CN1235846C - Method for preparing acetylene by hot plasma cracking methane containing gas - Google Patents
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Abstract
The present invention discloses a method for preparing acetylene by cracking gas containing methane by hot plasma. Argon, nitrogen or hydrogen gas is ionized into plasma jets by a plasma generator, and high temperature environment is formed in the reactor; an air inlet device for raw gas is opposite to and symmetrical with multiple air inlet rings, and raw gas is sprayed into the reactor via the air inlet rings to be mixed with the plasma jets penetrating the air inlet rings to be quickly and sufficiently soaked; the used reactor is a telescopic reactor, and mixed gas is limited in the reactor, which leads that a temperature in the reactor is unchanged; a used cooling device is a pneumatic cooling and expanding cavity and is combined with the reactor, and cracked gas is quenched in the expanding cavity; accordingly, a laboratory technique is successfully turned into an engineering technique. In the method, acetylene is mainly prepared together with black carbon, hydrogen gas is prepared in an auxiliary mode, and black carbon can also be mainly prepared. When the method is used for preparing acetylene, major techniques and economic indicator achieve or exceed the existing experiment level of abroad laboratories, and the present invention has the advantages of good economic and environmental benefits.
Description
Technical field
The present invention relates to the preparation method of acetylene, relate in particular to a kind of method of plasma pyrolysis methane-containing gas system acetylene.Technical scheme of the present invention is sophisticated commercial run, and can directly apply to the methane-containing gas is the chemical engineering field that raw material is produced acetylene.
Background technology
At present, the method for domestic production acetylene is calcium carbide hydrolysis method and gas by partial oxidation of natural method, also has arc process abroad.
Producing acetylene with the calcium carbide hydrolysis method, at first is melting lime carbonate (CaCO in electric arc furnace
3) obtain calcium oxide (CaO), calcium oxide again with water (H
2O) reaction generates acetylene.Whole process has a large amount of CO
2And carbide slag (CaOH) generation, very big to the pollution of environment, and be difficult to concentrate improvement.The gas by partial oxidation of natural method is that Sweet natural gas incomplete combustion in aerobic environment is obtained acetylene.Process also has a large amount of CO
2, waste gas such as CO produces, and the Sweet natural gas consumption of unit product is big, yield is low, usually, 6500 side's Sweet natural gases could produce one ton of acetylene, and is low to the utilization ratio of Nonrenewable energy resources.Electrocracking gas production acetylene method makes the conversion of natural gas rate low because of temperature of reaction is limited, the acetylene yield is low, the gas consumption height of unit product, the typical case's representative with electrocracking gas production acetylene abroad has German Huels company and U.S. Dupont company, the specific energy of Huels company report is 12.1KWh/kg, per pass conversion is about 50%, and yield is about 33%, and one ton of acetylene of every production consumes Sweet natural gas 4500m
3
The plasma jet preparation of acetylene by cracking natural gas is a kind of new method, it is the plasma jet that the discharge starting the arc forms high-velocity jet in working gas (nitrogen, argon, hydrogen etc.), produce hot environment, the methane composition of Sweet natural gas in this anaerobic, high temperature, atmospheric pressure environment by the dehydrogenation coupling, generation contains the splitting gas of acetylene, handles obtaining target product acetylene through subsequent handling.It is compared with calcium carbide hydrolysis system acetylene processing method has no something in common; Compare with the gas by partial oxidation of natural method, the thermal source that uses has the difference of essence, the gas by partial oxidation of natural method adopts Sweet natural gas incendiary mode in aerobic environment to obtain heat energy, and plasma jet preparation of acetylene by cracking natural gas method adopts and under arcing electric energy is converted into heat energy; Compare with the electrocracking method, plasma method can form the temperature environment that is more suitable for natural gas pyrolysis, obtain higher once through yield, the electrocracking method is the starting the arc formation hot environment of directly discharging in Sweet natural gas, do not need other working gas, but the temperature that produces is lower, and methane cracking is not thorough.
Carry out the research work of plasma jet preparation of acetylene by cracking natural gas representative be to be positioned at the national project of U.S. Idaho and the national energy technology experiment chamber (NETL) of environmental laboratory (INEEL) and Pittsburgh.The best result that they delivered in 2002 is plasma power 60KW, per hour cracking natural gas 7.25m
3, conversion of natural gas rate 96%, acetylene yield 93%.Calculate with this, one ton of acetylene of every production consumes Sweet natural gas 1550m
3, specific energy 12.9KWh/kg.
At present, the method for plasma jet preparation of acetylene by cracking natural gas does not enter the industrially scalable stage as yet still at laboratory stage.Its reason is: the essence of the method for plasma jet preparation of acetylene by cracking natural gas is the high-temperature chemical reaction process, speed of response is exceedingly fast, with millisecond meter, can be considered thermodynamic process in theory, the technical application and the laboratory technique of industrially scalable have a great difference, when the big flow unstripped gas of industrially scalable enters reaction, there is following difficulty:
After unstripped gas enters reactor, can not be fast with become the gas soaking, directly have influence on the reaction effect of unstripped gas, methane conversion is low, product yield is low; It is stable that temperature in the reactor is difficult for keeping, the bad control of the residence time of unstripped gas in reactor, and the productive rate of target product acetylene and byproduct carbon black can't be controlled as required; Reacted splitting gas does not have economy, effectively rapid cooling provision, and the acetylene of generation is cracked into carbon black again, and the acetylene yield is low; Reactor has knot carbon phenomenon, bad processing.
Summary of the invention
The present invention proposes a kind of new method, and this method has overcome above-mentioned difficulties effectively, has avoided corresponding negative consequence, is the sophisticated commercial run that can implement.Present method main product acetylene, coproduction carbon black, by-product hydrogen (H
2↑); Use present method to produce acetylene, major technique, economic target all will meet or exceed external breadboard experimental level, and comprehensive benefits such as economic benefit, environmental benefit all will obviously improve than the commercial run of existing any production acetylene.
Thermal plasma cracking methane-containing gas system acetylene method of the present invention, be that the one-tenth gas of working gas is sent into plasma generator, under the effect of highfield, formed the high-temperature plasma jet by discharge ionization, this high temp jet forms the hot environment more than the 5000K in reactor, the unstripped gas that contains methane enters reactor through diffuser, with the working gas contact heat transfer, mixture temperature 2000-4500K after the soaking, the methane composition of unstripped gas in this temperature by the dehydrogenation coupling, generation contains the splitting gas of acetylene, splitting gas is reduced to 350-1000K through refrigerating unit chilling temperature, remove carbon black in the splitting gas through gas-solid separator, isolate the acetylene in the splitting gas more according to a conventional method, it is characterized in that: described diffuser is symmetrical in opposite directions multiple tracks air inlet ring, and unstripped gas is gone into reactor through the air inlet ring spray, and its movement locus points to the center of circle by circumference and is the radiation convergent manner, mix with the plasma jet that runs through the air inlet ring, rapidly fully soaking; Described reactor is funnel-form chorate " Y " type reactor, and the gas mixture after the soaking is restrained in " Y " type reactor, makes the temperature in the reactor remain on 2000-4500K; Described refrigerating unit is pneumatic cooling expansion chamber, and splitting gas is cushioned in expansion chamber, and volume expands suddenly, and flow velocity falls sharply, with heat-eliminating medium big area contact heat-exchanging by chilling, temperature is reduced to 350-1000K; The throughput ratio of described unstripped gas and working gas is 0.7-2: 1; The residence time 0.4-40ms of described unstripped gas in reactor.
The temperature of described plasma jet is preferably 5000-30000K, preferably 8000-20000K.
Mixture temperature after the described soaking is preferably 2800--4000K, preferably 3100-3500K.
Described splitting gas is reduced to through the chilling temperature and is preferably 400-800K, preferably 500-700K;
The throughput ratio of described unstripped gas and working gas is preferably 0.7-1.5: 1, and 0.7-1 preferably: 1.
Described working gas is argon gas, nitrogen or hydrogen.
Described unstripped gas is any or several methane-containing gas of Sweet natural gas, coal-seam gas, coal tar gas.
The method main product acetylene of described system acetylene, the coproduction carbon black, by-product hydrogen by changing the envrionment temperature or the residence time of gas mixture in reactor in the reactor, changes the selectivity of acetylene or carbon black.
The selectivity of described acetylene or carbon black realizes by the input electric power that changes plasma generator.
The selectivity of described acetylene or carbon black realizes by the flow that changes unstripped gas.
The selectivity of described acetylene or carbon black by changing unstripped gas simultaneously flow and the input electric power of plasma generator realize.
The selectivity of described acetylene or carbon black realizes by the geometrical dimension that changes reactor.
The beneficial effect of present method is:
1. adopt symmetrical in opposite directions multiple tracks intake method, by fully soaking, methane is thorough in the high temperature reaction zone cracking, transformation efficiency height, product yield height when entering reaction for unstripped gas and high temp jet.
2. adopt funnel-form chorate " Y " type reactor, the gas mixture after the soaking is restrained in " Y " type reactor, makes the temperature in the reactor keep stable, and scission reaction is controlled fully, and production process is stablized; And the residence time of gas mixture in reactor can be controlled and adjust, thereby satisfy the acetylene of producing different yields, the needs of carbon black product.
3. adopt chorate " Y " type reactor and pneumatic cooling expansion chamber to organically combine, form rational cooling structure, avoided acetylene to be cracked into carbon black effectively, the acetylene yield is improved, also avoided reactor knot carbon simultaneously.
By solving the technical problem of above-mentioned three aspects, make present method become sophisticated commercial run, can directly in actual engineering, use.Present design scale is single complete equipment power 200KW, 100 tons of acetylene/years of throughput, conversion of natural gas rate 97%, acetylene yield 90%, specific energy 13KW/kg, acetylene power consumption 12987 degree per ton, Sweet natural gas 1558m
3, the concentration of acetylene in gaseous products is greater than 13%.
Description of drawings
Fig. 1 is the process flow sheet of present method.
Fig. 2 is that air inlet ring structure and unstripped gas, working gas flow to synoptic diagram.
Fig. 3 is the structure of reactor synoptic diagram.
Fig. 4 is a cooling expansion chamber structural representation.
Embodiment
Below describe the present invention in detail.
Referring to Fig. 1: the method for implementing this plasma pyrolysis methane-containing gas system acetylene, at first be that a device of implementing present method is set, this device comprises high-power DC power supply 1, plasma generator 2, unstripped gas diffuser 4, reactor 5, refrigerating unit 6, gas-solid separator 7, and plasma generator 2 is provided with working gas inlet 3.
Present method comprises the steps: to provide the energy by direct supply 1 to plasma generator 2, the one-tenth gas of working gas 3 is sent into plasma generator 2 through entering the mouth, the one-tenth gas of working gas is formed the high-temperature plasma jet by discharge ionization under the effect of highfield, this high temp jet forms the hot environment more than the 5000K in reactor 5, the unstripped gas that contains methane enters reactor 5 through diffuser 4, with working gas plasma jet contact heat transfer, mixture temperature 2000-4500K after the soaking, the methane composition of unstripped gas in this temperature by the dehydrogenation coupling, generation contains the splitting gas of acetylene, also contain carbon black, H in the splitting gas
2, CH
4, C
2H
4, C
2H
6, reach for example N of working gas component
2, splitting gas is through refrigerating unit 6 chillings, and temperature is reduced to 350-1000K, removes carbon black in the splitting gas through gas-solid separator 7, isolates the acetylene in the splitting gas more according to a conventional method, and whole process is carried out in anaerobic, atmospheric pressure environment.
More than be the common-base eigen of preparation of acetylene by cracking natural gas with plasma method, belong to existing known laboratory technique.
The present invention also has following distinguishing characteristics beyond above-mentioned essential characteristic, these distinguishing characteristicss constitute the inventive point of present method, are the keys that laboratory technique is transformed into engineering.Comprise
Referring to Fig. 2: unstripped gas diffuser 4 is ring-type multiple tracks structures, 2. unstripped gas goes into reactor 5 through the air inlet ring spray, form symmetrical in opposite directions intake method, the movement locus that is unstripped gas is the radiation convergent manner by the circumference sensing center of circle, 1. mix with the plasma jet that runs through the air inlet ring, make unstripped gas 2. with 1. rapidly fully soaking of working gas, thereby methane is thorough in the high temperature reaction zone cracking, the transformation efficiency height, the product yield height.
Referring to Fig. 3: reactor 5 is chorate " Y " type reactors, and promptly funnel shaped reactor, its leading portion are pyramidal structures, and back segment is the very little and length longer pipe shape structure of a latus rectum, and is very big to the resistance of medium.Gas mixture after the soaking is 3. restrained in " Y " type reactor 5, and temperature in the reactor 5 is remained in the scope of design requirements (2000-4500K), and reaction process is able to effectively stable carrying out.(annotate: the tubular sections outer wall of reactor 5 has water coolant 6. to cool off.)
Referring to Fig. 4: refrigerating unit 6 is pneumatic cooling expansion chambers, and its volume is very big, is built-in with interchanger 5., and the expansion chamber outer wall has water coolant 6. to cool off, built-in heat exchanger 5. in also logical water coolant 6., so the thermal capacitance of expansion chamber is also very big.Pneumatic cooling expansion chamber organically combines with " Y " type reactor 5, realizes splitting gas chilling 4..Its principle is, " Y " type reactor 5 long and narrow tubular sections constitute throttling range, and 4. splitting gas forms high-speed jet in throttling range, sprays to enter pneumatic cooling expansion chamber 6, and volume expands suddenly, and temperature sharply descends, and realizes cooling for the first time; Simultaneously, the splitting gas after the expansion 4. flow velocity falls sharply, and with big contact heat-exchanging of heat-eliminating medium, realizes cooling for the second time; Splitting gas 4. under this dual function by chilling, temperature is reduced to 350-1000K, thereby has avoided acetylene to be cracked into carbon black effectively, and the acetylene yield is improved.Simultaneously, because 4. splitting gas forms high-speed jet in throttling range, 5 generations are washed away to reactor, have also avoided reactor 5 knot carbon.(annotate: cooling expansion chamber inwall and interchanger 5. surface have knot carbon phenomenon, therefore cool off expansion chamber and also are provided with the mechanism that removes knot carbon, and be not shown.)
Through above-mentioned reaction process, unstripped gas methane composition 2. is by the dehydrogenation coupling, generate contain acetylene splitting gas 4., splitting gas also contains carbon black, H in 4.
2, CH
4, C
2H
4, C
2H
6, reach for example N of working gas component
2Remove carbon black in the splitting gas through gas-solid separator 7, gas-solid separator 7 can adopt for example cloth bag trap of common separating device, has separated the splitting gas of carbon black and has 4. isolated acetylene more according to a conventional method.
The correlation parameter of each step is as follows:
It is plasma jet that working gas becomes gas ionization, more than the temperature 5000K, and 5000-30000K preferably, preferred 8000-20000K.
The mixed temperature 2000-4500K of unstripped gas and working gas, 2800-4000K, preferably 3100-3500K preferably.
Splitting gas is reduced to 350-1000K through the chilling temperature, is preferably 400-800K, preferably 500-700K.
The throughput ratio of unstripped gas and working gas is 0.7-2: 1, be preferably 0.7-1.5: and 1,0.7-1 preferably: 1.
The residence time 0.4-40ms of unstripped gas in reactor.
The carbon black that present method generates has two kinds, and the one, the carbon black that the direct cracking of Sweet natural gas generates produces when temperature is low; The 2nd, the acetylene that has generated in the splitting gas fails in time to leave the high-temperature zone cooling, is cracked into carbon black again voluntarily, and the quality of this carbon black is better than the carbon black that the direct cracking of Sweet natural gas generates, and more approaches acetylene carbon black.
When implementing present method, can be by changing the geometrical dimension of reactor, or raw gas flow, or the electric power of input plasma generator, to change envrionment temperature in the reactor or/and the residence time of gas mixture in reactor, the selectivity of acetylene or carbon black be can change, the acetylene of producing different yields, the needs of carbon black product satisfied.For example
The electric power of raw gas flow, input plasma generator is constant, strengthens the length of reactor, and the resistance of medium increases, and flow velocity slows down, and the residence time of unstripped gas in reactor is elongated, reaction tendency carbon black selectivity;
Geometrical dimension, the raw gas flow of reactor are constant, strengthen the electric power of input plasma generator, and temperature of reaction raises, and the reaction required time shortens, when reactor is longer, and reaction tendency carbon black selectivity;
The electric power of the geometrical dimension of reactor, input plasma generator is constant, strengthens raw gas flow, is equivalent to reduce temperature of reaction in fact, reaction tendency carbon black selectivity.
For given reactor, its geometrical dimension is set, therefore, just adopts the back dual mode to change the selectivity of acetylene or carbon black usually.
Thus, present method also can be utilized the method main product carbon black of above-mentioned change product selectivity, uses a kind of or comprehensively uses several method, realizes the purpose of main product carbon black.But if the main product carbon black is a long-term objective, preferably adopt the reactor of longer dimension, the lengthening residence time of splitting gas in reactor, make the acetylene in the splitting gas also be cracked into carbon black, obtain high-quality carbon black.
The working gas that present method adopts can be an argon gas, or nitrogen, or hydrogen.Usually without argon gas, and adopt the relatively low nitrogen of cost, preferably adopt hydrogen, because its enthalpy is than nitrogen height, the effect of methane cracking can be better, and hydrogen can need not prepare or buy in addition directly from the divided gas flow in this flow process; Simultaneously, do not have components such as nitrogen, argon gas in the splitting gas, sepn process also will be simpler, easy.Working gas also can use nitrogen, hydrogen gas mixture, and the methane cracking effect was both good, and is economical again.
The unstripped gas that present method adopts can be any gas or several mixed gass that contain methane that contain methane such as Sweet natural gas, coal-seam gas, coal tar gas.
The described all gases metering of present method is (the standard M of unit with the standard volume
3), flow metering unit is standard volume/unit time.
Claims (10)
1. thermal plasma cracking methane-containing gas system acetylene method, be that the one-tenth gas of working gas is sent into plasma generator, ionization forms the high-temperature plasma jet under the effect of highfield, this high temp jet forms the hot environment more than the 5000K in reactor, the unstripped gas that contains methane enters reactor through diffuser, with the working gas contact heat transfer, mixture temperature 2000-4500K after the soaking, the methane composition of unstripped gas in this temperature by the dehydrogenation coupling, generation contains the splitting gas of acetylene, splitting gas is reduced to 350-1000K through refrigerating unit chilling temperature, remove carbon black in the splitting gas through gas-solid separator, isolate the acetylene in the splitting gas more according to a conventional method, it is characterized in that: described diffuser is symmetrical in opposite directions multiple tracks air inlet ring, and unstripped gas sprays into reactor through each road of air inlet ring, and its movement locus points to the center of circle by circumference and is the radiation convergent manner, mix with the plasma jet that runs through the air inlet ring, by fully soaking rapidly; Described reactor is to be funnelform chorate " Y " type reactor, and the gas mixture after the soaking is restrained in " Y " type reactor, makes the temperature in the reactor remain on 2000-4500K; Described refrigerating unit is pneumatic cooling expansion chamber, and splitting gas is cushioned in expansion chamber, and flow velocity is die-offed by chilling, and temperature is reduced to 350-1000K; The throughput ratio of described unstripped gas and working gas is 0.7-2: 1; The residence time of described unstripped gas in reactor is 0.4-40ms.
2. thermal plasma cracking methane-containing gas system acetylene method according to claim 1, it is characterized in that: the temperature of described plasma jet is 5000-30000K, mixture temperature 2800-4000K after the described soaking, described splitting gas is reduced to 400-800K through the chilling temperature, and the throughput ratio of described unstripped gas and working gas is 0.7-1.5: 1.
3. thermal plasma cracking methane-containing gas system acetylene method according to claim 1, it is characterized in that: the temperature of described plasma jet is 8000-20000K, mixture temperature 3100-3500K after the described soaking, described splitting gas is reduced to 500-700K through the chilling temperature, and the throughput ratio of described unstripped gas and working gas is 0.7-1: 1.
4. according to claim 1 to 3 each described thermal plasma cracking methane-containing gas system acetylene method wherein, it is characterized in that: described working gas is argon gas, nitrogen or hydrogen.
5. according to claim 1 to 3 each described thermal plasma cracking methane-containing gas system acetylene method wherein, it is characterized in that: described unstripped gas is any or several methane-containing gas of Sweet natural gas, coal-seam gas, coal tar gas.
6. thermal plasma cracking methane-containing gas system acetylene method according to claim 1, it is characterized in that: the method main product acetylene of described system acetylene, the coproduction carbon black, by-product hydrogen, by changing the envrionment temperature or the residence time of gas mixture in reactor in the reactor, change the selectivity of acetylene or carbon black.
7. thermal plasma cracking methane-containing gas system acetylene method according to claim 6 is characterized in that: the selectivity of described acetylene or carbon black realizes by the input electric power that changes plasma generator.
8. thermal plasma cracking methane-containing gas system acetylene method according to claim 6 is characterized in that: the selectivity of described acetylene or carbon black realizes by the flow that changes unstripped gas.
9. thermal plasma cracking methane-containing gas system acetylene method according to claim 6 is characterized in that: the selectivity of described acetylene or carbon black by changing unstripped gas simultaneously flow and the input electric power of plasma generator realize.
10. thermal plasma cracking methane-containing gas system acetylene method according to claim 6 is characterized in that: the selectivity of described acetylene or carbon black realizes by the geometrical dimension that changes reactor.
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