CN116496137A - Method for catalyzing natural gas to produce olefin through thermal radiation - Google Patents
Method for catalyzing natural gas to produce olefin through thermal radiation Download PDFInfo
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- CN116496137A CN116496137A CN202310212300.5A CN202310212300A CN116496137A CN 116496137 A CN116496137 A CN 116496137A CN 202310212300 A CN202310212300 A CN 202310212300A CN 116496137 A CN116496137 A CN 116496137A
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- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 title claims abstract description 185
- 230000005855 radiation Effects 0.000 title claims abstract description 157
- 239000003345 natural gas Substances 0.000 title claims abstract description 56
- 150000001336 alkenes Chemical class 0.000 title claims abstract description 55
- 238000000034 method Methods 0.000 title claims abstract description 55
- JRZJOMJEPLMPRA-UHFFFAOYSA-N olefin Natural products CCCCCCCC=C JRZJOMJEPLMPRA-UHFFFAOYSA-N 0.000 title claims abstract description 41
- 238000006243 chemical reaction Methods 0.000 claims abstract description 217
- 239000007789 gas Substances 0.000 claims abstract description 38
- 230000003197 catalytic effect Effects 0.000 claims abstract description 22
- 238000001228 spectrum Methods 0.000 claims abstract description 19
- 238000006555 catalytic reaction Methods 0.000 claims abstract description 16
- 238000004519 manufacturing process Methods 0.000 claims abstract description 14
- 239000007788 liquid Substances 0.000 claims abstract description 11
- 239000011949 solid catalyst Substances 0.000 claims abstract description 10
- 238000010521 absorption reaction Methods 0.000 claims abstract description 9
- 239000012495 reaction gas Substances 0.000 claims description 90
- 239000003054 catalyst Substances 0.000 claims description 68
- 238000010438 heat treatment Methods 0.000 claims description 30
- OTMSDBZUPAUEDD-UHFFFAOYSA-N Ethane Chemical compound CC OTMSDBZUPAUEDD-UHFFFAOYSA-N 0.000 claims description 26
- 239000000463 material Substances 0.000 claims description 19
- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 claims description 10
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 8
- 239000002184 metal Substances 0.000 claims description 7
- 239000001569 carbon dioxide Substances 0.000 claims description 5
- 229910002092 carbon dioxide Inorganic materials 0.000 claims description 5
- 239000010431 corundum Substances 0.000 claims description 5
- 229910052593 corundum Inorganic materials 0.000 claims description 5
- 239000000919 ceramic Substances 0.000 claims description 4
- 230000003595 spectral effect Effects 0.000 claims description 4
- 229910001120 nichrome Inorganic materials 0.000 claims description 3
- 239000000126 substance Substances 0.000 abstract description 6
- 238000005265 energy consumption Methods 0.000 abstract description 5
- 238000012986 modification Methods 0.000 abstract description 5
- 230000004048 modification Effects 0.000 abstract description 5
- 238000007146 photocatalysis Methods 0.000 abstract description 4
- 230000001699 photocatalysis Effects 0.000 abstract description 4
- 230000036632 reaction speed Effects 0.000 abstract description 3
- 230000035484 reaction time Effects 0.000 abstract description 3
- 239000000203 mixture Substances 0.000 description 23
- VGGSQFUCUMXWEO-UHFFFAOYSA-N Ethene Chemical compound C=C VGGSQFUCUMXWEO-UHFFFAOYSA-N 0.000 description 22
- 239000005977 Ethylene Substances 0.000 description 22
- 238000004817 gas chromatography Methods 0.000 description 20
- OKKJLVBELUTLKV-UHFFFAOYSA-N Methanol Chemical compound OC OKKJLVBELUTLKV-UHFFFAOYSA-N 0.000 description 6
- 230000004913 activation Effects 0.000 description 3
- 238000009434 installation Methods 0.000 description 3
- 239000000047 product Substances 0.000 description 3
- 239000010453 quartz Substances 0.000 description 3
- 239000002994 raw material Substances 0.000 description 3
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N silicon dioxide Inorganic materials O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 3
- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 description 2
- 230000009286 beneficial effect Effects 0.000 description 2
- 230000015572 biosynthetic process Effects 0.000 description 2
- NEHMKBQYUWJMIP-UHFFFAOYSA-N chloromethane Chemical compound ClC NEHMKBQYUWJMIP-UHFFFAOYSA-N 0.000 description 2
- 239000000446 fuel Substances 0.000 description 2
- 238000005286 illumination Methods 0.000 description 2
- 239000002574 poison Substances 0.000 description 2
- 231100000614 poison Toxicity 0.000 description 2
- 238000003786 synthesis reaction Methods 0.000 description 2
- 238000012546 transfer Methods 0.000 description 2
- 230000005457 Black-body radiation Effects 0.000 description 1
- 229910000831 Steel Inorganic materials 0.000 description 1
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 description 1
- 229910021529 ammonia Inorganic materials 0.000 description 1
- 230000005540 biological transmission Effects 0.000 description 1
- 239000006227 byproduct Substances 0.000 description 1
- 239000000969 carrier Substances 0.000 description 1
- 239000003153 chemical reaction reagent Substances 0.000 description 1
- 238000001514 detection method Methods 0.000 description 1
- 238000011161 development Methods 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 238000005485 electric heating Methods 0.000 description 1
- 238000002474 experimental method Methods 0.000 description 1
- 230000002349 favourable effect Effects 0.000 description 1
- 239000003502 gasoline Substances 0.000 description 1
- 239000012535 impurity Substances 0.000 description 1
- 230000001788 irregular Effects 0.000 description 1
- 238000005259 measurement Methods 0.000 description 1
- 230000008018 melting Effects 0.000 description 1
- 238000002844 melting Methods 0.000 description 1
- 239000007769 metal material Substances 0.000 description 1
- WSFSSNUMVMOOMR-NJFSPNSNSA-N methanone Chemical compound O=[14CH2] WSFSSNUMVMOOMR-NJFSPNSNSA-N 0.000 description 1
- 229940050176 methyl chloride Drugs 0.000 description 1
- -1 natural gas olefin Chemical class 0.000 description 1
- 239000003973 paint Substances 0.000 description 1
- 239000003208 petroleum Substances 0.000 description 1
- 238000002360 preparation method Methods 0.000 description 1
- 239000000523 sample Substances 0.000 description 1
- 239000007787 solid Substances 0.000 description 1
- 229910001220 stainless steel Inorganic materials 0.000 description 1
- 239000010935 stainless steel Substances 0.000 description 1
- 239000010959 steel Substances 0.000 description 1
- 238000006467 substitution reaction Methods 0.000 description 1
- 230000002195 synergetic effect Effects 0.000 description 1
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Classifications
-
- C—CHEMISTRY; METALLURGY
- C07—ORGANIC CHEMISTRY
- C07C—ACYCLIC OR CARBOCYCLIC COMPOUNDS
- C07C2/00—Preparation of hydrocarbons from hydrocarbons containing a smaller number of carbon atoms
- C07C2/76—Preparation of hydrocarbons from hydrocarbons containing a smaller number of carbon atoms by condensation of hydrocarbons with partial elimination of hydrogen
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- Chemical & Material Sciences (AREA)
- Organic Chemistry (AREA)
- Organic Low-Molecular-Weight Compounds And Preparation Thereof (AREA)
Abstract
The application provides a method for catalyzing natural gas to produce olefin through thermal radiation, and relates to the field of chemical industry. According to the method for producing olefin by catalyzing natural gas through thermal radiation, photocatalysis generated by thermal radiation is added into traditional thermal catalysis, so that the catalytic performance of the method is improved, the reaction speed is accelerated, the conversion rate is improved, the catalytic reaction selectivity is improved, and the reaction time and the energy consumption are reduced. In the catalytic process participated in aiming at gas, liquid and solid catalysts with heat radiation spectrum absorption capacity, the method can further improve the characteristics of catalytic performance, selectivity, stability and the like on the basis of the original catalytic performance. The method is mainly aimed at improving the catalytic performance of the natural gas for producing olefin, has the characteristics of simple and convenient operation and stable operation, and does not need excessive modification on the prior industrial equipment.
Description
Technical Field
The application relates to the field of chemical industry, in particular to a method for catalyzing natural gas to produce olefin through thermal radiation.
Background
With the growing shortage of petroleum resources, further development and utilization of natural gas resources are attracting more and more attention. The natural gas can be used as fuel, high-efficiency, high-quality and clean energy and chemical raw materials. The main composition of natural gas is methane, and the comprehensive utilization of methane is largely divided into two main types, namely a direct conversion method and an indirect conversion method. The direct conversion method is to directly convert methane into chemical raw materials such as ethylene, methanol, formaldehyde, methyl chloride and the like, and the indirect conversion method is to firstly convert methane into synthesis gas, and then prepare liquid fuels such as methanol, gasoline and the like and synthetic ammonia and the like from the synthesis gas.
The methane indirect conversion method needs a long time to complete conversion, and has the advantages of relatively large investment and large energy consumption. The direct conversion method of methane has a higher energy efficiency process, and the difficulty is the selective activation and directional conversion of methane.
Disclosure of Invention
The invention aims to provide a method for catalyzing natural gas to produce olefin through thermal radiation, which aims to solve the problems that the existing methane indirect conversion method needs to take a long time to finish conversion, the investment is relatively large, the energy consumption is large and the selective activation and directional conversion of methane by a direct methane conversion method are difficult.
In order to achieve the above purpose, the present application provides a method for producing olefins by catalyzing natural gas through thermal radiation, wherein a reaction gas is introduced into a reaction device, the volume ratio of methane in the reaction gas is greater than or equal to 20% and less than 100%, the volume ratio of ethane is greater than 0 and less than or equal to 80%, and the reaction gas is catalyzed under the conditions of heating and thermal radiation to prepare the olefins; the thermal radiation includes a first thermal radiation generated by the heated heat source.
Preferably, the temperature of the reaction gas heating is 300-1000 ℃;
preferably, the temperature of the reaction gas heating is 450-650 ℃.
Preferably, a radiation source is further arranged in the reaction device, and the heat radiation further comprises second heat radiation generated by the radiation source;
preferably, the temperature of the radiation source is 300-1500 ℃;
preferably, the temperature of the radiation source is 500-1000 ℃.
Preferably, the introducing the reaction gas into the reaction device further comprises: adding a catalyst into a reaction device, wherein the catalyst can absorb the spectrum of the thermal radiation so as to raise the surface temperature of the catalyst and improve the internal energy of a reaction system; the catalyst includes any one or more of a gas catalyst, a solid catalyst, and a liquid catalyst.
Preferably, the catalyst comprises a gas catalyst which is a gas molecule having strong spectral absorption of thermal radiation;
preferably, the gas catalyst comprises either or both of carbon dioxide and water vapor;
preferably, the volume ratio of the reaction gas to the gas catalyst is (1000:1) to (1:1000).
Preferably, the temperature of the reaction gas is 550-650 ℃, and the reaction gas is introduced into the reaction device further comprises: adding a catalyst into a reaction device, wherein the catalyst can absorb the spectrum of the thermal radiation so as to raise the surface temperature of the catalyst and improve the internal energy of a reaction system; the catalyst comprises any one or more of a gas catalyst, a solid catalyst and a liquid catalyst;
preferably, the catalyst comprises a gas catalyst which is a gas molecule having strong spectral absorption of thermal radiation;
preferably, the gas catalyst comprises either or both of carbon dioxide and water vapor;
preferably, the volume ratio of the reaction gas to the gas catalyst is (1000:1) to (1:1000).
Preferably, the reaction device is a tubular reactor, the reaction gas is introduced into a reaction tube of the reaction device, and the reaction tube is prepared from a transparent high-temperature-resistant material or a high-emissivity material.
Preferably, the reaction device is a tubular reactor, the reaction gas is introduced into a reaction tube of the reaction device, the reaction tube is made of transparent high-temperature resistant material or high-emissivity material, and the distances between the radiation source and the reaction tube and between the radiation source and the reaction tube are respectively 0-100cm.
Preferably, the radiation source is a wound heating wire or heating rod, and the heat source is a wound heating wire or heating rod; the radiation source is made of metal; the outer surface of the heat source is wrapped with corundum and/or ceramic.
Preferably, the flow rate of the reaction gas is 1-1000ml/min.
Compared with the prior art, the beneficial effects of this application include:
according to the method for producing olefin by catalyzing natural gas through thermal radiation, photocatalysis generated by thermal radiation is added into traditional thermal catalysis, so that the catalytic performance of the method is improved, the reaction speed is accelerated, the conversion rate is improved, the catalytic reaction selectivity is improved, and the reaction time and the energy consumption are reduced.
In the catalytic process participated in aiming at gas, liquid and solid catalysts with heat radiation spectrum absorption capacity, the method can further improve the characteristics of catalytic performance, selectivity, stability and the like on the basis of the original catalytic performance.
The method is mainly aimed at improving the catalytic performance of the natural gas for producing olefin, has the characteristics of simple and convenient operation and stable operation, and does not need excessive modification on the prior industrial equipment.
Drawings
In order to more clearly illustrate the technical solutions of the embodiments of the present application, the drawings that are needed in the embodiments will be briefly described below, it being understood that the following drawings only illustrate certain embodiments of the present application and therefore should not be considered as limiting the scope of the present application.
FIG. 1 is a schematic structural view of an embodiment of a reaction apparatus of the present application;
FIG. 2 is a schematic structural view of another embodiment of the reaction apparatus of the present application.
The reference numerals are:
10-a reaction tube; 11-air inlet; 12-an air outlet; 20-a heat source; 30-cavity; 40-a housing.
Detailed Description
The term as used herein:
"prepared from … …" is synonymous with "comprising". The terms "comprising," "including," "having," "containing," or any other variation thereof, as used herein, are intended to cover a non-exclusive inclusion. For example, a composition, step, method, article, or apparatus that comprises a list of elements is not necessarily limited to only those elements but may include other elements not expressly listed or inherent to such composition, step, method, article, or apparatus.
The conjunction "consisting of … …" excludes any unspecified element, step or component. If used in a claim, such phrase will cause the claim to be closed, such that it does not include materials other than those described, except for conventional impurities associated therewith. When the phrase "consisting of … …" appears in a clause of the claim body, rather than immediately following the subject, it is limited to only the elements described in that clause; other elements are not excluded from the stated claims as a whole.
When an equivalent, concentration, or other value or parameter is expressed as a range, preferred range, or a range bounded by a list of upper preferable values and lower preferable values, this is to be understood as specifically disclosing all ranges formed from any pair of any upper range limit or preferred value and any lower range limit or preferred value, regardless of whether ranges are separately disclosed. For example, when ranges of "1 to 5" are disclosed, the described ranges should be construed to include ranges of "1 to 4", "1 to 3", "1 to 2 and 4 to 5", "1 to 3 and 5", and the like. When a numerical range is described herein, unless otherwise indicated, the range is intended to include its endpoints and all integers and fractions within the range.
In these examples, the parts and percentages are by mass unless otherwise indicated.
"parts by mass" means a basic unit of measurement showing the mass ratio of a plurality of components, and 1 part may be any unit mass, for example, 1g may be expressed, 2.689g may be expressed, and the like. If we say that the mass part of the a component is a part and the mass part of the B component is B part, the ratio a of the mass of the a component to the mass of the B component is represented as: b. alternatively, the mass of the A component is aK, and the mass of the B component is bK (K is an arbitrary number and represents a multiple factor). It is not misunderstood that the sum of the parts by mass of all the components is not limited to 100 parts, unlike the parts by mass.
"and/or" is used to indicate that one or both of the illustrated cases may occur, e.g., a and/or B include (a and B) and (a or B).
The application provides a method for producing olefin by catalyzing natural gas through thermal radiation, which comprises the steps of introducing reaction gas into a reaction device, wherein the volume ratio of methane in the reaction gas is more than or equal to 20% and less than 100%, the volume ratio of ethane is more than 0 and less than or equal to 80%, and the reaction gas is catalyzed to prepare olefin under the conditions of heating and thermal radiation; the thermal radiation includes a first thermal radiation generated by the heated heat source.
The reaction gas may be mainly methane and ethane, and the volume ratio of methane may be, for example, 20%, 30%, 40%, 50%, 60%, 70%, 80%, or 90%, and the volume ratio of ethane may be, for example, 10%, 20%, 30%, 40%, 50%, 60%, 70%, or 80%. Preferably, the reaction gas in the embodiment satisfies that the volume ratio of methane is 80% or more and less than 100%, and the volume ratio of ethane is 0% or more and 20% or less.
The reaction device is a device for catalyzing natural gas to produce olefin by heat radiation, and the shape, structure and the like of the reaction device are not particularly limited, and may be, for example, a cube, a cuboid, a cylinder, or other irregular shapes and the like. The reaction device may be, for example, a cavity reactor or a tube reactor. The reaction device is a cavity type reactor, and then the reaction gas is introduced into the reaction cavity for catalytic reaction, and the reaction device is a tubular type reactor, and then the reaction gas is introduced into the reaction tube for catalytic reaction.
Preferably, referring to fig. 1 and 2, the reaction apparatus is a tubular reactor, and includes a housing 40, the reaction gas is introduced into a reaction tube 10 of the reaction apparatus through a gas inlet 11 and is communicated with a detection device through a gas outlet 12, and the reaction tube 10 is made of a transparent high temperature resistant material or a high emissivity material. The transparent high temperature resistant material for preparing the reaction tube can be, for example, transparent quartz, so that the transparent quartz tube is prepared; the high emissivity material for preparing the reaction tube can be corundum, a sand-blasted stainless steel tube or a steel tube sprayed with black body radiation paint, for example.
The distance between the heat source 20 and the reaction tube 10 may be 0 to 100cm, for example, may be 0cm, 5cm, 10cm, 20cm, 30cm, 40cm, 50cm, 60cm, 70cm, 80cm, 90cm or 100cm, or any value between 0 and 100cm. The installation distance determines the temperature and the thermal radiation spectrum of the reaction tube 10, so that the installation distance can be adjusted according to the temperature and the thermal radiation spectrum required for practical use. Wherein, the closer the heat source 20 is to the reaction tube 10, the more favorable the heat radiation transmission, and the catalyst or reaction molecule is convenient to absorb the heat radiation spectrum.
The thermal radiation catalytic natural gas olefin production index is mainly evaluated in two aspects, including conversion rate and selectivity, wherein the conversion rate is the ratio of the amount of a product to the amount of input raw materials, and the higher the conversion rate is, the more the obtained olefin is; selectivity refers to the probability of selecting the desired product relative to the byproducts when a reaction is performed. The conversion rate and selectivity of the natural gas to olefin by thermal radiation catalysis can be measured by a gas chromatograph externally connected with a reaction furnace.
The existing preparation of olefin by natural gas mainly uses heating and solid metal catalyst to make catalytic reaction, and the reaction cavity or reaction tube of the existing reaction device is usually prepared by using opaque common high-temperature-resistant material. The applicant has found that the heat source for heating provides a temperature and also radiates heat, which can produce a spectrum of heat radiation, and also has a catalytic effect. The thermal radiation catalysis is mainly divided into two parts, namely, the thermal radiation is used for transferring heat energy, and the thermal radiation spectrum can be used for driving photocatalysis to achieve the effect of photo-thermal synergistic catalysis, so that the molecular bond vibration of the reaction gas is enhanced, the internal energy of a reaction system is improved, and the natural gas can be used for preparing olefin under the condition of no catalyst.
Wherein, the heat radiation is the phenomenon that the object radiates electromagnetic waves due to the temperature, and is one of three modes of heat transfer, all objects with the temperature higher than absolute zero can generate heat radiation, and the higher the temperature, the larger the total energy radiated by the object, and the more short wave components. The spectrum of thermal radiation is a continuum spectrum, and the wavelength coverage can theoretically range from 0 up to +.. Thus, the heat source used for heating of the present application may also generate heat radiation, i.e. first heat radiation, as one of the conditions of the process for catalyzing the production of olefins from natural gas. It can be understood that in order to improve the energy of heat radiation, a radiation source can be additionally arranged on the basis of a heat source, so that the reaction efficiency is improved.
According to the method for producing olefin by catalyzing natural gas through thermal radiation, photocatalysis generated by thermal radiation is added into traditional thermal catalysis, so that the catalytic performance of the method is improved, the reaction speed is accelerated, the conversion rate is improved, the catalytic reaction selectivity is improved, and the reaction time and the energy consumption are reduced.
Wherein heating means heating the reaction gas at a temperature of 300 to 1000 ℃, for example, 300 to 700 ℃, or 500 to 1000 ℃, or 400 to 800 ℃, or 450 to 650 ℃. Preferably, the temperature at which the reaction gas is heated is 450 to 650 ℃, and may be, for example, (450, 500, 550, 600, or 650) °c, or any value between 450 and 650 ℃, and the temperature at which the reaction gas is heated may also be referred to as the reaction temperature thereof. The reaction temperature may be maintained at a set reaction temperature by, for example, disposing a temperature sensing probe in the reaction tube or the reaction chamber and heating the reaction tube or the reaction chamber by a heat source in the reaction apparatus.
It is understood that the reaction tube 10 may be heated by an external heat source, or the reaction tube 10 itself may be electrically heated to heat the reaction gas in the reaction tube 10. The reaction tube 10 is made of a transparent high temperature resistant material so as to be penetrated by heat radiation of more external heat sources to perform heat radiation illumination on the reaction gas in the reaction tube 10. The reaction tube 10 may also be made of a high emissivity material so that the reaction tube 10 itself may be heat-radiated as a heat source after being heated to light the reaction gas inside the reaction tube 10.
In other embodiments, when the reaction device is a cavity reactor, the reaction gas is directly introduced into the reaction cavity to react, and the heat source directly heats and radiates the reaction gas. Similar to the tubular reactor, the reaction chamber may be self-energized to heat as a heat source, or a heat source structure including a high emissivity material such as a heating rod or a heating wire may be installed in the reaction chamber, so that heat radiation illumination is generated by the heating rod or the heating wire to act on the reaction gas.
In a preferred embodiment, a radiation source is further arranged in the reaction device, the heat radiation further comprises second heat radiation generated by the radiation source, and the catalytic reaction efficiency can be improved by adding one radiation source on the basis of the heat source.
Wherein the temperature of the radiation source is 300-1500deg.C, such as 300-800deg.C, or 700-1300 deg.C, or 600-1000 deg.C, or 500-1500deg.C. Preferably, the temperature of the radiation source is 500-1000 ℃, for example 500 ℃, 600 ℃, 700 ℃, 800 ℃, 900 ℃ or 1000 ℃.
Optionally, with continued reference to fig. 1 and 2, a cavity 30 structure may be provided in the tubular reactor, with the reactor tube 10 being mounted within the cavity 30 structure, and the heat source 20 and the radiation source being mounted within the cavity 30 structure for releasing thermal radiation.
The distance between the radiation source and the reaction tube 10 is 0-100cm, for example, may be any value between 0cm, 5cm, 10cm, 20cm, 30cm, 40cm, 50cm, 60cm, 70cm, 80cm, 90cm or 100cm, or between 0-100cm, and the installation distance determines the size of the second heat radiation and may be adjusted according to the actual application.
The radiation source can be a wound heating wire or a heating rod, and the heat source can also be a wound heating wire (shown in figure 1) or a heating rod (shown in figure 2); the radiation source is made of metal, and the emissivity of the radiation source is between 0.5 and 0.99, so that the radiation source has high heat radiation. Preferably, the radiation source is made of nichrome. Wherein emissivity is generally called emissivity, which means that the ratio of the radiation capacity of an object to the radiation capacity of a black body at the same temperature is called emissivity of the object, generally in the range of [0,1], and the higher the emissivity, the higher the thermal radiation of the object.
The heat source can only provide heat and can also provide heat radiation, the heat source can provide heat radiation by wrapping corundum and/or ceramic on the outer surface of the heat source, the corundum and the ceramic are made of high-emissivity materials, the emissivity of the heat source can be improved, or the heat source also adopts a metal material with high emissivity.
The method is mainly aimed at improving the catalytic performance of the natural gas for producing olefin, has the characteristics of simple and convenient operation and stable operation, and does not need excessive modification on the prior industrial equipment.
In a preferred embodiment, the introducing the reaction gas into the reaction apparatus further comprises: adding a catalyst into a reaction device, wherein the catalyst can absorb the spectrum of the thermal radiation so as to raise the surface temperature of the catalyst and improve the internal energy of a reaction system; the catalyst includes any one or more of a gas catalyst, a solid catalyst, and a liquid catalyst.
Specifically, the catalyst is added in the thermal radiation catalytic reaction process to improve the catalytic rate, and the catalyst has the characteristics of absorbing the spectrum generated by thermal radiation, namely absorbing the thermal radiation, so that the self surface temperature is increased, vibration is enhanced, the solid catalyst and the liquid catalyst can also excite the generation of photo-generated carriers or surface plasma, and the activation of reactive gas molecules is promoted, thereby accelerating the reaction rate.
In the catalytic process participated in aiming at gas, liquid and solid catalysts with heat radiation spectrum absorption capacity, the method can further improve the characteristics of catalytic performance, selectivity, stability and the like on the basis of the original catalytic performance.
The specific form of the catalyst is not limited, and may be a gas having an absorption capacity for the thermal radiation spectrum (a substance having a vaporization temperature lower than the catalytic temperature), or a liquid having an absorption capacity for the thermal radiation spectrum (a substance having a melting temperature lower than the catalytic temperature), or a solid catalyst.
In one embodiment, the catalyst comprises a gas catalyst that is a gas molecule that is strongly spectrally absorptive of thermal radiation; the internal energy of the gas catalyst molecules is increased, which is beneficial to the transfer of kinetic energy in the process of molecular collision. The gas catalyst comprises either or both of carbon dioxide and water vapor, as well as any other gas molecules that can absorb the spectrum of thermal radiation.
More preferably, the gas catalyst is water vapor, and the spectral absorption characteristics of water vapor are better, so that the catalytic performance is better.
Preferably, the volume ratio of the reaction gas and the gas catalyst is (1000:1) - (1:1000), for example, may be 2:1, 3:2, 5:3, 10:3, 50:3, 50:23, 100:33, 200:55, 300:57, 400:1 or 500:1.
In another preferred embodiment, the temperature of the reaction gas heating is 550-650 ℃, for example, 550 ℃, 600 ℃ or 650 ℃, and the step of introducing the reaction gas into the reaction device without an external radiation source further comprises: the catalyst is added into the reaction device, and the characteristics of the catalyst are the same as those of the catalyst in the above embodiment, and will not be described in detail here. Experiments have shown that in the absence of sufficient heat radiation to provide sufficient energy to deactivate the catalyst steam, the steam can poison the reaction at low temperatures, slowing the reaction.
Preferably, the flow rate of the reaction gas is 1 to 1000ml/min, and may be, for example, (1, 2, 3, 4, 5, 6, 7, 8, 9, 10, 20, 30, 50, 100, 200, 300, 400, 500, 600, 700, 800, 900 or 1000) ml/min, or any value between 1 and 1000ml/min.
Embodiments of the present application will be described in detail below with reference to specific examples, but it will be understood by those skilled in the art that the following examples are only for illustration of the present application and should not be construed as limiting the scope of the present application. The specific conditions are not noted in the examples and are carried out according to conventional conditions or conditions recommended by the manufacturer. The reagents or apparatus used were conventional products commercially available without the manufacturer's attention.
For convenience of description, the reaction apparatus for catalyzing natural gas to produce olefins by heat radiation according to the embodiment of the present invention is illustrated by taking a tube reactor similar to that of fig. 2 as an example, the reaction apparatus includes a housing 40 and is provided with a cavity structure 30, a reaction tube 10 and a heat source 20 are provided in the cavity structure 30, the reaction tube 10 includes an air inlet 11 and an air outlet 12 for introducing a reaction gas, a transparent quartz tube is used as the reaction tube 10, the heat source 20 is alumina-based electric heating rods with high heat emissivity, the total number of the heat sources 20 is 6, and the distance between the heating rods and the reaction tube 10 is about 5cm, unlike fig. 2 in which the heat source 20 and the reaction tube 10 are uniformly installed around the reaction tube 10 in parallel. The radiation source is a spiral winding metal wire with the length of 14.5cm and the material of nichrome, and the metal wire and the reaction tube 10 are arranged in parallel with each other, and the distance is about 5 cm.
It will be appreciated by those skilled in the art that the structure of the reaction apparatus described herein is merely for illustrating the present application, and should not be construed as limiting the scope of the present application, and that the specific structure, parameters, etc. of the reaction apparatus may be modified or replaced according to practical applications, and these modifications or replacements do not deviate the essence of the corresponding technical solutions from the scope of the technical solutions of the embodiments of the present application.
Example 1
A method for catalyzing natural gas to produce olefin by heat radiation comprises the following specific steps:
after the reaction gas was mixed in a volume ratio of 42.5% methane, 7.5% ethane and 50% Ar, the reaction temperature was set to 450℃and the total reaction gas flow rate was set to 4mL/min, and the mixture was introduced into a reaction apparatus shown in FIG. 1. After 1 hour of reaction, the initial conversion was about 0.86% and the ethylene selectivity was 100% as indicated by the results of external gas chromatography.
Example 2
A method for catalyzing natural gas to produce olefin by heat radiation comprises the following specific steps:
after the reaction gas was mixed in a volume ratio of 42.5% methane, 7.5% ethane and 50% Ar, the reaction temperature was set at 500℃and the total reaction gas flow rate was set at 4mL/min, and the mixture was introduced into a reaction apparatus shown in FIG. 1. After 1 hour of reaction, the initial conversion was about 1.25% and the ethylene selectivity was 100% as determined by the results of external gas chromatography.
Example 3
A method for catalyzing natural gas to produce olefin by heat radiation comprises the following specific steps:
after the reaction gas was mixed in a volume ratio of 42.5% methane, 7.5% ethane and 50% Ar, the reaction temperature was set to 550℃and the total reaction gas flow rate was set to 4mL/min, and the mixture was introduced into a reaction apparatus shown in FIG. 1. After 1 hour of reaction, the initial conversion was about 1.17% and the ethylene selectivity was 81.06% as determined by the external gas chromatography.
Example 4
A method for catalyzing natural gas to produce olefin by heat radiation comprises the following specific steps:
after the reaction gas was mixed in a volume ratio of 42.5% methane, 7.5% ethane and 50% Ar, the reaction temperature was set at 600℃and the total reaction gas flow rate was set at 4mL/min, and the mixture was introduced into a reaction apparatus shown in FIG. 1. After 1 hour of reaction, the initial conversion was about 1.15% and the ethylene selectivity was 79.31% as indicated by the results of external gas chromatography.
Example 5
A method for catalyzing natural gas to produce olefin by heat radiation comprises the following specific steps:
after the reaction gas was mixed in a volume ratio of 42.5% methane, 7.5% ethane and 50% Ar, the reaction temperature was set to 650℃and the total reaction gas flow rate was set to 4mL/min, and the mixture was introduced into a reaction apparatus shown in FIG. 1. After 1 hour of reaction, the initial conversion was about 1.65% and the ethylene selectivity was 80.89% as determined by the external gas chromatography.
Example 6
A method for catalyzing natural gas to produce olefin by heat radiation comprises the following specific steps:
after the reaction gas was mixed in a volume ratio of 42.5% methane, 7.5% ethane and 50% Ar, the reaction temperature was set to 450℃and the heat radiation temperature was set to 700℃to set the total reaction gas flow rate to 4mL/min, and the mixture was introduced into a reaction apparatus shown in FIG. 1. After 1 hour of reaction, the initial conversion was about 1.71% and the ethylene selectivity was 100% as determined by the external gas chromatography.
Example 7
A method for catalyzing natural gas to produce olefin by heat radiation comprises the following specific steps:
after the reaction gas was mixed in a volume ratio of 42.5% methane, 7.5% ethane and 50% Ar, the reaction temperature was set to 500℃and the heat radiation temperature was set to 700℃to set the total reaction gas flow rate to 4mL/min, and the mixture was introduced into a reaction apparatus shown in FIG. 1. After 1 hour of reaction, the initial conversion was about 2.18% and the ethylene selectivity was 100% as seen from the results of external gas chromatography.
Example 8
A method for catalyzing natural gas to produce olefin by heat radiation comprises the following specific steps:
after the reaction gas was mixed in a volume ratio of 42.5% methane, 7.5% ethane and 50% Ar, the reaction temperature was set to 550℃and the heat radiation temperature was set to 700℃to set the total reaction gas flow rate to 4mL/min, and the mixture was introduced into a reaction apparatus shown in FIG. 1. After 1 hour of reaction, the initial conversion was about 2.66% and the ethylene selectivity was 89.54% as determined by the external gas chromatography.
Example 9
A method for catalyzing natural gas to produce olefin by heat radiation comprises the following specific steps:
after the reaction gas was mixed in a volume ratio of 42.5% methane, 7.5% ethane and 50% Ar, the reaction temperature was set to 600℃and the heat radiation temperature was set to 700℃to set the total reaction gas flow rate to 4mL/min, and the mixture was introduced into a reaction apparatus shown in FIG. 1. After 1 hour of reaction, the initial conversion was about 3.01% and the ethylene selectivity was 85.25% as indicated by the results of external gas chromatography.
Example 10
A method for catalyzing natural gas to produce olefin by heat radiation comprises the following specific steps:
after the reaction gas was mixed in a volume ratio of 42.5% methane, 7.5% ethane and 50% Ar, the reaction temperature was set to 650 ℃, the heat radiation temperature was set to 700 ℃, and the total reaction gas flow rate was set to 4mL/min, and the mixture was introduced into a reaction apparatus shown in FIG. 1. After 1 hour of reaction, the initial conversion was about 3.72% and the ethylene selectivity was 88.45% as indicated by the results of external gas chromatography.
Example 11
A method for catalyzing natural gas to produce olefin by heat radiation comprises the following specific steps:
after the reaction gas was mixed according to the volume ratio of 42.5% methane, 7.5% ethane and 47.4% Ar, 2.6% steam, the reaction temperature was set to 450℃and the heat radiation temperature was set to 700℃to set the total reaction gas flow rate to 4mL/min, and the mixture was introduced into the reaction apparatus shown in FIG. 1. After 1 hour of reaction, the initial conversion was about 2.30% and the ethylene selectivity was 100% as seen from the results of external gas chromatography.
Example 12
A method for catalyzing natural gas to produce olefin by heat radiation comprises the following specific steps:
after the reaction gas was mixed according to the volume ratio of 42.5% methane, 7.5% ethane and 47.4% Ar, 2.6% steam, the reaction temperature was set to 500℃and the heat radiation temperature was set to 700℃to set the total reaction gas flow rate to 4mL/min, and the mixture was introduced into the reaction apparatus shown in FIG. 1. After 1 hour of reaction, the initial conversion was about 2.54% and the ethylene selectivity was 100% as seen from the results of external gas chromatography.
Example 13
A method for catalyzing natural gas to produce olefin by heat radiation comprises the following specific steps:
after the reaction gas was mixed according to the volume ratio of 42.5% methane, 7.5% ethane and 47.4% Ar, 2.6% steam, the reaction temperature was set to 550℃and the heat radiation temperature was set to 700℃to set the total reaction gas flow rate to 4mL/min, and the mixture was introduced into the reaction apparatus shown in FIG. 1. After 1 hour of reaction, the initial conversion was about 4.19% and the ethylene selectivity was 100% as seen from the results of external gas chromatography.
Example 14
A method for catalyzing natural gas to produce olefin by heat radiation comprises the following specific steps:
after the reaction gas was mixed according to the volume ratio of 42.5% methane, 7.5% ethane and 47.4% Ar, 2.6% steam, the reaction temperature was set at 600℃and the heat radiation temperature was set at 700℃to set the total reaction gas flow rate at 4mL/min, and the mixture was introduced into the reaction apparatus shown in FIG. 1. After 1 hour of reaction, the initial conversion was about 5.17% and the ethylene selectivity was 100% as indicated by the results of external gas chromatography.
Example 15
A method for catalyzing natural gas to produce olefin by heat radiation comprises the following specific steps:
after the reaction gas was mixed according to the volume ratio of 42.5% methane, 7.5% ethane and 47.4% Ar, 2.6% steam, the reaction temperature was set to 650 ℃, the heat radiation temperature was set to 700 ℃, and the total reaction gas flow rate was set to 4mL/min, and the mixture was introduced into the reaction apparatus shown in FIG. 1. After 1 hour of reaction, the initial conversion was about 5.71% and the ethylene selectivity was 100% as determined by the external gas chromatography.
Example 16
A method for catalyzing natural gas to produce olefin by heat radiation comprises the following specific steps:
after the reaction gas was mixed in a volume ratio of 42.5% methane, 7.5% ethane and 47.4% Ar and 2.6% steam, the reaction temperature was set at 450℃and the total reaction gas flow rate was set at 4mL/min, and the mixture was introduced into a reaction apparatus shown in FIG. 1. After 1 hour of reaction, the initial conversion was about 0% and the ethylene selectivity was 0% as indicated by the results of external gas chromatography.
Example 17
A method for catalyzing natural gas to produce olefin by heat radiation comprises the following specific steps:
after the reaction gas was mixed in a volume ratio of 42.5% methane, 7.5% ethane and 47.4% Ar and 2.6% steam, the reaction temperature was set at 500℃and the total reaction gas flow rate was set at 4mL/min, and the mixture was introduced into a reaction apparatus shown in FIG. 1. After 1 hour of reaction, the initial conversion was about 0% and the ethylene selectivity was 0% as indicated by the results of external gas chromatography.
Example 18
A method for catalyzing natural gas to produce olefin by heat radiation comprises the following specific steps:
after the reaction gas was mixed in a volume ratio of 42.5% methane, 7.5% ethane and 47.4% Ar and 2.6% steam, the reaction temperature was set to 550℃and the total reaction gas flow rate was set to 4mL/min, and the mixture was introduced into a reaction apparatus shown in FIG. 1. After 1 hour of reaction, the initial conversion was about 1.32% and the ethylene selectivity was 100% as indicated by the results of external gas chromatography.
Example 19
A method for catalyzing natural gas to produce olefin by heat radiation comprises the following specific steps:
after the reaction gas was mixed in a volume ratio of 42.5% methane, 7.5% ethane and 47.4% Ar and 2.6% steam, the reaction temperature was set at 600℃and the total reaction gas flow rate was set at 4mL/min, and the mixture was introduced into a reaction apparatus shown in FIG. 1. After 1 hour of reaction, the initial conversion was about 2.34% and the ethylene selectivity was 100% as indicated by the results of external gas chromatography.
Example 20
A method for catalyzing natural gas to produce olefin by heat radiation comprises the following specific steps:
after the reaction gas was mixed in a volume ratio of 42.5% methane, 7.5% ethane and 47.4% Ar and 2.6% steam, the reaction temperature was set at 650℃and the total reaction gas flow rate was set at 4mL/min, and the mixture was introduced into a reaction apparatus shown in FIG. 1. After 1 hour of reaction, the initial conversion was about 3.26% and the ethylene selectivity was 100% as seen from the results of external gas chromatography.
Table 1 shows the experimental results of examples 1 to 20 for catalyzing natural gas to produce olefins by heat radiation, and it is understood from table 1 that examples 1 to 5 can catalyze natural gas to produce olefins by only providing heat radiation by a heated heat source without adding steam as a catalyst or providing heat radiation by an external radiation source, and the conversion rate can reach 0.86% to 1.65%; examples 6 to 10 are provided with a radiation source to provide heat radiation on the basis of examples 1 to 5, and the corresponding conversion rate is improved to 1.71 to 3.72 percent at the corresponding reaction temperature; examples 11 to 15, based on examples 6 to 10, steam was added as a catalyst, and the corresponding conversion was improved at the corresponding reaction temperature, which could be 2.30% to 5.71%.
In addition, examples 16 to 20 added steam as a catalyst on the basis of examples 1 to 5, but no additional radiation source, and as a result, no conversion occurred at the reaction temperatures of 450 ℃ and 500 ℃, but the conversion rates were improved by 1.32%, 2.34%, 3.26% with respect to examples 3 to 5 at 550 to 650 ℃, respectively; it is shown that steam can be used as a catalyst to increase the conversion of the reaction, but when insufficient heat radiation is available to activate the steam, the steam can poison the reaction at low temperatures, slowing the reaction.
Table 1 experimental results for the production of ethylene from natural gas of examples 1 to 20
The data in table 1 shows that: with the increase of the reaction temperature, the methane conversion rate is gradually increased, and finally reaches 5.71% under the condition that the additional water vapor is used as a catalyst and an additional radiation source is adopted.
Finally, it should be noted that: the above embodiments are only for illustrating the technical solution of the present application, and not for limiting the same; although the present application has been described in detail with reference to the foregoing embodiments, it should be understood by those of ordinary skill in the art that: the technical scheme described in the foregoing embodiments can be modified or some or all of the technical features thereof can be replaced by equivalents; such modifications and substitutions do not depart from the spirit of the corresponding technical solutions from the scope of the technical solutions of the embodiments of the present application.
Furthermore, those skilled in the art will appreciate that while some embodiments herein include some features but not others included in other embodiments, combinations of features of different embodiments are meant to be within the scope of the present application and form different embodiments. For example, in the claims below, any of the claimed embodiments may be used in any combination. The information disclosed in this background section is only for enhancement of understanding of the general background of the application and should not be taken as an acknowledgement or any form of suggestion that this information forms the prior art already known to a person skilled in the art.
Claims (10)
1. A method for catalyzing natural gas to produce olefin through heat radiation is characterized in that reaction gas is introduced into a reaction device, wherein the volume ratio of methane in the reaction gas is more than or equal to 20% and less than 100%, the volume ratio of ethane is more than 0 and less than or equal to 80%, and the reaction gas is catalyzed to prepare olefin under the conditions of heating and heat radiation; the thermal radiation includes a first thermal radiation generated by the heated heat source.
2. The method for producing olefins by heat radiation catalytic natural gas according to claim 1, wherein the temperature of heating the reaction gas is 300 to 1000 ℃;
preferably, the temperature of the reaction gas heating is 450-650 ℃.
3. The method for producing olefins from natural gas by thermal radiation according to claim 1 or 2, wherein a radiation source is further arranged in the reaction device, and the thermal radiation further comprises a second thermal radiation generated by the radiation source;
preferably, the temperature of the radiation source is 300-1500 ℃;
preferably, the temperature of the radiation source is 500-1000 ℃.
4. The method for producing olefins from natural gas by thermal radiation catalysis according to claim 3, wherein introducing a reaction gas into the reaction device further comprises: adding a catalyst into a reaction device, wherein the catalyst can absorb the spectrum of the thermal radiation so as to raise the surface temperature of the catalyst and improve the internal energy of a reaction system; the catalyst includes any one or more of a gas catalyst, a solid catalyst, and a liquid catalyst.
5. The method of catalyzing natural gas for producing olefins by thermal radiation according to claim 4, wherein the catalyst comprises a gas catalyst that is a gas molecule that is strongly spectrally absorptive of thermal radiation;
preferably, the gas catalyst comprises either or both of carbon dioxide and water vapor;
preferably, the volume ratio of the reaction gas to the gas catalyst is (1000:1) to (1:1000).
6. The method for producing olefins from natural gas by thermal radiation catalysis according to claim 2, wherein the temperature of heating the reaction gas is 550-650 ℃, and the introducing the reaction gas into the reaction device further comprises: adding a catalyst into a reaction device, wherein the catalyst can absorb the spectrum of the thermal radiation so as to raise the surface temperature of the catalyst and improve the internal energy of a reaction system; the catalyst comprises any one or more of a gas catalyst, a solid catalyst and a liquid catalyst;
preferably, the catalyst comprises a gas catalyst which is a gas molecule having strong spectral absorption of thermal radiation;
preferably, the gas catalyst comprises either or both of carbon dioxide and water vapor;
preferably, the volume ratio of the reaction gas to the gas catalyst is (1000:1) to (1:1000).
7. The method for producing olefins by catalyzing natural gas with thermal radiation according to claim 1, wherein the reaction device is a tubular reactor, the reaction gas is introduced into a reaction tube of the reaction device, and the reaction tube is made of transparent high temperature resistant material or high emissivity material.
8. A method for catalyzing natural gas to produce olefins by thermal radiation according to claim 3, characterized in that the reaction device is a tubular reactor, the reaction gas is introduced into a reaction tube of the reaction device, the reaction tube is made of transparent high temperature resistant material or high emissivity material, and the distance between the radiation source and the heat source and the reaction tube is 0-100cm, respectively.
9. The method of catalyzing natural gas for producing olefins by thermal radiation according to claim 8, wherein the radiation source is a wound heating wire or rod and the heat source is a wound heating wire or rod; the radiation source is made of metal, and the emissivity of the metal is between 0.5 and 0.99;
preferably, the outer surface of the heat source is wrapped with corundum and/or ceramic;
preferably, the radiation source is made of nichrome.
10. The method for producing olefins from natural gas by thermal radiation according to claim 1, wherein the flow rate of the reaction gas is 1-1000ml/min.
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