1. A double-tower-plate chemical-looping hydrogen production device for treating sludge biomass solid waste is characterized by comprising a tower body, an upper-layer tower plate, a lower-layer tower plate, a low-temperature plasma generator, a cyclone separator and a gas separator; the middle part of the tower body is provided with an upper layer tower plate, and the lower part of the tower body is provided with a lower layer tower plate; the upper space of the tower body separated by the upper tower plate is a chemical-looping hydrogen production reaction zone, the inner space of the tower body between the lower tower plate and the upper tower plate is a low-temperature plasma reaction zone, and an oxygen carrier is tiled on the upper tower plate; the upper part of the chemical looping hydrogen production reaction zone is provided with a dust-containing gas outlet, the lower part of the chemical looping hydrogen production reaction zone is provided with an oxygen carrier feeding hole and a solid particle returning hole, wherein the dust-containing gas outlet is connected with a dust-containing gas inlet of the cyclone separator, and the solid particle returning hole is connected with an outlet of a dust discharge pipe at the bottom of the cyclone separator; the top of the cyclone separator is provided with a mixed gas outlet and an externally discharged hydrogen outlet, wherein the mixed gas outlet is connected with a mixed gas inlet of the gas separator through a mixed gas pipeline, and the externally discharged hydrogen outlet is connected with an externally discharged hydrogen pipeline; a solid waste fuel inlet is arranged on one side of the upper part of the low-temperature plasma reaction zone, and a low-temperature plasma generator is arranged on the periphery of the low-temperature plasma reaction zone; the inner space of the tower body below the lower tower plate is an air inlet ash discharging chamber, one side of the air inlet ash discharging chamber is provided with a working gas inlet, and the bottom of the air inlet ash discharging chamber is provided with an ash discharging port; the working gas inlet is respectively connected with the air pipeline, the water vapor pipeline and the argon pipeline through a working gas pipeline, wherein the argon pipeline is connected with the argon outlet of the gas separator.

2. The double-tower plate chemical looping hydrogen production device for treating sludge biomass solid waste according to claim 1, wherein the low-temperature plasma generator is a plate-type dielectric barrier discharge reactor and consists of a dielectric I, a dielectric II, a high-voltage electrode, a grounding electrode and an alternating-current high-voltage generator; the medium I and the medium II are oppositely arranged on two sides of the tower body, the high-voltage electrode is arranged on the outer side of the medium I, the grounding electrode is arranged on the outer side of the medium II, and the high-voltage electrode and the grounding electrode are respectively connected with the alternating-current high-voltage generator; the first medium and the second medium are both made of quartz.

3. The double-tower plate chemical looping hydrogen production device for treating sludge biomass solid waste according to claim 1, characterized in that the upper-layer tower plate is a porous steel plate, and a plurality of wind caps are uniformly arranged on the upper-layer tower plate; the hood comprises cap head and spliced pipe, and the bottom of spliced pipe is pegged graft with the jack on the upper tower board, and the top of spliced pipe links to each other with the cap head, is equipped with the round exhaust vent along the hoop between spliced pipe and the cap head, and the air-out direction of exhaust vent is towards the outer below slope.

4. The double-tower-plate chemical-looping hydrogen production device for treating sludge biomass solid waste according to claim 1, characterized in that the lower tower plate is a porous steel plate; a divergent section is arranged between the low-temperature plasma reaction zone and the chemical-looping hydrogen production reaction zone, the cross section of the divergent section is gradually enlarged from bottom to top, and the inclination angle of the side wall of the tower body of the divergent section is 30-60 degrees; the bottom plate of the air inlet ash discharge chamber is obliquely arranged, and the working gas inlet and the ash discharge port are arranged at the lower end of the bottom plate.

5. The double-tower plate chemical looping hydrogen production device for treating sludge biomass solid waste according to claim 2, characterized in that a protective cover is arranged outside the plate type dielectric barrier discharge reactor, and the protective cover is made of polytetrafluoroethylene material.

6. The double-tower plate chemical looping hydrogen production device for treating sludge biomass solid waste according to claim 1, characterized in that an air valve is arranged on the air pipeline; the water vapor pipeline is connected with the water vapor generator and is provided with a water vapor valve; an argon gas cylinder and an argon gas valve are sequentially arranged on the argon gas pipeline along the flowing direction of argon gas; a mixed gas valve is arranged on the mixed gas pipeline; and a hydrogen valve is arranged on the hydrogen discharge pipeline.

7. The double-tower-plate chemical-looping hydrogen production method based on the device of any one of claims 1 to 6 is characterized by comprising three reaction stages, specifically as follows:

the first stage is a fuel reaction stage, and argon is used as working gas; in the stage, an argon valve and a low-temperature plasma generator are opened, argon is introduced into a low-temperature plasma reaction area to carry out pyrolytic oxidation reaction with solid waste fuel to generate CO and H₂And CH₄The synthesis gas and the unionized argon gas enter a chemical-looping hydrogen production reaction zone through an upper tower plate to perform reduction reaction with an oxygen carrier to generate CO₂And H₂O, enabling dust-containing gas carrying a small part of oxygen carrier particles to enter a cyclone separator, separating solid particles carried in the gas flow, sending the solid particles back to the chemical-looping hydrogen production reaction zone to participate in the reaction again; the purified mixed gas enters a gas separator to separate argon, and the residual gas is discharged into subsequent CO₂A capture system; the separated argon is used as working gas for cyclic utilization; closing an argon valve and a low-temperature plasma generator after the first-stage reaction is finished;

the second stage is a hydrogen production reaction stage, and water vapor is used as working gas; in the stage, a water vapor generator, a water vapor valve and a hydrogen valve are opened, and a mixed gas valve is closed; introducing steam into a chemical-looping hydrogen production reaction zone, fully contacting with the oxygen carrier reduced in the first stage for oxidation reaction, and allowing the produced hydrogen to enter a subsequent hydrogen collecting system through an externally discharged hydrogen pipeline; after the second stage reaction is finished, closing the water vapor generator, the water vapor valve and the hydrogen valve;

the third stage is an oxidation reaction stage, and air is used as working gas; opening an air valve at the stage, introducing air into a chemical-looping hydrogen production reaction zone, and fully contacting with the partially oxidized oxygen carrier to carry out oxidation reaction; after the reaction in the third stage is finished, closing the air valve;

the three stages are circularly repeated.

8. The method for producing hydrogen by the double-tower-plate chemical looping according to claim 7, wherein the particle size of the solid waste fuel is below 8 mm.

9. The method for producing hydrogen by using the double-tower plate chemical looping according to claim 7, wherein a lossless standard capacitor is connected in series with the grounding end of the plate-type dielectric barrier discharge reactor, the frequency is adjusted by using a CTP-2000K type low-temperature plasma experimental power supply, and the electrical parameters are acquired by a TBS 1052B Tak oscilloscope; the pressure regulating range of the low-temperature plasma experiment power supply is 0-220V, and the regulating range of the output frequency is 5-20 KHz.

Background

With the rapid development of urban construction in China and the stricter laws and regulations related to solid waste disposal, the search for a high-efficiency solid waste treatment mode and the recycling of energy in the solid waste treatment mode become the key research direction of solid waste disposal technology. Sludge is a by-product of water treatment, and the main treatment modes at present are sanitary landfill, agricultural composting and incineration. However, the side effects of these treatments include pollution of the land, accumulation of heavy metals such as N and P, and harmful polluting gases (e.g. containing SO)_x、NO_xAnd gases of dioxins, etc.). Annual sludge production in china is high and the economic cost of traditional treatment is usually high. Therefore, it is very important to find an economic and efficient treatment mode for the sludge. In addition, the waste produced by production and consumption of human beings in the process of utilizing biomass is waste biomass, such as wood chips, straws and the like. Waste biomass has the characteristics of large yield and heavy pollution. If the waste biomass can be reasonably utilized and the resource recovery is enhanced, the win-win result of environmental protection and energy problems can be achieved. The chemical looping hydrogen production technology is a novel hydrogen production technology developed on the basis of the chemical looping combustion technology, and the chemical looping technology is applied to treat sludge and waste biomass to reduce the emission of pollutants.

Chemical looping hydrogen production (CLHG) combines hydrogen production by a steam-iron method and chemical looping combustion, and has the advantages of low energy consumption, low pollutant emission and the like. The reaction principle is as follows: reaction of metal oxides with fuel instead of air to produce H₂O and CO₂(ii) a Then, the low-valence metal oxide can react with water vapor to prepare high-purity hydrogen; finally, the oxygen carrier reacts with air and is oxidized to an initial state. In the process, the fuel does not contact with air, and CO in the flue gas can be realized₂The internal separation of (2) and the preparation of high-purity hydrogen without an additional hydrogen purification process, so that the CLHG technology has a very wide development space. Because the ash content of the sludge is high (about 50 percent can be achieved), the sludge and active components in the oxygen carrier generally react to inactivate part of the oxygen carrier and reduce the use efficiency of the oxygen carrier, so that the ash content is highBecomes one of the potential factors limiting the development of the sludge chemical chain technology. The low-temperature plasma technology has the advantages of low energy consumption, high efficiency, no secondary pollution and the like, and has great potential in the aspect of treating solid waste. Due to the excellent characteristic of low temperature, no toxic substances such as dioxin and the like are generated in the gasification process, and the method is environment-friendly. Dielectric barrier discharge refers to a non-equilibrium gas discharge form after an insulating material is inserted between metal electrodes, the generated electrons have high density, can be performed under normal pressure, and has the advantages of uniform and stable discharge, easy operation, loose requirements on plasma generating conditions and the like.

Disclosure of Invention

The invention provides a double-tower-plate chemical-looping hydrogen production device and method for treating sludge biomass solid waste, which are based on the principles of reduction, harmlessness and recycling of sludge, biomass and other solid waste treatment processes, and are combined with a low-temperature plasma technology to carry out pyrolysis on solid waste fuel.

In order to achieve the purpose, the invention adopts the following technical scheme:

a double-tower-plate chemical-looping hydrogen production device for treating sludge biomass solid waste comprises a tower body, an upper-layer tower plate, a lower-layer tower plate, a low-temperature plasma generator, a cyclone separator and a gas separator; the middle part of the tower body is provided with an upper layer tower plate, and the lower part of the tower body is provided with a lower layer tower plate; the upper space of the tower body separated by the upper tower plate is a chemical-looping hydrogen production reaction zone, the inner space of the tower body between the lower tower plate and the upper tower plate is a low-temperature plasma reaction zone, and an oxygen carrier is tiled on the upper tower plate; the upper part of the chemical looping hydrogen production reaction zone is provided with a dust-containing gas outlet, the lower part of the chemical looping hydrogen production reaction zone is provided with an oxygen carrier feeding hole and a solid particle returning hole, wherein the dust-containing gas outlet is connected with a dust-containing gas inlet of the cyclone separator, and the solid particle returning hole is connected with an outlet of a dust discharge pipe at the bottom of the cyclone separator; the top of the cyclone separator is provided with a mixed gas outlet and an externally discharged hydrogen outlet, wherein the mixed gas outlet is connected with a mixed gas inlet of the gas separator through a mixed gas pipeline, and the externally discharged hydrogen outlet is connected with an externally discharged hydrogen pipeline; a solid waste fuel inlet is arranged on one side of the upper part of the low-temperature plasma reaction zone, and a low-temperature plasma generator is arranged on the periphery of the low-temperature plasma reaction zone; the inner space of the tower body below the lower tower plate is an air inlet ash discharging chamber, one side of the air inlet ash discharging chamber is provided with a working gas inlet, and the bottom of the air inlet ash discharging chamber is provided with an ash discharging port; the working gas inlet is respectively connected with the air pipeline, the water vapor pipeline and the argon pipeline through a working gas pipeline, wherein the argon pipeline is connected with the argon outlet of the gas separator.

The low-temperature plasma generator is a plate-type dielectric barrier discharge reactor and consists of a dielectric I, a dielectric II, a high-voltage electrode, a grounding electrode and an alternating-current high-voltage generator; the medium I and the medium II are oppositely arranged on two sides of the tower body, the high-voltage electrode is arranged on the outer side of the medium I, the grounding electrode is arranged on the outer side of the medium II, and the high-voltage electrode and the grounding electrode are respectively connected with the alternating-current high-voltage generator; the first medium and the second medium are both made of quartz.

The upper-layer tower plate is a porous steel plate, and a plurality of wind caps are uniformly arranged on the upper-layer tower plate; the hood comprises cap head and spliced pipe, and the bottom of spliced pipe is pegged graft with the jack on the upper tower board, and the top of spliced pipe links to each other with the cap head, is equipped with the round exhaust vent along the hoop between spliced pipe and the cap head, and the air-out direction of exhaust vent is towards the outer below slope.

The lower tower plate is a porous steel plate; a divergent section is arranged between the low-temperature plasma reaction zone and the chemical-looping hydrogen production reaction zone, the cross section of the divergent section is gradually enlarged from bottom to top, and the inclination angle of the side wall of the tower body of the divergent section is 30-60 degrees; the bottom plate of the air inlet ash discharge chamber is obliquely arranged, and the working gas inlet and the ash discharge port are arranged at the lower end of the bottom plate.

And a protective cover is arranged outside the plate-type dielectric barrier discharge reactor and is made of polytetrafluoroethylene materials.

An air valve is arranged on the air pipeline; the water vapor pipeline is connected with the water vapor generator and is provided with a water vapor valve; an argon gas cylinder and an argon gas valve are sequentially arranged on the argon gas pipeline along the flowing direction of argon gas; a mixed gas valve is arranged on the mixed gas pipeline; and a hydrogen valve is arranged on the hydrogen discharge pipeline.

A double-tower-plate chemical-looping hydrogen production method is divided into three reaction stages, and specifically comprises the following steps:

the first stage is a fuel reaction stage, and argon is used as working gas; in the stage, an argon valve and a low-temperature plasma generator are opened, argon is introduced into a low-temperature plasma reaction area to carry out pyrolytic oxidation reaction with solid waste fuel to generate CO and H₂And CH₄The synthesis gas and the unionized argon gas enter a chemical-looping hydrogen production reaction zone through an upper tower plate to perform reduction reaction with an oxygen carrier to generate CO₂And H₂O, enabling dust-containing gas carrying a small part of oxygen carrier particles to enter a cyclone separator, separating solid particles carried in the gas flow, sending the solid particles back to the chemical-looping hydrogen production reaction zone to participate in the reaction again; the purified mixed gas enters a gas separator to separate argon, and the residual gas is discharged into subsequent CO₂A capture system; the separated argon is used as working gas for cyclic utilization; closing an argon valve and a low-temperature plasma generator after the first-stage reaction is finished;

the second stage is a hydrogen production reaction stage, and water vapor is used as working gas; in the stage, a water vapor generator, a water vapor valve and a hydrogen valve are opened, and a mixed gas valve is closed; introducing steam into a chemical-looping hydrogen production reaction zone, fully contacting with the oxygen carrier reduced in the first stage for oxidation reaction, and allowing the produced hydrogen to enter a subsequent hydrogen collecting system through an externally discharged hydrogen pipeline; after the second stage reaction is finished, closing the water vapor generator, the water vapor valve and the hydrogen valve;

the third stage is an oxidation reaction stage, and air is used as working gas; opening an air valve at the stage, introducing air into a chemical-looping hydrogen production reaction zone, and fully contacting with the partially oxidized oxygen carrier to carry out oxidation reaction; after the reaction in the third stage is finished, closing the air valve;

the three stages are circularly repeated.

The particle size of the solid waste fuel is below 8 mm.

The grounding end of the plate-type dielectric barrier discharge reactor is connected with a lossless standard capacitor in series, the frequency is adjusted by adopting a CTP-2000K type low-temperature plasma experiment power supply, and the electrical parameters are collected by a TBS 1052B Take oscilloscope; the pressure regulating range of the low-temperature plasma experiment power supply is 0-220V, and the regulating range of the output frequency is 5-20 KHz.

Compared with the prior art, the invention has the beneficial effects that:

1) the method is characterized in that the tower body is divided into an upper chemical-looping hydrogen production reaction zone and a lower low-temperature plasma reaction zone by arranging double-layer tower plates in the same tower body, solid waste fuel and oxygen carrier react with the furnace, and the solid waste fuel and the oxygen carrier are not in direct contact with each other, so that ash in the solid waste fuel is prevented from polluting the oxygen carrier, and the reaction efficiency is improved;

2) the pyrolysis of the solid waste fuel is realized by combining a low-temperature plasma technology, and the formation and the emission of pollutants are reduced;

3) the reduction, harmlessness and reclamation of solid waste treatment processes such as sludge, biomass and the like are realized.

Drawings

FIG. 1 is a schematic structural diagram of a double-tower plate chemical-looping hydrogen production device for treating sludge biomass solid waste.

FIG. 2 is a schematic diagram of a plate-type dielectric barrier discharge reactor according to the present invention.

In the figure: 1. tower body 2, upper tower plate 3, lower tower plate 4, oxygen carrier 5, plate type dielectric barrier discharge reactor 51, medium I52, medium II 53, high voltage electrode 54, grounding electrode 55, alternating current high voltage generator 6, ash discharge port 7, working gas inlet 8, cyclone separator 9, gas separator 10, argon gas cylinder 11, water vapor generator 12, hood I, boiling section of low temperature plasma reaction

Detailed Description

The following further describes embodiments of the present invention with reference to the accompanying drawings:

as shown in figure 1, the double-tower-plate chemical-looping hydrogen production device for treating sludge biomass solid waste comprises a tower body 1, an upper-layer tower plate 2, a lower-layer tower plate 3, a low-temperature plasma generator, a cyclone separator 8 and a gas separator 9; the middle part of the tower body 1 is provided with an upper layer tower plate 2, and the lower part is provided with a lower layer tower plate 3; the upper space of the tower body 1 separated by the upper tower plate 2 is a chemical chain hydrogen production reaction zone, the inner space of the tower body 1 between the lower tower plate 3 and the upper tower plate 2 is a low-temperature plasma reaction zone, and an oxygen carrier 4 is tiled on the upper tower plate 2; the upper part of the chemical looping hydrogen production reaction zone is provided with a dust-containing gas outlet, the lower part of the chemical looping hydrogen production reaction zone is provided with an oxygen carrier feeding hole and a solid particle returning hole, wherein the dust-containing gas outlet is connected with a dust-containing gas inlet of the cyclone separator 8, and the solid particle returning hole is connected with an outlet of a dust discharge pipe at the bottom of the cyclone separator 8; the top of the cyclone separator 8 is provided with a mixed gas outlet and an externally discharged hydrogen outlet, wherein the mixed gas outlet is connected with a mixed gas inlet of the gas separator 9 through a mixed gas pipeline, and the externally discharged hydrogen outlet is connected with an externally discharged hydrogen pipeline; a solid waste fuel inlet is arranged on one side of the upper part of the low-temperature plasma reaction zone, and a low-temperature plasma generator is arranged on the periphery of the low-temperature plasma reaction zone; the inner space of the tower body 1 below the lower layer tower plate 3 is an air inlet ash discharging chamber, one side of the air inlet ash discharging chamber is provided with a working gas inlet 7, and the bottom of the air inlet ash discharging chamber is provided with an ash discharging port 6; the working gas inlet 7 is connected with an air pipeline, a water vapor pipeline and an argon pipeline through a working gas pipeline respectively, wherein the argon pipeline is connected with an argon outlet of the gas separator 9.

As shown in fig. 2, the low-temperature plasma generator is a plate-type dielectric barrier discharge reactor 5, and is composed of a first dielectric 51, a second dielectric 52, a high-voltage electrode 53, a ground electrode 54 and an alternating-current high-voltage generator 55; the medium I51 and the medium II 52 are oppositely arranged at two sides of the tower body 1, the high-voltage electrode 53 is arranged at the outer side of the medium I51, the grounding electrode 54 is arranged at the outer side of the medium II 52, and the high-voltage electrode 53 and the grounding electrode 54 are respectively connected with an alternating-current high-voltage generator 55; the first medium 51 and the second medium 52 are both made of quartz.

The upper tower plate 2 is a porous steel plate, and a plurality of air hoods are uniformly arranged on the upper tower plate; the hood comprises cap head and spliced pipe, and the bottom of spliced pipe is pegged graft with the jack on the upper tower board 2, and the top of spliced pipe links to each other with the cap head, is equipped with the round exhaust vent along the hoop between spliced pipe and the cap head, and the air-out direction of exhaust vent is towards the outer below slope.

The lower tower plate 3 is a porous steel plate; a divergent section is arranged between the low-temperature plasma reaction zone and the chemical chain hydrogen production reaction zone, the cross section of the divergent section is gradually enlarged from bottom to top, and the inclination angle of the side wall of the tower body 1 of the divergent section is 30-60 degrees; the bottom plate of the air inlet ash discharge chamber is obliquely arranged, and the working gas inlet 7 and the ash discharge port 6 are arranged at the lower end of the bottom plate.

And a protective cover is arranged outside the plate-type dielectric barrier discharge reactor 5 and is made of polytetrafluoroethylene materials.

An air valve is arranged on the air pipeline; the water vapor pipeline is connected with the water vapor generator 11, and a water vapor valve is arranged on the water vapor pipeline; an argon gas cylinder 10 and an argon gas valve are sequentially arranged on the argon gas pipeline along the flowing direction of argon gas; a mixed gas valve is arranged on the mixed gas pipeline; and a hydrogen valve is arranged on the hydrogen discharge pipeline.

A double-tower plate chemical chain hydrogen production method is divided into three reaction stages, specifically the following steps;

the first stage is a fuel reaction stage, and argon is used as working gas; in the stage, an argon valve and a low-temperature plasma generator are opened, argon is introduced into a low-temperature plasma reaction area to carry out pyrolytic oxidation reaction with solid waste fuel to generate CO and H₂And CH₄The synthesis gas in the reaction zone enters the chemical-looping hydrogen production reaction zone through the upper tower plate 2 together with the non-ionized argon gas to perform reduction reaction with the oxygen carrier to generate CO₂And H₂O, the dust-containing gas carrying a small part of oxygen carrier particles enters a cyclone separator 8, and solid particles carried in the gas flow are separated and sent back to the chemical chain hydrogen production reaction zone to participate in the reaction again; the purified mixed gas enters a gas separator 9 to separate argon, and the rest gas is discharged into subsequent CO₂A capture system; the separated argon is used as working gas for cyclic utilization; closing an argon valve and a low-temperature plasma generator after the first-stage reaction is finished;

the second stage is a hydrogen production reaction stage, and water vapor is used as working gas; in the stage, the water vapor generator 11, the water vapor valve and the hydrogen valve are opened, and the mixed gas valve is closed; introducing steam into a chemical-looping hydrogen production reaction zone, fully contacting with the oxygen carrier reduced in the first stage for oxidation reaction, and allowing the produced hydrogen to enter a subsequent hydrogen collecting system through an externally discharged hydrogen pipeline; after the second stage reaction is finished, closing the water vapor generator 11, the water vapor valve and the hydrogen valve;

the third stage is an oxidation reaction stage, and air is used as working gas; opening an air valve at the stage, introducing air into a chemical-looping hydrogen production reaction zone, and fully contacting with the partially oxidized oxygen carrier to carry out oxidation reaction; after the reaction in the third stage is finished, closing the air valve;

the three stages are circularly repeated.

The particle size of the solid waste fuel is below 8 mm.

The grounding end of the plate-type dielectric barrier discharge reactor 5 is connected with a lossless standard capacitor in series, the frequency is adjusted by adopting a CTP-2000K type low-temperature plasma experiment power supply, and the electrical parameters are collected by a TBS 1052B Tak oscilloscope; the pressure regulating range of the low-temperature plasma experiment power supply is 0-220V, and the regulating range of the output frequency is 5-20 KHz.

The following examples are carried out on the premise of the technical scheme of the invention, and detailed embodiments and specific operation processes are given, but the scope of the invention is not limited to the following examples.

[ examples ] A method for producing a compound

In this embodiment, the double-tower-plate chemical-looping hydrogen production device for treating sludge biomass solid waste comprises a tower body, a lower-layer tower plate, an upper-layer tower plate, a plate-type dielectric barrier discharge reactor, a cyclone separator, a gas separator, a water vapor generator and an argon gas cylinder. The gas supply system for supplying working gas into the tower body is divided into three paths, namely an argon gas path, an air path and a water vapor path, and the three gas paths are respectively provided with a switch valve for control; the exhaust gas of the cyclone separator is divided into two paths, the exhaust gas in the fuel reaction stage flows to the gas separator after passing through the cyclone separator, and the separated argon gas and the residual gas are respectively discharged; the exhaust gas of the hydrogen production reaction stage and the oxidation reaction stage is directly discharged after passing through a cyclone separator.

The tower body is divided into an upper reaction zone and a lower reaction zone by double layers of tower plates, namely an upper layer of tower plate and a lower layer of tower plate, the upper layer of tower plate is loaded with an oxygen carrier, and the upper space of the tower body is used as a chemical-looping hydrogen production reaction zone for carrying out chemical-looping hydrogen production circulation reaction. The lower layer space is provided with a plate type dielectric barrier discharge reactor as a low-temperature plasma reaction area. A transition section with variable cross section is arranged between the two reaction zones, the side wall of the tower body of the transition section is of an inclined structure expanding outwards and upwards, and the inclination angle is 45 degrees.

The lower tower plate is a porous flat plate made of steel plates, and the upper tower plate is a porous flat plate with a hood structure. The solid waste fuel is fed in a positive pressure feeding mode, working gas is introduced into the tower body through the lower tower plate, and reaction gas in the low-temperature plasma reaction zone moves upwards along with the gas flow and enters the chemical-looping hydrogen production reaction zone through the blast cap on the upper tower plate.

In this embodiment, the tower body is of a full-boiling furnace type with a fixed air distribution form. The working gas uniformly enters the low-temperature plasma reaction zone through the holes on the lower tower plate (the lower tower plate is equivalent to an air distribution plate) through the air inlet ash discharge chamber and flows from bottom to top. The air inlet and ash discharge chamber adopts an isobaric air chamber structure with an inclined bottom surface, so that the uniform distribution of air quantity is improved, and meanwhile, the collection and discharge of ash are facilitated.

The solid waste fuel with the particle size of less than 8mm is sent into the tower body from the solid waste fuel inlet and flows downwards. The feeding mode of the solid waste fuel is positive pressure feeding so as to improve the burnout rate of the solid waste fuel. The transition section is arranged between the boiling section I of the low-temperature plasma reaction and the upper layer tower plate, the section of the tower body of the transition section is in a cone shape, the area of the cross section of the transition section is enlarged from bottom to top, and the purpose of the transition section is to reduce the air velocity, so that the retention time of solid waste fuel particles in a low-temperature plasma reaction area can be prolonged, the gasification quality is ensured, and meanwhile, the effective separation of fly ash in the tower body can be enhanced.

The upper tower plate is a porous flat plate made of steel plates, and a wind cap is arranged on the upper tower plate to achieve the purpose of uniform wind distribution. The shape and size of the upper layer tower plate are adapted to the shape and size of the inner section of the corresponding part of the tower body, and the thickness is 30 mm. In this embodiment, the upper end of the blast cap is sealed by the cap head, and the opening of the insertion tube at the lower end is open and is vertically inserted into the insertion hole on the upper tower plate. The joint of the hood head and the splicing pipe is provided with a circle of air outlet holes which are slightly inclined downwards. The synthetic gas generated by the pyrolysis and gasification of the fuel flows in through the lower end opening of the blast cap plug-in pipe and is sprayed out from the air outlet hole in all directions at high speed. This high velocity gas stream with high dispersion and strong turbulence can be uniformly and sufficiently contacted with the oxygen carrier placed on the upper tray to perform the chemical chain reaction.

The dusty gas outlet at the upper part of the tower body is connected with an externally arranged cyclone separator to separate solid particles carried in the dusty gas, and the solid particles are sent back to the upper-layer tower plate through the material returning device to react again. And the mixed gas after the solid particles are separated by the cyclone separator enters a gas separator for further separation, and the separated argon is sent to an argon gas cylinder for storage and finally returned to the tower body as working gas.

In this embodiment, three gas supply systems are provided as working gases in three reaction stages, respectively, according to the entire reaction process.

The first stage is a fuel reaction stage, argon gas is used as working gas and enters a low-temperature plasma reaction zone from an air inlet ash discharge chamber through a lower tower plate, an ion atmosphere is generated under the action of low-temperature plasma, solid waste fuel is subjected to pyrolysis oxidation, and generated CO and H₂And CH₄The synthesis gas and the non-ionized argon gas enter a chemical-looping hydrogen production reaction zone through a blast cap on an upper tower plate together to perform reduction reaction with an oxygen carrier to generate CO₂And H₂O, then the mixed gas carries a small fraction of the oxygen carrier particles into the cyclone. The clean gas outlet at the top of the cyclone separator is provided with two channels which are respectively controlled by a mixed gas valve and a hydrogen valve. In the first stage, a mixed gas valve connected with a gas separator is opened, the mixed gas is separated from argon gas by the gas separator, and the rest gas is discharged into subsequent CO₂A capture system. The separated argon is re-sent into the tower body through an argon passage for reaction. The time for the fuel reaction phase was 1 hour.

The second stage is a hydrogen production reaction stage, after the fuel reaction stage is finished, an argon valve on an argon passage and a plate type dielectric barrier discharge reactor are closed, a steam generating device and a steam valve on a steam passage are opened, the steam enters an upper chemical chain hydrogen production reaction zone after passing through a lower tower plate and an upper tower plate, and is fully contacted with the oxygen carrier reduced in the first stage for oxidation reaction, and hydrogen is produced. At the moment, the mixing gas valve connected with the gas separator is closed, the hydrogen valve on the other path of hydrogen discharge pipeline is opened, and hydrogen is directly discharged into a subsequent hydrogen collecting system. The time for the hydrogen production reaction stage was 30 minutes.

And the third stage is an oxidation reaction stage, after the hydrogen production reaction stage is finished, a steam valve on a steam pipeline is closed, an air valve on an air pipeline is opened, and air enters an upper chemical chain hydrogen production reaction zone after passing through a lower tower plate and an upper tower plate and is fully contacted with the partially oxidized oxygen carrier to carry out oxidation reaction. The operation temperature of the chemical chain hydrogen production reaction zone is controlled to be about 900 ℃, and the reaction time is 30 minutes. The metal oxide oxygen carrier reacts with oxygen in the air to obtain metal oxide in a complete oxidation state, and reaction heat is generated to enable the oxygen carrier to have higher temperature. The reacted gas carries solid particles into a cyclone separator, the purified mixed gas is discharged into the gas separator, and the solid particles return to an oxygen carrier layer in the tower body. After the reaction at the stage is finished, the air valve is closed, the argon valve is opened, the fuel reaction stage is started again, and the process is circulated and repeated.

In this embodiment, the low-temperature plasma generator is a plate-type dielectric barrier discharge reactor (DBD) which is composed of a high-voltage electrode, a ground electrode, an ac high-voltage generator, a first dielectric, and a second dielectric. The DBD selects a quartz material double-layer medium structure, namely a medium I and a medium II are both made of quartz materials, and discharge occurs between the medium I and the medium II, so that the electrode can be well protected, and ash residues of discharge plasma and solid waste fuel are prevented from contacting the electrode. Meanwhile, the structure is beneficial to the deposition and diffusion of charges. The grounding end of the DBD is connected with a lossless standard capacitor in series, the frequency is adjusted by adopting a CTP-2000K type low-temperature plasma experiment power supply, and the electrical parameters are acquired by a TBS 1052B Take oscilloscope. The pressure regulation range of the low-temperature plasma experiment power supply is 0-220V, and the regulation range of the output frequencyThe enclosure is 5-20 KHz. By storing oscilloscopes CH under different atmospheres and different frequency conditions₁、CH₂And (5) obtaining the Lissajous area data through channel data, and further calculating the discharge power and the energy density. A polytetrafluoroethylene protective cover is arranged outside the DBD reactor, so that the influence of surrounding environment factors on the electrodes in the reaction process is prevented.

The power calculation in the reaction process of the plate-type dielectric barrier discharge reactor is calculated according to the following method:

firstly, through Lissajous method calculation, probes of the oscilloscope are respectively connected to a high-voltage output voltage detection interface and a high-voltage output current detection interface, and the oscilloscope can record curves of instantaneous voltage and current. Measuring the sampling capacitance (C) during discharge_m) The process of discharging can be expressed as:

in the formula: i is the current, Q is the charge delivered during discharge, C is the measurement sampling capacitor during discharge, and U is the voltage applied to the capacitor.

And drawing a Lissajous diagram by using Origin software according to data recorded by an oscilloscope to obtain an approximate parallelogram, wherein the diagram contains data of 2.5 periods, and the discharge power input into the reactor in a discharge period can be obtained by calculating the area of the diagram. In the lissajous diagram, the product of the area (a) of the closed curve and the discharge frequency is the discharge frequency of the plate-type dielectric barrier discharge reactor. The calculation formula is as follows:

P＝f×C_m×A

in the above formula, P is the discharge power of the plate-type dielectric barrier discharge reactor, f is the AC power frequency, C_mIs the sampling capacitance (0.47. mu.F), and A is the Lissajous area of the graph. To prevent inaccurate power calculation, the average value needs to be calculated three times.

The Energy Density (SED) of the input plasma can be calculated from the discharge power P, and the calculation formula is as follows:

in the above formula, V is the gas flow rate through the plate-type dielectric barrier discharge reactor.

In the present example, 2 kinds of solid waste treatment were performed, and the oxygen carrier component in example 1 was CuO-Fe₂O₃The solid waste fuel is sludge/corncobs; the hydrogen production purity is 94 percent, the cycle experiment times are 20 times, and no obvious sintering phenomenon is found. Example 2 the oxygen carrier component was CuFe₂O₄/MgAl₂O₄The solid waste fuel is sludge/biomass semicoke, the hydrogen production purity is 97%, the cycle experiment times are 30 times, and no obvious sintering phenomenon is seen.