CN102351144A - Method and equipment for preparing hydrogen-rich gas through plasma/chemical catalytic composite reforming - Google Patents
Method and equipment for preparing hydrogen-rich gas through plasma/chemical catalytic composite reforming Download PDFInfo
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- CN102351144A CN102351144A CN2011101744922A CN201110174492A CN102351144A CN 102351144 A CN102351144 A CN 102351144A CN 2011101744922 A CN2011101744922 A CN 2011101744922A CN 201110174492 A CN201110174492 A CN 201110174492A CN 102351144 A CN102351144 A CN 102351144A
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Abstract
The invention discloses a method and equipment for preparing hydrogen-rich gas through plasma/chemical catalytic composite reforming. The method is as follows: droplets of a hydrocarbon fuel are introduced into an annular plasma discharge zone constructed by a tubular inner electrode and a tubular external electrode and are subjected to a plasma reforming reaction based on free radicals so as to produce considerable active particles and micromolecular mixtures; resultants of the plasma reforming reaction are introduced into a chemical catalytic reaction bed layer filled in the cavity of the tubular inner electrode, more and smaller micromolecular mixtures are produced through a catalytic reaction, and therefore, high concentration hydrogen-rich gas can be obtained. The equipment mainly comprises the tubular inner electrode, the tubular external electrode and the chemical catalytic reaction bed layer filled in the cavity of the tubular inner electrode. The equipment in the invention has the advantages of a compact structure, a small volume and low cost. The method in the invention has the advantages of a fast reaction speed, slim possibility of toxicosis resulting from a catalyst, high overall reforming efficiency and a high utilization rate of energy.
Description
Technical field
The present invention relates to the hydrocarbon fuel reforming technology, refer to that particularly the compound reformation of a kind of plasma body and chemical catalysis prepares the method and apparatus of hydrogen-rich combustion gas.
Background technology
At present, the method for utilizing hydrocarbon fuel to produce hydrogen-rich combustion gas mainly contains chemical catalysis and reforming plasma method.The chemical catalysis reformation hydrogen production is under the effect of catalyzer, becomes hydrogen after making the hydrocarbon fuel after chemical reaction, and it includes steam reforming, partial oxidation is reformed and self-heating recapitalization.
Steam reforming method comparative maturity, the hydrogen content of producing is high, is present the most frequently used a kind of reformation hydrogen production mode.Adopt this method, fuel is mixed the back get into reformer with water vapour, reforming reaction takes place under the effect of high temperature and catalyzer produce hydrogen.But this reaction is thermo-negative reaction, and institute's heat requirement is by the part of fuel generation of externally burning, the carrying out that needs outside heat supply just can keep reforming reaction; In total system, the fuel of participating in combustion reactions accounts for 25% of total fuel greatly, and capacity usage ratio is lower; The time of response of chemical catalysis reforming reaction while is long, and catalyzer is poisoned easily.
Partial oxidation is reformed and is utilized fuel under oxygen situation, redox reaction to take place, and produces carbon monoxide and hydrogen.This reaction is thermopositive reaction, thereby does not need external thermal source to supply with.But this method need lose efficacy to avoid poisoning of catalyst before reaction in sulphur removal; And the reaction mechanism that partial oxidation is reformed is very complicated, and by product is many, and the hydrogen purity of generation is low, product hydrogen rate is low.
Self-heating recapitalization is the partial oxidation of the steam reforming of heat absorption and heat release to be reformed combine, and realizes the self-equilibrating of heat under certain condition.Though this method can make the efficient of system improve, self-heating recapitalization requires the ratio between oxygen, water vapour and the fuel that regulates simultaneously, and control ratio is difficulty, and in reformation, is prone to produce the carbon distribution phenomenon and damages catalyzer.
Reforming plasma hydrogen manufacturing is a kind of advanced person's hydrogen producing technology, and its adopts the generation of excitation of plasma reforming reaction, and the high-energy electron in the plasma body acts on hydrocarbon molecules, wherein hydrocarbon chain is interrupted forming little molecule, like hydrogen etc.Because isoionic energy density is very high, make this mode have characteristics such as starting is fast, dynamic response is quick, reformer is simple and compact for structure.But the employed high-frequency and high-voltage power supply of reformer can produce great amount of heat and expended energy on electrode, and capacity usage ratio is not high.
Summary of the invention
The objective of the invention is to overcome the existing in prior technology deficiency, provide a kind of speed of response is fast, reformation efficient high, capacity usage ratio is high plasma body cooperative catalysis complex reaction to prepare the method and apparatus of hydrogen-rich combustion gas.
For realizing above-mentioned purpose, the compound reformation of plasma body that the present invention designed and chemical catalysis prepares the method for hydrogen-rich combustion gas, comprises the steps:
1) will pass through hydrocarbon fuel droplet that atomizing handles imports in the toroidal plasma region of discharge that electrode and tubular outer electrode are constituted in the tubular of coaxial arrangement; Make the hydrocarbon fuel droplet that the reforming plasma reaction based on free radical take place under the effect of impact of high-energy electron; Wherein most macromole hydrocarbon chain material is interrupted and is activated, and produces a large amount of active particle and small-molecule mixture;
2) active particle that produced and small-molecule mixture are directly imported together with a small amount of unreacted macromole hydrocarbon chain material be filled in the tubular in the chemical catalysis reaction bed in the electrode cavity again; Make them rapid catalyzed reaction take place on the surface of chemical catalyst; Produce more and littler small-molecule mixture, the heat that electrode produces in the while tubular can be the chemical catalysis reaction bed and adds thermal utilization;
3) at last the small-molecule mixture that is produced is derived, can obtain the hydrogen-rich combustion gas of high density.
Particularly, said hydrocarbon fuel is aqueous ethanol, methane, methyl alcohol or petroleum naphtha.
Further, the voltage that applies of said toroidal plasma region of discharge is that 5～20KV, frequency are that 7～15KHz, electrode discharge spacing are 0.5～4mm.
Further, said chemical catalyst is nickel-base catalyst or copper-based catalysts, and the temperature of said chemical catalysis reaction is 320～400 ℃.
For realizing that custom-designed plasma of said method and the compound reformation of chemical catalysis prepare the equipment of hydrogen-rich combustion gas; The interior electrode of tubular and the tubular external electrode that comprise coaxial arrangement; Form the toroidal plasma region of discharge in the said tubular between electrode and the tubular external electrode; One end of said toroidal plasma region of discharge is the region of discharge import; The other end of said toroidal plasma region of discharge is the region of discharge outlet; Be filled with the chemical catalysis reaction bed in the cavity of electrode in the said tubular; The reaction bed import of said chemical catalysis reaction bed is positioned at the same side with the outlet of the region of discharge of toroidal plasma region of discharge and is connected, and the reaction bed outlet of said chemical catalysis reaction bed is positioned at the same side also separately with the region of discharge inlet of toroidal plasma region of discharge.
As preferred version, be provided with tubular block media layer between electrode and the tubular outer electrode in the said tubular, said tubular outer electrode is sleeved on the tubular block media layer.
Particularly, said tubular block media layer is the alumina-ceramic or the quartz of high insulating material, and its resistivity is greater than 10
14Ω/cm, dielectric constant values>=9, thickness are 0.4～1.0mm, and critical breakdown electric field intensity>=400KV/cm, water-intake rate are 0.0%.
Further, a side of electrode and tubular outer electrode is provided with end cover in the said tubular.Like this, it is simple and practical, through end cover stop with guide functions under, the reaction bed import that can make said chemical catalysis reaction bed is connected in the shortest distance with the outlet of the region of discharge of toroidal plasma region of discharge.
Further, be provided with well heater in the said chemical catalysis reaction bed.Like this, during shortage of heat in interior electrode offers the chemical catalysis reaction bed, can pass through the well heater heat supply.
Again further, be provided with temperature sensor in the said chemical catalysis reaction bed.Like this, can monitor the temperature in the chemical catalysis reaction bed, and in time temperature of reaction regulated in view of the above, make heat energy utilization reach best.
The preparation method that the present invention designed is that the hydrocarbon fuel atomizing is imported in the toroidal plasma region of discharge, makes the hydrocarbon fuel molecule receive the impact of high-energy electron, and wherein the chemical bond that is contained ruptures, and forms H, OH, CH
3, C
2H
5, CH
2OH, CH
3CHOH, CH
2CH
2The free radical that OH etc. are bigger after these free radicals receive further impact, fragments into littler free radical.Hydrocarbon fuel droplet through after the Cement Composite Treated by Plasma directly enters into the chemical catalysis reaction bed; Wherein a large amount of active particles also together enters into the chemical catalysis reaction bed; Contain a large amount of active particles owing to enter into the material of chemical catalysis reaction bed; The heat of electrode can be heated for the catalytic bed layer simultaneously; Thereby can lower the energy consumption of catalyzed reaction, the efficient of raising catalyzed reaction, and then improve compound reformation efficient and capacity usage ratio.
The compound reformer apparatus that the present invention designed; The region of discharge outlet of its toroidal plasma region of discharge directly links to each other with the reaction bed import that with interior electrode is the chemical catalysis reaction bed of outer cover, makes through the product after the Cement Composite Treated by Plasma and enters into the chemical catalysis reaction bed at once; Through containing a large amount of active particles in the fuel after the Cement Composite Treated by Plasma; After these active particles together enter into the chemical catalysis reaction bed along with the hydrogen-rich gas that generates; Can reduce the activation temperature of catalytic reforming; Improve the reaction efficiency of catalytic reforming; The high temperature that produces because of high-frequency current on the electrode simultaneously; Can become the thermal source of catalyzed reaction, heat, overall reformation efficient and capacity usage ratio are improved for catalyzed reaction.
The invention has the advantages that: designed method combines reforming plasma method and chemical catalysis reforming process produces hydrogen-rich combustion gas; Overcome the defective of available technology adopting single method; Not only speed of response is fast, catalyzer is not easy to poison, and reformation efficient and capacity usage ratio can obviously improve.Simultaneously, the simple and compact equipment structure, the lightweight and portable in volume that are designed are small and exquisite, and be cheap for manufacturing cost.
Description of drawings
Fig. 1 prepares the sectional structure synoptic diagram of the equipment of hydrogen-rich combustion gas for a kind of plasma body and the compound reformation of chemical catalysis.
Fig. 2 is the A-A sectional structure synoptic diagram among Fig. 1.
Embodiment
Below in conjunction with accompanying drawing and specific embodiment the present invention is described in further detail.
The compound reformation of plasma body shown in the figure and chemical catalysis prepares the equipment of hydrogen-rich combustion gas, comprises the interior electrode 2 of tubular and tubular outer electrode 1 of coaxial arrangement, is provided with tubular block media layer 3 between electrode 2 and the tubular outer electrode 1 in the tubular.Alumina-ceramic or quartz that tubular block media layer 3 adopts high insulating material, its resistivity is greater than 10
14Ω/cm, dielectric constant values>=9, thickness are 0.4～1.0mm, and critical breakdown electric field intensity>=400KV/cm, water-intake rate are 0.0%.Tubular outer electrode 1 is sleeved on the tubular block media layer 3, in tubular, forms the toroidal plasma region of discharge 4 of dielectric impedance structure thus between electrode 2 and the tubular outer electrode 1.One end of toroidal plasma region of discharge 4 is region of discharge import 8, and the other end of toroidal plasma region of discharge 4 is region of discharge outlet 10.
A side of electrode 2 and tubular outer electrode 1 is provided with end cover 6 in tubular, and end cover 6 is fixed on the extended tubular block media of this side layer 3 end.In tubular, be filled with chemical catalysis reaction bed 5 in the cavity of electrode 2; The reaction bed import 11 of chemical catalysis reaction bed 5 is positioned at the same side with the region of discharge of toroidal plasma region of discharge 4 outlet 10, and end cover 6 stop with guide functions under be connected.9 region of discharge inlets 8 with toroidal plasma region of discharge 4 of the reaction bed outlet of chemical catalysis reaction bed 5 are positioned at the same side also separately.In chemical catalysis reaction bed 5, also be provided with well heater 7 and temperature sensor 12.Well heater 7 adopts electrothermal tube, and the one of which end is fixed on the end cover 6.12 of temperature sensors pass through signal wire and link to each other with extraneous pilot circuit, in order to regulate the temperature of reaction of chemical catalysis reaction bed 5.
It is following that the compound reformation of above-mentioned plasma body and chemical catalysis prepares the concrete design variable of equipment of hydrogen-rich combustion gas:
Embodiment 1:
Be that 122mm, thickness are that the high insulating alumina-ceramic of 0.5mm is a tubular block media layer 3 with the internal diameter, tubular outer electrode 1 is sleeved on the external diameter of tubular block media layer 3.Electrode 2 external diameters are that 120mm, length are 300mm in the tubular, and the electrode discharge spacing in the tubular between electrode 2 and the tubular block media layer 3 is 1mm, and discharge length is 280mm.The high-frequency high-voltage of loading frequency 10KHz, voltage 15KV between internal and external electrode.Be filled with chemical catalysis reaction bed 5 in the cavity of electrode 2 in the tubular, used chemical catalyst is a nickel-base catalyst.The electric heating tubular heater 7 and temperature sensor 12 of diameter 12mm are installed in the chemical catalysis reaction bed 5, and there is metal guard stagnant catalyst at two ends, form the catalytic reaction chamber that diameter is 100mm.
Embodiment 2:
Be that 123mm, thickness are that the quartz of 0.8mm is a tubular block media layer 3 with the internal diameter, tubular outer electrode 1 is sleeved on the external diameter of tubular block media layer 3.In the tubular external diameter of electrode 2 be 120mm,, length is 300mm, the electrode discharge spacing in the tubular between electrode 2 and the tubular block media layer 3 is 1.5mm, discharge length is 280mm.The high-frequency high-voltage of loading frequency 15KHz, voltage 15KV between internal and external electrode.Be filled with chemical catalysis reaction bed 5 in the cavity of electrode 2 in the tubular, used chemical catalyst is a copper-based catalysts.Be provided with the electric heating tubular heater 7 and temperature sensor 12 of diameter 12mm in the chemical catalysis reaction bed 5, there is metal guard stagnant catalyst at two ends, form the catalytic reaction chamber that diameter is 100mm.
When adopting above-mentioned compound reformer apparatus to prepare hydrogen-rich combustion gas:
1) will pass through hydrocarbon fuel droplet that atomizing handles imports in the toroidal plasma region of discharge 4 that electrode 2 and tubular outer electrode 1 are constituted in the tubular of coaxial arrangement; Make the hydrocarbon fuel droplet that the reforming plasma reaction based on free radical take place under the effect of impact of high-energy electron; Wherein most macromole hydrocarbon chain material is interrupted and is activated, and produces a large amount of active particle and small-molecule mixture;
2) active particle that produced and small-molecule mixture are directly imported together with a small amount of unreacted macromole hydrocarbon chain material be filled in the tubular in the chemical catalysis reaction bed 5 in electrode 2 cavitys again; Make them rapid catalyzed reaction take place on the surface of chemical catalyst; Produce more and littler small-molecule mixture, the heat that electrode 2 produces in the while tubular can be chemical catalysis reaction bed 5 and adds thermal utilization;
3) at last the small-molecule mixture that is produced is derived, can obtain the hydrogen-rich combustion gas of high density.
Comparative Examples
With plasma body of the present invention and the compound reformation of chemical catalysis prepares the method for hydrogen-rich combustion gas and traditional chemical catalysis and reforming plasma method compares, the result is as shown in table 1.
Table 1: the comparison of three kinds of methods
| Method | Temperature of reaction (℃) | Energy efficiency % | Reformation efficient % |
| Traditional plasma is reformed | Normal temperature | 35 | 45 |
| The traditional chemical catalytic reforming | 450～550 | 42 | 50 |
| Compound reformation of the present invention | 320～400 | 56 | 75 |
By finding out in the table 1: the temperature of reaction of compound reforming process of the present invention is than low 100～150 ℃ of single chemical catalysis reforming process, and energy efficiency and reformation efficient are all high than single chemical catalysis reforming process and reforming plasma method.Therefore, the collaborative compound reformation of chemical catalysis of the using plasma of the present invention method for preparing hydrogen-rich fuel has the speed of response high characteristics of efficient and capacity usage ratio of soon, totally reforming.
Claims (10)
1. plasma body and the compound reformation of chemical catalysis prepare the method for hydrogen-rich combustion gas, comprise the steps:
1) will pass through hydrocarbon fuel droplet that atomizing handles imports in the toroidal plasma region of discharge that electrode and tubular outer electrode are constituted in the tubular of coaxial arrangement; Make the hydrocarbon fuel droplet that the reforming plasma reaction based on free radical take place under the effect of impact of high-energy electron; Wherein most macromole hydrocarbon chain material is interrupted and is activated, and produces a large amount of active particle and small-molecule mixture;
2) active particle that produced and small-molecule mixture are directly imported together with a small amount of unreacted macromole hydrocarbon chain material be filled in the tubular in the chemical catalysis reaction bed in the electrode cavity again; Make them rapid catalyzed reaction take place on the surface of chemical catalyst; Produce more and littler small-molecule mixture, the heat that electrode produces in the while tubular can be the chemical catalysis reaction bed and adds thermal utilization;
3) at last the small-molecule mixture that is produced is derived, can obtain the hydrogen-rich combustion gas of high density.
2. plasma body according to claim 1 and the compound reformation of chemical catalysis prepare the method for hydrogen-rich combustion gas, it is characterized in that: said hydrocarbon fuel is aqueous ethanol, methane, methyl alcohol or petroleum naphtha.
3. plasma body according to claim 1 and 2 and the compound reformation of chemical catalysis prepare the method for hydrogen-rich combustion gas, it is characterized in that: the voltage that applies of said toroidal plasma region of discharge is that 5～20KV, frequency are that 7～15KHz, electrode discharge spacing are 0.5～4mm.
4. plasma body according to claim 1 and 2 and the compound reformation of chemical catalysis prepare the method for hydrogen-rich combustion gas, it is characterized in that: said chemical catalyst is nickel-base catalyst or copper-based catalysts, and the temperature of said chemical catalysis reaction is 320～400 ℃.
5. plasma and the compound reformation of chemical catalysis prepare the equipment of hydrogen-rich combustion gas; The interior electrode (2) of tubular and the tubular external electrode (1) that comprise coaxial arrangement; Form toroidal plasma region of discharge (4) in the said tubular between electrode (2) and the tubular external electrode (1); One end of said toroidal plasma region of discharge (4) is region of discharge import (8); The other end of said toroidal plasma region of discharge (4) is region of discharge outlet (10); It is characterized in that: be filled with chemical catalysis reaction bed (5) in the cavity of electrode (2) in the said tubular; The reaction bed import (11) of said chemical catalysis reaction bed (5) is positioned at the same side with the region of discharge of toroidal plasma region of discharge (4) outlet (10) and is connected, and the reaction bed outlet (9) of said chemical catalysis reaction bed (5) is positioned at the same side also separately with the region of discharge inlet (8) of toroidal plasma region of discharge (4).
6. plasma body according to claim 5 and the compound reformation of chemical catalysis prepare the equipment of hydrogen-rich combustion gas; It is characterized in that: be provided with tubular block media layer (3) between electrode (2) and the tubular outer electrode (1) in the said tubular, said tubular outer electrode (1) is sleeved on the tubular block media layer (3).
7. plasma body according to claim 6 and the compound reformation of chemical catalysis prepare the equipment of hydrogen-rich combustion gas, it is characterized in that: said tubular block media layer (3) is the alumina-ceramic of high insulating material or quartz, and its resistivity is greater than 10
14Ω/cm, dielectric constant values>=9, thickness are 0.4～1.0mm, and critical breakdown electric field intensity 400KV/cm, water-intake rate are 0.0%.
8. the equipment for preparing hydrogen-rich combustion gas according to claim 5 or 6 or 7 described plasma bodys and the compound reformation of chemical catalysis; It is characterized in that: a side of electrode (2) and tubular outer electrode (1) is provided with end cover (6) in the said tubular, the reaction bed import (11) of said chemical catalysis reaction bed (5) and the region of discharge of toroidal plasma region of discharge (4) export (10) end cover (6) stop with guide functions under be connected.
9. prepare the equipment of hydrogen-rich combustion gas according to claim 5 or 6 or 7 described plasma bodys and the compound reformation of chemical catalysis, it is characterized in that: be provided with well heater (7) in the said chemical catalysis reaction bed (5).
10. prepare the equipment of hydrogen-rich combustion gas according to claim 5 or 6 or 7 described plasma bodys and the compound reformation of chemical catalysis, it is characterized in that: be provided with temperature sensor (12) in the said chemical catalysis reaction bed (5).
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| CN105056858A (en) * | 2015-07-20 | 2015-11-18 | 浙江工商大学 | Reactor and method for preparing synthesis gases through reforming greenhouse gases |
| CN106006553A (en) * | 2016-05-09 | 2016-10-12 | 大连理工大学 | Online hydrogen production method and equipment with methanol oxidation and steam reforming segmental combined |
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| CN103216336B (en) * | 2013-03-22 | 2015-06-24 | 哈尔滨工程大学 | Chemical heat regenerator |
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| CN106006553A (en) * | 2016-05-09 | 2016-10-12 | 大连理工大学 | Online hydrogen production method and equipment with methanol oxidation and steam reforming segmental combined |
| CN106006553B (en) * | 2016-05-09 | 2018-07-13 | 大连理工大学 | Methanol is aoxidized combines online production hydrogen methods and equipment with steam reformation segmentation |
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| CN110255496B (en) * | 2019-06-27 | 2022-03-25 | 大连民族大学 | Array type non-equilibrium plasma reformer |
| CN110255496A (en) * | 2019-06-27 | 2019-09-20 | 大连民族大学 | A kind of array nonequilibrium plasma reformer |
| CN112322317A (en) * | 2020-09-29 | 2021-02-05 | 上海工程技术大学 | Method and device for coupling low-temperature plasma methane activation and oil shale pyrolysis |
| CN112250040A (en) * | 2020-11-18 | 2021-01-22 | 天津大学 | Hydrogen production device and method for reforming organic compound through low-temperature plasma |
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