CN115504846A - Method for preparing organic matter by catalyzing carbon dioxide synthesis gas through ionizing radiation - Google Patents

Method for preparing organic matter by catalyzing carbon dioxide synthesis gas through ionizing radiation Download PDF

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CN115504846A
CN115504846A CN202211140391.8A CN202211140391A CN115504846A CN 115504846 A CN115504846 A CN 115504846A CN 202211140391 A CN202211140391 A CN 202211140391A CN 115504846 A CN115504846 A CN 115504846A
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ionizing radiation
carbon dioxide
gas
source
synthesis gas
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蒙大桥
沈崇雨
罗文华
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Institute of Materials of CAEP
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    • C—CHEMISTRY; METALLURGY
    • C07—ORGANIC CHEMISTRY
    • C07C—ACYCLIC OR CARBOCYCLIC COMPOUNDS
    • C07C1/00—Preparation of hydrocarbons from one or more compounds, none of them being a hydrocarbon
    • C07C1/02—Preparation of hydrocarbons from one or more compounds, none of them being a hydrocarbon from oxides of a carbon
    • C07C1/12—Preparation of hydrocarbons from one or more compounds, none of them being a hydrocarbon from oxides of a carbon from carbon dioxide with hydrogen
    • C—CHEMISTRY; METALLURGY
    • C07—ORGANIC CHEMISTRY
    • C07C—ACYCLIC OR CARBOCYCLIC COMPOUNDS
    • C07C1/00—Preparation of hydrocarbons from one or more compounds, none of them being a hydrocarbon
    • C07C1/02—Preparation of hydrocarbons from one or more compounds, none of them being a hydrocarbon from oxides of a carbon
    • C07C1/04—Preparation of hydrocarbons from one or more compounds, none of them being a hydrocarbon from oxides of a carbon from carbon monoxide with hydrogen
    • C—CHEMISTRY; METALLURGY
    • C07—ORGANIC CHEMISTRY
    • C07C—ACYCLIC OR CARBOCYCLIC COMPOUNDS
    • C07C1/00—Preparation of hydrocarbons from one or more compounds, none of them being a hydrocarbon
    • C07C1/02—Preparation of hydrocarbons from one or more compounds, none of them being a hydrocarbon from oxides of a carbon
    • C07C1/04—Preparation of hydrocarbons from one or more compounds, none of them being a hydrocarbon from oxides of a carbon from carbon monoxide with hydrogen
    • C07C1/0455—Reaction conditions
    • C—CHEMISTRY; METALLURGY
    • C07—ORGANIC CHEMISTRY
    • C07C—ACYCLIC OR CARBOCYCLIC COMPOUNDS
    • 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
    • C—CHEMISTRY; METALLURGY
    • C07—ORGANIC CHEMISTRY
    • C07C—ACYCLIC OR CARBOCYCLIC COMPOUNDS
    • 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
    • C07C29/1512—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 reaction conditions
    • C—CHEMISTRY; METALLURGY
    • C07—ORGANIC CHEMISTRY
    • C07C—ACYCLIC OR CARBOCYCLIC COMPOUNDS
    • C07C45/00—Preparation of compounds having >C = O groups bound only to carbon or hydrogen atoms; Preparation of chelates of such compounds
    • C—CHEMISTRY; METALLURGY
    • C07—ORGANIC CHEMISTRY
    • C07C—ACYCLIC OR CARBOCYCLIC COMPOUNDS
    • C07C45/00—Preparation of compounds having >C = O groups bound only to carbon or hydrogen atoms; Preparation of chelates of such compounds
    • C07C45/49—Preparation of compounds having >C = O groups bound only to carbon or hydrogen atoms; Preparation of chelates of such compounds by reaction with carbon monoxide
    • C—CHEMISTRY; METALLURGY
    • C07—ORGANIC CHEMISTRY
    • C07C—ACYCLIC OR CARBOCYCLIC COMPOUNDS
    • C07C51/00—Preparation of carboxylic acids or their salts, halides or anhydrides
    • C—CHEMISTRY; METALLURGY
    • C07—ORGANIC CHEMISTRY
    • C07C—ACYCLIC OR CARBOCYCLIC COMPOUNDS
    • C07C51/00—Preparation of carboxylic acids or their salts, halides or anhydrides
    • C07C51/10—Preparation of carboxylic acids or their salts, halides or anhydrides by reaction with carbon monoxide

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  • Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Engineering & Computer Science (AREA)
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  • General Chemical & Material Sciences (AREA)
  • Organic Low-Molecular-Weight Compounds And Preparation Thereof (AREA)
  • Carbon And Carbon Compounds (AREA)

Abstract

The invention belongs to the technical field of irradiation processing, and provides a method for preparing organic matters by catalyzing carbon dioxide synthesis gas with ionizing radiation. When the method provided by the invention is used for preparing organic matters, carbon dioxide synthesis gas is taken as a preparation raw material and is carried out under the action of ionizing radiation; since the ray energy of the ionizing radiation is generally much higher than the chemical bond energy in the carbon dioxide synthesis gas and the organic matter, under the action of the ionizing radiation, the carbon-containing gas (carbon monoxide and/or carbon dioxide) in the carbon dioxide synthesis gas is subjected to chemical bond breakage and combined with the hydrogen isotope gas (the hydrogen isotope gas comprises one or more of protium, deuterium and tritium) to be converted into the organic matter. Compared with other chemical catalysts, the ionizing radiation can provide energy required by chemical reaction and is the catalyst, and other catalysts and heating treatment are not needed, so that the chemical reaction cost and energy consumption are reduced.

Description

Method for preparing organic matter by catalyzing carbon dioxide synthesis gas through ionizing radiation
Technical Field
The invention relates to the technical field of irradiation processing, in particular to a method for preparing organic matters by catalyzing carbon dioxide synthesis gas with ionizing radiation.
Background
With the rapid development of modern industry, the energy consumption supporting the development of the industry is increasing. The fuel such as natural gas, petroleum, coal, charcoal and the like is combusted to obtain industrial heat energy, and simultaneously, a large amount of carbon dioxide greenhouse gas is discharged to the environment. At present, global climate problems caused by greenhouse gas emission of carbon dioxide have become common knowledge, and reduction of greenhouse gas emission of carbon dioxide and the like is considered to be an imminent effective approach to cope with global climate problems. Carbon dioxide emission reduction is mainly achieved through two ways, one is energy substitution, namely, fuel for generating carbon dioxide is not used or is used in a reduced mode; secondly, carbon dioxide released by combustion is converted into other substances through a carbon dioxide conversion technology, so that the emission of carbon dioxide into the atmosphere is not emitted or reduced. Admittedly, under the condition that the new energy technology cannot completely replace the existing fuel system, the adoption of the carbon dioxide conversion technology to achieve the purpose of not discharging or reducing the discharged carbon dioxide is a technical approach for effectively dealing with the global climate problem caused by the carbon dioxide. The carbon dioxide conversion technology can effectively reduce the emission of carbon dioxide, change waste into valuable and convert the waste into other industrial raw materials or products.
The conversion of carbon dioxide into methane is used for the first time in the aerospace field, and is mainly used for solving the problem of oxygen required by the breathing of astronauts, and the specific solution is as follows: carbon dioxide exhaled by the astronauts is converted into methane and water through a catalytic reaction, and the water is further electrolyzed to prepare oxygen for the astronauts to breathe. Based on this, the reaction of converting carbon dioxide into other organic substances is regarded as important industrially, but the conversion of carbon dioxide by the conventional catalytic reaction is costly and consumes a lot of energy.
Disclosure of Invention
In view of the above, the present invention provides a method for preparing organic matters by catalyzing carbon dioxide synthesis gas with ionizing radiation. The method provided by the invention has low cost and low energy consumption.
In order to achieve the above object, the present invention provides the following technical solutions:
the invention provides a method for preparing organic matters by catalyzing carbon dioxide synthesis gas through ionizing radiation, which comprises the following steps:
taking carbon dioxide synthesis gas as a preparation raw material, and carrying out chemical reaction under the action of ionizing radiation to obtain an organic matter;
the carbon dioxide synthesis gas comprises hydrogen isotope gas and carbon-containing gas;
the hydrogen isotope gas comprises one or more of protium, deuterium and tritium hydrogen isotopes;
the carbon-containing gas comprises carbon monoxide and/or carbon dioxide.
Preferably, the hydrogen isotope gas includes hydrogen gas, deuterium gas, or tritium-containing hydrogen isotope gas.
Preferably, the tritium-hydrogen isotope-containing gas includes tritium gas or a tritium-hydrogen isotope-containing gas mixture.
Preferably, said ionizing radiation is generated by an ionizing radiation source; the source of ionizing radiation comprises one or more of alpha rays, beta rays, gamma rays, X rays, and n.
Preferably, the source of ionizing radiation comprises an endogenous source of ionizing radiation or an exogenous source of ionizing radiation.
Preferably, when the ionizing radiation is generated by an external ionizing radiation source, the dose rate of the ionizing radiation is more than or equal to 2Gy/h.
Preferably, the source of ionizing radiation is a radionuclide or a shielding ray; the shielding ray is a ray which needs to be shielded in a power station or a large-scale ray device.
Preferably, when the ionizing radiation source is an external ionizing radiation source, the pressure of the chemical reaction is more than or equal to 5MPa; when the ionizing radiation source is an endogenous ionizing radiation source, the pressure of the chemical reaction is more than or equal to 0.1MPa.
The invention provides a method for preparing organic matters by catalyzing carbon dioxide synthesis gas through ionizing radiation, which comprises the following steps: taking carbon dioxide synthesis gas as a preparation raw material, and reacting under the action of ionizing radiation to obtain an organic matter; the carbon dioxide synthesis gas comprises hydrogen isotope gas and carbon-containing gas; the hydrogen isotope gas comprises one or more of three hydrogen isotopes of protium, deuterium and tritium; the carbon-containing gas comprises carbon monoxide and/or carbon dioxide. When the method provided by the invention is used for preparing organic matters, carbon dioxide synthesis gas is used as a preparation raw material and is carried out under the action of ionizing radiation; since the ray energy of the ionizing radiation is generally much higher than the chemical bond energy in the carbon dioxide synthesis gas and the organic matter, under the action of the ionizing radiation, the carbon-containing gas (carbon monoxide and/or carbon dioxide) in the carbon dioxide synthesis gas is ionized or the chemical bond is broken and combined with the hydrogen isotope gas (the hydrogen isotope gas comprises one or more of protium, deuterium and tritium) to be converted into the organic matter. Compared with other chemical catalysts, the ionizing radiation can provide energy required by chemical reaction and is the catalyst, other catalysts and heating treatment are not needed, and the chemical reaction cost and energy consumption are reduced. When the hydrogen isotope gas of the carbon dioxide synthesis gas comprises isotope tritium, the carbon dioxide synthesis gas can directly synthesize tritium-substituted organic matter under the action of an ionization radiation source of tritium, and compared with the method in the prior art that tritium-substituted organic matter is prepared by taking a target compound as a raw material and carrying out tritium substitution reaction under the action of a catalyst, or tritium is added under the action of a hydrogenation catalyst to prepare the tritium-substituted organic matter by adopting unsaturated organic matter, the tritium substitution rate is higher; meanwhile, when the hydrogen isotope gas of the carbon dioxide synthesis gas comprises isotope tritium, because the tritium is a radioactive isotope of hydrogen and has a half-life period of 12.3 years, beta rays are emitted during decay, ionizing radiation of the beta rays can induce the chemical reaction, and additional ionizing radiation is not needed, so that the cost is further reduced.
Further, the ionizing radiation source is a radionuclide or a shielding ray; when the shielding rays are rays required to be shielded by a power station or a large-scale ray device, the cost of chemical reaction can be further reduced.
Drawings
FIG. 1 is a topographical view of the condensed product obtained in example 1;
FIG. 2 is a topographical view of the waxy product obtained in example 1;
FIG. 3 is the mass spectrometric detection of the gaseous products produced in example 1;
FIG. 4 is a graph showing the morphology of the condensed product obtained in example 2;
FIG. 5 is a schematic representation of the liquid product obtained in example 2;
FIG. 6 is a topographical view of the waxy product obtained in example 2;
FIG. 7 is the mass spectrometric detection of the gaseous products produced in example 2;
FIG. 8 is the mass spectrometric detection of the gaseous products produced in example 3.
Detailed Description
The invention provides a method for preparing organic matters by catalyzing carbon dioxide synthesis gas through ionizing radiation, which comprises the following steps:
taking carbon dioxide synthesis gas as a preparation raw material, and carrying out chemical reaction under the action of ionizing radiation to obtain an organic matter;
the carbon dioxide synthesis gas comprises hydrogen isotope gas and carbon-containing gas;
the hydrogen isotope gas comprises one or more of protium, deuterium and tritium hydrogen isotopes;
the carbon-containing gas comprises carbon monoxide and/or carbon dioxide.
In the present invention, the starting materials used in the present invention are preferably commercially available products unless otherwise specified.
In the present invention, the carbon dioxide synthesis gas includes hydrogen isotope gas and carbon-containing gas. In the present invention, the molar ratio of the hydrogen isotope gas to the carbon-containing gas in the carbon dioxide synthesis gas is preferably 1:1.
in the present invention, the hydrogen isotope gas preferably includes hydrogen gas, deuterium gas, or tritium-containing hydrogen isotope gas; the tritium-hydrogen-containing isotopeThe gas preferably comprises tritium gas or tritium-containing hydrogen isotope mixed gas (Q) 2 ). In the present invention, the carbon-containing gas comprises carbon monoxide and/or carbon dioxide.
In the present invention, the carbon dioxide synthesis gas is more preferably a tritium-carbon monoxide-carbon dioxide gas mixture or a tritium-containing hydrogen isotope gas mixture (Q) 2 ) -a mixture of carbon monoxide and carbon dioxide or a hydrogen-carbon dioxide mixture.
In the present invention, the ionizing radiation is preferably generated by a source of ionizing radiation; the source of ionizing radiation preferably comprises one or more of alpha rays, beta rays, gamma rays, X rays and n.
In the present invention, the ionizing radiation source preferably comprises an endogenous ionizing radiation source or an exogenous ionizing radiation source.
In the present invention, the endogenous ionizing radiation source is preferably gas generation in carbon dioxide synthesis gas, in particular hydrogen isotope-tritium generation in carbon dioxide synthesis gas. In the invention, tritium is a radioactive isotope of hydrogen, the half-life period is 12.3 years, beta rays are emitted during decay, and the ionizing radiation of the beta rays can induce the chemical reaction. In the invention, when tritium is contained in the carbon dioxide synthesis gas, preferably no additional ionizing radiation is applied, and the cost is further reduced.
In the invention, when the ionizing radiation is generated by an external ionizing radiation source, the dose rate of the ionizing radiation is preferably not less than 2Gy/h, and more preferably 2-10 Gy/h. In the present invention, it is preferred to use an external source of ionizing radiation when the carbon dioxide synthesis gas does not contain hydrogen isotope tritium. In the present invention, the ionizing radiation source is preferably a radionuclide or a shielded ray; the shielding ray is preferably a ray which needs to be shielded by a power station or a large ray device. In the invention, the ionizing radiation source is shielding rays, so that the cost of chemical reaction can be further reduced.
In the present invention, the higher the pressure of the chemical reaction is, the more favorable the reaction rate is, the higher the pressure is, the implementation is related to the ionizing radiation source used, and when an external ionizing radiation source is used, the pressure of the chemical reaction is preferably not less than 5MPa, more preferably 5 to 20MPa, and still more preferably 10MPa. In the present invention, when an endogenous ionizing radiation source is used, the pressure of the chemical reaction is preferably 0.1MPa or more, more preferably 0.1 to 2MPa, and still more preferably 1MPa.
The time of the chemical reaction is not particularly limited, and may be set according to the type of the carbon dioxide synthesis gas and the type of the organic substance to be produced.
In the present invention, the organic substance preferably contains one or more of a hydrocarbon, an aldehyde, an alcohol, and a carboxylic acid.
The method for preparing organic matters by catalyzing carbon dioxide synthesis gas with ionizing radiation according to the present invention will be described in detail with reference to the following examples, which should not be construed as limiting the scope of the present invention.
Example 1
Preparing tritiated organic matters by using a mixed gas of tritium gas, carbon monoxide and carbon dioxide:
evacuating the reactor with quartz visual window, cleaning the reactor with carbon dioxide gas for 3 times, respectively injecting carbon dioxide and carbon monoxide into the reactor, and injecting pure tritium gas into the reactor with total pressure of 1MPa and molar ratio of each gas (T/T) 2 ：CO：CO 2 ) Is that 2:1:1; the valve on the reactor is closed, the catalysis is carried out by utilizing beta rays generated by the decay of tritium, and the following can be observed through a visible window of the reactor: a condensed product was formed at the initial stage (as shown in FIG. 1), and a waxy product was observed as the reaction proceeded (as shown in FIG. 2); the composition of the gaseous products in the reactor was tested by quadrupole mass spectrometry and the results are shown in figure 3.
As can be seen from fig. 1 and 2: the initial chemical reaction produces a snowflake-like condensed product that continues to convert to a waxy product as shown in fig. 2 upon irradiation with beta rays from tritium decay.
FIG. 3 shows the mass spectrometric detection of the gaseous product obtained, from FIG. 3: the generated gaseous product comprises tritiated alkanes, tritiated alkenes, tritiated aldehydes, tritiated alcohols and other tritiated organic matters.
Example 2
Preparing tritiated organic matters by adopting a mixed gas containing tritium-hydrogen isotope gas, carbon monoxide and carbon dioxide:
evacuating the reactor with quartz viewing window, cleaning the reactor with carbon dioxide gas for 3 times, respectively injecting carbon dioxide and carbon monoxide into the reactor, and mixing hydrogen isotope gas containing tritium (using 'Q') 2 "refers to) was injected into the reactor, the total pressure was controlled at 1MPa, and the molar ratio (Q) of each gas was controlled 2 ：CO：CO 2 ) Is that 2:1:1. closing the valve on the reactor, it can be observed through the visible window of the reactor: a condensed product was formed at an early stage (as shown in fig. 4), and a liquid product was observed as the reaction proceeded (as shown in fig. 5); waxy products could be observed as the reaction proceeded further (as shown in fig. 6); the composition of the gaseous products in the reactor was tested by quadrupole mass spectrometry and the results are shown in figure 7.
As can be seen from fig. 4 to 6: the condensed product generated in the initial stage of the chemical reaction is continuously converted into the liquid organic matter as shown in fig. 5 under the irradiation of the beta ray generated by the decay of the tritium, and the liquid organic matter is finally converted into the waxy organic matter as shown in fig. 6.
As can be seen from fig. 7: the generated gaseous product mainly comprises tritiated alkane, tritiated olefin, tritiated aldehyde, tritiated alcohol, carboxylic acid and other tritiated organic matters.
Example 3
Preparing organic matters by catalyzing mixed gas of hydrogen and carbon dioxide by X-rays:
evacuating the reactor capable of bearing high-pressure gas, cleaning the reactor with carbon dioxide gas for 3 times, evacuating, injecting carbon dioxide into the reactor, injecting hydrogen into the reactor, controlling total pressure at 10MPa, and controlling gas molar ratio (H) 2 ：CO 2 ) Is 1:1. the valve on the reactor was closed, the reactor was irradiated exogenously with X-rays having an energy of 9MeV (dose rate of ionizing radiation of 2 Gy/h), and the composition of the gaseous products inside the reactor was tested by quadrupole mass spectrometry, the results of which are shown in FIG. 8.
As can be seen from fig. 8: the gaseous product is mainly alkane, and also comprises olefin, aldehyde, alcohol, carboxylic acid and other organic matters.
The foregoing is only a preferred embodiment of the present invention, and it should be noted that, for those skilled in the art, various modifications and decorations can be made without departing from the principle of the present invention, and these modifications and decorations should also be regarded as the protection scope of the present invention.

Claims (8)

1. A method for preparing organic matters by catalyzing carbon dioxide synthesis gas with ionizing radiation is characterized by comprising the following steps:
taking carbon dioxide synthesis gas as a preparation raw material, and carrying out chemical reaction under the action of ionizing radiation to obtain an organic matter;
the carbon dioxide synthesis gas comprises hydrogen isotope gas and carbon-containing gas;
the hydrogen isotope gas comprises one or more of protium, deuterium and tritium isotopes;
the carbon-containing gas comprises carbon monoxide and/or carbon dioxide.
2. The method of claim 1, wherein the hydrogen isotope gas comprises hydrogen gas, deuterium gas, or tritium-containing hydrogen isotope gas.
3. The method of claim 2, wherein the tritiated hydrogen isotope-containing gas comprises tritium gas or a tritiated hydrogen isotope-containing gas mixture.
4. The method of claim 1, wherein the ionizing radiation is generated by a source of ionizing radiation; the ionizing radiation source includes one or more of alpha rays, beta rays, gamma rays, X rays, and n.
5. The method of claim 4, wherein the source of ionizing radiation comprises an endogenous source of ionizing radiation or an exogenous source of ionizing radiation.
6. The method of claim 5, wherein the ionizing radiation is at a dose rate of at least 2Gy/h when generated by an external source of ionizing radiation.
7. The method according to any one of claims 4 to 6, wherein the ionizing radiation source is a radionuclide or a shielding ray; the shielding ray is the ray which needs to be shielded in a power station or a large-scale ray device.
8. The method of claim 5, wherein when the ionizing radiation source is an exogenous ionizing radiation source, the pressure of the chemical reaction is greater than or equal to 5MPa; when the ionizing radiation source is an endogenous ionizing radiation source, the pressure of the chemical reaction is more than or equal to 0.1MPa.
CN202211140391.8A 2022-09-20 2022-09-20 Method for preparing organic matter by catalyzing carbon dioxide synthesis gas through ionizing radiation Pending CN115504846A (en)

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