CN113788736A - High-efficiency conversion of CO2Catalyst for ethanol production - Google Patents
High-efficiency conversion of CO2Catalyst for ethanol production Download PDFInfo
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- CN113788736A CN113788736A CN202111237986.0A CN202111237986A CN113788736A CN 113788736 A CN113788736 A CN 113788736A CN 202111237986 A CN202111237986 A CN 202111237986A CN 113788736 A CN113788736 A CN 113788736A
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- C07C29/00—Preparation of compounds having hydroxy or O-metal groups bound to a carbon atom not belonging to a six-membered aromatic ring
- C07C29/15—Preparation of compounds having hydroxy or O-metal groups bound to a carbon atom not belonging to a six-membered aromatic ring by reduction of oxides of carbon exclusively
- C07C29/151—Preparation of compounds having hydroxy or O-metal groups bound to a carbon atom not belonging to a six-membered aromatic ring by reduction of oxides of carbon exclusively with hydrogen or hydrogen-containing gases
- C07C29/153—Preparation of compounds having hydroxy or O-metal groups bound to a carbon atom not belonging to a six-membered aromatic ring by reduction of oxides of carbon exclusively with hydrogen or hydrogen-containing gases characterised by the catalyst used
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Abstract
The invention relates to the technical field of catalysts, and particularly relates to a catalyst for efficiently converting co2 into ethanol. The composite material comprises the following raw materials in parts by weight: 5-10 parts of active component, 50-90 parts of carrier, 1-5 parts of metal ion, 1-3 parts of activating agent and 1-3 parts of third component. The balance of deionized water; in the catalyst for efficiently converting co2 into ethanol, the added activating agent can improve the catalytic activity of the active component by utilizing the electronic effect of the chloroalkoxy compound, and the added third component has stronger electron donating capability, can influence the molecular weight increase of the product in the reaction process, and simultaneously influences the interaction of the active component and the chloroalkoxy compound in the activating agent, thereby improving the activity of the catalyst.
Description
Technical Field
The invention relates to the technical field of catalysts, and particularly relates to a catalyst for efficiently converting co2 into ethanol.
Background
The utilization of carbon dioxide has an important influence on the development of carbon cycle and recycling economy, and the catalytic conversion thereof has attracted worldwide attention, wherein hydrogen production by photocatalysis and photoelectrocatalysis using renewable energy such as solar energy is an effective way for utilizing carbon dioxide in the hydrogenation of carbon dioxide. Among the numerous products of carbon dioxide conversion, methanol is the predominant product and has attracted extensive attention and research. In contrast, there has been less research on the hydrogenation of carbon dioxide to ethanol. Ethanol is not only non-toxic but also a more valuable product that can be easily converted to high value added chemicals such as ethylene. Ethanol can be obtained by hydrogenation of carbon dioxide or CO, and the main difference is that the former has reverse water gas shift reaction. For the preparation of ethanol by hydrogenation of carbon dioxide, a catalyst with high activity and high ethanol selectivity needs to be developed.
The existing catalyst for preparing ethanol generally needs higher temperature and pressure in the traditional process of preparing a multi-carbon product by thermally catalyzing carbon dioxide hydrogenation, the product distribution is wide, the selectivity is low, and the activity of the prepared catalyst is poor, so that the conversion effect of ethanol is poor, and therefore, a catalyst for efficiently converting co2 into ethanol is needed to overcome the defects in the prior art.
Disclosure of Invention
The invention aims to provide a catalyst for efficiently converting co2 into ethanol, so as to solve the problems in the background technology.
In order to achieve the above object, in one aspect, the present invention provides a catalyst for efficiently converting co2 into ethanol, comprising the following raw materials in parts by weight: 5-10 parts of active component, 50-90 parts of carrier, 1-5 parts of metal ion, 1-3 parts of activating agent, 1-3 parts of third component and the balance of deionized water.
As a further improvement of the technical scheme, the active component is selected from one or more of gold-copper alloy, fluorine modified copper, metal zinc, titanium and chlorine.
As a further improvement of the technical scheme, the carrier is selected from at least one of silicon carbide, magnesium oxide, silicon dioxide, aluminum oxide and ferric oxide.
As a further improvement of the technical scheme, the metal ions are at least one selected from divalent copper ions, divalent iron ions, trivalent iron ions, sodium ions, cobalt ions, potassium ions and ammonium ions, and are used as a promoter of the active component, so that the activity, selectivity, stability and service life of the catalyst can be improved.
As a further improvement of the technical scheme, the activating agent is a chloroalkoxy compound, and the catalytic activity of the active component is improved by utilizing the electronic effect of the chloroalkoxy compound.
As a further improvement of the technical scheme, the third component comprises at least one of ethylene imine, pyrrolidine, 2-naphthylamine and benzidine, and the compound has stronger electron donating capability, can influence the molecular weight increase of products in the reaction process, and simultaneously influences the interaction of the active component and the chloroalkoxy compound in the activator, thereby improving the activity of the catalyst.
In another aspect, the present invention provides a method for preparing a catalyst for efficiently converting co2 into ethanol, comprising the steps of:
s1, adding the carrier into a water solvent, carrying out ultrasonic treatment for 5-8h, then adding the active component into the solution, mixing and stirring for 10-15h to prepare a precursor solution;
s2, filtering the precursor solution to remove liquid, washing with water, drying, and roasting at high temperature to obtain a semi-finished catalyst;
s3, adding the semi-finished catalyst powder into the aqueous solution, carrying out ultrasonic treatment for 1-2h, then adding metal ions, an activating agent and a third component, mixing and stirring for 2-4h, finally filtering and drying the mixed solution, and roasting at high temperature to obtain the finished catalyst.
Preferably, in the S2, the roasting temperature is 200-300 ℃, and the time is 1-2 h.
Preferably, in the S3, the roasting temperature is 200-300 ℃, and the time is 1-2 h.
Compared with the prior art, the invention has the beneficial effects that:
in the catalyst for efficiently converting co2 into ethanol, the added activating agent can improve the catalytic activity of the active component by utilizing the electronic effect of the chloroalkoxy compound, and the added third component has stronger electron donating capability, can influence the molecular weight increase of the product in the reaction process, and simultaneously influences the interaction of the active component and the chloroalkoxy compound in the activating agent, thereby improving the activity of the catalyst.
Drawings
FIG. 1 is an overall flow diagram of the present invention.
Detailed Description
The technical solutions in the embodiments of the present invention will be clearly and completely described below with reference to the drawings in the embodiments of the present invention, and it is obvious that the described embodiments are only a part of the embodiments of the present invention, and not all of the embodiments. All other embodiments, which can be derived by a person skilled in the art from the embodiments given herein without making any creative effort, shall fall within the protection scope of the present invention.
Example 1 a catalyst for high efficiency conversion of co2 to ethanol comprising:
1. adding 90 parts of carrier into a hydrosolvent, carrying out ultrasonic treatment for 8h, then adding 5 parts of active component into the solution, mixing and stirring for 15h to prepare a precursor solution;
2. filtering the precursor solution to remove liquid, washing and drying, and roasting at the temperature of 300 ℃ for 4 hours to obtain a semi-finished catalyst;
3. adding the semi-finished catalyst powder into the aqueous solution, carrying out ultrasonic treatment for 2h, then adding 1 part of metal ions, 1 part of activating agent and 1 part of third component, mixing and stirring for 2h, finally filtering and drying the mixed solution, and roasting at the temperature of 300 ℃ for 4h to obtain the finished catalyst.
Example 2 a catalyst for high efficiency conversion of co2 to ethanol comprising:
1. adding 80 parts of carrier into a hydrosolvent, carrying out ultrasonic treatment for 7h, then adding 6 parts of active component into the solution, mixing and stirring for 14h to prepare a precursor solution;
2. filtering the precursor solution to remove liquid, washing and drying, and roasting at 280 ℃ for 3.5h to obtain a semi-finished catalyst;
3. adding the semi-finished catalyst powder into the aqueous solution, carrying out ultrasonic treatment for 2h, then adding 2 parts of metal ions, 1.5 parts of activating agent and 1.5 parts of third component, mixing and stirring for 2h, finally filtering and drying the mixed solution, and roasting at 280 ℃ for 3.5h to obtain the finished catalyst.
Example 3 a catalyst for high efficiency conversion of co2 to ethanol comprising:
1. adding 70 parts of carrier into a hydrosolvent, carrying out ultrasonic treatment for 6h, then adding 8 parts of active component into the solution, mixing and stirring for 13h to prepare a precursor solution;
2. filtering the precursor solution to remove liquid, washing and drying, and roasting at 250 ℃ for 3h to obtain a semi-finished catalyst;
3. adding the semi-finished catalyst powder into the aqueous solution, carrying out ultrasonic treatment for 1.5h, then adding 3 parts of metal ions, 2 parts of activating agent and 2 parts of third component, mixing and stirring for 3h, finally filtering and drying the mixed solution, and roasting at the temperature of 250 ℃ for 3h to obtain the finished catalyst.
Example 4 a catalyst for high efficiency conversion of co2 to ethanol comprising:
1. adding 60 parts of carrier into a hydrosolvent, carrying out ultrasonic treatment for 6h, then adding 9 parts of active component into the solution, mixing and stirring for 12h to prepare a precursor solution;
2. filtering the precursor solution to remove liquid, washing and drying, and roasting at 220 ℃ for 2h to obtain a semi-finished catalyst;
3. adding the semi-finished catalyst powder into the aqueous solution, carrying out ultrasonic treatment for 1h, then adding 4 parts of metal ions, 2.5 parts of activating agent and 2.5 parts of third component, mixing and stirring for 3.54h, finally filtering and drying the mixed solution, and roasting at 220 ℃ for 2.5h to obtain the finished catalyst.
Example 5 a catalyst for high efficiency conversion of co2 to ethanol comprising:
1. adding 50 parts of carrier into a hydrosolvent, carrying out ultrasonic treatment for 5h, then adding 10 parts of active component into the solution, mixing and stirring for 10h to prepare a precursor solution;
2. filtering the precursor solution to remove liquid, washing and drying, and roasting at 200 ℃ for 2h to obtain a semi-finished catalyst;
3. adding the semi-finished catalyst powder into the aqueous solution, carrying out ultrasonic treatment for 1h, then adding 5 parts of metal ions, 3 parts of activating agent and 3 parts of third component, mixing and stirring for 4h, finally filtering and drying the mixed solution, and roasting for 2h at the temperature of 200 ℃ to obtain the finished catalyst.
In the above examples 1 to 5, the active component is selected from one or more of gold-copper alloy, fluorine modified copper, metallic zinc, titanium and chlorine;
the carrier is selected from at least one of silicon carbide, magnesium oxide, silicon dioxide, aluminum oxide and ferric oxide;
the activator is a chloroalkoxy compound, and the catalytic activity of the active component is improved by utilizing the electronic effect of the chloroalkoxy compound;
the third component comprises at least one of ethylene imine, pyrrolidine, 2-naphthylamine and benzidine, and the compounds have stronger electron donating capability, can influence the molecular weight increase of products in the reaction process, and influence the interaction of the active component and the chlorinated alkoxy compound in the activator, thereby improving the activity of the catalyst.
The relevant indexes of the catalyst for efficiently converting co2 into ethanol are shown in the table 1:
TABLE 1
As shown in Table 1, examples 1-5 all had better carbon dioxide conversion, while ethanol conversion was 80% or more, with the catalyst in example 3 performing best. The data in table 1 can show that the catalyst provided by the invention has better activity and selectivity.
Comparative example 1 a catalyst for the conversion of co2 to ethanol comprising:
1. adding 70 parts of carrier into a hydrosolvent, carrying out ultrasonic treatment for 6h, then adding 8 parts of active component into the solution, mixing and stirring for 13h to prepare a precursor solution;
2. filtering the precursor solution to remove liquid, washing and drying, and roasting at 250 ℃ for 3h to obtain a semi-finished catalyst;
3. adding the semi-finished catalyst powder into the aqueous solution, carrying out ultrasonic treatment for 1.5h, then adding 3 parts of metal ions and 2 parts of a third component, mixing and stirring for 3h, finally filtering and drying the mixed solution, and roasting at the temperature of 250 ℃ for 3h to obtain the finished catalyst.
Comparative example 2 a catalyst for the conversion of co2 to ethanol comprising:
1. adding 70 parts of carrier into a hydrosolvent, carrying out ultrasonic treatment for 6h, then adding 8 parts of active component into the solution, mixing and stirring for 13h to prepare a precursor solution;
2. filtering the precursor solution to remove liquid, washing and drying, and roasting at 250 ℃ for 3h to obtain a semi-finished catalyst;
3. adding the semi-finished catalyst powder into the aqueous solution, carrying out ultrasonic treatment for 1.5h, then adding 3 parts of metal ions and 2 parts of activating agent, mixing and stirring for 3h, finally filtering and drying the mixed solution, and roasting at the temperature of 250 ℃ for 3h to obtain the finished catalyst.
Comparative example 3 a catalyst for the conversion of co2 to ethanol comprising:
1. adding 70 parts of carrier into a hydrosolvent, carrying out ultrasonic treatment for 6h, then adding 8 parts of active component into the solution, mixing and stirring for 13h to prepare a precursor solution;
2. filtering the precursor solution to remove liquid, washing and drying, and roasting at 250 ℃ for 3h to obtain a semi-finished catalyst;
3. adding the semi-finished catalyst powder into the aqueous solution, carrying out ultrasonic treatment for 1.5h, then adding 3 parts of metal ions, mixing and stirring for 3h, finally filtering and drying the mixed solution, and roasting at the temperature of 250 ℃ for 3h to obtain the finished catalyst.
The catalyst for efficiently converting co2 into ethanol prepared by the invention has better activity and selectivity, and has a great relationship with the added activating agent and the third component, and in order to verify the related technical scheme, the applicant performs the following tests:
comparative examples 1 to 3: by using the method of example 3, the prepared catalyst was tested for its associated indicators with the removal of the activator and third component, as shown in table 2:
TABLE 2
As shown in table 2, in comparative examples 1 to 3, the carbon dioxide conversion rate and the selectivity of ethanol conversion were decreased to different degrees when the activating agent and the third component were removed separately as compared to example 3, and in comparative example 1 and comparative example 2, the carbon dioxide conversion rate and the selectivity of ethanol conversion were most significantly decreased when the activating agent and the third component were removed simultaneously as in comparative example 3, and thus it can be illustrated that the addition of the activating agent and the third component is an important factor for improving the catalyst activity and selectivity in the present invention.
The foregoing shows and describes the general principles, essential features, and advantages of the invention. It will be understood by those skilled in the art that the present invention is not limited to the embodiments described above, and the preferred embodiments of the present invention are described in the above embodiments and the description, and are not intended to limit the present invention. The scope of the invention is defined by the appended claims and equivalents thereof.
Claims (9)
1. The catalyst for efficiently converting co2 into ethanol is characterized by comprising the following raw materials in parts by weight: 5-10 parts of active component, 50-90 parts of carrier, 1-5 parts of metal ion, 1-3 parts of activating agent, 1-3 parts of third component and the balance of deionized water.
2. The catalyst for highly efficient conversion of co2 into ethanol as claimed in claim 1, wherein: the active component is selected from one or more of gold-copper alloy, fluorine modified copper, metal zinc, titanium and chlorine.
3. The catalyst for highly efficient conversion of co2 into ethanol as claimed in claim 1, wherein: the carrier is selected from at least one of silicon carbide, magnesium oxide, silicon dioxide, aluminum oxide and ferric oxide.
4. The catalyst for highly efficient conversion of co2 into ethanol as claimed in claim 1, wherein: the metal ion is selected from at least one of divalent copper ion, divalent iron ion, trivalent iron ion, sodium ion, cobalt ion, potassium ion and ammonium ion.
5. The catalyst for highly efficient conversion of co2 into ethanol as claimed in claim 1, wherein: the activating agent is a chloroalkoxy compound.
6. The catalyst for highly efficient conversion of co2 into ethanol as claimed in claim 1, wherein: the third component includes at least one of an ethyleneimine, a pyrrolidine, a 2-naphthylamine, and a benzidine.
7. The catalyst for highly efficient conversion of co2 into ethanol according to any one of claims 1-6, wherein the preparation method comprises the following steps:
s1, adding the carrier into a water solvent, carrying out ultrasonic treatment for 5-8h, then adding the active component into the solution, mixing and stirring for 10-15h to prepare a precursor solution;
s2, filtering the precursor solution to remove liquid, washing with water, drying, and roasting at high temperature to obtain a semi-finished catalyst;
s3, adding the semi-finished catalyst powder into the aqueous solution, carrying out ultrasonic treatment for 1-2h, then adding metal ions, an activating agent and a third component, mixing and stirring for 2-4h, finally filtering and drying the mixed solution, and roasting at high temperature to obtain the finished catalyst.
8. The catalyst for highly efficient conversion of co2 into ethanol as claimed in claim 7, wherein: in the S2, the roasting temperature is 200-300 ℃, and the time is 1-2 h.
9. The catalyst for highly efficient conversion of co2 into ethanol as claimed in claim 7, wherein: in the S3, the roasting temperature is 200-300 ℃, and the time is 1-2 h.
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| CN202111237986.0A CN113788736A (en) | 2021-10-25 | 2021-10-25 | High-efficiency conversion of CO2Catalyst for ethanol production |
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Citations (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN1087571A (en) * | 1992-12-03 | 1994-06-08 | 默蒙特股份有限公司 | The propylene polymer film of biax orientation or sheet articles |
| CN103314017A (en) * | 2010-12-27 | 2013-09-18 | 维尔萨利斯股份公司 | Solid catalyst component, catalyst comprising said solid component, and process for the (co)polymerization of alpha-olefins |
| CN113058596A (en) * | 2021-03-09 | 2021-07-02 | 江南大学 | High-stability CO2Preparation and application of catalyst for preparing ethanol by hydrogenation |
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- 2021-10-25 CN CN202111237986.0A patent/CN113788736A/en active Pending
Patent Citations (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN1087571A (en) * | 1992-12-03 | 1994-06-08 | 默蒙特股份有限公司 | The propylene polymer film of biax orientation or sheet articles |
| CN103314017A (en) * | 2010-12-27 | 2013-09-18 | 维尔萨利斯股份公司 | Solid catalyst component, catalyst comprising said solid component, and process for the (co)polymerization of alpha-olefins |
| CN113058596A (en) * | 2021-03-09 | 2021-07-02 | 江南大学 | High-stability CO2Preparation and application of catalyst for preparing ethanol by hydrogenation |
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