an auxiliary agent, wherein:

[0281] The mass ratio of high-temperature desulfurizer, water and additive is 30:30:1, referred to as "HDSF44 group".

[0282] Furthermore, the auxiliary agent is a composition of antioxidant, corrosion inhibitor, pH regulator, defoamer and dispersant of equal mass.

[0283] Furthermore, the antioxidant is a hindered phenol antioxidant. In another embodiment, the antioxidant is an amine antioxidant.

[0284] Furthermore, the corrosion inhibitor is nitrite. In another embodiment, the corrosion inhibitor is silicate. In another embodiment, the corrosion inhibitor is phosphoric acid. In another embodiment, the corrosion inhibitor is phosphate.

[0285] Furthermore, the pH adjusting agent is sodium hydroxide. In another embodiment, the pH adjusting agent is sodium carbonate. In another embodiment, the pH adjusting agent is hydrochloric acid. In another embodiment, the pH adjusting agent is phosphoric acid.

[0286] Furthermore, the defoamer is a polysiloxane defoamer. In another embodiment, the defoamer is a polyether-modified silicone oil.

[0287] Furthermore, the dispersant is sodium tripolyphosphate. In another embodiment, the dispersant is sodium hexametaphosphate. In another embodiment, the dispersant is triethylhexyl phosphoric acid. In another embodiment, the dispersant is sodium dodecyl sulfate.

[0288] The high-temperature desulfurizer prepared by the above preparation method and the above-mentioned high-temperature desulfurizer composition are used as desulfurizers.

[0289] Embodiment 45

[0290] A method for synthesizing a high-temperature desulfurizer, in terms of molar parts, comprises the following steps:

[0291] (1) 1.3 parts of a compound having a structure represented by formula (Y), 1.0 parts of a compound having a structure represented by formula (Z) and 2 parts of a first catalyst are reacted at 300° C. for 5 hours to generate an amide reaction product, wherein:

[0292] The compound represented by the structure of formula (Y):

[0293]

[0294] R4 is C 10 of alkylene;

[0295] A' is OR a , where R a is methyl;

[0296] A″ is OR a , where R a is methyl;

[0297] The compound represented by the structure of formula (Z):

[0298] in:

[0299] R5 is C 10 of alkylene;

[0300] B is C 20 The hydrocarbon group;

[0301] (2) 1.3 parts of the compound of formula (X) are placed in the amide reaction product obtained in step (1), and then reacted at 300° C. for 5 hours to produce a high-temperature desulfurization agent, referred to as “HDSF45”, wherein:

[0302] The compound represented by the structure of formula (X):

[0303] in:

[0304] R3 is a C8 alkylene group;

[0305] R8 is methyl;

[0306] R9 is methyl.

[0307] Furthermore, the first catalyst is HBTU.

[0308] In another embodiment, the reaction temperature of step (1) is 200° C., and the reaction time is 5 h. In yet another embodiment, the reaction temperature of step (1) is 110° C., and the reaction time is 5 h.

[0309] In another embodiment, the reaction temperature of step (2) is 200° C. and the reaction time is 5 h.

[0310] Furthermore, 0.12 parts of a second catalyst is added in step (2).

[0311] Furthermore, the second catalyst is an inorganic acid.

[0312] Furthermore, the inorganic acid is a mixture of equal masses of sulfuric acid, hydrochloric acid, nitric acid, phosphoric acid, boric acid and heteropoly acid.

[0313] The high-temperature desulfurization agent composition is composed of the above-mentioned high-temperature desulfurization agent, water and an auxiliary agent, wherein:

[0314] The mass ratio of high-temperature desulfurizer, water and additive is 40:50:10, referred to as "HDSF45 group".

[0315] Furthermore, the auxiliary agent is an antioxidant.

[0316] Furthermore, the antioxidant is an amine antioxidant.

[0317] The high-temperature desulfurizer prepared by the above preparation method and the above-mentioned high-temperature desulfurizer composition are used as desulfurizers.

[0318] Embodiment 46

[0319] A method for synthesizing a high-temperature desulfurizer, in terms of molar parts, comprises the following steps:

[0320] (1) reacting 1 part of the compound represented by the structure of formula (Y), 0.9 parts of the compound represented by the structure of formula (Z) and 1 part of the first catalyst at 0° C. for 30 hours to generate an amide reaction product, wherein:

[0321] The compound represented by the structure of formula (Y):

[0322]

[0323] R4 is a C5 alkylene group;

[0324] A' is OR a , where R a is n-butyl;

[0325] A″ is OR a , where R a is n-butyl;

[0326] The compound represented by the structure of formula (Z):

[0327] in:

[0328] R5 is C4 alkylene;

[0329] B is n-pentyl;

[0330] (2) placing one part of the compound having the structure represented by formula (X) into the amide reaction product obtained in step (1), and then reacting at 50° C. for 24 hours to generate a high-temperature desulfurization agent, referred to as “HDSF46”, wherein:

[0331] The compound represented by the structure of formula (X):

[0332] in:

[0333] R3 is C3;

[0334] R8 is n-butyl;

[0335] R9 is n-butyl.

[0336] Furthermore, the first catalyst is DMC.

[0337] In another embodiment, the first catalyst is HOBT. In another embodiment, the first catalyst is HATU. In another embodiment, the first catalyst is DCC. In another embodiment, the first catalyst is CDI. In another embodiment, the first catalyst is propyl chloroformate.

[0338] In another embodiment, the reaction temperature of step (1) is 100° C. and the reaction time is 6 h.

[0339] Furthermore, the reaction temperature of step (2) is 100° C. and the reaction time is 8 h.

[0340] Furthermore, 0.1 parts of a second catalyst is added in step (2).

[0341] Furthermore, the second catalyst is an organic acid.

[0342] Furthermore, the organic acid is a mixture of equal masses of benzenesulfonic acid, cyclohexanecarboxylic acid and methanesulfonic acid.

[0343] The high-temperature desulfurization agent composition is composed of the above-mentioned high-temperature desulfurization agent, water and an auxiliary agent, wherein:

[0344] The mass ratio of high-temperature desulfurizer, water and additive is 35:40:5, referred to as "HDSF46 group".

[0345] Furthermore, the auxiliary agent is a corrosion inhibitor.

[0346] Furthermore, the corrosion inhibitor is silicate.

[0347] The high-temperature desulfurizer prepared by the above preparation method and the above high-temperature desulfurizer composition are used as desulfurizers.

[0348] Examples 47-50

[0349] The same as Example 44, the only difference is that the substituents R4, A', A" in the compound of the structure represented by formula (Y) are different:

[0350]

[0351] in:

[0352] The high-temperature desulfurization agent prepared in Example 47 is named as "HDSF47". The high-temperature desulfurization composition prepared in Example 47 is referred to as "HDSF47 Group" for short, and the following examples are similar.

[0353] Examples 51-57

[0354] The same as Example 44, the only difference is that the substituents R5 and B in the compound represented by the structure of formula (Z) are different:

[0355] <![CDATA[R5]]> B Embodiment 51 <![CDATA[C 10 Alkylene]]> <![CDATA[C 20 Hydrocarbon]]> Embodiment 52 <![CDATA[C6 alkylene]]> <![CDATA[C 10 Hydrocarbon]]> Embodiment 53 <![CDATA[The alkylene group of C3]]> <![CDATA[Hydrocarbyl group of C5]]> Embodiment 54 <![CDATA[The alkylene group of C2]]> n-propyl Embodiment 55 <![CDATA[C7 alkylene]]> <![CDATA[C 20 H 41 -OH]]> Embodiment 56 <![CDATA[C4 alkylene]]> <![CDATA[C 10 H 21 -COOH]]> Embodiment 57 <![CDATA[The alkylene of C1]]> <![CDATA[C5H 11 -NH2]]>

[0356] Examples 58-65

[0357] The same as Example 44, the only difference is that the substituents R3, R8, and R9 in the compound of the structure represented by formula (X) are different:

[0358] <![CDATA[R3]]> <![CDATA[R8]]> <![CDATA[R9]]> Embodiment 58 <![CDATA[C8 alkylene]]> methyl methyl Embodiment 59 <![CDATA[C6 alkylene]]> n-octyl n-octyl Embodiment 60 <![CDATA[The alkylene group of C3]]> n-Hexyl n-Hexyl Embodiment 61 <![CDATA[The alkylene of C2]]> n-propyl n-propyl Embodiment 62 <![CDATA[The alkylene group of C1]]> <![CDATA[CH3OH]]> <![CDATA[CH3OH]]> Embodiment 63 <![CDATA[C6 alkylene]]> <![CDATA[C6H 13 NH2]]> <![CDATA[C6H 13 NH2]]> Embodiment 64 <![CDATA[The alkylene group of C3]]> <![CDATA[C8H 17 COOH]]> <![CDATA[C8H 17 COOH]]> Embodiment 65 <![CDATA[The alkylene group of C2]]> <![CDATA[C3H7OH]]> <![CDATA[C3H7OH]]>

[0359] Embodiment 66

[0360] A method for synthesizing a high-temperature desulfurizer, in terms of molar parts, comprises the following steps:

[0361] (1) 0.8 parts of an anhydride of a compound of formula (Y') and 0.8 parts of a compound of formula (Z) are reacted at 0°C for 30 hours to generate an amide reaction product, wherein:

[0362] The structure of the acid anhydride of the compound represented by the structure of formula (Y') is as follows:

[0363]

[0364] Where: R a is H;

[0365] The compound represented by the structure of formula (Z):

[0366] in:

[0367] R5 is C1 alkylene;

[0368] B is a methyl group;

[0369] (2) adding 0.8 parts of the compound represented by the formula (X) to the amide reaction product obtained in step (1), and reacting at 50° C. for 24 hours to generate a high-temperature desulfurization agent, referred to as “HDSF66”, wherein:

[0370] The compound represented by the structure of formula (X):

[0371] in:

[0372] R3 is a C1 alkylene group;

[0373] R8 is H;

[0374] R9 is H.

[0375] In another embodiment, the reaction temperature in step (1) is 0°C and the reaction time is 20 hours. In another embodiment, the reaction temperature in step (1) is 0°C and the reaction time is 12 hours.

[0376] In another embodiment, the reaction temperature of step (2) is 0°C and the reaction time is 12h.

[0377] Furthermore, 0.08 parts of a second catalyst is added in step (2).

[0378] Furthermore, the second catalyst is a mixture of an inorganic acid, an organic acid, a metal salt of an organic acid, and an acidic resin in equal mass ratios.

[0379] Further, the inorganic acid is sulfuric acid. In another embodiment, the inorganic acid is hydrochloric acid or nitric acid. In another embodiment, the inorganic acid is nitric acid. In another embodiment, the inorganic acid is phosphoric acid. In another embodiment, the inorganic acid is boric acid. In another embodiment, the inorganic acid is a heteropoly acid.

[0380] In yet another embodiment, the organic acid is benzenesulfonic acid. In another embodiment, the organic acid is cyclohexane acid. In another embodiment, the organic acid is methanesulfonic acid.

[0381] Further, the metal salt of the organic acid is a zinc salt of the organic acid. In another embodiment, the metal salt of the organic acid is a potassium salt of the organic acid. In another embodiment, the metal salt of the organic acid is a sodium salt of the organic acid.

[0382] The high-temperature desulfurization agent composition is composed of the above-mentioned high-temperature desulfurization agent, water and an auxiliary agent, wherein:

[0383] The mass ratio of high-temperature desulfurizer, water and additive is 30:30:1, referred to as "HDSF66 group".

[0384] Furthermore, the auxiliary agent is a mixture of antioxidant, corrosion inhibitor, pH regulator, defoamer and dispersant of equal mass.

[0385] Furthermore, the antioxidant is a hindered phenol antioxidant. In another embodiment, the antioxidant is an amine antioxidant.

[0386] Furthermore, the corrosion inhibitor is nitrite. In another embodiment, the corrosion inhibitor is silicate. In another embodiment, the corrosion inhibitor is phosphoric acid. In another embodiment, the corrosion inhibitor is phosphate.

[0387] Furthermore, the pH adjusting agent is sodium hydroxide. In another embodiment, the pH adjusting agent is sodium carbonate. In another embodiment, the pH adjusting agent is hydrochloric acid. In another embodiment, the pH adjusting agent is phosphoric acid.

[0388] Furthermore, the defoamer is a polysiloxane defoamer. In another embodiment, the defoamer is a polyether-modified silicone oil.

[0389] Furthermore, the dispersant is sodium tripolyphosphate. In another embodiment, the dispersant is sodium hexametaphosphate. In another embodiment, the dispersant is triethylhexyl phosphoric acid. In another embodiment, the dispersant is sodium dodecyl sulfate.

[0390] The high-temperature desulfurizer prepared by the above preparation method and the above-mentioned high-temperature desulfurizer composition are used as desulfurizers.

[0391] Embodiment 67

[0392] A method for synthesizing the above-mentioned high-temperature desulfurizer, in terms of molar parts, comprises the following steps:

[0393] (1) 1.3 parts of an anhydride of a compound of formula (Y') and 1.0 parts of a compound of formula (Z) are reacted at 300° C. for 5 h to generate an amide reaction product, wherein:

[0394] The structure of the acid anhydride of the compound represented by the structure of formula (Y') is as follows:

[0395]

[0396] Where: R ais H; in another embodiment, R a is methyl; in another embodiment, R a is n-butyl;

[0397] The compound represented by the structure of formula (Z):

[0398] in:

[0399] R5 is C 10 In another embodiment, R5 is a C6 alkylene; In another embodiment, R5 is a C4 alkylene;

[0400] B is C 20 In another embodiment, B is a C containing a substituent 20 A hydrocarbon group, wherein: a C containing a substituent 20 The substituent of the hydrocarbon group is hydroxyl; in another embodiment, B is C containing a substituent 10 A hydrocarbon group, wherein: a C containing a substituent 10 The substituent of the hydrocarbon group is a carboxyl group; in another embodiment, B is a C5 hydrocarbon group containing a substituent, wherein: the substituent of the C5 hydrocarbon group containing a substituent is an amine group;

[0401] (2) 1.3 parts of the compound represented by formula (X) are added to the amide reaction product obtained in step (1), and reacted at 300° C. for 5 h to generate a high-temperature desulfurization agent, referred to as “HDSF67”, wherein:

[0402] The compound represented by the structure of formula (X):

[0403] in:

[0404] R3 is C8 alkylene; in another embodiment, R3 is C6 alkylene; in another embodiment, R3 is C3 alkylene;

[0405] R8 is n-octyl; in another embodiment, R8 is a C8 hydrocarbon group containing a substituent, wherein the substituent of the C8 hydrocarbon group containing a substituent is a hydroxyl group; in another embodiment, R8 is a C8 hydrocarbon group containing a substituent, wherein the substituent of the C8 hydrocarbon group containing a substituent is a carboxyl group; in another embodiment, R8 is a C6 hydrocarbon group containing a substituent, wherein the substituent of the C6 hydrocarbon group containing a substituent is an amine group;

[0406] R9 is n-octyl; in another embodiment, R9 is a C8 hydrocarbon group containing a substituent, wherein the substituent of the C8 hydrocarbon group containing a substituent is a hydroxyl group; in another embodiment, R9 is a C8 hydrocarbon group containing a substituent, wherein the substituent of the C8 hydrocarbon group containing a substituent is a carboxyl group; in another embodiment, R9 is a C8 hydrocarbon group containing a substituent, wherein the substituent of the C8 hydrocarbon group containing a substituent is an amino group; in another embodiment, R9 is a C6 hydrocarbon group containing a substituent, wherein the substituent of the C6 hydrocarbon group containing a substituent is a hydroxyl group.

[0407] In another embodiment, the reaction temperature in step (1) is 200° C., and the reaction time is 5 h; in another embodiment, the reaction temperature in step (1) is 110° C., and the reaction time is 5 h.

[0408] In another embodiment, the reaction temperature of step (2) is 200° C. and the reaction time is 5 h.

[0409] Furthermore, 0.12 parts of a second catalyst is added in step (2).

[0410] Furthermore, the second catalyst is an inorganic acid.

[0411] Furthermore, the inorganic acid is nitric acid.

[0412] The high-temperature desulfurization agent composition is composed of the above-mentioned high-temperature desulfurization agent, water and an auxiliary agent, wherein:

[0413] The mass ratio of high-temperature desulfurizer, water and additive is 40:50:10, referred to as "HDSF67 group".

[0414] Furthermore, the auxiliary agent is a dispersant.

[0415] Furthermore, the dispersant is triethylhexyl phosphoric acid.

[0416] The high-temperature desulfurizer prepared by the above preparation method and the above-mentioned high-temperature desulfurizer composition are used as desulfurizers.

[0417] Embodiment 68

[0418] A method for synthesizing the above-mentioned high-temperature desulfurizer, in terms of molar parts, comprises the following steps:

[0419] (1) One part of the anhydride of the compound of the structure represented by formula (Y') is reacted with 0.85 parts of the compound of the structure represented by formula (Z) at 200° C. for 8 hours to generate an amide reaction product, wherein:

[0420] The structure of the acid anhydride of the compound represented by the structure of formula (Y') is as follows:

[0421]

[0422] Where: R a Ethyl;

[0423] The compound represented by the structure of formula (Z):

[0424] in:

[0425] R5 is a C2 alkylene group;

[0426] B is ethyl; in another embodiment, B is a C3 hydrocarbon group containing a substituent, wherein: the substituent of the C3 hydrocarbon group containing a substituent is a hydroxyl group; in another embodiment, B is a C3 hydrocarbon group containing a substituent, wherein: the substituent of the C3 hydrocarbon group containing a substituent is a carboxyl group; in another embodiment, B is a C3 hydrocarbon group containing a substituent, wherein: the substituent of the C3 hydrocarbon group containing a substituent is an amine group;

[0427] (2) Adding 1 part of the compound represented by the structure of formula (X) to the amide reaction product obtained in step (1), reacting at 200° C. for 12 hours to generate a high-temperature desulfurization agent, referred to as “HDSF68”, wherein:

[0428] The compound represented by the structure of formula (X):

[0429] in:

[0430] R3 is a C2 alkylene group;

[0431] R8 is ethyl; in another embodiment, R8 is a C3 hydrocarbon group containing a substituent, wherein the substituent of the C3 hydrocarbon group containing a substituent is a hydroxyl group; in another embodiment, R8 is a C3 hydrocarbon group containing a substituent, wherein the substituent of the C3 hydrocarbon group containing a substituent is a carboxyl group; in another embodiment, R8 is a C3 hydrocarbon group containing a substituent, wherein the substituent of the C3 hydrocarbon group containing a substituent is an amine group;

[0432] R9 is ethyl; in another embodiment, R9 is a C3 hydrocarbon group containing a substituent, wherein the substituent of the C3 hydrocarbon group containing a substituent is hydroxyl; in another embodiment, R9 is a C3 hydrocarbon group containing a substituent, wherein the substituent of the C3 hydrocarbon group containing a substituent is carboxyl; in another embodiment, R9 is a C3 hydrocarbon group containing a substituent, wherein the substituent of the C3 hydrocarbon group containing a substituent is amine.

[0433] In another embodiment, the reaction temperature in step (1) is 100° C., and the reaction time is 6 h; in another embodiment, the reaction temperature in step (1) is 80° C., and the reaction time is 10 h.

[0434] In another embodiment, the reaction temperature of step (2) is 100° C. and the reaction time is 7 h.

[0435] Furthermore, 0.1 parts of a second catalyst is added in step (2).

[0436] Furthermore, the second catalyst is an organic acid.

[0437] Furthermore, the organic acid is methanesulfonic acid.

[0438] The high-temperature desulfurization agent composition is composed of the above-mentioned high-temperature desulfurization agent, water and an auxiliary agent, wherein:

[0439] The mass ratio of high-temperature desulfurizer, water and additive is 35:40:5, referred to as "HDSF68 group".

[0440] Furthermore, the auxiliary agent is an antioxidant.

[0441] Furthermore, the antioxidant is an amine antioxidant.

[0442] The high-temperature desulfurizer prepared by the above preparation method and the above-mentioned high-temperature desulfurizer composition are used as desulfurizers.

[0443] Embodiment 69

[0444] A method for synthesizing a high-temperature desulfurizer, in terms of molar parts, comprises the following steps:

[0445] (1) 0.8 parts of a compound having a structure represented by formula (X), 0.8 parts of a compound having a structure represented by formula (Y), and 0.05 parts of a second catalyst are reacted at 50° C. for 24 hours to generate an ester reaction product, wherein:

[0446] The compound represented by the structure of formula (X):

[0447] in:

[0448] R3 is an alkylene group of C;

[0449] R8 is H; in another embodiment, R8 is methyl; in another embodiment, R8 is a C1 hydrocarbon group containing a substituent, wherein the substituent of the C1 hydrocarbon group containing a substituent is a hydroxyl group; in another embodiment, R8 is a C1 hydrocarbon group containing a substituent, wherein the substituent of the C1 hydrocarbon group containing a substituent is a carboxyl group; in another embodiment, R8 is a C1 hydrocarbon group containing a substituent, wherein the substituent of the C1 hydrocarbon group containing a substituent is an amine group;

[0450] R9 is H; in another embodiment, R9 is methyl; in another embodiment, R9 is a C1 hydrocarbon group containing a substituent, wherein the substituent of the C1 hydrocarbon group containing a substituent is hydroxyl; in another embodiment, R9 is a C1 hydrocarbon group containing a substituent, wherein the substituent of the C1 hydrocarbon group containing a substituent is carboxyl; in another embodiment, R9 is a C1 hydrocarbon group containing a substituent, wherein the substituent of the C1 hydrocarbon group containing a substituent is amine;

[0451] The compound represented by the structure of formula (Y):

[0452]

[0453] R4 is a C1 alkylene group;

[0454] A′ is OH;

[0455] A″ is OH;

[0456] (2) 0.8 parts of the compound represented by formula (Z) is placed in the ester reaction product obtained in step (1), and reacted at 0°C for 30 hours to generate a high-temperature desulfurization agent, referred to as "HDSF69", wherein:

[0457] The compound represented by the structure of formula (Z):

[0458] in:

[0459] R5 is a C1 alkylene group;

[0460] B is methyl; in another embodiment, B is a C1 hydrocarbon group containing a substituent, wherein: the substituent of the C1 hydrocarbon group containing a substituent is hydroxyl; in another embodiment, B is a C1 hydrocarbon group containing a substituent, wherein: the substituent of the C1 hydrocarbon group containing a substituent is carboxyl; in another embodiment, B is a C1 hydrocarbon group containing a substituent, wherein: the substituent of the C1 hydrocarbon group containing a substituent is amine.

[0461] In another embodiment, the reaction temperature of step (1) is 0°C and the reaction time is 12h.

[0462] In another embodiment, in step (1), the second catalyst is a mixture of an inorganic acid, an organic acid, a metal salt of an organic acid and an acidic resin in equal mass ratios.

[0463] Furthermore, the inorganic acid is a mixture of sulfuric acid, hydrochloric acid, nitric acid, phosphoric acid, boric acid and heteropoly acid in equal mass ratio. In another embodiment, the inorganic acid is sulfuric acid. In another embodiment, the inorganic acid is hydrochloric acid. In another embodiment, the inorganic acid is nitric acid. In another embodiment, the inorganic acid is phosphoric acid. In another embodiment, the inorganic acid is boric acid. In another embodiment, the inorganic acid is heteropoly acid.

[0464] Furthermore, the organic acid is a mixture of equal masses of benzenesulfonic acid, cyclohexane acid and methanesulfonic acid. In another embodiment, the organic acid is benzenesulfonic acid. In another embodiment, the organic acid is cyclohexane acid. In another embodiment, the organic acid is methanesulfonic acid.

[0465] Furthermore, the metal salt of the organic acid is a mixture of an organic acid zinc salt, an organic acid potassium salt and an organic acid sodium salt in equal mass ratios. In another embodiment, the metal salt of the organic acid is an organic acid zinc salt. In another embodiment, the metal salt of the organic acid is an organic acid potassium salt. In another embodiment, the metal salt of the organic acid is an organic acid sodium salt.

[0466] In another embodiment, the reaction temperature of step (2) is 0°C, and the reaction time is 20 hours. In another embodiment, the reaction temperature of step (2) is 0°C, and the reaction time is 12 hours.

[0467] In another embodiment, 0.5 parts of the first catalyst are further added in step (2), and the first catalyst is a mixture of HBTU, DMC, HOBT, HATU, DCC, CDI and propyl chloroformate in equal mass ratios. In another embodiment, 0.5 parts of the first catalyst are further added in step (2), and the first catalyst is HBTU. In another embodiment, 0.5 parts of the first catalyst are further added in step (2), and the first catalyst is DMC. In another embodiment, 0.5 parts of the first catalyst are further added in step (2), and the first catalyst is HOBT. In another embodiment, 0.5 parts of the first catalyst are further added in step (2), and the first catalyst is HATU. In another embodiment, 0.5 parts of the first catalyst are further added in step (2), and the first catalyst is DCC. In another embodiment, 0.5 parts of the first catalyst are further added in step (2), and the first catalyst is CDI. In another embodiment, 0.5 parts of the first catalyst are further added in step (2), and the first catalyst is propyl chloroformate.

[0468] The high-temperature desulfurization agent composition is composed of the above-mentioned high-temperature desulfurization agent, water and an auxiliary agent, wherein:

[0469] The mass ratio of high-temperature desulfurizer, water and additive is 30:30:1, referred to as "HDSF69 group".

[0470] Furthermore, the auxiliary agent is a mixture of an antioxidant, a corrosion inhibitor, a pH regulator, a defoaming agent, and a dispersant in equal mass ratios.

[0471] Furthermore, the antioxidant is a hindered phenol antioxidant. In another embodiment, the antioxidant is an amine antioxidant.

[0472] Furthermore, the corrosion inhibitor is nitrite. In another embodiment, the corrosion inhibitor is silicate. In another embodiment, the corrosion inhibitor is phosphoric acid. In another embodiment, the corrosion inhibitor is phosphate.

[0473] Furthermore, the pH adjusting agent is sodium hydroxide. In another embodiment, the pH adjusting agent is sodium carbonate. In another embodiment, the pH adjusting agent is hydrochloric acid. In another embodiment, the pH adjusting agent is phosphoric acid.

[0474] Furthermore, the defoamer is a polysiloxane defoamer. In another embodiment, the defoamer is a polyether-modified silicone oil.

[0475] Furthermore, the dispersant is sodium tripolyphosphate. In another embodiment, the dispersant is sodium hexametaphosphate. In another embodiment, the dispersant is triethylhexyl phosphoric acid. In another embodiment, the dispersant is sodium dodecyl sulfate.

[0476] The high-temperature desulfurizer prepared by the above preparation method and the above-mentioned high-temperature desulfurizer composition are used as desulfurizers.

[0477] Embodiment 70

[0478] A method for synthesizing a high-temperature desulfurizer, in terms of molar parts, comprises the following steps:

[0479] (1) 1.3 parts of a compound having a structure represented by formula (X), 1.0 parts of a compound having a structure represented by formula (Y), and 0.12 parts of a second catalyst are reacted at 300° C. for 5 hours to generate an ester reaction product, wherein:

[0480] The compound represented by the structure of formula (X):

[0481] in:

[0482] R3 is C8 alkylene; in another embodiment, R3 is C6 alkylene; in another embodiment, R3 is C3 alkylene;

[0483] R8 is methyl; in another embodiment, R8 is n-octyl; in another embodiment, R8 is a C8 hydrocarbon group containing a substituent, wherein the substituent of the C8 hydrocarbon group containing a substituent is a hydroxyl group; in another embodiment, R8 is a C8 hydrocarbon group containing a substituent, wherein the substituent of the C8 hydrocarbon group containing a substituent is a carboxyl group; in another embodiment, R8 is a C8 hydrocarbon group containing a substituent, wherein the substituent of the C8 hydrocarbon group containing a substituent is an amine group; in another embodiment, R8 is n-hexyl; in another embodiment, R8 is a C6 hydrocarbon group containing a substituent, wherein the substituent of the C6 hydrocarbon group containing a substituent is a hydroxyl group; in another embodiment, R8 is a C6 hydrocarbon group containing a substituent, wherein the substituent of the C6 hydrocarbon group containing a substituent is a carboxyl group; in another embodiment, R8 is a C6 hydrocarbon group containing a substituent, wherein the substituent of the C6 hydrocarbon group containing a substituent is an amine group;

[0484] R9 is methyl; in another embodiment, R9 is n-octyl; in another embodiment, R9 is a C8 hydrocarbon group containing a substituent, wherein the substituent of the C8 hydrocarbon group containing a substituent is a hydroxyl group; in another embodiment, R9 is a C8 hydrocarbon group containing a substituent, wherein the substituent of the C8 hydrocarbon group containing a substituent is a carboxyl group; in another embodiment, R9 is a C8 hydrocarbon group containing a substituent, wherein the substituent of the C8 hydrocarbon group containing a substituent is an amine group; in another embodiment, R9 is n-hexyl; in another embodiment, R9 is a C6 hydrocarbon group containing a substituent, wherein the substituent of the C6 hydrocarbon group containing a substituent is a hydroxyl group; in another embodiment, R9 is a C6 hydrocarbon group containing a substituent, wherein the substituent of the C6 hydrocarbon group containing a substituent is a carboxyl group; in another embodiment, R9 is a C6 hydrocarbon group containing a substituent, wherein the substituent of the C6 hydrocarbon group containing a substituent is an amine group;

[0485] The compound represented by the structure of formula (Y):

[0486]

[0487] R4 is C 10 In another embodiment, R4 is a C6 alkylene; In another embodiment, R4 is a C4 alkylene;

[0488] A' is OH; in another embodiment, A' is OCH3; in another embodiment, A' is OR a , where R a is C4 alkyl; in another embodiment, A′ is F; in another embodiment, A′ is Cl; in another embodiment, A′ is Br; in another embodiment, A′ is I.

[0489] A" is OH; in another embodiment, A" is OCH3; in another embodiment, A" is OR a , where R a is C4 alkyl; in another embodiment, A″ is F; in another embodiment, A″ is Cl; in another embodiment, A″ is Br; in another embodiment, A″ is I.

[0490] (2) 1.3 parts of the compound represented by formula (Z) are placed in the ester reaction product obtained in step (1), and reacted at 300° C. for 5 hours to generate a high-temperature desulfurization agent, referred to as “HDSF70”, wherein:

[0491] The compound represented by the structure of formula (Z):

[0492] in:

[0493] R5 is C 10 In another embodiment, R5 is a C6 alkylene; In another embodiment, R5 is a C4 alkylene;

[0494] B is C 20 In another embodiment, B is C 10 In another embodiment, B is a C1 hydrocarbon group containing a substituent, wherein: the substituent of the C1 hydrocarbon group containing a substituent is a hydroxyl group; In another embodiment, B is a C1 hydrocarbon group containing a substituent 20 A hydrocarbon group, wherein: a C containing a substituent 20 In another embodiment, B is a C8 hydrocarbon group containing a substituent, wherein the substituent of the C8 hydrocarbon group containing a substituent is an amine group; in another embodiment, B is a C5 normal hydrocarbon group; in another embodiment, B is one of the C1 hydrocarbon groups containing a substituent, wherein the substituent of the C1 hydrocarbon group containing a substituent is a hydroxyl group; in another embodiment, B is a C5 normal hydrocarbon group. 10 One of the hydrocarbon groups, wherein: C 10 The substituent of the hydrocarbon group is a carboxyl group; in another embodiment, B is one of the C5 hydrocarbon groups containing a substituent, wherein: the substituent of the C5 hydrocarbon group containing a substituent is an amine group; in another embodiment, B is a C3 hydrocarbon group.

[0495] In another embodiment, the reaction temperature of step (1) is 200° C. and the reaction time is 5 h.

[0496] Furthermore, in step (1), the second catalyst is an inorganic acid.

[0497] Furthermore, the inorganic acid is hydrochloric acid.

[0498] In another embodiment, the reaction temperature of step (2) is 00°C, and the reaction time is 5 hours; in another embodiment, the reaction temperature of step (2) is 110°C, and the reaction time is 5 hours.

[0499] Further, in step (2), 2 parts of a first catalyst are added, and the first catalyst is a mixture of equal masses of HBTU, DMC, HOBT, HATU, DCC, CDI and propyl chloroformate. In another embodiment, the first catalyst is HBTU. In another embodiment, the first catalyst is DMC. In another embodiment, the first catalyst is HOBT. In another embodiment, the first catalyst is HATU. In another embodiment, the first catalyst is DCC. In another embodiment, the first catalyst is CDI. In another embodiment, the first catalyst is propyl chloroformate.

[0500] The high-temperature desulfurization agent composition is composed of the above-mentioned high-temperature desulfurization agent, water and an auxiliary agent, wherein:

[0501] The mass ratio of high-temperature desulfurizer, water and additive is 40:50:10, referred to as "HDSF70 group".

[0502] Furthermore, the auxiliary agent is an antioxidant.

[0503] Furthermore, the antioxidant is an amine antioxidant.

[0504] The high-temperature desulfurizer prepared by the above preparation method and the above-mentioned high-temperature desulfurizer composition are used as desulfurizers.

[0505] Embodiment 71

[0506] A method for synthesizing a high-temperature desulfurizer, in terms of molar parts, comprises the following steps:

[0507] (1) 1 part of a compound having a structure represented by formula (X), 0.9 parts of a compound having a structure represented by formula (Y), and 0.08 parts of a second catalyst are reacted at 150° C. for 12 hours to generate an ester reaction product, wherein:

[0508] The compound represented by the structure of formula (X):

[0509] in:

[0510] R3 is a C2 alkylene group;

[0511] R8 is ethyl. In another embodiment, R8 is one of the C4 hydrocarbon groups containing substituents, wherein the substituent of the C4 hydrocarbon group containing substituents is hydroxyl. In another embodiment, R8 is one of the C4 hydrocarbon groups containing substituents, wherein the substituent of the C4 hydrocarbon group containing substituents is carboxyl. In another embodiment, R8 is one of the C4 hydrocarbon groups containing substituents, wherein the substituent of the C4 hydrocarbon group containing substituents is amine;

[0512] R9 is ethyl. In another embodiment, R9 is a C3 hydrocarbon group containing a substituent, wherein the substituent of the C3 hydrocarbon group containing a substituent is a hydroxyl group. In another embodiment, R9 is a C3 hydrocarbon group containing a substituent, wherein the substituent of the C3 hydrocarbon group containing a substituent is a carboxyl group. In another embodiment, R9 is a C3 hydrocarbon group containing a substituent, wherein the substituent of the C3 hydrocarbon group containing a substituent is an amine group;

[0513] The compound represented by the structure of formula (Y):

[0514]

[0515] R4 is a C2 alkylene group;

[0516] A′ is OH;

[0517] A″ is OH;

[0518] (2) Place 1 part of the compound represented by formula (Z) in the ester reaction product obtained in step (1), and react at 150° C. for 12 hours to generate a high-temperature desulfurization agent, referred to as “HDSF71”, wherein:

[0519] The compound represented by the structure of formula (Z):

[0520] in:

[0521]

[0522] R5 is a C2 alkylene group;

[0523] In another embodiment, B is a C3 hydrocarbon group containing a substituent, wherein: 30 In another embodiment, B is a C3 hydrocarbon group containing a substituent, wherein: 30 In another embodiment, B is a C3 hydrocarbon group containing a substituent, wherein: 30 The substituent of the hydrocarbon group is an amine group.

[0524] In another embodiment, the reaction temperature of step (1) is 80° C. and the reaction time is 10 h.

[0525] Furthermore, in step (1), the second catalyst is a mixture of an inorganic acid, an organic acid, a metal salt of an organic acid and an acidic resin in equal mass ratios.

[0526] Furthermore, the inorganic acid is selected from a mixture of sulfuric acid, hydrochloric acid, nitric acid, phosphoric acid, boric acid and heteropolyacid. In another embodiment, the inorganic acid is selected from sulfuric acid. In another embodiment, the inorganic acid is selected from hydrochloric acid. In another embodiment, the inorganic acid is selected from nitric acid. In another embodiment, the inorganic acid is selected from phosphoric acid. In another embodiment, the inorganic acid is selected from boric acid. In another embodiment, the inorganic acid is selected from heteropolyacid.

[0527] Furthermore, the organic acid is a mixture of benzenesulfonic acid, cyclohexane acid and methanesulfonic acid. In another embodiment, the organic acid is benzenesulfonic acid. In another embodiment, the organic acid is cyclohexane acid. In another embodiment, the organic acid is methanesulfonic acid.

[0528] Furthermore, the metal salt of the organic acid is selected from a mixture of a zinc salt of an organic acid, a potassium salt of an organic acid and a sodium salt of an organic acid. In another embodiment, the metal salt of the organic acid is selected from a zinc salt of an organic acid. In another embodiment, the metal salt of the organic acid is selected from a potassium salt of an organic acid. In another embodiment, the metal salt of the organic acid is selected from a sodium salt of an organic acid.

[0529] In another embodiment, the reaction temperature of step (2) is 100° C. and the reaction time is 12 h. In another embodiment, the reaction temperature of step (2) is 80° C. and the reaction time is 8 h.

[0530] Furthermore, 0.5 parts of the first catalyst is added in step (2).

[0531] Furthermore, the first catalyst is HBTU.

[0532] The high-temperature desulfurization agent composition is composed of the above-mentioned high-temperature desulfurization agent, water and an auxiliary agent, wherein:

[0533] The mass ratio of high-temperature desulfurizer, water and additive is 35:45:5, referred to as "HDSF71 group".

[0534] Furthermore, the auxiliary agent is an antioxidant.

[0535] Furthermore, the antioxidant is a hindered phenol antioxidant.

[0536] The high-temperature desulfurizer prepared by the above preparation method and the above-mentioned high-temperature desulfurizer composition are used as desulfurizers.

[0537] Embodiment 72

[0538] A method for synthesizing a high-temperature desulfurizer, in terms of molar parts, comprises the following steps:

[0539] (1) 0.8 parts of a compound of formula (X) and 0.8 parts of an anhydride of a compound of formula (Y') are reacted at 50° C. for 24 hours to generate an ester reaction product, wherein:

[0540] The compound represented by the structure of formula (X):

[0541] in:

[0542] R3 is a C1 alkylene group;

[0543] R8 is H; in another embodiment, R8 is methyl. In another embodiment, R8 is a C1 hydrocarbon group containing a substituent, wherein the substituent of the C1 hydrocarbon group containing a substituent is hydroxyl. In another embodiment, R8 is a C1 hydrocarbon group containing a substituent, wherein the substituent of the C1 hydrocarbon group containing a substituent is carboxyl. In another embodiment, R8 is a C1 hydrocarbon group containing a substituent, wherein the substituent of the C1 hydrocarbon group containing a substituent is amine;

[0544] R9 is H. In another embodiment, R9 is methyl. In another embodiment, R9 is a C1 hydrocarbon group containing a substituent, wherein the substituent of the C1 hydrocarbon group containing a substituent is hydroxyl. In another embodiment, R9 is a C1 hydrocarbon group containing a substituent, wherein the substituent of the C1 hydrocarbon group containing a substituent is carboxyl. In another embodiment, R9 is a C1 hydrocarbon group containing a substituent, wherein the substituent of the C1 hydrocarbon group containing a substituent is amine;

[0545] The structure of the acid anhydride of the compound represented by the structure of formula (Y') is as follows:

[0546]

[0547] Where: R a is H. In another embodiment, R a is methyl;

[0548] (2) 0.8 parts of the compound represented by formula (Z) is added to the ester reaction product obtained in step (1) and reacted at 0°C for 30 hours to produce a high-temperature desulfurization agent, referred to as "HDSF72", wherein:

[0549] The compound represented by the structure of formula (Z):

[0550] in:

[0551] R5 is C1 alkylene;

[0552] In another embodiment, B is a C1 hydrocarbon group containing a substituent, wherein: 20 In another embodiment, B is a C1-C1 hydrocarbon group containing a substituent, wherein: 20 In another embodiment, B is a C1 hydrocarbon group containing a substituent, wherein: 20 The substituent of the hydrocarbon group is an amine group.

[0553] In another embodiment, the reaction temperature of step (1) is 0°C and the reaction time is 12h.

[0554] In another embodiment, the reaction temperature of step (2) is 0°C and the reaction time is 20 hours; in another embodiment, the reaction temperature of step (2) is 0°C and the reaction time is 12 hours.

[0555] Furthermore, 0.5 parts of the first catalyst is added in step (2).

[0556] Further, the first catalyst is selected from a mixture of HBTU, DMC, HOBT, HATU, DCC, CDI and propyl chloroformate. In another embodiment, the first catalyst is selected from HBTU. In another embodiment, the first catalyst is selected from DMC. In another embodiment, the first catalyst is selected from HOBT. In another embodiment, the first catalyst is selected from HATU. In another embodiment, the first catalyst is selected from DCC. In another embodiment, the first catalyst is selected from CDI. In another embodiment, the first catalyst is selected from propyl chloroformate.

[0557] The high-temperature desulfurization agent composition is composed of the above-mentioned high-temperature desulfurization agent, water and an auxiliary agent, wherein:

[0558] The mass ratio of high-temperature desulfurizer, water and additive is 30:30:1, referred to as "HDSF72 group".

[0559] Further, the auxiliary agent is a mixture of an antioxidant, a corrosion inhibitor, a pH regulator, a defoamer, and a dispersant in equal mass ratios. In another embodiment, the auxiliary agent is an antioxidant. In another embodiment, the auxiliary agent is a corrosion inhibitor. In another embodiment, the auxiliary agent is a pH regulator. In another embodiment, the auxiliary agent is a defoamer. In another embodiment, the auxiliary agent is a dispersant.

[0560] Furthermore, the antioxidant is a hindered phenol antioxidant. In another embodiment, the antioxidant is an amine antioxidant.

[0561] Furthermore, the corrosion inhibitor is nitrite. In another embodiment, the corrosion inhibitor is silicate. In another embodiment, the corrosion inhibitor is phosphoric acid. In another embodiment, the corrosion inhibitor is phosphate.

[0562] Furthermore, the pH adjusting agent is sodium hydroxide. In another embodiment, the pH adjusting agent is sodium carbonate. In another embodiment, the pH adjusting agent is hydrochloric acid. In another embodiment, the pH adjusting agent is phosphoric acid.

[0563] Furthermore, the defoamer is a polysiloxane defoamer. In another embodiment, the defoamer is a polyether-modified silicone oil.

[0564] Furthermore, the dispersant is sodium tripolyphosphate. In another embodiment, the dispersant is sodium hexametaphosphate. In another embodiment, the dispersant is triethylhexyl phosphoric acid. In another embodiment, the dispersant is sodium dodecyl sulfate.

[0565] The high-temperature desulfurizer prepared by the above preparation method and the above-mentioned high-temperature desulfurizer composition are used as desulfurizers.

[0566] Embodiment 73

[0567] A method for synthesizing a high-temperature desulfurizer, in terms of molar parts, comprises the following steps:

[0568] (1) 1.3 parts of a compound of formula (X) and 1.0 parts of an anhydride of a compound of formula (Y') are reacted at 300° C. for 5 hours to generate an ester reaction product, wherein:

[0569] The compound represented by the structure of formula (X):

[0570] in:

[0571] R3 is C8 alkylene. In another embodiment, R3 is C6 alkylene. In another embodiment, R3 is C3 alkylene;

[0572] R8 is n-octyl. In another embodiment, R8 is a C8 hydrocarbon group containing a substituent, wherein the substituent of the C8 hydrocarbon group containing a substituent is a hydroxyl group. In another embodiment, R8 is a C8 hydrocarbon group containing a substituent, wherein the substituent of the C8 hydrocarbon group containing a substituent is a carboxyl group. In another embodiment, R8 is a C8 hydrocarbon group containing a substituent, wherein the substituent of the C8 hydrocarbon group containing a substituent is an amine group;

[0573] R9 is n-octyl. In another embodiment, R9 is a C8 hydrocarbon group containing a substituent, wherein the substituent of the C8 hydrocarbon group containing a substituent is a hydroxyl group. In another embodiment, R9 is a C8 hydrocarbon group containing a substituent, wherein the substituent of the C8 hydrocarbon group containing a substituent is a carboxyl group. In another embodiment, R9 is a C8 hydrocarbon group containing a substituent, wherein the substituent of the C8 hydrocarbon group containing a substituent is an amine group;

[0574] The structure of the acid anhydride of the compound represented by the structure of formula (Y') is as follows:

[0575]

[0576] Where: R a is n-butyl;

[0577] (2) 1.3 parts of the compound represented by formula (Z) are added to the ester reaction product obtained in step (1) and reacted at 300° C. for 5 h to produce a high-temperature desulfurization agent, referred to as “HDSF73”, wherein:

[0578] The compound represented by the structure of formula (Z):

[0579] in:

[0580] R5 is C 10 In another embodiment, R5 is a C6 alkylene. In another embodiment, R5 is a C4 alkylene;

[0581] B is C 20 In another embodiment, B is a C containing a substituent. 20 A hydrocarbon group, wherein: a C containing a substituent 20 In another embodiment, B is a C having a substituent group. 10 A hydrocarbon group, wherein: a C containing a substituent 10 The substituent of the hydrocarbon group is a carboxyl group. In another embodiment, B is a C5 hydrocarbon group containing a substituent, wherein the substituent of the C5 hydrocarbon group containing a substituent is an amine group.

[0582] In another embodiment, the reaction temperature of step (1) is 200° C. and the reaction time is 5 h.

[0583] In another embodiment, the reaction temperature of step (2) is 200° C. and the reaction time is 5 h. In another embodiment, the reaction temperature of step (2) is 110° C. and the reaction time is 8 h.

[0584] Furthermore, one portion of the first catalyst is added in step (2).

[0585] Furthermore, the first catalyst is selected from a mixture of HBTU, DMC, HOBT, HATU, DCC, CDI and propyl chloroformate in equal mass ratios. In another embodiment, the first catalyst is selected from HBTU. In another embodiment, the first catalyst is selected from DMC. In another embodiment, the first catalyst is selected from HOBT. In another embodiment, the first catalyst is selected from HATU. In another embodiment, the first catalyst is selected from DCC. In another embodiment, the first catalyst is selected from CDI. In another embodiment, the first catalyst is selected from propyl chloroformate.

[0586] The high-temperature desulfurization agent composition is composed of the above-mentioned high-temperature desulfurization agent, water and an auxiliary agent, wherein:

[0587] The mass ratio of high-temperature desulfurizer, water and additive is 35:40:5, referred to as "HDSF73 group".

[0588] Furthermore, the auxiliary agent is a dispersant.

[0589] Furthermore, the dispersant is sodium dodecyl sulfate.

[0590] The high-temperature desulfurizer prepared by the above preparation method and the above-mentioned high-temperature desulfurizer composition are used as desulfurizers.

[0591] Embodiment 74

[0592] A method for synthesizing a high-temperature desulfurizer, in terms of molar parts, comprises the following steps:

[0593] (1) One part of the compound represented by the formula (X) and 0.9 parts of the anhydride of the compound represented by the formula (Y') are reacted at 120° C. for 10 hours to generate an ester reaction product, wherein:

[0594] The compound represented by the structure of formula (X):

[0595] in:

[0596] R3 is a C2 alkylene group;

[0597] R8 is n-butyl; in another embodiment, R8 is a C4 hydrocarbon group containing a substituent, wherein the substituent of the C4 hydrocarbon group containing a substituent is a hydroxyl group; in another embodiment, R8 is a C4 hydrocarbon group containing a substituent, wherein the substituent of the C4 hydrocarbon group containing a substituent is a carboxyl group; in another embodiment, R8 is a C4 hydrocarbon group containing a substituent, wherein the substituent of the C4 hydrocarbon group containing a substituent is an amine group;

[0598] R9 is n-butyl; in another embodiment, R9 is a C4 hydrocarbon group containing a substituent, wherein the substituent of the C4 hydrocarbon group containing a substituent is a hydroxyl group; in another embodiment, R9 is a C4 hydrocarbon group containing a substituent, wherein the substituent of the C4 hydrocarbon group containing a substituent is a carboxyl group; in another embodiment, R9 is a C4 hydrocarbon group containing a substituent, wherein the substituent of the C4 hydrocarbon group containing a substituent is an amine group;

[0599] The structure of the acid anhydride of the compound represented by the structure of formula (Y') is as follows:

[0600]

[0601] Where: R a is H; in another embodiment, R a is methyl; in another embodiment, R a is n-butyl;

[0602] (2) Add 1 part of the compound represented by formula (Z) to the ester reaction product obtained in step (1) and react at 100° C. for 12 hours to generate a high-temperature desulfurization agent, referred to as “HDSF74”, wherein:

[0603] The compound represented by the structure of formula (Z):

[0604] in:

[0605] R5 is a C3 alkylene group;

[0606] B is n-butyl; in another embodiment, B is a C3 hydrocarbon group containing a substituent, wherein: the C1-C 20 The substituent of the hydrocarbon group is hydroxyl; in another embodiment, B is a C3 hydrocarbon group containing a substituent, wherein: the C1-C 20 The substituent of the hydrocarbon group is a carboxyl group; in another embodiment, B is a C3 hydrocarbon group containing a substituent, wherein: the C1-C 20 The substituent of the hydrocarbon group is an amine group.

[0607] In another embodiment, the reaction temperature of step (1) is 80° C. and the reaction time is 6.5 h.

[0608] In another embodiment, the reaction temperature of step (2) is 100° C., and the reaction time is 10 h; in another embodiment, the reaction temperature of step (2) is 60° C., and the reaction time is 8 h.

[0609] Furthermore, in step (2), 1 part of a first catalyst is added, and the first catalyst is a mixture of equal masses of HBTU, DMC, HOBT, HATU, DCC, CDI and propyl chloroformate; in another embodiment, the first catalyst is HBTU; in another embodiment, the first catalyst is DMC; in another embodiment, the first catalyst is HOBT; in another embodiment, the first catalyst is HATU; in another embodiment, the first catalyst is DCC; in another embodiment, the first catalyst is CDI; in another embodiment, the first catalyst is propyl chloroformate.

[0610] The high-temperature desulfurization agent composition is composed of the above-mentioned high-temperature desulfurization agent, water and an auxiliary agent, wherein:

[0611] The mass ratio of high-temperature desulfurizer, water and additive is 35:45:5, referred to as "HDSF74 group".

[0612] Furthermore, the auxiliary agent is a dispersant.

[0613] Furthermore, the dispersant is sodium hexametaphosphate.

[0614] The high-temperature desulfurizer prepared by the above preparation method and any of the above high-temperature desulfurizer compositions are used as desulfurizers.

[0615] Desulfurization effect evaluation

[0616] Preparation method of desulfurizer: add 40g of the sample to be tested, 0.1g of defoaming agent, and 0.8g of pH adjuster into 100g of water, and stir at 60℃ for 2h to mix the solution evenly.

[0617] The desulfurizing agents were prepared using triazine, HDSF44-HDSF74, and HDSF44 group-HDSF74 group, respectively (ie, the samples to be tested were selected from triazine, HDSF44-HDSF74, and HDSF44 group-HDSF74 group, respectively).

[0618] Desulfurization effect method: Weigh 3g of chemically pure Na2S·9H2O, add it to a 1000mL wide-mouth bottle, then add about 200g of desalted water, cover it with a rubber stopper connected to the detection tube and the constant pressure dropping funnel, and keep the detection tube of the pump suction hydrogen sulfide detector above the reaction liquid surface. Add a stirring magnet, put the wide-mouth bottle in a 95°C water bath, turn on the magnetic stirring, and then drip a certain amount of H2SO4 solution into the constant pressure dropping funnel, add a certain amount of solution, and use the hydrogen sulfide detector to detect the concentration of hydrogen sulfide in the wide-mouth bottle after 5 minutes as the initial concentration. Quickly drip 3g of the sample to be tested, turn on the hydrogen sulfide detector to detect the concentration of hydrogen sulfide in the wide-mouth bottle at intervals, end the test after 30 minutes, and record the hydrogen sulfide concentration. The experimental results are shown in Table 1.

[0619] Table 1 Desulfurization agent indoor desulfurization test results

[0620]

[0621]

[0622]

[0623] It can be seen from Table 1 that the high-temperature desulfurizer of the present invention has a good indoor desulfurization effect, with a desulfurization rate of more than 90%; while the desulfurization rate of triazine is 78.9%, which is significantly lower than the desulfurization rate of the high-temperature desulfurizer of the present invention.

[0624] (2) Field test

[0625] Oil well A of an oil production plant in Shengli Oilfield 13 , liquid volume 25m 3 / d, wellhead hydrogen sulfide content 2500ppm, reservoir temperature 145℃. Field tests were conducted using triazine desulfurizer and "HDSF46 group" high-temperature desulfurizer, respectively, with a dosage of 40kg / d. After 20 days, the hydrogen sulfide content was tested, and the results are shown in Table 2.

[0626] Table 2 Desulfurization agent on-site desulfurization test results

[0627] Desulfurization agent type Hydrogen sulfide concentration (ppm) Desulfurization rate (%) Triazine 320 87.2 HDSF46 Group 20 99.2%

[0628] It can be seen from Table 2 that the high-temperature desulfurizer of the present invention has a good on-site desulfurization effect, and the desulfurization rate of the desulfurizer HDSF3 reaches 99.2%; while the desulfurization rate of triazine is 87.2%, which is significantly lower than the desulfurization rate of the high-temperature desulfurizer of the present invention.

[0629] The above describes the embodiments of the present invention in detail. However, the present invention is not limited to the above embodiments, and various changes can be made within the knowledge of ordinary technicians in the relevant technical field without departing from the purpose of the present invention.

Claims

1. A high temperature desulfurizing agent, characterized in that: Its molecular structure is shown in formula (1): R'-ML Formula (1), where R' is a structure shown in formula (2): in: R1 is one of H, C1-C8 hydrocarbon group, and C1-C8 hydrocarbon group containing a substituent, wherein the substituent of the C1-C8 hydrocarbon group containing a substituent is one or more of hydroxyl group, carboxyl group, and amine group; R1 is preferably H, C1-C6 hydrocarbon group, and C1-C6 hydrocarbon group containing a substituent, wherein the substituent of the C1-C6 hydrocarbon group containing a substituent is one or more of hydroxyl group, carboxyl group, and amine group; R2 is one of H, C1-C8 hydrocarbon group, and C1-C8 hydrocarbon group containing a substituent, wherein the substituent of the C1-C8 hydrocarbon group containing a substituent is one or more of hydroxyl, carboxyl, and amine; R2 is preferably H, C1-C6 hydrocarbon group, and C1-C6 hydrocarbon group containing a substituent, wherein the substituent of the C1-C6 hydrocarbon group containing a substituent is one or more of hydroxyl, carboxyl, and amine; R3 is a C1-C8 alkylene group, preferably a C1-C6 alkylene group, more preferably a C1-C3 alkylene group; M is a structure shown in formula (3): in: R4 is C1-C 10 An alkylene group, preferably a C1-C6 alkylene group, more preferably a C1-C4 alkylene group; R5 is C1-C 10 An alkylene group, preferably a C1-C6 alkylene group, more preferably a C1-C4 alkylene group; L is a structure shown in formula (4): In the formula, B is C1-C 20 Hydrocarbon groups, C1-C 20 One of the hydrocarbon groups, wherein: a C1-C 20 The substituent of the hydrocarbon group is one or more of hydroxyl, carboxyl, and amine; B is preferably C1-C 10 Hydrocarbon groups, C1-C 10 One of the hydrocarbon groups, wherein: a C1-C 10 The substituent of the hydrocarbon group is one or more of hydroxyl, carboxyl and amine groups, and B is more preferably a C1-C5 hydrocarbon group or a C1-C5 hydrocarbon group containing a substituent, wherein the substituent of the C1-C5 hydrocarbon group containing a substituent is one or more of hydroxyl, carboxyl and amine groups.

2. A high temperature desulfurization agent as claimed in claim 1, characterized in that: The high-temperature desulfurizing agent is one of the compounds of formula (5), formula (6), and formula (7):

3. A high temperature desulfurizing agent, characterized in that: The molecular structure is shown in formula (8): in: R1 is one of H, C1-C8 hydrocarbon group, and C1-C8 hydrocarbon group containing a substituent, wherein the substituent of the C1-C8 hydrocarbon group containing a substituent is one or more of hydroxyl group, carboxyl group, and amine group; R1 is preferably H, C1-C6 hydrocarbon group, and C1-C6 hydrocarbon group containing a substituent, wherein the substituent of the C1-C6 hydrocarbon group containing a substituent is one or more of hydroxyl group, carboxyl group, and amine group; R2 is one of H, C1-C8 hydrocarbon group, and C1-C8 hydrocarbon group containing a substituent, wherein the substituent of the C1-C8 hydrocarbon group containing a substituent is one or more of hydroxyl, carboxyl, and amine; R2 is preferably H, C1-C6 hydrocarbon group, and C1-C6 hydrocarbon group containing a substituent, wherein the substituent of the C1-C6 hydrocarbon group containing a substituent is one or more of hydroxyl, carboxyl, and amine; R3 is a C1-C8 alkylene group, preferably a C1-C6 alkylene group, more preferably a C1-C3 alkylene group; R4 is C1-C 10 An alkylene group, preferably a C1-C6 alkylene group, more preferably a C1-C4 alkylene group; R5 is C1-C 10 The alkylene group is preferably a C1-C6 alkylene group, and more preferably a C1-C4 alkylene group.

4. A high-temperature desulfurizing agent, characterized in that: The molecular structure is shown in formula (9): in: B is C1-C 20 Hydrocarbon groups, C1-C 20 One of the hydrocarbon groups, wherein: a C1-C 20 The substituent of the hydrocarbon group is one or more of hydroxyl, carboxyl, and amine; B is preferably C1-C 10 Hydrocarbon groups, C1-C 10 One of the hydrocarbon groups, wherein: a C1-C 10 The substituent of the hydrocarbon group is one or more of hydroxyl, carboxyl, and amine. B is more preferably a C1-C5 hydrocarbon group or a C1-C5 hydrocarbon group containing a substituent, wherein the substituent of the C1-C5 hydrocarbon group containing a substituent is one or more of hydroxyl, carboxyl, and amine. R3 is a C1-C8 alkylene group, preferably a C1-C6 alkylene group, more preferably a C1-C3 alkylene group; R4 is C1-C 10 An alkylene group, preferably a C1-C6 alkylene group, more preferably a C1-C4 alkylene group; R5 is C1-C 10 An alkylene group, preferably a C1-C6 alkylene group, more preferably a C1-C4 alkylene group; R6 is a C1-C8 alkylene group, preferably a C1-C6 alkylene group, and more preferably a C1-C3 alkylene group; R7 is a C1-C8 alkylene group, preferably a C1-C6 alkylene group, and more preferably a C1-C3 alkylene group.

5. A method for synthesizing the high-temperature desulfurizer according to any one of claims 1 to 4, characterized in that: In terms of molar parts, the steps are as follows: (1) 0.8-1.3 parts of a compound having a structure represented by formula (Y), 0.8-1.0 parts of a compound having a structure represented by formula (Z) and 0.5-2 parts of a first catalyst are reacted at 0-300° C. for 5-30 hours to generate an amide reaction product, wherein: The compound represented by the structure of formula (Y): R4 is C1-C 10 An alkylene group, preferably a C1-C6 alkylene group, more preferably a C1-C4 alkylene group; A' is OR a , F, Cl, Br, I, where R a H, C 1~ One of the C4 alkyl groups; A″ is OR a , F, Cl, Br, I, where R a H, C 1~ One of the C4 alkyl groups; The compound represented by the structure of formula (Z): in: R5 is C1-C 10 An alkylene group, preferably a C1-C6 alkylene group, more preferably a C1-C4 alkylene group; B is C1-C 20 Hydrocarbon groups, C1-C 20 One of the hydrocarbon groups, wherein: a C1-C 20 The substituent of the hydrocarbon group is one or more of hydroxyl, carboxyl, and amine; B is preferably C1-C 10 Hydrocarbon groups, C1-C 10 One of the hydrocarbon groups, wherein: a C1-C 10 The substituent of the hydrocarbon group is one or more of hydroxyl, carboxyl, and amine. B is more preferably a C1-C5 hydrocarbon group or a C1-C5 hydrocarbon group containing a substituent, wherein the substituent of the C1-C5 hydrocarbon group containing a substituent is one or more of hydroxyl, carboxyl, and amine. (2) placing 0.8-1.3 parts of the compound having the structure represented by formula (X) into the amide reaction product obtained in step (1), and then reacting at 50-300° C. for 5-24 hours to generate a high-temperature desulfurization agent, wherein: The compound represented by the structure of formula (X): in: R3 is a C1-C8 alkylene group, preferably a C1-C6 alkylene group, more preferably a C1-C3 alkylene group; R8 is one of H, C1-C8 hydrocarbon group, and C1-C8 hydrocarbon group containing a substituent, wherein the substituent of the C1-C8 hydrocarbon group containing a substituent is one or more of hydroxyl, carboxyl, and amine; R8 is preferably one of H, C1-C6 hydrocarbon group, and C1-C6 hydrocarbon group containing a substituent, wherein the substituent of the C1-C6 hydrocarbon group containing a substituent is one or more of hydroxyl, carboxyl, and amine; R9 is one of H, C1-C8 hydrocarbon group, and C1-C8 hydrocarbon group containing substituents, wherein the substituents of the C1-C8 hydrocarbon group containing substituents are one or more of hydroxyl, carboxyl, and amine groups; R9 is preferably one of H, C1-C6 hydrocarbon group, and C1-C6 hydrocarbon group containing substituents, wherein the substituents of the C1-C6 hydrocarbon group containing substituents are one or more of hydroxyl, carboxyl, and amine groups.

6. The method for synthesizing a high-temperature desulfurizing agent according to claim 5, characterized in that: The first catalyst is one or more of HBTU, DMC, HOBT, HATU, DCC, CDI and propyl chloroformate.

7. The method for synthesizing a high-temperature desulfurizing agent according to claim 5, characterized in that: The reaction temperature of step (1) is 0-200°C, and the reaction time is 5-20h. More preferably, the reaction temperature of step (1) is 0-110°C, and the reaction time is 5-12h. The reaction temperature of step (2) is 0-200° C., and the reaction time is 5-12 h.

8. The method for synthesizing a high-temperature desulfurizing agent according to claim 5, characterized in that: In step (2), 0.05-0.12 parts of a second catalyst are also added.

9. The method for synthesizing a high-temperature desulfurizing agent according to claim 8, characterized in that: The second catalyst is one or more of an inorganic acid, an organic acid, a metal salt of an organic acid, and an acidic resin.

10. The method for synthesizing a high-temperature desulfurizing agent according to claim 9, characterized in that: The inorganic acid is one or more of sulfuric acid, hydrochloric acid, nitric acid, phosphoric acid, boric acid and heteropoly acid; The organic acid is one or more of benzenesulfonic acid, cyclohexanesulfonic acid and methanesulfonic acid; The metal salt of the organic acid is one or more of a zinc salt of the organic acid, a potassium salt of the organic acid and a sodium salt of the organic acid.

11. A method for synthesizing the high-temperature desulfurizing agent according to any one of claims 1 to 4, characterized in that: In terms of molar parts, the steps are as follows: (1) reacting 0.8-1.3 parts of an anhydride of a compound of formula (Y') with 0.8-1.0 parts of a compound of formula (Z) at 0-300° C. for 5-30 hours to generate an amide reaction product, wherein: The structure of the acid anhydride of the compound represented by the structure of formula (Y') is as follows: Where: R a H, C 1~ One of the C4 alkyl groups; The compound represented by the structure of formula (Z): in: R5 is C1-C 10 An alkylene group, preferably a C1-C6 alkylene group, more preferably a C1-C4 alkylene group; B is C1-C 20 Hydrocarbon groups, C1-C 20 One of the hydrocarbon groups, wherein: a C1-C 20 The substituent of the hydrocarbon group is one or more of hydroxyl, carboxyl, and amine; B is preferably C1-C 10 Hydrocarbon groups, C1-C 10 One of the hydrocarbon groups, wherein: a C1-C 10 The substituent of the hydrocarbon group is one or more of hydroxyl, carboxyl, and amine. B is more preferably a C1-C5 hydrocarbon group or a C1-C5 hydrocarbon group containing a substituent, wherein the substituent of the C1-C5 hydrocarbon group containing a substituent is one or more of hydroxyl, carboxyl, and amine. (2) adding 0.8-1.3 parts of the compound having the structure represented by formula (X) to the amide reaction product obtained in step (1), and reacting at 50-300° C. for 5-24 hours to generate a high-temperature desulfurization agent, wherein: The compound represented by the structure of formula (X): in: R3 is a C1-C8 alkylene group, preferably a C1-C6 alkylene group, more preferably a C1-C3 alkylene group; R8 is one of H, C1-C8 hydrocarbon group, and C1-C8 hydrocarbon group containing a substituent, wherein the substituent of the C1-C8 hydrocarbon group containing a substituent is one or more of hydroxyl, carboxyl, and amine; R8 is preferably one of H, C1-C6 hydrocarbon group, and C1-C6 hydrocarbon group containing a substituent, wherein the substituent of the C1-C6 hydrocarbon group containing a substituent is one or more of hydroxyl, carboxyl, and amine; R9 is one of H, C1-C8 hydrocarbon group, and C1-C8 hydrocarbon group containing substituents, wherein the substituents of the C1-C8 hydrocarbon group containing substituents are one or more of hydroxyl, carboxyl, and amine groups; R9 is preferably one of H, C1-C6 hydrocarbon group, and C1-C6 hydrocarbon group containing substituents, wherein the substituents of the C1-C6 hydrocarbon group containing substituents are one or more of hydroxyl, carboxyl, and amine groups.

12. The method for synthesizing a high-temperature desulfurizing agent according to claim 11, characterized in that: The reaction temperature in step (1) is 0-200° C., and the reaction time is 5-20 h. Preferably, the reaction temperature in step (1) is 0-110° C., and the reaction time is 5-12 h. The reaction temperature of step (2) is 0-200° C., and the reaction time is 5-12 h.

13. The method for synthesizing a high-temperature desulfurizing agent according to claim 11, characterized in that: In step (2), 0.08-0.12 parts of a second catalyst are also added.

14. The method for synthesizing a high-temperature desulfurizing agent according to claim 13, characterized in that: The second catalyst is one or more of an inorganic acid, an organic acid, a metal salt of an organic acid, and an acidic resin.

15. The method for synthesizing a high-temperature desulfurizing agent according to claim 14, characterized in that: The inorganic acid is one or more of sulfuric acid, hydrochloric acid, nitric acid, phosphoric acid, boric acid and heteropoly acid; Still further, the organic acid is one or more of benzenesulfonic acid, cyclohexanesulfonic acid and methanesulfonic acid; Furthermore, the metal salt of the organic acid is one or more of a zinc salt of an organic acid, a potassium salt of an organic acid and a sodium salt of an organic acid.

16. A method for synthesizing the high-temperature desulfurizing agent according to any one of claims 1 to 4, characterized in that: In terms of molar parts, the steps are as follows: (1) 0.8-1.3 parts of a compound having a structure represented by formula (X), 0.8-1.0 parts of a compound having a structure represented by formula (Y), and 0.05-0.12 parts of a second catalyst are reacted at 50-300° C. for 5-24 hours to generate an ester reaction product, wherein: The compound represented by the structure of formula (X): in: R3 is a C1-C8 alkylene group, preferably a C1-C6 alkylene group, more preferably a C1-C3 alkylene group; R8 is one of H, C1-C8 hydrocarbon group, and C1-C8 hydrocarbon group containing a substituent, wherein the substituent of the C1-C8 hydrocarbon group containing a substituent is one or more of hydroxyl, carboxyl, and amine; R8 is preferably one of H, C1-C6 hydrocarbon group, and C1-C6 hydrocarbon group containing a substituent, wherein the substituent of the C1-C6 hydrocarbon group containing a substituent is one or more of hydroxyl, carboxyl, and amine; R9 is one of H, C1-C8 hydrocarbon group, and C1-C8 hydrocarbon group containing a substituent, wherein the substituent of the C1-C8 hydrocarbon group containing a substituent is one or more of hydroxyl group, carboxyl group, and amine group; R9 is preferably one of H, C1-C6 hydrocarbon group, and C1-C6 hydrocarbon group containing a substituent, wherein the substituent of the C1-C6 hydrocarbon group containing a substituent is one or more of hydroxyl group, carboxyl group, and amine group; The compound represented by the structure of formula (Y): R4 is C1-C 10 An alkylene group, preferably a C1-C6 alkylene group, more preferably a C1-C4 alkylene group; A' is OR a , F, Cl, Br, I, where R a H, C 1~ One of the C4 alkyl groups; A″ is OR a , F, Cl, Br, I, where R a H, C 1~ One of the C4 alkyl groups; (2) Place 0.8-1.3 parts of the compound having the structure represented by formula (Z) in the ester reaction product obtained in step (1), and react at 0-300° C. for 5-30 hours to generate a high-temperature desulfurization agent, wherein: The compound represented by the structure of formula (Z): in: R5 is C1-C 10 An alkylene group, preferably a C1-C6 alkylene group, more preferably a C1-C4 alkylene group; B is C1-C 20 Hydrocarbon groups, C1-C 20 One of the hydrocarbon groups, wherein: a C1-C 20 The substituent of the hydrocarbon group is one or more of hydroxyl, carboxyl, and amine; B is preferably C1-C 10 Hydrocarbon groups, C1-C 10 One of the hydrocarbon groups, wherein: a C1-C 10 The substituent of the hydrocarbon group is one or more of hydroxyl, carboxyl and amine groups, and B is more preferably a C1-C5 hydrocarbon group or a C1-C5 hydrocarbon group containing a substituent, wherein the substituent of the C1-C5 hydrocarbon group containing a substituent is one or more of hydroxyl, carboxyl and amine groups.

17. The method for synthesizing a high-temperature desulfurizing agent according to claim 16, characterized in that: The reaction temperature of step (1) is 0-200° C. and the reaction time is 5-12 h; The reaction temperature of step (2) is 0-200° C., and the reaction time is 5-20 h. Preferably, the reaction temperature is 0-110° C., and the reaction time is 5-12 h.

18. The method for synthesizing a high-temperature desulfurizing agent according to claim 16, characterized in that: In step (1), the second catalyst is one or more of an inorganic acid, an organic acid, a metal salt of an organic acid and an acidic resin.

19. The method for synthesizing a high-temperature desulfurizing agent according to claim 18, characterized in that: The inorganic acid is selected from one or more of sulfuric acid, hydrochloric acid, nitric acid, phosphoric acid, boric acid and heteropoly acid; The organic acid is selected from one or more of benzenesulfonic acid, cyclohexanesulfonic acid and methanesulfonic acid; The metal salt of the organic acid is selected from one or more of the zinc salt of the organic acid, the potassium salt of the organic acid and the sodium salt of the organic acid.

20. The method for synthesizing a high-temperature desulfurizing agent according to claim 16, characterized in that: In step (2), 0.5-2 parts of a first catalyst are also added, wherein the first catalyst is one or more of HBTU, DMC, HOBT, HATU, DCC, CDI and propyl chloroformate.

21. A method for synthesizing the high-temperature desulfurizing agent according to any one of claims 1 to 4, characterized in that: In terms of molar parts, the steps are as follows: (1) reacting 0.8-1.3 parts of a compound of formula (X) with 0.8-1.0 parts of an anhydride of a compound of formula (Y') at 50-300° C. for 5-24 hours to produce an ester reaction product, wherein: The compound represented by the structure of formula (X): in: R3 is a C1-C8 alkylene group, preferably a C1-C6 alkylene group, more preferably a C1-C3 alkylene group; R8 is one of H, C1-C8 hydrocarbon group, and C1-C8 hydrocarbon group containing a substituent, wherein the substituent of the C1-C8 hydrocarbon group containing a substituent is one or more of hydroxyl, carboxyl, and amine; R8 is preferably one of H, C1-C6 hydrocarbon group, and C1-C6 hydrocarbon group containing a substituent, wherein the substituent of the C1-C6 hydrocarbon group containing a substituent is one or more of hydroxyl, carboxyl, and amine; R9 is one of H, C1-C8 hydrocarbon group, and C1-C8 hydrocarbon group containing a substituent, wherein the substituent of the C1-C8 hydrocarbon group containing a substituent is one or more of hydroxyl group, carboxyl group, and amine group; R9 is preferably one of H, C1-C6 hydrocarbon group, and C1-C6 hydrocarbon group containing a substituent, wherein the substituent of the C1-C6 hydrocarbon group containing a substituent is one or more of hydroxyl group, carboxyl group, and amine group; The structure of the acid anhydride of the compound represented by the structure of formula (Y') is as follows: Where: R a H, C 1~ One of the C4 alkyl groups; (2) adding 0.8-1.3 parts of the compound having the structure represented by formula (Z) to the ester reaction product obtained in step (1) and reacting at 0-300° C. for 5-30 hours to generate a high-temperature desulfurization agent, wherein: The compound represented by the structure of formula (Z): in: R5 is C1-C 10 An alkylene group, preferably a C1-C6 alkylene group, more preferably a C1-C4 alkylene group; B is C1-C 20 Hydrocarbon groups, C1-C 20 One of the hydrocarbon groups, wherein: a C1-C 20 The substituent of the hydrocarbon group is one or more of hydroxyl, carboxyl, and amine; B is preferably C1-C 10 Hydrocarbon groups, C1-C 10 One of the hydrocarbon groups, wherein: a C1-C 10 The substituent of the hydrocarbon group is one or more of hydroxyl, carboxyl and amine groups, and B is more preferably a C1-C5 hydrocarbon group or a C1-C5 hydrocarbon group containing a substituent, wherein the substituent of the C1-C5 hydrocarbon group containing a substituent is one or more of hydroxyl, carboxyl and amine groups.

22. The method for synthesizing a high-temperature desulfurizing agent according to claim 21, characterized in that: The reaction temperature of step (1) is 0-200° C. and the reaction time is 5-12 h; The reaction temperature of step (2) is 0-200° C., and the reaction time is 5-20 h. Preferably, the reaction temperature is 0-110° C., and the reaction time is 5-12 h.

23. The method for synthesizing a high-temperature desulfurizing agent according to claim 21, characterized in that: In step (2), 0.5-2 parts of a first catalyst are also added, wherein the first catalyst is one or more of HBTU, DMC, HOBT, HATU, DCC, CDI and propyl chloroformate.

24. A high-temperature desulfurization agent composition, characterized in that: It is composed of the high-temperature desulfurizer according to any one of claims 1 to 4, water and an additive, wherein: The mass ratio of the high-temperature desulfurizer, water and auxiliary agent is (30-40): (30-50): (1-10).

25. The high-temperature desulfurization agent composition according to claim 24, characterized in that: The auxiliary agent is one or more of an antioxidant, a corrosion inhibitor, a pH regulator, a defoaming agent, and a dispersant.

26. The high-temperature desulfurization agent composition according to claim 24, characterized in that: The antioxidant is one of a hindered phenol antioxidant and an amine antioxidant; The corrosion inhibitor is one of nitrite, silicate, phosphoric acid, and phosphate; The pH regulator is one of sodium hydroxide, sodium carbonate, hydrochloric acid and phosphoric acid; The defoamer is one of polysiloxane defoamer and polyether modified silicone oil; The dispersant is one of sodium tripolyphosphate, sodium hexametaphosphate, triethylhexyl phosphate and sodium dodecyl sulfate.

27. Use of the high-temperature desulfurizer according to any one of claims 1 to 4, the high-temperature desulfurizer prepared by the preparation method according to any one of claims 5 to 22, or the high-temperature desulfurizer composition according to any one of claims 24 to 26 as a desulfurizer.

Citation Information

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