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CN111233796A - Preparation method of 2, 5-furandimethanol - Google Patents

Preparation method of 2, 5-furandimethanol Download PDF

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Publication number
CN111233796A
CN111233796A CN202010130668.3A CN202010130668A CN111233796A CN 111233796 A CN111233796 A CN 111233796A CN 202010130668 A CN202010130668 A CN 202010130668A CN 111233796 A CN111233796 A CN 111233796A
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solvent
hydroxymethylfurfural
solution
furandimethanol
preparation
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王磊
何凤林
金海涛
张建
胡华雷
杨勇
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Zhejiang Tangneng Technology Co ltd
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Zhejiang Tangneng Technology Co ltd
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    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07DHETEROCYCLIC COMPOUNDS
    • C07D307/00Heterocyclic compounds containing five-membered rings having one oxygen atom as the only ring hetero atom
    • C07D307/02Heterocyclic compounds containing five-membered rings having one oxygen atom as the only ring hetero atom not condensed with other rings
    • C07D307/34Heterocyclic compounds containing five-membered rings having one oxygen atom as the only ring hetero atom not condensed with other rings having two or three double bonds between ring members or between ring members and non-ring members
    • C07D307/38Heterocyclic compounds containing five-membered rings having one oxygen atom as the only ring hetero atom not condensed with other rings having two or three double bonds between ring members or between ring members and non-ring members with substituted hydrocarbon radicals attached to ring carbon atoms
    • C07D307/40Radicals substituted by oxygen atoms
    • C07D307/42Singly bound oxygen atoms

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  • Organic Chemistry (AREA)
  • Organic Low-Molecular-Weight Compounds And Preparation Thereof (AREA)

Abstract

The application discloses a preparation method of 2, 5-furandimethanol, which at least comprises the following steps: reacting a material A containing 5-hydroxymethylfurfural with sodium borohydride in a solvent to obtain 2, 5-furandimethanol; the solvent contains water. The preparation method for reducing sodium borohydride provided by the invention has the characteristics of simple system, low energy consumption and suitability for industrial production.

Description

Preparation method of 2, 5-furandimethanol
Technical Field
The application relates to a preparation method of 2, 5-furandimethanol, belonging to the field of biomass energy chemical industry.
Background
5-Hydroxymethylfurfural (HMF) is used as an important platform compound in the field of biomass energy, the molecule of the HMF contains a furan ring, an aldehyde group and a hydroxymethyl group, the chemical property is active, and a series of other novel furan derivatives with high added values can be synthesized through chemical actions such as hydrogenation, oxidative dehydrogenation, esterification, halogenation, polymerization and the like.
2, 5-furandimethanol (BHMF) is an important selective hydrogenation product of HMF, can be applied to adhesives, plasticizers, surfactants, drug intermediates and the like, can also be used as monomer synthetic resin materials, fiber materials, foam materials and the like (CN107442177A), and has wide application value.
At present, in the research of preparing 2, 5-furandimethanol by selective hydrogenation of 5-hydroxymethylfurfural, noble metals (Pt, Pd, Ru and the like) or non-noble metals (Ag, Co, Ni, Cu and the like) are mainly used as catalysts, and hydrogen is directly hydrogenated or is subjected to catalytic transfer hydrogenation, but some problems are inevitable. If the catalyst is complicated in preparation process, high in cost and poor in recycling effect; the hydrogenation reaction process has long high-temperature and high-pressure time, high energy consumption, high requirement on equipment and the like.
In addition, the current reports mainly focus on the selective hydrogenation of pure HMF raw materials to prepare BHMF, and the reports on the recovery and utilization of HMF from HMF with low purity and even production waste have not been found yet.
Disclosure of Invention
According to one aspect of the application, the simple method for recovering and preparing the 2, 5-furandimethanol from the 5-hydroxymethylfurfural production waste is simple in system, low in energy consumption and suitable for industrial production.
According to one aspect of the present application, there is provided a process for the preparation of 2, 5-furandimethanol, said process comprising at least: reacting a material A containing 5-hydroxymethylfurfural with sodium borohydride in a solvent to obtain the 2, 5-furandimethanol;
the solvent contains water.
Optionally, the mass ratio of the 5-hydroxymethylfurfural to the sodium borohydride is 2-13: 1.
alternatively, the upper limit of the mass ratio of 5-hydroxymethylfurfural to sodium borohydride is independently selected from 13: 1. 12: 1. 11: 1. 10: 1. 9: 1. 8: 1. 7: 1. 6: 1. 5: 1. 4: 1. 3: 1; the lower limit is independently selected from 12: 1. 10: 1. 8: 1. 6: 1. 4: 1. 2: 1.
optionally, the reaction conditions are: the reaction temperature is 7-50 ℃; the reaction time is 1-8 h.
Optionally, the upper reaction temperature limit is independently selected from 50 ℃, 40 ℃, 30 ℃, 20 ℃, 10 ℃; the lower limit is independently selected from 7 deg.C, 10 deg.C, 20 deg.C, 30 deg.C, and 40 deg.C.
Optionally, the upper reaction time limit is independently selected from 8h, 6h, 4h, 2 h; the lower limit is independently selected from 7h, 5h, 3h, 1 h.
Optionally, the method comprises at least: mixing a material A containing 5-hydroxymethylfurfural, a solution B containing sodium borohydride and a solvent I, and reacting to obtain the 2, 5-furandimethanol.
Optionally, the method comprises at least: and sequentially adding a material A containing 5-hydroxymethylfurfural, a solvent I and a solution B containing sodium borohydride into a reactor with a stirrer and a thermocouple for reaction to obtain the 2, 5-furandimethanol.
Optionally, the stirring is mechanical stirring, and the speed of the mechanical stirring is 100-500 rmp/min.
Optionally, the mass ratio of the solvent I to the material A is 1-10: 1.
optionally, the upper limit of the mass ratio of the solvent I to the material A is independently selected from 10: 1. 9: 1. 8: 1. 7: 1. 6: 1. 5: 1. 4: 1. 3: 1. 2: 1; the lower limit is independently selected from 9: 1. 8: 1. 7: 1. 6: 1. 5: 1. 4: 1. 3: 1. 2: 1. 1: 1.
preferably, the solvent I is water.
Optionally, the mass content of the 5-hydroxymethylfurfural in the material A is 20-100%.
Optionally, the upper limit of the mass content of the 5-hydroxymethylfurfural in the material A is independently selected from 100%, 90%, 80%, 70%, 60%, 50%, 40%, 30%; the lower limit is independently selected from 90%, 80%, 70%, 60%, 50%, 40%, 30%, 20%.
Optionally, the material A containing 5-hydroxymethylfurfural is at least one selected from production waste with 5-hydroxymethylfurfural remaining, crude 5-hydroxymethylfurfural with more impurities, and waste liquid with 5-hydroxymethylfurfural remaining.
Optionally, the waste material also contains impurities such as acetic acid, ethyl acetate, n-hexane and the like.
Optionally, the waste material is present in the form of a solid or liquid.
Optionally, the solution B includes a solvent II, and a mass ratio of the sodium borohydride to the solvent II in the solution B is 1: 2-10;
alternatively, the upper limit of the mass ratio of the sodium borohydride to the solvent II in the solution B is independently selected from 1: 2. 1: 4. 1: 6. 1: 8; the lower limit is independently selected from 1: 3. 1: 5. 1: 7. 1: 9. 1: 10.
preferably, the solvent II is water.
Optionally, the method comprises at least the following steps:
(1) mixing a material A containing 5-hydroxymethylfurfural with a solvent I to obtain a solution C;
(2) obtaining solution B containing sodium borohydride;
(3) and mixing the solution C with the solution B, and reacting to obtain the 2, 5-furandimethanol.
Optionally, the step (3) comprises at least the following steps:
and mixing the solution C with the solution B, reacting, performing rotary evaporation, extracting, performing rotary evaporation, and centrifuging to obtain the 2, 5-furandimethanol.
Optionally, the step (3) comprises at least the following steps: and mixing the solution C with the solution B, reacting, standing, filtering, performing rotary evaporation, extracting, performing rotary evaporation, and centrifuging to obtain the 2, 5-furandimethanol.
Optionally, the standing time is 5-48 h, so as to wait for solid-liquid layering.
Optionally, the conditions of the rotary evaporation are as follows: the rotary evaporation temperature is 30-80 ℃; the rotary evaporation speed is 40-100 rmp/min.
Preferably, the conditions of the centrifugation are: the centrifugal rotating speed is 1000-2500 rmp/min; centrifuging for 10-60 min; the mesh number of the filter cloth is 600-2000 meshes.
Preferably, the extraction is carried out with solvent III; the solvent III is at least one selected from ethyl acetate and petroleum ether.
Preferably, the method comprises at least:
1) sequentially adding a material A containing 5-hydroxymethylfurfural, a solvent I and a solution B containing sodium borohydride into a reactor with a stirrer and a thermocouple for reaction;
2) standing the material obtained in the step 1) for a period of time, and then taking the upper layer liquid for rotary evaporation to remove most of the solvent;
3) extracting the material obtained in the step 2) by using a solvent III, then carrying out rotary evaporation to remove the solvent III, and then centrifuging to obtain the 2, 5-furandimethanol.
The beneficial effects that this application can produce include:
(1) the method can be suitable for waste materials containing 5-hydroxymethylfurfural produced by different production modes, has low requirements on the purity and the content of the 5-hydroxymethylfurfural in the raw materials, has wide adaptability, can effectively realize the large-scale recycling and conversion of important biological platform compounds of the 5-hydroxymethylfurfural, and avoids resource waste;
(2) the preparation method for reducing sodium borohydride provided by the application has the characteristics of simple system, low energy consumption and suitability for industrial production.
(3) The method for preparing 2, 5-furandimethanol (BHMF) from 5-Hydroxymethylfurfural (HMF) provided by the application has high HMF conversion rate, high BHMF yield and excellent stability; the reaction product is simple to separate, and the high-purity BHMF product can be obtained by extraction, rotary evaporation and centrifugation.
Detailed Description
The present application will be described in detail with reference to examples, but the present application is not limited to these examples.
The raw materials in the examples of the present application were all purchased commercially, unless otherwise specified.
In the examples, a product obtained by selective hydrogenation of 5-Hydroxymethylfurfural (HMF) to 2, 5-furandimethanol (BHMF) was analyzed by a model 1260 high performance liquid chromatograph from Agilent, and quantified by an external standard method.
The conversion rate of 5-hydroxymethylfurfural and the yield of 2, 5-furandimethanol in the reaction for preparing 2, 5-furandimethanol (BHMF) by selective hydrogenation of 5-Hydroxymethylfurfural (HMF) are calculated as follows:
the 5-hydroxymethylfurfural conversion and 2, 5-furandimethanol yield were calculated based on the moles of molecules tested:
Figure BDA0002395694570000041
Figure BDA0002395694570000042
example 1
100g of purified liquid waste A1 (containing impurities such as acetic acid, ethyl acetate and n-hexane except HMF) containing 5-hydroxymethylfurfural (80 wt%) is added into a 2L beaker, and then 300ml of solvent water is added and stirred for 30min, which is recorded as C1 liquid. Then 40g of sodium borohydride is weighed and slowly and completely dissolved in 100ml of water with stirring, and the solution is marked as B1 solution. Then the B1 liquid is slowly dripped into the C1 liquid, the reaction process releases heat, the dripping speed is controlled so as to avoid overheating, and the temperature is 30 ℃. After the liquid B1 was completely added, the reaction was started for 5 hours and recorded as liquid D1. And standing the D1 liquid material overnight, taking the upper layer liquid, carrying out rotary evaporation at 65 ℃ and 80rmp/min, removing most of solvent to obtain a viscous substance, extracting with ethyl acetate, carrying out rotary evaporation at 45 ℃ and 100rmp/min, and carrying out centrifugal separation with 1000-mesh filter cloth (the centrifugal rotation speed is 1500rmp/min, the centrifugal time is 30min) to remove ethyl acetate, thus obtaining the 2, 5-furandimethanol. And (3) testing and analyzing the liquid taken before and after the hydrogenation reaction by using a high performance liquid chromatograph, and calculating the conversion rate of 5-hydroxymethylfurfural to be 100% and the yield of 2, 5-furandimethanol to be 99%.
Example 2
100g of production centrifugal waste A2 (except HMF, the waste contains impurities such as OBMF, acetic acid, ethyl acetate, n-hexane and the like) containing 5-hydroxymethylfurfural (50 wt%) is added into a 2L beaker, and then 300ml of solvent water is added and stirred for 30min, which is recorded as C2 liquid. Then 25g of sodium borohydride is weighed and slowly and completely dissolved in 100ml of water with stirring, and the solution is marked as B2 solution. Then the B2 liquid is slowly dripped into the C2 liquid, the reaction process releases heat, the dripping speed is controlled so as to avoid overheating, and the temperature is 40 ℃. After the liquid B2 was completely added, the reaction was started for 5 hours and recorded as liquid D2. And standing the D2 liquid material overnight, taking the upper layer liquid, carrying out rotary evaporation at 65 ℃ and 80rmp/min, removing most of solvent to obtain a viscous substance, extracting with ethyl acetate, carrying out rotary evaporation at 45 ℃ and 100rmp/min, and carrying out centrifugal separation with 1000-mesh filter cloth (the centrifugal rotation speed is 1500rmp/min, the centrifugal time is 30min) to remove ethyl acetate, thus obtaining the 2, 5-furandimethanol. And (3) testing and analyzing the liquid taken before and after the hydrogenation reaction by using a high performance liquid chromatograph, and calculating the conversion rate of 5-hydroxymethylfurfural to be 100% and the yield of 2, 5-furandimethanol to be 98%.
Example 3
100g of production waste A3 (except HMF, black carbonaceous matter containing impurities, 5-AMF, OBMF, acetic acid, ethyl acetate, n-hexane and the like) containing 5-hydroxymethylfurfural (30 wt%) is added into a 2L beaker, and then 300ml of solvent water is added and stirred for 30min, which is marked as C3 liquid. Then 14g of sodium borohydride was weighed out and dissolved in 100ml of water slowly and completely with stirring, and the solution is recorded as B3 solution. Then the B3 liquid is slowly dripped into the C3 liquid, the reaction process releases heat, the dripping speed is controlled so as to avoid overheating, and the temperature is 50 ℃. After the liquid B3 was completely added, the reaction was started for 2 hours and recorded as liquid D3. And standing the D3 liquid material overnight, taking the upper layer liquid, carrying out rotary evaporation at 65 ℃ and 80rmp/min, removing most of solvent to obtain a viscous substance, extracting with ethyl acetate, carrying out rotary evaporation at 45 ℃ and 100rmp/min, and carrying out centrifugal separation with 1000-mesh filter cloth (the centrifugal speed is 1500rmp/min, the centrifugal time is 20min) to remove ethyl acetate, thus obtaining the 2, 5-furandimethanol. And (3) testing and analyzing the liquid taken before and after the hydrogenation reaction by using a high performance liquid chromatograph, and calculating that the conversion rate of the 5-hydroxymethylfurfural is 100% and the yield of the 2, 5-furandimethanol is 85%.
Example 4
22kg of a crystallized and purified liquid waste material A4 (the waste material contains impurities such as acetic acid, ethyl acetate and n-hexane except HMF) containing 5-hydroxymethylfurfural (80 wt%) is added into a 100L reactor, 50L of solvent water is added, and the mixture is stirred for 30min and is marked as C4 liquid. Then, 1.6kg of sodium borohydride was weighed out and slowly and completely dissolved in 6L of water with stirring, and the solution was recorded as B4 solution. Then, the B4 liquid is slowly dripped into the C4 liquid, the reaction process releases heat, the dripping speed is controlled so as to avoid overheating, and the temperature is 9 ℃. After the liquid B4 was completely added, the reaction was started for 8 hours and recorded as liquid D4. And after the reaction is finished, discharging the D4 liquid into a plastic barrel, standing for one day, after solid-liquid separation, taking the upper layer liquid, carrying out rotary evaporation at 65 ℃ and 65rmp/min, removing most of solvent to obtain a viscous substance, then extracting with ethyl acetate, continuing to carry out rotary evaporation at 45 ℃ and 100rmp/min, and then carrying out centrifugal separation (the centrifugal rotation speed is 2500rmp/min and the centrifugal time is 60min) by using 2000-mesh filter cloth to remove the ethyl acetate to obtain the 2, 5-furandimethanol. And (3) testing and analyzing the liquid taken before and after the hydrogenation reaction by using a high performance liquid chromatograph, and calculating the conversion rate of 5-hydroxymethylfurfural to be 100% and the yield of 2, 5-furandimethanol to be 98%.
Example 5
100g of purified liquid waste A5 (containing impurities such as acetic acid, ethyl acetate and n-hexane except HMF) containing 5-hydroxymethylfurfural (80 wt%) is added into a 2L beaker, and then 800ml of solvent water is added and stirred for 30min, which is recorded as C5 liquid. Then 40g of sodium borohydride is weighed and slowly and completely dissolved in 400ml of water with stirring, and the solution is marked as B5 solution. Then the B5 liquid is slowly dripped into the C5 liquid, the reaction process generates heat, the dripping speed is controlled so as to avoid overheating, and the temperature is 20 ℃. After the liquid B5 was completely added, the reaction was started for 1h and recorded as liquid D5. And standing the D5 liquid material overnight, taking the upper layer liquid, carrying out rotary evaporation at 65 ℃ and 80rmp/min, removing most of solvent to obtain a viscous substance, extracting with ethyl acetate, carrying out rotary evaporation at 40 ℃ and 100rmp/min, and carrying out centrifugal separation with 1000-mesh filter cloth (the centrifugal rotation speed is 1500rmp/min, the centrifugal time is 30min) to remove ethyl acetate, thus obtaining the 2, 5-furandimethanol. And (3) testing and analyzing the liquid taken before and after the hydrogenation reaction by using a high performance liquid chromatograph, and calculating the conversion rate of 5-hydroxymethylfurfural to be 100% and the yield of 2, 5-furandimethanol to be 99%.
Although the present application has been described with reference to a few embodiments, it should be understood that various changes, substitutions and alterations can be made herein without departing from the spirit and scope of the application as defined by the appended claims.

Claims (10)

1. A process for the preparation of 2, 5-furandimethanol, which comprises at least: reacting a material A containing 5-hydroxymethylfurfural with sodium borohydride in a solvent to obtain the 2, 5-furandimethanol;
the solvent contains water.
2. The preparation method according to claim 1, wherein the mass ratio of the 5-hydroxymethylfurfural to the sodium borohydride is 2-13: 1.
3. the method according to claim 1, wherein the reaction conditions are as follows: the reaction temperature is 7-50 ℃; the reaction time is 1-8 h.
4. The method for preparing according to claim 1, characterized in that it comprises at least: mixing a material A containing 5-hydroxymethylfurfural, a solution B containing sodium borohydride and a solvent I, and reacting to obtain the 2, 5-furandimethanol.
5. The preparation method according to claim 4, wherein the mass ratio of the solvent I to the material A is 1-10: 1;
preferably, the solvent I is water.
6. The preparation method according to claim 1 or 4, wherein the mass content of 5-hydroxymethylfurfural in the 5-hydroxymethylfurfural-containing material A is 20-100%;
preferably, the material A of the 5-hydroxymethylfurfural is at least one selected from production waste liquid containing the 5-hydroxymethylfurfural.
7. The preparation method according to claim 4, wherein the solution B comprises a solvent II, and the mass ratio of the sodium borohydride to the solvent II in the solution B is 1: 2-10;
preferably, the solvent II is water.
8. Preparation process according to claim 4, characterized in that it comprises at least the following steps:
(1) mixing a material A containing 5-hydroxymethylfurfural with a solvent I to obtain a solution C;
(2) obtaining solution B containing sodium borohydride;
(3) and mixing the solution C with the solution B, and reacting to obtain the 2, 5-furandimethanol.
9. The method for preparing as claimed in claim 8, wherein the step (3) comprises at least the steps of:
and mixing the solution C with the solution B, reacting, performing rotary evaporation, extracting, performing rotary evaporation, and centrifuging to obtain the 2, 5-furandimethanol.
10. The preparation method according to claim 9, wherein the conditions of the rotary evaporation are as follows: the rotary evaporation temperature is 30-80 ℃; the rotary evaporation speed is 40-100 rmp/min;
preferably, the conditions of the centrifugation are: the centrifugal rotating speed is 1000-2500 rmp/min; centrifuging for 10-60 min; the mesh number of the filter cloth is 600-2000 meshes;
preferably, the extraction is carried out with solvent III; the solvent III is at least one selected from ethyl acetate and petroleum ether.
CN202010130668.3A 2020-02-28 2020-02-28 Preparation method of 2, 5-furandimethanol Pending CN111233796A (en)

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Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN112812080A (en) * 2021-01-13 2021-05-18 湖南师范大学 A kind of method for preparing 2,5-furandimethanol from 5-hydroxymethylfurfural

Non-Patent Citations (3)

* Cited by examiner, † Cited by third party
Title
F. A. KUCHEROV ET AL.: "Efficient route for the construction of polycyclic systems from bioderived HMF", 《GREEN CHEMISTRY》 *
JINGJING MENG ET AL.: "Sustainable bio-based furan epoxy resin with flame retardancy", 《POLYM. CHEM.》 *
SUDIPTA DE ET AL.: "Furan-based acetylating agent for the chemical modification of proteins", 《BIOORGANIC & MEDICINAL CHEMISTRY》 *

Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN112812080A (en) * 2021-01-13 2021-05-18 湖南师范大学 A kind of method for preparing 2,5-furandimethanol from 5-hydroxymethylfurfural

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