CN101734620A - Method for producing hydrogen gas by methane-rich plasma - Google Patents
Method for producing hydrogen gas by methane-rich plasma Download PDFInfo
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Abstract
The invention relates to a method for producing hydrogen gas by methane-rich plasma. The method comprises the following steps: firstly, exchanging heat between methane-rich gas and reaction high-temperature tail gas; secondly, exchanging heat between the methane-rich gas and a wall of a plasma pyrolysis gasification reactor; and finally, introducing the methane-rich gas to the plasma pyrolysis gasification reactor to have action with a plasma jet generated by a plasma generator to generate gas taking the hydrogen gas as a main composition. The method solves the difficult problems that a traditional process needs a catalyst which is easy to have carbon precipitation and sulphur, halogen and arsenic poisoning and also solves the problems of high energy consumption and the protection of the wall of the reactor in the process of producing hydrogen by plasma. The method has the advantages of short process flow, simple operation, high thermal efficiency and light environmental pollution and is applicable to the fields of fuel gas chemical engineering and plasma chemical engineering.
Description
Technical field
The present invention relates to a kind of method of methane gas hydrogen, particularly a kind of method that under the plasma jet effect, makes hydrogen with high methane gas.
Technical background
The Application Areas of hydrogen is very wide, mainly is the hydrogenation reaction that is used to produce synthetic ammonia, methyl alcohol and petroleum refining process.In addition, also there is a lot of application in field such as, aerospace industry synthetic in electronic industry, metallurgical industry, food-processing, float glass, fine chemistry industry.Along with the pay attention to day by day of society to environmental quality, the sulfide that allows in the gasoline, diesel, the content of aromatic hydroxy compound progressively reduce, and this makes the demand of hydrogen be growing trend.Hydrogen has very high combustion heat value as a kind of clean fuel gas, and the product after the burning is water, can be to the environmental emission greenhouse gases, and be a kind of comparatively ideal secondary energy therefore.In addition, the use of hydrogen energy source also can increase the demand of market to hydrogen, and especially hydrogen is as chemical industry synthetic intermediates gas or unstripped gas, and increasing in the last few years scientific research institution is the development and utilization of the fuel cell of the energy with hydrogen putting forth effort on research.
Mainly contain four kinds with the high methane gas for the raw material hydrogen production process: the CO 2 reformation method of the steam reforming method of methane, the partial oxidation process of methane, methane and the non-catalytic partial oxidation method of methane.The steam reforming method is the existing main method of producing hydrogen.Wherein the technological process of three kinds of methods all needs catalysis system, and catalyzer is all analysed carbon easily, and sulphur, halogen, arseniasis.The non-catalytic partial oxidation rule needs pure oxygen or oxygen-rich air, simultaneously quite a few hydrogen is converted into water, has reduced the productive rate of hydrogen.Methane is one of the most stable organic molecule of occurring in nature, hydrocarbon key bond energy in the methane is big, structure is quite firm, so in methane hydrogen process, the fracture of hydrocarbon key needs lot of energy, therefore, the hydrogen manufacturing of tradition methane conversion generally needs catalyzer, and reactor is huge, is rich in the introducing of active particle plasma body, solved this problem, but effective utilization of high-grade energy of plasma has become problem again.If utilize badly, new energy wastage will be caused.
The arc heat plasma body, belong to thermal plasma, its jet has that energy height is concentrated, ultrahigh-temperature, the atom that is rich in excited state, molecule, electronics isoreactivity particle, speed and the high characteristics of pressure gradient, plasma jets etc. are very suitable to the ultrashort catalytic thermal source of ultrahigh-temperature, with the plasma hydrogen preparing technology that plasma technique combines with methane conversion, overcome many shortcomings of traditional methane conversion process, have flow process and lack, do not need characteristics such as catalyzer.Because energy consumption does not have industrialization so far.Because temperature of reactor is higher, the temperature of reaction back gas is also high in the plasma hydrogen preparing technology, will reclaim wherein heat with interchanger usually.U.S. Pat 6,881,363 are provided with aheat exchanger in plasma reactor comes regenerator section air or part of fuel, thereby has reduced the energy supply.But problem is this interchanger exists the air-flow skewness, interchanger next-door neighbour plasma arc causes carbon distribution in the interchanger easily simultaneously, have a strong impact on heat exchange effect and interchanger life-span, even cause plasma arc to extinguish when interchanger is big by gas flow, system is out of service.
U.S. Pat 7,597,860 are connected with a shell and tube heat exchanger below plasma reactor, be used for reducing the temperature of hydrogen-rich gas, and preheated air, unstripped gas or both gas mixtures reach the purpose that cuts down the consumption of energy.In this invention, the hydrogen-rich gas that reaction produces is lower through temperature behind the beds, and is relatively poor to the pre-heat effect of unstripped gas; Unstripped gas after preheating enters high frequency discharge zone between plasma generator the two poles of the earth by the connecting leg outside the reactor, and the gas that is preheated in connecting leg has certain calorific loss again; Cause the air-flow turbulence greatly or owing to heating if be preheated gas tolerance, the steady running of electric arc and system will be destroyed.
In the above-mentioned prior art, the tail gas behind the plasma hydrogen preparing is entered beds, can improve the productive rate of hydrogen, but catalyzer is poisoned easily, in order to overcome the problem of poisoning of catalyst, need to purify the working gas of unstripped gas and plasma generator, make the technical process complexity so again.
Summary of the invention
In order to overcome above-mentioned the deficiencies in the prior art, the invention provides a kind of method of producing hydrogen gas by methane-rich plasma.
The method of producing hydrogen gas by methane-rich plasma of the present invention is with high methane gas or its gas mixture elder generation and reaction end gas heat exchange, then with the heat exchange of plasma reactor wall, enter the plasma jet that produces with plasma generator in the plasma reactor again and interact, generating with hydrogen is the gas of main component.The concrete steps of this method are as follows:
I. methane content is at 10%～100% high methane gas, or the gas mixture of itself and water vapour, carbonic acid gas, enter in the interchanger of plasma reactor bottom, carry out heat exchange with reacted 600 ℃-1500 ℃ hydrogen-rich gas, high methane gas or gas mixture are heated to 300 ℃-600 ℃;
II. heated high methane gas or gas mixture enter interchanger and the heat exchange of plasma reactor wall in the plasma reactor wall, high methane gas or gas mixture by second-heating after, temperature rises to 600 ℃-1200 ℃;
III. entered plasma reactor by the high methane gas of second-heating or gas mixture, act on mutually at the plasma jet that is rich in active particle of reaction zone with 2500 ℃-5000 ℃ plasma generator generation, generating with hydrogen in the 0.5-500ms under normal pressure is the hydrogen-rich gas of main component, and temperature is reduced to 200 ℃-300 ℃ after this hydrogen-rich gas and wall of reactor, high methane gas or the gas mixture heat exchange;
IV. the hydrogen-rich gas after the cooling enters separator, isolates solid impurity, further separates making with hydrogen then.
In technique scheme, described high methane gas is Sweet natural gas, coal-seam gas, coke-oven gas or its gas mixture arbitrarily; Described high methane gas or its gas mixture and the heat exchange of plasma reactor wall are to carry out heat exchange by the spiral tube exchanger that is imbedded in the plasma reactor inwall flame-proof thermal insulation material layer; Described plasma generator is non-mobile model arc plasma producer; The working gas of described plasma generator is hydrogen, argon gas, oxygen, carbonic acid gas, nitrogen, water vapour and airborne a kind of or its any gas mixture.
The present invention's method of high methane gas hydrogen manufacturing under the plasma jet effect, compare with the method for existing plasma-converted methane hydrogen, high methane gas or gas mixture are before entering the plasma reactor reaction, by reacted hydrogen-rich gas and the preheating of plasma reactor wall secondary, after high methane gas or gas mixture are preheated activation, enter reactor and plasma jet action-reaction again, made full use of and be rich in high reactivity particle (ion, electronics, atom, the molecule of excited state etc.) plasma jet energy has improved the temperature of reaction and the speed of reaction of chemical reaction.In this reaction process, the heat lost by radiation of wall of reactor since in established interchanger and effectively reduced, the energy of product rich, high temperature hydrogen is fully utilized, because high methane gas is preheated activation, the high problem of needed plasma body energy consumption when having solved high methane gas hydrogen manufacturing effectively, promptly when energy of plasma is constant, improved the treatment capacity of high methane gas effectively; In this reaction process, the heat energy of reactor wall is continuously absorbed by refractory insulating layer, has protected reactor effectively, has prolonged the life-span of reactor.And, shortened technical process owing to adopted the top and the bottom interchanger to be integrated in the plasma reactor, simplified working method.
In the processing method of hydrogen manufacturing of the present invention, save the cleaning and desulfurization technology of high methane gas, gas mixture and work gas, avoided the use catalyzer, overcome the difficult problem of poisoning of catalyst.Simultaneously, improve the energy utilization efficiency of high methane gas hydrogen, solved plasma method hydrogen manufacturing energy consumption problem of higher, taken into account the protection plasma reactor again, guaranteed the normal steady running of plasma hydrogen preparing system.
In the processing method of hydrogen manufacturing of the present invention, can be according to the different purposes of obtained rich hydrogen unstripped gas, what the working gas of gas mixture that can adopt different components as required and different plasma generators made heterogeneity content is the target unstripped gas of main component with hydrogen.
In the processing method of hydrogen manufacturing of the present invention, by measuring various high methane gass, gas mixture, the work gas of plasma generator, the hydrogen-rich gas temperature of isolated solid impurity, pressure, flow, and adopt gas-chromatography to record the percentage composition of the various compositions in the hydrogen-rich gas, calculate the inventive method hydrogen manufacturing, its methane conversion has reached 90%-99.9%, the productive rate of hydrogen has reached 80%-95% (not using under the situation of water vapour), under the situation of using water vapour, the productive rate of hydrogen surpassed for 100% (calculating of yield does not comprise the hydrogen in the water vapour), and the specific energy consumption of hydrogen has reduced 11MJ/kg.
Description of drawings
Fig. 1 is the apparatus structure synoptic diagram of high methane gas of the present invention hydrogen method under action of plasma
Among the figure: 1: plasma electrical source; 2: plasma generator; 3: the plasma body working gas; 4: plasma jet; 5: flame-proof thermal insulation material; 6: plasma reactor; 7: thermal insulation layer; 8: high methane gas or gas mixture; 9: the bottom interchanger; 10; The top interchanger; 11: high methane gas or gas mixture after the pre-thermal activation; 12: cooled hydrogen-rich gas; 13: gas separator; 14: the hydrogen-rich gas of isolating solid impurity.
Embodiment
A kind of method of the present invention with high methane gas hydrogen under the plasma jet effect, different purposes according to its obtained rich hydrogen unstripped gas, can adopt the working gas of different gas mixture of composition and different plasma generator as required, for example: pure if desired hydrogen, use higher Sweet natural gas of methane purity or coal-seam gas as raw material, adopt hydrogen as working gas, this process can also generate the nano level carbon black of by product, do not produce simultaneously the greenhouse gases Carbon emission, it is a significant low-carbon (LC) process, because the hydrogen starting the arc is had any problem, can in the working gas of plasma generator, mix a certain proportion of argon gas, be convenient to the starting the arc and stable arc; Preparing synthetic gas if desired, be used for oxygenatedchemicalss such as synthesizing methanol, can adopt high methane gas to add carbonic acid gas, or high methane gas adds water vapour, or high methane gas adds carbonic acid gas and adds water vapour as gas mixture, and high methane gas wherein can be Sweet natural gas, coal-seam gas, coke-oven gas or its any mixing.Adopt the working gas of oxygen-containing gas as plasma generator, as oxygen, carbonic acid gas, oxygen, or air, or water vapour, or oxygen adds water vapour, or the air oxygen etc., the additional proportion of oxygen-containing gas is decided on the hydrogen-carbon ratio of gas mixture gas composition and the hydrogen-carbon ratio of needed synthetic gas; Synthetic ammonia adopts high methane gas as raw material if desired, nitrogenous gas such as nitrogen, and air is as the working gas of plasma generator.Using of oxygen and air can provide more energy as this process of plasma hydrogen preparing, reduces the degree of dependence of reaction pair energy of plasma, does so certainly to have carbon monoxide and carbonic acid gas generation.Because above-mentioned gas mixture composition and plasma body work gas kind are more, and the kind of the gas mixture that can be made up of oxygen, carbonic acid gas, oxygen, air, water vapour and argon gas is more, needn't enumerate one by one in the present invention, typical case with regard to embodiment is described in detail in conjunction with the accompanying drawings below, those skilled in the art is after having read specific embodiment, can realize that the present invention is conspicuous down, its described effect also can access embodiment simultaneously.
Embodiment 1
As Fig. 1, when implementing the method for hydrogen manufacturing of the present invention, opening valve is that 98% Sweet natural gas 8 is sent in the interchanger 9 of plasma reactor bottom with methane content, compression hydrogen 3 is delivered in the plasma generator 2, start high frequency ignition and light plasma generator electric arc, form plasma jet 4.Deng reach steady state to system, enter the Sweet natural gas 8 of plasma reactor 6 bottom interchanger 9, with the rich, high temperature hydrogen heat exchange after the plasma reaction, Sweet natural gas is heated to 300 ℃-600 ℃, heated Sweet natural gas continues the wall heat exchange at the spiral tube exchanger and the plasma reactor 6 on plasma reactor 6 tops, the Sweet natural gas secondary is heated pre-activation, temperature rises to 600 ℃-900 ℃, Sweet natural gas 11 after the pre-thermal activation enters in the plasma reactor 6, the plasma jet 4 of the temperature that is rich in active particle up to 3000 ℃-4000 ℃ that produces with plasma generator in reaction zone acts on mutually, under normal pressure, be the hydrogen-rich gas of main component less than generating in the time of 100ms with hydrogen, temperature is bottom and interchanger 9 heat exchange that 900 ℃ of-1200 ℃ of hydrogen-rich gases enter the plasma gas reactor, hydrogen-rich gas temperature after the cooling is reduced to 200 ℃-300 ℃, cooled hydrogen-rich gas 12 is through gas-solid separator 13, isolate by product carbon black in the hydrogen-rich gas, gas-solid separator is separating device commonly used, as cyclonic separator, sack cleaner, hydrogen-rich gas 14 hydrogen contents after the dedusting are for reaching 90%-98%, all the other are a spot of methane, carbon monoxide, nitrogen etc., hydrogen-rich gas is according to the method for routine, as membrane sepn, the transformation fractionation by adsorption goes out hydrogen, part is as product output, and part is used as the working gas of plasma generator.
In order to cut down the consumption of energy, guard reactor is covered with flame-proof thermal insulation material 5 at the inwall of reactor 6, and the interchanger 10 on reactor top is embedded in wherein, except wall that can guard reactor 6, prolongs the life-span of refractory materials; In addition, 7 coatings of the outer wall of reactor employing lagging material are in order to reduce the reactor thermosteresis equally.
As Fig. 1, when implementing the method for hydrogen manufacturing of the present invention, opening valve is the interchanger 9 that 98% coal-seam gas 8 enters the plasma reactor bottom with methane content, compressed nitrogen 3 is delivered to plasma generator 2, start high frequency ignition and light plasma generator electric arc, form plasma jet 4.Deng reach stable state to system, enter the coal-seam gas of plasma reactor bottom interchanger 9, with 900 ℃ of-1300 ℃ of gas converting heats after the plasma reaction, coal-seam gas is heated to 300 ℃-600 ℃, heated coal-seam gas continues in top interchanger 10 and the heat exchange of plasma reactor wall, the coal-seam gas secondary is heated pre-activation, temperature rises to 600 ℃-900 ℃, preheating activatory coal-seam gas 11 enters in the plasma reactor 6, the plasma jet 4 of the temperature that is rich in active particle up to 3500 ℃-4500 ℃ that produces with plasma generator in reaction zone acts on mutually, under normal pressure, be the hydrogen-rich gas of main component less than generating in the time of 100ms with hydrogen, hydrogen-rich gas enters the bottom of plasma gas reactor, heat exchange in bottom interchanger 9, temperature is reduced to 200 ℃-300 ℃, through gas-solid separator 13, isolate by product carbon black in the hydrogen-rich gas 12, gas-solid separator 13 is separating device commonly used, as cyclonic separator, sack cleaner, the amount of hydrogen and nitrogen is for reaching 90%-97% in the hydrogen-rich gas 14 after the dedusting, all the other are a spot of methane, carbon monoxide etc., the ratio 2.7-3 of hydrogen and nitrogen.Hydrogen-rich gas 14 enters gas separation system, and this separation system is the isolation of purified technology of present synthetic ammonia factory routine, isolate gases such as carbon monoxide, carbonic acid gas, hydrogen sulfide after, as the unstripped gas of synthetic ammonia.
In order to cut down the consumption of energy, guard reactor is provided with flame-proof thermal insulation material 5 at the inwall of reactor 6, and the interchanger 10 on reactor top just is embedded in wherein, except can guard reactor 6 walls, prolongs the life-span of refractory materials; In addition, 7 coatings of the outer wall of reactor employing lagging material are in order to reduce the reactor thermosteresis equally.
As Fig. 1, when implementing the method for hydrogen manufacturing of the present invention, with methane content is 26.3%, hydrogen content is the interchanger 9 that the gas mixture 8 that forms after 55.6% coke-oven gas and the carbon dioxide mix enters plasma reactor 6 bottoms, water vapour and mixing as working gas 3 of oxygen are delivered to plasma generator 2, start high frequency ignition and light plasma generator electric arc, form plasma jet 4.Deng reach stable state to system, enter the gas mixture of plasma reactor 6 bottom interchanger, with 1000 ℃ of-1500 ℃ of gas converting heats after the plasma reaction, gas mixture is heated to 300 ℃-800 ℃, heated gas mixture continues and the heat exchange of plasma reactor wall, gas mixture is heated by secondary, temperature rises to 600 ℃-1000 ℃, gas mixture 11 after the pre-thermal activation enters in the plasma reactor, the plasma jet of the temperature that is rich in active particle up to 2000 ℃-3500 ℃ that produces with plasma generator in reaction zone acts on mutually, under normal pressure, be the gas of main component less than generating in the time of 100ms with hydrogen, hydrogen-rich gas enters the bottom of plasma gas reactor, with 9 heat exchange of bottom interchanger, temperature is reduced to 200 ℃ below-300 ℃, hydrogen-rich gas 12 after the cooling is through gas-solid separator 13, isolate a spot of carbon black in the hydrogen-rich gas, gas-solid separator is separating device commonly used, as cyclonic separator, sack cleaner, the content of hydrogen and carbon monoxide reaches 92%-98% in the hydrogen-rich gas 14 after the dedusting, the ratio of hydrogen and carbon monoxide is 1.8-2.3, all the other are a spot of carbon monoxide, carbonic acid gas, nitrogen etc., hydrogen-rich gas is according to the method for routine, as low-temperature rectisol, remove carbonic acid gas, gases such as hydrogen sulfide, output is used to produce methyl alcohol as synthetic gas, dme, fuel or industrial chemicals such as alkene.
In order to cut down the consumption of energy, guard reactor is covered with flame-proof thermal insulation material 5 at the inwall of reactor 6, and the interchanger 10 on reactor top just is embedded in wherein, except can guard reactor 6 walls, prolongs the life-span of refractory materials; In addition, 7 coatings of the outer wall of reactor employing lagging material are in order to reduce the reactor thermosteresis equally.
Claims (5)
1. the method for a producing hydrogen gas by methane-rich plasma, the concrete processing step of this method is as follows:
I. methane content is at 10%～100% high methane gas, or the gas mixture of itself and water vapour, carbonic acid gas, enter in the interchanger of plasma reactor bottom, carry out heat exchange with reacted 600 ℃-1500 ℃ hydrogen-rich gas, high methane gas or gas mixture are heated to 300 ℃-600 ℃;
II. heated high methane gas or gas mixture enter interchanger and the heat exchange of plasma reactor wall in the plasma reactor wall, high methane gas or gas mixture by second-heating after, temperature rises to 600 ℃-1200 ℃;
III. entered plasma reactor by the high methane gas of second-heating or gas mixture, act on mutually at the plasma jet that is rich in active particle of reaction zone with 2500 ℃-5000 ℃ plasma generator generation, generating with hydrogen in the 0.5-500ms under normal pressure is the hydrogen-rich gas of main component, and temperature is reduced to 200 ℃-300 ℃ after this hydrogen-rich gas and wall of reactor, high methane gas or the gas mixture heat exchange;
IV. the hydrogen-rich gas after the cooling enters separator, isolates solid impurity, further separates making hydrogen then.
2. a kind of method as claimed in claim 1, its high methane gas are Sweet natural gas, coal-seam gas, coke-oven gas or its any mixing.
3. interchanger and the heat exchange of plasma reactor wall that a kind of method as claimed in claim 1 or 2, its high methane gas or gas mixture enter in the plasma reactor wall are to carry out heat exchange by the spiral tube exchanger in the flame-proof thermal insulation material layer that is arranged on the plasma reactor inwall.
4. a kind of method as claimed in claim 1, its plasma generator are non-mobile model arc plasma producers.
5. as claim 1 or 4 described a kind of methods, the working gas of its plasma generator is hydrogen, argon gas, oxygen, carbonic acid gas, nitrogen, water vapour and airborne a kind of or its any mixing.
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| CN101734620B (en) | 2011-10-05 |
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