CN111377401A - Multi-reaction-tube low-temperature plasma equipment and method for decomposing hydrogen sulfide - Google Patents
Multi-reaction-tube low-temperature plasma equipment and method for decomposing hydrogen sulfide Download PDFInfo
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- CN111377401A CN111377401A CN201811642924.6A CN201811642924A CN111377401A CN 111377401 A CN111377401 A CN 111377401A CN 201811642924 A CN201811642924 A CN 201811642924A CN 111377401 A CN111377401 A CN 111377401A
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- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B3/00—Hydrogen; Gaseous mixtures containing hydrogen; Separation of hydrogen from mixtures containing it; Purification of hydrogen
- C01B3/02—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen
- C01B3/04—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by decomposition of inorganic compounds, e.g. ammonia
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- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B17/00—Sulfur; Compounds thereof
- C01B17/02—Preparation of sulfur; Purification
- C01B17/04—Preparation of sulfur; Purification from gaseous sulfur compounds including gaseous sulfides
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- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B17/00—Sulfur; Compounds thereof
- C01B17/02—Preparation of sulfur; Purification
- C01B17/04—Preparation of sulfur; Purification from gaseous sulfur compounds including gaseous sulfides
- C01B17/0404—Preparation of sulfur; Purification from gaseous sulfur compounds including gaseous sulfides by processes comprising a dry catalytic conversion of hydrogen sulfide-containing gases, e.g. the Claus process
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- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/30—Hydrogen technology
- Y02E60/36—Hydrogen production from non-carbon containing sources, e.g. by water electrolysis
Abstract
The invention relates to the field of plasma chemistry, and discloses a multi-reaction-tube low-temperature plasma device and a method for decomposing hydrogen sulfide, which comprise the following steps: a first cavity (1) formed by at least two parallel reaction tubes; a second cavity (2) nested inside the first cavity (1); a third cavity (7) nested outside the first cavity (1); an inner electrode (3), an outer electrode (4) and a blocking medium (6) are respectively arranged in each reaction tube. The multi-reaction-tube low-temperature plasma reaction equipment provided by the invention can be used for plasma decomposition of hydrogen sulfide, and the reactor can generate uniform and efficient dielectric barrier discharge, so that hydrogen sulfide is directly decomposed to generate hydrogen and sulfur.
Description
Technical Field
The invention relates to the field of plasma chemistry, in particular to a multi-reaction-tube low-temperature plasma device and a method for decomposing hydrogen sulfide.
Background
Hydrogen sulfide (H)2S) is a highly toxic and malodorous acid gas, which not only can cause the corrosion of materials such as metal, but also can harm the health of human bodies and pollute the environment. At present, the traditional Claus method (Claus) is adopted by large and medium-sized oil refineries in China to treat H-containing oil2And (4) tail gas of S, and recovering sulfur. The process recovers only the sulfur in the hydrogen sulfide, but converts valuable hydrogen to water. From the viewpoint of comprehensive utilization of resources, in the conventional hydrogen sulfide recovery process, hydrogen resources are not effectively utilized.
Therefore, the decomposition of hydrogen sulfide into sulfur and hydrogen gradually becomes a technical field of great attention of domestic and foreign researchers.
At present, the hydrogen sulfide decomposition method mainly comprises the following steps: high temperature decomposition, electrochemical, photocatalytic, and low temperature plasma methods. Among the aforementioned methods, the pyrolysis method is relatively mature in industrial technology, but the thermal decomposition of hydrogen sulfide strongly depends on the reaction temperature and is limited by the thermodynamic equilibrium, and the conversion rate of hydrogen sulfide is only 20% even if the reaction temperature is 1000 ℃ or higher. In addition, the high temperature conditions place high demands on reactor materials, which also increases operating costs. In addition, since the thermal decomposition conversion of hydrogen sulfide is low, a large amount of hydrogen sulfide gas needs to be separated from the tail gas and circulated in the system, thereby reducing the efficiency of the apparatus and increasing the energy consumption, which all bring difficulties to large-scale industrial application thereof. Although the adoption of the membrane technology can effectively separate products, thereby breaking balance limitation and improving the conversion rate of hydrogen sulfide, the thermal decomposition temperature often exceeds the limit heat-resistant temperature of the membrane, so that the structure of the membrane material is damaged. The electrochemical method has the defects of multiple operation steps, serious equipment corrosion, poor reaction stability, low efficiency and the like. The photocatalytic method for decomposing hydrogen sulfide mainly refers to the research of photocatalytic water decomposition, and the research focuses on the aspects of developing high-efficiency semiconductor photocatalysts and the like. The method for decomposing the hydrogen sulfide by utilizing the solar energy has the advantages of low energy consumption, mild reaction conditions, simple operation and the like, and is a relatively economic method. However, this method has problems such as a small treatment amount, low catalytic efficiency, and easy deactivation of the catalyst.
Compared with other decomposition methods, the low-temperature plasma method has the advantages of simple operation, small device volume, high energy efficiency and the like, and the involved reaction has high controllability and can be flexibly applied under the conditions of small treatment capacity and difficult centralized treatment. In addition, the hydrogen sulfide decomposition device has the characteristics of high energy density and shortened reaction time, can realize effective decomposition of hydrogen sulfide at a lower temperature, and is suitable for occasions with different scales, dispersed layouts and variable production conditions. Besides, the low-temperature plasma method recovers hydrogen resources while recovering sulfur, and can realize resource utilization of hydrogen sulfide.
At present, researchers at home and abroad carry out extensive research on the technology of decomposing hydrogen sulfide by low-temperature plasma, and the used discharge forms mainly comprise glow discharge, corona discharge, sliding arc discharge, microwave plasma, radio frequency plasma, dielectric barrier discharge and the like.
CN102408095A uses dielectric barrier discharge and photocatalyst to synergistically decompose hydrogen sulfide by filling a solid catalyst with photocatalytic activity in a plasma region. However, this process has the disadvantage that sulphur produced by the decomposition of hydrogen sulphide is deposited below the catalyst bed.
CN103204466A discloses a temperature-controlled hydrogen sulfide decomposition device and method, the device is characterized in that a central electrode is made of metal, a grounding electrode is made of temperature-controlled circulating liquid, and the hydrogen sulfide decomposition process can be continuously and stably carried out through temperature control of a liquid grounding electrode. In addition, CN103204467A discloses a device and a method for preparing hydrogen by continuously and stably decomposing hydrogen sulfide, which is characterized in that a central electrode is made of metal, a ground electrode is used as temperature-controllable circulating liquid, temperature control is performed through a liquid ground electrode, raw material is fed in a circumferential direction and reversely passes through a discharge area in a spiral mode along an axial direction, so that generated sulfur is timely and centrifugally separated. However, in order to ensure that the hydrogen sulfide is decomposed as sufficiently as possible in the methods disclosed in CN103204466A and CN103204467A, it is necessary to control the flow rate of the hydrogen sulfide so that the residence time of the hydrogen sulfide in the inner cylinder of the reactor is longer and to control the size of the inner cylinder so that more electric energy is obtained per unit volume of gas in the inner cylinder, and since the current prior art cannot provide a more powerful power source, the methods disclosed in CN103204466A and CN103204467A can only achieve the highest conversion rate of the hydrogen sulfide of about 20% even if the residence time of the hydrogen sulfide is longer and the size of the inner cylinder is controlled so that more electric energy is obtained per unit volume of gas in the inner cylinder, and when the highest conversion rate of the hydrogen sulfide reaches about 20%, the energy consumption of the decomposition reaction of the hydrogen sulfide is considerably high and is not suitable for large-scale industrial applications. Further, the methods disclosed in CN103204466A and CN103204467A have the drawback that the kinds of the liquid-applicable ground electrodes are very few, and the disclosed salt solutions and the like can generally only maintain the temperature of the reactor at 100 ℃ or lower, whereas elemental sulfur is generally solid at 100 ℃ or lower, which is likely to cause the reactor to be clogged.
Disclosure of Invention
The invention aims to overcome the defects of low hydrogen sulfide conversion rate and high decomposition energy consumption of low-temperature plasma reaction equipment provided by the prior art when the low-temperature plasma reaction equipment is used for decomposing hydrogen sulfide, and provides novel multi-reaction-tube low-temperature plasma reaction equipment capable of improving the hydrogen sulfide conversion rate and reducing the decomposition energy consumption and a method for decomposing hydrogen sulfide by using the same.
The differences between the "side wall" and the "outer side wall" and the "inner side wall" of the present invention are: "outer sidewall" and "inner sidewall" mean "sidewall" outer and inner surfaces, respectively, and if "sidewall" means "outer sidewall" and/or "inner sidewall".
In order to achieve the above object, the present invention provides, in a first aspect, a multi-reaction-tube low-temperature plasma reaction apparatus, comprising:
the first cavity is formed by at least two reaction tubes which are arranged in parallel and are correspondingly communicated at the top and the bottom respectively, an inner electrode, an outer electrode and a blocking medium are arranged in each reaction tube respectively, and a first inlet and a first outlet are arranged on the first cavity respectively;
the second cavity is nested in the first cavity, and a second inlet and a second outlet are respectively arranged on the second cavity;
the third cavity is nested outside the first cavity, and a third inlet and a third outlet are respectively arranged on the third cavity;
wherein, in each of the reaction tubes,
at least part of the inner electrode extends into the reaction tube;
the outer electrode forms at least part of the side wall of the reaction tube or is arranged on the side wall of the reaction tube in a surrounding way; and
the barrier dielectric is disposed between the inner electrode and the outer electrode such that a discharge region between the inner electrode and the outer electrode is separated by the barrier dielectric;
the inner electrode and the outer electrode are both solid electrodes, and the shapes of the inner electrode and the outer electrode are matched with each other to form an isodiametric structure;
the distance between the outer side wall of the inner electrode and the inner side wall of the outer electrode is L1The thickness of the barrier medium is D1，L2＝L1-D1And L is2And D1The ratio of (0.1-100): 1, preferably L2And D1The ratio of the two components is (0.1-30)): 1; more preferably (0.2-15): 1.
"isodiametric structure" means: the minimum distance between any point of the outer side wall of the inner electrode and the inner side wall of the outer electrode is equal to the minimum distance between other points of the outer side wall of the inner electrode and the inner side wall of the outer electrode.
Preferably, the inner electrodes in the respective reaction tubes are connected in parallel with each other.
Preferably, the external electrodes in the respective reaction tubes are connected in parallel with each other.
Preferably, in each of the reaction tubes, the inner electrode forms at least a part of a side wall of the second cavity.
Preferably, in each of the reaction tubes, the inner electrode is circumferentially disposed on a sidewall of the second cavity.
Preferably, in each of the reaction tubes, the inner electrode is circumferentially disposed on an outer sidewall of the second cavity.
Preferably, in each of the reaction tubes, the barrier medium forms at least part of the side wall of the reaction tube or is circumferentially disposed on the inner side wall of the reaction tube; more preferably, the reaction tube is formed of a barrier medium.
Preferably, in each of the reaction tubes, the external electrode is disposed around an outer sidewall of the reaction tube, and the blocking medium forms at least a part of the sidewall of the reaction tube.
Preferably, the barrier medium is disposed on at least a portion of the outer surface of the inner electrode, such that at least a portion of the outer surface of the inner electrode is wrapped with the barrier medium. The barrier medium may be fixed to the outer surface of the inner electrode in any manner that allows it to be fixed, or the barrier medium may be applied to the outer surface of the inner electrode in the form of a coating.
In the present invention, the shape of the first cavity and the second cavity may be, for example, cylindrical, serpentine, fin-shaped, S-shaped, wave-shaped.
According to another preferred embodiment, the blocking dielectric is disposed around the inner electrode and the outer electrode, and the distances between the blocking dielectric and the inner electrode and the distances between the blocking dielectric and the outer electrode are both greater than 0. In this preferred embodiment, it is preferred that the barrier medium is fixedly attached to the top and/or bottom of the first cavity; more preferably, a hole structure is arranged at one end of the blocking medium fixedly connected with the first cavity. The aperture structure enables the flow of material in the first cavity to be accessed by the aperture structure. The fixing manner of the blocking medium is not particularly limited in the present invention, as long as the blocking medium can be disposed between the inner electrode and the outer electrode in a surrounding manner.
In the present invention, the inner electrode may be, for example, a cylindrical shape, the first cavity is a hollow cylinder extending along an axial direction with a constant diameter, and the inner electrode and the first cavity are coaxial.
The low-temperature plasma reaction equipment provided by the invention is preferably jacket type dielectric barrier discharge reaction equipment with a coaxial structure, the basic structure of the low-temperature plasma reaction equipment mainly comprises an inner electrode, an outer electrode, a barrier medium and the like, and the sleeve type structure can enable the heat-conducting medium to circularly heat or cool the discharge reaction equipment, so that flexible temperature control of a discharge area is realized. In particular, the present invention is achieved by controlling L2And thickness D of barrier medium1The proportion relation of (A) is in a specific range, and when a solid inner electrode and a solid outer electrode are applied, the conversion rate of hydrogen sulfide can be obviously improved and the decomposition energy consumption can be reduced compared with the prior art.
The jacket structure design of the invention can lead the heat-conducting medium to circularly flow in the shell layer, ensure the discharge intensity and simultaneously maintain the whole reaction equipment within a certain temperature range, lead the generated sulfur to flow out of the reaction equipment in a liquid state, effectively avoid the solidification of the sulfur generated by the decomposition of the hydrogen sulfide, and lead the decomposition process to continuously and stably realize long-period operation while achieving higher conversion rate.
Preferably, the number of the first cavities is 1.
According to another particularly preferred embodiment, the number of the first cavities is more than 2, and each of the first cavities is respectively composed of at least two reaction tubes which are arranged in parallel and the top and the bottom of each reaction tube are respectively and correspondingly communicated. In this particularly preferred embodiment, it is preferred that the respective inner electrodes are connected in parallel with each other. In this particularly preferred embodiment, the individual outer electrodes are preferably connected in parallel with one another.
Preferably, the material of the blocking medium is an electrical insulating material. More preferably at least one selected from the group consisting of glass, quartz, ceramic, enamel, polytetrafluoroethylene and mica. The glass can be quartz glass or hard glass; the material forming the barrier medium can also be other metal and non-metal composite materials with high-voltage electric insulation design, and the like. The ceramic may be an alumina ceramic.
Preferably, the outer electrode and the inner electrode are conductive materials. Preferably, the outer electrode and the inner electrode may each independently be at least one selected from the group consisting of a graphite tube, graphite powder, a metal rod, a metal foil, a metal mesh, a metal tube, metal powder, and a graphite rod.
The metal rod and the metal pipe can comprise an elemental metal rod, an alloy metal rod, an elemental metal pipe and an alloy metal pipe. The metal powder may comprise elemental metal powder, alloy metal powder, or a mechanical mixture of elemental and/or alloy metal powders. The material forming the electrodes (including the inner electrode and the outer electrode) can also be other rod-shaped and tubular materials with conductive performance.
In the present invention, it is preferable that one of the inner electrode and the outer electrode is a ground electrode and the other is a high voltage electrode. The material of the inner electrode and the outer electrode can be determined by those skilled in the art according to application requirements.
Preferably, the reaction apparatus of the present invention further comprises a ground line, one end of which is electrically connected to the outer electrode or the inner electrode.
Preferably, the first inlet is provided at an upper portion of the first cavity, and the first outlet is provided at a lower portion and/or a bottom portion of the first cavity.
Preferably, the first outlet includes a gaseous product outlet and a liquid product outlet, and the gaseous product outlet is disposed at a lower portion of the first cavity, and the liquid product outlet is disposed at a bottom of the first cavity.
Preferably, the gas product outlet is arranged below the discharge area, and the gas product outlet is arranged at a position corresponding to the height H of the bottom of the first cavity1And the length L of the discharge region3The proportion relation between the components is as follows: h1：L31: (0.05 to 25000); preferably H1：L31: (0.1 to 10000); more preferably H1：L3＝1：(0.5～1000)。
In the present invention, the "discharge region" refers to a region where the inner electrode, the outer electrode, and the blocking dielectric completely overlap.
The ratio of the inner diameter of the first cavity to the aperture of the first outlet may be (0.1 to 100): 1.
the ratio of the aperture of the first inlet to the aperture of the first outlet may be (0.1 to 120): 1.
the ratio of the length of the first cavity to the inner diameter of the first cavity can be (0.5-500): 1. the inner diameter of the first cavity represents the distance from the axis of the first cavity to the outer side wall of the first cavity.
Preferably, the second inlet and the second outlet are provided at a lower portion and an upper portion of the second cavity, respectively.
Preferably, the third inlet and the third outlet are disposed at a lower portion and an upper portion of the third cavity, respectively.
The first inlet of the present invention may be arranged such that the feed gas entering the first cavity is parallel to the inner diameter of the first cavity or at an angle, for example, may be arranged tangentially.
The invention can lead the temperature of the reaction equipment with the jacket structure to be maintained between 119 and 444.6 ℃ for example by introducing the heat-conducting medium into the second cavity and the third cavity. In this case, the sulfur produced can be continuously discharged in a liquid form.
The low-temperature plasma reaction equipment can be filled with a catalyst capable of catalyzing the hydrogen sulfide to be decomposed into elemental sulfur and hydrogen, and the catalyst is preferably filled in the first cavity of the reaction equipment. The present invention has no particular requirement on the loading volume and the loading type of the catalyst, and the type of the catalyst may be, for example, any one or more of the catalysts disclosed in CN102408095A, CN101590410A, and CN 103495427A.
The low-temperature plasma reaction equipment provided by the invention can be used for plasma decomposition of hydrogen sulfide, and the reaction equipment can generate uniform and efficient dielectric barrier discharge, so that hydrogen sulfide is directly decomposed to generate hydrogen and sulfur.
In a second aspect, the present invention provides a method for decomposing hydrogen sulfide, the method being implemented in the multi-reaction-tube low-temperature plasma reaction apparatus according to the first aspect of the present invention, the method comprising: and one of an outer electrode and an inner electrode of the reaction equipment is connected with a high-voltage power supply, the other one is grounded, dielectric barrier discharge is carried out, raw material gas containing hydrogen sulfide is introduced into a first cavity from a first inlet of the first cavity of the reaction equipment to carry out decomposition reaction of the hydrogen sulfide, material flow obtained after decomposition is led out from a first outlet, and heat-conducting medium is continuously introduced into a second cavity and a third cavity of the reaction equipment from a second inlet and a third inlet and is led out from the second outlet and the third outlet to control the temperature of the first cavity of the reaction equipment.
Preferably, the conditions of the dielectric barrier discharge include: the discharge voltage is 2kV to 80kV, preferably 5kV to 30kV, more preferably 5kV to 20kV, and even more preferably 5kV to 15 kV; the discharge frequency is 200 to 30000Hz, preferably 500 to 15000Hz, and more preferably 500 to 13000 Hz.
Preferably, the conditions of the decomposition reaction include: the reaction temperature is 0-800 ℃, preferably 40-500 ℃, and more preferably 119-444.6 ℃; the reaction pressure is 0 to 0.6MPa, preferably 0 to 0.3 MPa.
Preferably, the residence time of the feed gas containing hydrogen sulphide in the discharge zone of the reaction device is 1 × 10-5120s, preferably 2 × 10-5～60s。
Preferably, the decomposition reaction of hydrogen sulfide is carried out in the presence of a carrier gas selected from at least one of nitrogen, hydrogen, helium, argon, water vapor, carbon monoxide, carbon dioxide, methane, ethane and propane; more preferably, the carrier gas is selected from at least one of hydrogen, argon, helium, and nitrogen.
Particularly preferably, the carrier gas is selected from at least one of hydrogen, argon, helium, and nitrogen.
Preferably, the content of the hydrogen sulfide gas in the feed gas is such that the content of the hydrogen sulfide gas at the first inlet of the low-temperature plasma reaction device is 1 × 10-8-100% by volume; more preferably 10 to 100% by volume.
In the present invention, the raw material gas does not include the aforementioned carrier gas of the present invention, the raw material gas is pure hydrogen sulfide gas or industrial waste gas containing hydrogen sulfide and other gases obtained in industrial production, and the carrier gas defined in the present invention is a gas that is actively added to be mixed with the raw material gas, although the raw material gas may contain the same kind of gas as the carrier gas defined in the present invention, and the method of the present invention can control the amount of the carrier gas added as needed.
The following provides a preferred embodiment for decomposing hydrogen sulfide by using the multi-reaction-tube low-temperature plasma reaction device of the invention:
a protective gas, for example nitrogen, is introduced into the first cavity of the reaction device from the first inlet to remove air from the discharge region, and the gas is withdrawn from the first outlet. And meanwhile, heat-conducting media are introduced into the second cavity and the third cavity from the second inlet and the third inlet, and the introduced heat-conducting media are respectively led out from the second outlet and the third outlet. The temperature of the heat transfer medium is maintained at the temperature required for the system reaction. Then introducing raw material gas containing hydrogen sulfide into a first cavity of the reaction equipment from a first inlet, switching on a high-voltage power supply after the raw material gas flow is stable, and forming a plasma discharge field between the inner electrode and the outer electrode by adjusting voltage and frequency. The hydrogen sulfide gas is ionized in the discharge area and decomposed into hydrogen and elemental sulfur, and the elemental sulfur generated by discharge slowly flows down along the wall of the first cavity and flows out from the first outlet.
The low-temperature plasma reaction equipment provided by the invention can realize continuous and stable hydrogen sulfide decomposition process under the condition of obviously higher hydrogen sulfide conversion rate, and the device can realize long-period operation.
And the low-temperature plasma reaction equipment provided by the invention can also be used for a hydrogen sulfide treatment process with high flow rate and high concentration.
Drawings
Fig. 1 is a schematic structural diagram of a preferred embodiment of a multi-reaction-tube low-temperature plasma reaction device provided by the invention.
Description of the reference numerals
1. A first cavity 2 and a second cavity
11. First inlet 21, second inlet
12. Gas product outlet 22, second outlet
13. Liquid product outlet
3. Inner electrode
4. External electrode
5. Grounding wire
6. Barrier dielectric
7. Third cavity 71, third inlet
72. A third outlet
Detailed Description
The endpoints of the ranges and any values disclosed herein are not limited to the precise range or value, and such ranges or values should be understood to encompass values close to those ranges or values. For ranges of values, between the endpoints of each of the ranges and the individual points, and between the individual points may be combined with each other to give one or more new ranges of values, and these ranges of values should be considered as specifically disclosed herein.
The structure of a preferred embodiment of the multi-reaction-tube low-temperature plasma reaction apparatus of the present invention is provided below with reference to fig. 1, specifically:
the reaction apparatus comprises:
the device comprises a first cavity 1, a second cavity and a third cavity, wherein the first cavity is composed of at least two reaction tubes which are arranged in parallel and are respectively and correspondingly communicated at the top and the bottom, an inner electrode 3, an outer electrode 4 and a blocking medium 6 are respectively arranged in each reaction tube, and a first inlet 11 and a first outlet are respectively arranged on the first cavity 1;
the second cavity 2 is nested inside the first cavity 1, and a second inlet 21 and a second outlet 22 are respectively arranged on the second cavity 2;
the third cavity 7 is nested outside the first cavity 1, and a third inlet 71 and a third outlet 72 are respectively arranged on the third cavity 7;
wherein, in each of the reaction tubes,
at least part of the inner electrode 3 extends into the reaction tube;
the outer electrode 4 forms at least part of the side wall of the reaction tube or is arranged around the reaction tube
The side wall of the reaction tube; and
the blocking medium 6 is arranged between the inner electrode 3 and the outer electrode 4 such that
The discharge area between the inner electrode 3 and the outer electrode 4 is separated by the barrier medium 6;
the inner electrode 3 and the outer electrode 4 are both solid electrodes, and the shapes of the two electrodes are matched with each other
Synthesizing to form an isometric structure;
the distance between the outer side wall of the inner electrode 3 and the inner side wall of the outer electrode 4 is L1，
The thickness of the barrier medium 6 is D1，L2＝L1-D1And L is2And D1The ratio of (0.1-100): 1, preferably L2And D1The ratio of (0.1-30): 1; more preferably
1 is (0.2-15).
It is preferable that the inner electrodes 3 in the respective reaction tubes are connected in parallel with each other.
Preferably, the external electrodes 4 in the respective reaction tubes are connected in parallel with each other.
Preferably, in each of the reaction tubes, the inner electrode 3 forms at least a part of a side wall of the second cavity 2.
According to a preferred embodiment, in each of the reaction tubes, the inner electrode 3 is circumferentially disposed on the side wall of the second cavity 2; more preferably, in each of the reaction tubes, the inner electrode 3 is circumferentially disposed on an outer sidewall of the second cavity 2.
According to a preferred embodiment, in each of said reaction tubes, said barrier medium 6 forms at least part of the side wall of said reaction tube or is circumferentially arranged on the inner side wall of said reaction tube; more preferably, the reaction tube is formed by a barrier medium 6.
Preferably, in each of the reaction tubes, the external electrode 4 is circumferentially disposed on an outer sidewall of the reaction tube, and the blocking medium forms at least a part of the sidewall of the reaction tube.
Preferably, in each reaction tube, the barrier medium 6 is disposed on at least part of the outer surface of the inner electrode 3, so that at least part of the outer surface of the inner electrode 3 is wrapped with the barrier medium 6.
Preferably, in each reaction tube, the blocking medium 6 is arranged between the inner electrode 3 and the outer electrode 4 in a surrounding manner, and the distances between the blocking medium and the inner electrode 3 and the outer electrode 4 are respectively larger than 0.
According to a preferred embodiment, the number of first cavities 1 is 1.
According to another preferred embodiment, the number of the first cavities 1 is more than 2, and each of the first cavities 1 is respectively composed of at least two reaction tubes which are arranged in parallel and the top and the bottom of each reaction tube are respectively and correspondingly communicated.
Preferably, the reaction apparatus further comprises a ground line 5, and one end of the ground line 5 is electrically connected to the inner electrode 3 or the outer electrode 4.
In the present invention, one of the inner electrode 3 and the outer electrode 4 is a ground electrode, and the other is a high voltage electrode.
Preferably, the first inlet 11 is arranged at an upper portion of the first cavity 1 and the first outlet is arranged at a lower portion and/or a bottom portion of the first cavity 1.
Preferably, the second inlet 21 and the second outlet 22 are provided at a lower portion and an upper portion of the second cavity 2, respectively.
Preferably, the third inlet 71 and the third outlet 72 are provided at a lower portion and an upper portion of the third cavity 7, respectively.
Preferably, the first outlet includes a gaseous product outlet 12 and a liquid product outlet 13, and the gaseous product outlet is disposed at a lower portion of all the reaction tubes, and the liquid product outlet is disposed at a bottom portion of all the reaction tubes. Preferably, the reaction tubes are the same size.
Preferably, the gas product outlet is arranged below all the discharge area, and the gas product outlet is arranged at a position corresponding to the height H of the bottom of the first cavity 11And the length L of the discharge region3The proportion relation between the components is as follows: h1：L31: (0.05 to 25000); preferably H1：L31: (0.1 to 10000); more preferably H1：L3＝1：(0.5～1000)。
The pressure in the present invention means absolute pressure unless otherwise specified.
The multi-reaction-tube low-temperature plasma reaction equipment provided by the invention also has the following specific advantages:
(1) compared with a liquid grounding electrode, the solid grounding electrode has larger micro-discharge current generated by discharge when matched with the structure of the invention, and is more beneficial to the discharge decomposition reaction of hydrogen sulfide molecules.
(2) This reaction equipment sets up jacket structure, and the accessible is pressed from both sides the heat-conducting medium temperature in the cover and is carried out temperature control to reaction equipment, can make the sulphur that hydrogen sulfide discharge decomposition produced flow out the discharge region smoothly, avoids sulphur solidification to block up reaction equipment, makes the continuation of discharging stable going on.
(3) The reaction equipment is characterized in that L in each reaction tube is controlled2And the thickness D of the barrier medium1The proportion relation is as follows: (0.1-100): 1, preferably (0.1 to 30): 1, more preferably (0.2-15): 1, and the other structures of the reaction equipment can obviously improve the conversion rate of the hydrogen sulfide and reduce the energy consumption for decomposition.
The present invention will be described in detail below by way of examples. In the following examples, various raw materials used were commercially available unless otherwise specified.
The thickness of the barrier dielectric is the same in the following examples and comparative examples.
The hydrogen sulfide conversion in the following examples was calculated according to the following formula:
the decomposition rate of hydrogen sulfide (% of converted hydrogen sulfide/initial hydrogen sulfide) is × 100%
The energy consumption for decomposing hydrogen sulfide in the following examples was measured by an oscilloscope and calculated using lissajous figures.
Example 1
The reaction equipment with a structure similar to that of the low-temperature plasma reaction equipment shown in fig. 1 is adopted for hydrogen sulfide decomposition reaction, and the specific structure and structural parameters of the low-temperature plasma reaction equipment are as follows:
the reaction apparatus comprises:
the reactor comprises a first cavity, a second cavity and a third cavity, wherein a reactor inlet, a gas product outlet and a liquid product outlet are respectively arranged on the first cavity, the first cavity contains 4 reaction tubes which are arranged in parallel, the top and the bottom of each reaction tube are respectively and correspondingly communicated, so that raw materials entering from the reactor inlet can respectively enter each reaction tube, gaseous products generated in each reaction tube can be led out from the gas product outlet, liquid products generated in each reaction tube can be led out from the liquid product outlet, the sizes of the 4 reaction tubes are completely the same, all side walls of the reaction tubes are formed by blocking media, and the material forming the blocking media is hard glass;
the second cavity is nested in the first cavity, a second inlet and a second outlet are respectively arranged on the second cavity, a heat-conducting medium introduced from the second inlet can be distributed among the reaction tubes of the first cavity, the heat-conducting medium is led out from the second outlet, the side wall of each reaction tube is completely formed by an inner electrode, the material forming the inner electrode is stainless steel, the inner electrodes in the reaction tubes are connected in parallel, and the inner electrodes are connected with a high-voltage power supply;
the second cavity is nested outside the first cavity, a third inlet and a third outlet are respectively formed in the third cavity, the third cavity is made of stainless steel, and the third cavity is not electrically connected with the inner electrode;
the outer electrode, the outer electrode encircles respectively and sets up on each the lateral wall of reaction tube, forms the material of outer electrode is the stainless steel foil, will outer electrode ground connection, and the lower edge of the inner electrode in this embodiment with the lower edge of outer electrode flushes.
L2And the thickness D of the barrier medium1The ratio of (A) to (B) is 8: 1; and H1：L3＝1：32；
The volume of the first cavity of the entire reactor of this example was 1L.
In the embodiment, the mixed gas enters the first cavity of the reactor from the upper part of the first cavity of the reaction equipment, a gas product is led out from a gas product outlet positioned at the lower part of the first cavity of the reaction equipment, and elemental sulfur is led out from a liquid product outlet positioned at the bottom of the reaction equipment; and the heat-conducting medium of the embodiment is introduced from the lower parts of the second cavity and the third cavity of the reaction equipment and is extracted from the upper parts of the second cavity and the third cavity of the reaction equipment.
The method comprises the following operation steps:
nitrogen gas is fed into the first cavity of the reaction device from the inlet of the reaction device to purge the discharge region of air, and the gas is led out from the gaseous product outlet and the liquid product outlet. Meanwhile, heat-conducting media (specifically, dimethyl silicone oil) are respectively introduced into the second cavity and the third cavity from the second inlet and the third inlet, the introduced heat-conducting media are respectively led out from the second outlet and the third outlet, and the temperature of the heat-conducting media is kept at 145 ℃.
Then introducing H into the first cavity of the high-flux low-temperature plasma reactor from the inlet of the reactor2S/Ar mixed gas, in which H2The volume fraction of S was 27%, and the flow rate of the mixed gas was controlled so that the average residence time of the gas in the discharge zone was 12.5S and the pressure was 0.23 MPa. H2And (3) introducing the S/Ar mixed gas into the reactor for 30min, switching on an alternating-current high-voltage power supply, and adjusting the voltage and the frequency to form a plasma discharge field between the inner electrode and the solid grounding electrode. Wherein the discharge conditions are as follows: the voltage was 19.5kV, the frequency was 0.8kHz, and the current was 2.6A. The hydrogen sulfide gas is ionized in the discharge area and decomposed into hydrogen and elemental sulfur, and the elemental sulfur generated by discharge slowly flows down along the wall of the first cavity and flows out from the outlet of the liquid product. The gas flows out from the gas product outlet after the reaction.
As a result: in this example, H was measured after the hydrogen sulfide decomposition reaction was continued for 20min2The S conversion was 74.2%; and the discharge state and H are not abnormal after the discharge lasts for 100H2The S conversion rate is kept stable. And the decomposition energy consumption of the embodiment is 14.6eV/H2S molecule (1 molecule of H per decomposition)2S requires 14.6eV as energy).
Comparative example 1
This comparative example used a low temperature plasma reaction apparatus similar to that of example 1 for the hydrogen sulfide decomposition reaction, except that:
the ground electrode in this comparative example was a liquid ground electrode, and LiCl were used in a molar ratio of 1:1 in a molten stateAlCl3The liquid grounding electrode is also a heat-conducting medium, keeps the temperature at 145 ℃, and is placed in the second cavity and the third cavity of the reactor; the outer electrode in the comparative example is arranged on the outer side wall of each reaction tube in a surrounding way, and is connected with a high-voltage power supply; however, the heat transfer medium in the third cavity is not grounded and does not make an electrical connection with the high voltage electrode.
The flow rate of the mixed gas was controlled so that the mean residence time of the gas in the discharge zone was 26.8 s.
The volume of the first cavity of the entire reactor of this comparative example was 0.05L.
The rest is the same as in example 1.
And this comparative example carried out the hydrogen sulfide decomposition reaction in the same operation as in example 1.
As a result: h was measured after the hydrogen sulfide decomposition reaction of this comparative example was continued for 20min2S conversion rate is 13.2%, and H is generated after 1.5H of continuous discharge2The S conversion decreased to 5.3%.
The energy consumption for decomposition of this comparative example was 122eV/H2And (3) an S molecule.
Comparative example 2
This comparative example was carried out using a low temperature plasma reaction apparatus similar to that of comparative example 1, except that:
L2and thickness D of barrier medium1The ratio of (A) to (B) is 0.08: 1.
the flow rate of the mixed gas was controlled so that the mean residence time of the gas in the discharge zone was 27.1 s.
The volume of the first cavity of this comparative example was 0.02L.
The rest is the same as in comparative example 1.
As a result: h was measured after the hydrogen sulfide decomposition reaction of this comparative example was continued for 20min2S conversion rate is 18.4%, H after 1.5H of continuous discharge2The S conversion decreased to 7.2%.
The energy consumption for decomposition of this comparative example was 135eV/H2And (3) an S molecule.
Example 2
This example uses a plasma reactor similar to that of example 1 to carry out the decomposition reaction of hydrogen sulfide, except that in this example:
all the side walls of each reaction tube are formed by outer electrodes, the materials forming the outer electrodes are stainless steel metal foils, the outer electrodes are connected with a high-voltage power supply, and the inner electrodes are grounded;
the blocking medium is arranged on the inner side wall of each reaction tube in a surrounding manner;
L2and D1The ratio of (A) to (B) is 15: 1; and H1：L3＝1：85；
In this example, H was introduced into the inner tube of the high flux low temperature plasma reactor from the inlet of the reactor2S/Ar mixed gas, in which H2The volume fraction of S was 65%, and the flow rate of the mixed gas was controlled so that the average residence time of the gas in the discharge zone was 17.9S and the pressure was 0.12 MPa. H2And (3) introducing the S/Ar mixed gas into the reactor for 30min, switching on an alternating-current high-voltage power supply, and adjusting the voltage and the frequency to form a plasma discharge field between the central high-voltage electrode and the grounding electrode. Wherein the discharge conditions are as follows: the voltage was 9.7kV, the frequency was 4.2kHz, and the current was 2.9A.
The rest is the same as in example 1.
As a result: in this example, H was measured after the hydrogen sulfide decomposition reaction was continued for 20min2The S conversion was 75.1%; and the discharge state and H are not abnormal after the discharge lasts for 100H2The S conversion rate is kept stable. And the decomposition energy consumption of the embodiment is 13.9eV/H2And (3) an S molecule.
Example 3
This example uses a plasma reactor similar to that of example 1 to carry out the decomposition reaction of hydrogen sulfide, except that in this example:
all the side walls of each reaction tube are formed by outer electrodes, the material forming the outer electrodes is copper foil, the outer electrodes are grounded, and the inner electrodes are connected with a high-voltage power supply;
the barrier medium is arranged in the middle of each reaction tube in a surrounding way and is not in direct contact with the side wall of the reaction tube;
L2and D1The ratio of (A) to (B) is 0.5: 1; and H1：L3＝1：220；
In this example, H was introduced into the inner tube of the high flux low temperature plasma reactor from the inlet of the reactor2S/Ar mixed gas, in which H2The volume fraction of S is 65%, the flow rate of the mixed gas is controlled so that the mean residence time of the gas in the discharge zone is 15.3S and the pressure is 0.07 MPa. H2And (3) introducing the S/Ar mixed gas into the reactor for 30min, switching on an alternating-current high-voltage power supply, and adjusting the voltage and the frequency to form a plasma discharge field between the central high-voltage electrode and the grounding electrode. Wherein the discharge conditions are as follows: the voltage was 11.0kV, the frequency was 5.4kHz, and the current was 2.5A.
The rest is the same as in example 1.
As a result: in this example, H was measured after the hydrogen sulfide decomposition reaction was continued for 20min2The S conversion was 73.1%; and the discharge state and H are not abnormal after the discharge lasts for 100H2The S conversion rate is kept stable. And the decomposition energy consumption of the embodiment is 15.4eV/H2And (3) an S molecule.
Example 4
This example uses a plasma reactor similar to that of example 1 to carry out the decomposition reaction of hydrogen sulfide, except that in this example:
L2and D1The ratio of (A) to (B) is 35: 1;
the rest is the same as in example 1.
As a result: in this example, H was measured after the hydrogen sulfide decomposition reaction was continued for 20min2The S conversion was 66.4%; and the discharge state and H are not abnormal after the discharge lasts for 100H2The S conversion rate is kept stable. And the decomposition energy consumption of the embodiment is 20.7eV/H2And (3) an S molecule.
Example 5
This example uses a plasma reactor similar to that of example 1 to carry out the decomposition reaction of hydrogen sulfide, except that in this example:
H1：L3＝1：1200。
the rest is the same as in example 1.
As a result: the hydrogen sulfide decomposition reaction of this example continuedH is measured after 20min2The S conversion was 69.5%; and the discharge state and H are not abnormal after the discharge lasts for 100H2The S conversion rate is kept stable. And the decomposition energy consumption of the embodiment is 18.8eV/H2And (3) an S molecule.
From the above results, it can be seen that the hydrogen sulfide conversion rate can be significantly improved when the low-temperature plasma reaction device provided by the present invention is applied to the decomposition of hydrogen sulfide, compared with the prior art, and the reaction device provided by the present invention can maintain the high hydrogen sulfide conversion rate for a long period with low decomposition energy consumption.
The preferred embodiments of the present invention have been described above in detail, but the present invention is not limited thereto. Within the scope of the technical idea of the invention, many simple modifications can be made to the technical solution of the invention, including combinations of various technical features in any other suitable way, and these simple modifications and combinations should also be regarded as the disclosure of the invention, and all fall within the scope of the invention.
Claims (19)
1. A multi-reactor tube low temperature plasma apparatus, the apparatus comprising:
the device comprises a first cavity (1) and a second cavity (1), wherein the first cavity is composed of at least two reaction tubes which are arranged in parallel and are correspondingly communicated at the top and the bottom respectively, an inner electrode (3), an outer electrode (4) and a blocking medium (6) are respectively arranged in each reaction tube, and a first inlet (11) and a first outlet are respectively arranged on the first cavity (1);
the second cavity (2) is nested inside the first cavity (1), and a second inlet (21) and a second outlet (22) are respectively arranged on the second cavity (2);
the third cavity (7) is nested outside the first cavity (1), and a third inlet (71) and a third outlet (72) are respectively arranged on the third cavity (7);
wherein, in each of the reaction tubes,
at least part of the inner electrode (3) extends into the reaction tube;
the outer electrode (4) forms at least part of the side wall of the reaction tube or is arranged on the side wall of the reaction tube in a surrounding way; and
the barrier medium (6) is arranged between the inner electrode (3) and the outer electrode (4) such that a discharge area between the inner electrode (3) and the outer electrode (4) is separated by the barrier medium (6);
the inner electrode (3) and the outer electrode (4) are both solid electrodes, and the shapes of the inner electrode and the outer electrode are matched with each other to form an isodiametric structure;
the distance between the outer side wall of the inner electrode (3) and the inner side wall of the outer electrode (4) is L1The thickness of the barrier medium (6) is D1，L2＝L1-D1And L is2And D1The ratio of (0.1-100): 1, preferably L2And D1The ratio of (0.1-30): 1; more preferably (0.2-15): 1.
2. The apparatus according to claim 1, wherein the inner electrodes (3) in each of the reaction tubes are connected in parallel with each other;
preferably, the external electrodes (4) in the respective reaction tubes are connected in parallel with each other.
3. The apparatus according to claim 1 or 2, wherein in each of the reaction tubes the inner electrode (3) forms at least part of a side wall of the second cavity (2).
4. The apparatus according to claim 1 or 2, wherein in each of the reaction tubes the inner electrode (3) is circumferentially arranged on a side wall of the second cavity (2);
preferably, in each reaction tube, the inner electrode (3) is circumferentially disposed on an outer side wall of the second cavity (2).
5. The apparatus according to any one of claims 1-4, wherein in each of the reaction tubes the barrier medium (6) forms at least part of the side wall of the reaction tube or is arranged circumferentially on the inner side wall of the reaction tube;
preferably, the reaction tube is formed by a barrier medium (6).
6. The apparatus according to any one of claims 1-4, wherein in each of the reaction tubes the outer electrode (4) is circumferentially arranged on an outer sidewall of the reaction tube and the barrier medium forms at least part of the sidewall of the reaction tube.
7. The apparatus according to any one of claims 1 to 4, wherein in each of the reaction tubes, the barrier medium (6) is disposed on at least part of the outer surface of the inner electrode (3) such that at least part of the outer surface of the inner electrode (3) is wrapped with the barrier medium (6).
8. The apparatus according to any of claims 1-4, wherein in each of the reaction tubes the barrier medium (6) is arranged circumferentially between the inner electrode (3) and the outer electrode (4) with a distance to the inner electrode (3) and the outer electrode (4), respectively, of more than 0.
9. The device according to any of claims 1-8, wherein the number of first cavities (1) is 1.
10. The apparatus according to any one of claims 1 to 8, wherein the number of said first cavities (1) is more than 2, and each of said first cavities (1) is composed of at least two reaction tubes disposed in parallel and having top and bottom portions respectively communicated with each other.
11. The apparatus of any of claims 1-10, wherein the blocking dielectric is an electrically insulating material; preferably at least one selected from the group consisting of glass, quartz, ceramic, enamel, polytetrafluoroethylene, and mica;
the outer electrode (4) and the inner electrode (3) are each independently selected from conductive materials: preferably, each is independently selected from at least one of a graphite tube, graphite powder, a metal rod, a metal foil, a metal mesh, a metal tube, metal powder, and a graphite rod.
12. The device according to any one of claims 1-11, further comprising a ground wire (5) having one end electrically connected to a ground electrode, the ground electrode being the outer electrode (4) or the inner electrode (3), and the other of the outer electrode (4) and the inner electrode (3) being a high voltage electrode.
13. The device according to any of claims 1-12, wherein the first inlet (11) is arranged in an upper part of the first cavity (1) and the first outlet is arranged in a lower part and/or in a bottom part of the first cavity (1).
14. An apparatus according to claim 13, wherein the first outlet comprises a gaseous product outlet (12) and a liquid product outlet (13), and the gaseous product outlet (12) is arranged at a lower portion of the first cavity (1), and the liquid product outlet (13) is arranged at a bottom portion of the first cavity (1).
15. Apparatus according to claim 14, wherein the gas product outlet (12) is arranged below the discharge area and the gas product outlet (12) is arranged in a position with respect to the height H of the bottom of the first cavity (1)1And the length L of the discharge region3The proportion relation between the components is as follows: h1：L31: (0.05 to 25000); preferably H1：L31: (0.1 to 10000); more preferably H1：L3＝1：(0.5～1000)。
16. The apparatus according to any one of claims 1-15, wherein the second inlet (21) and the second outlet (22) are provided in a lower portion and an upper portion, respectively, of the second cavity (2);
preferably, the third inlet (71) and the third outlet (72) are provided at a lower portion and an upper portion of the third cavity (7), respectively.
17. A method of decomposing hydrogen sulfide, the method being carried out in the multi-reactor tube low temperature plasma apparatus of any one of claims 1 to 16, the method comprising: one of an outer electrode (4) and an inner electrode (3) of the device is connected with a high-voltage power supply, the other one is grounded, dielectric barrier discharge is carried out, raw material gas containing hydrogen sulfide is introduced into a first cavity (1) of the device from a first inlet (11) of the first cavity (1) to carry out decomposition reaction of the hydrogen sulfide, a material flow obtained after decomposition is led out from a first outlet, and heat-conducting medium is continuously introduced into a second cavity (2) and a third cavity (7) of the device from a second inlet (21) and a third inlet (71) and is continuously led out from a second outlet (22) and a third outlet (72) to control the temperature of the first cavity (1) of the device.
18. The method of claim 17, wherein the condition of the dielectric barrier discharge comprises: the discharge voltage is 2kV to 80kV, preferably 5kV to 30kV, more preferably 5kV to 20kV, and even more preferably 5kV to 15 kV; the discharge frequency is 200-30000 Hz, preferably 500-15000 Hz, and more preferably 500-13000 Hz;
the conditions of the decomposition reaction include: the reaction temperature is 0-800 ℃, preferably 40-500 ℃, more preferably 119-444.6 ℃, the reaction pressure is 0-0.6MPa, preferably 0-0.3MPa,
the residence time of the feed gas containing hydrogen sulphide in the discharge zone of the apparatus was 1 × 10-5120s, preferably 2 × 10-5～60s。
19. The method according to claim 17 or 18, wherein the decomposition reaction of hydrogen sulfide is carried out in the presence of a carrier gas selected from at least one of nitrogen, hydrogen, helium, argon, water vapor, carbon monoxide, carbon dioxide, methane, ethane and propane, preferably the carrier gas is selected from at least one of hydrogen, argon, helium and nitrogen.
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