CN102351144B - 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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- CN102351144B CN102351144B CN 201110174492 CN201110174492A CN102351144B CN 102351144 B CN102351144 B CN 102351144B CN 201110174492 CN201110174492 CN 201110174492 CN 201110174492 A CN201110174492 A CN 201110174492A CN 102351144 B CN102351144 B CN 102351144B
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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 height of producing is present the most frequently used a kind of reformation hydrogen production mode.Adopt this method, with fuel with enter reformer after water vapour mixes, 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 that participates 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 to regulate simultaneously the ratio between oxygen, water vapour and the fuel, and control ratio is difficulty, and easily produces the carbon distribution phenomenon and damage catalyzer in reformation.
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, as 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 a large amount of heats and expended energy at 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, the method and apparatus that provide that a kind of speed of response is fast, reformation efficient height, plasma body cooperative catalysis complex reaction that capacity usage ratio is high prepares hydrogen-rich combustion gas.
For achieving the above object, the compound reformation of the plasma body that the present invention is designed and chemical catalysis prepares the method for hydrogen-rich combustion gas, comprises the steps:
In the toroidal plasma region of discharge that electrode and tubular outer electrode constitute in the tubular of the hydrocarbon fuel droplet importing coaxial arrangement that 1) will handle through atomizing, make the hydrocarbon fuel droplet under the effect of impact of high-energy electron, take place to react based on the reforming plasma of free radical, 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 produces 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 on the surface of chemical catalyst rapid catalyzed reaction take place, produce more and littler small-molecule mixture, the heat of the interior electrode generation of tubular simultaneously can be the chemical catalysis reaction bed and adds thermal utilization;
3) at last the small-molecule mixture that produces is derived, can obtain the hydrogen-rich combustion gas of high density.
Particularly, described hydrocarbon fuel is aqueous ethanol, methane, methyl alcohol or petroleum naphtha.
Further, the voltage that applies of described toroidal plasma region of discharge is that 5～20KV, frequency are that 7～15KHz, electrode discharge spacing are 0.5～4mm.
Further, described chemical catalyst is nickel-base catalyst or copper-based catalysts, and the temperature of described chemical catalysis reaction is 320～400 ℃.
For realizing that the custom-designed plasma body of aforesaid method and the compound reformation of chemical catalysis prepare the equipment of hydrogen-rich combustion gas, the interior electrode of tubular and the tubular outer electrode that comprise coaxial arrangement, form the toroidal plasma region of discharge in the described tubular between electrode and the tubular outer electrode, one end of described toroidal plasma region of discharge is the region of discharge import, the other end of described 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 described tubular, the reaction bed import of described 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 described chemical catalysis reaction bed is positioned at the same side also separately with the region of discharge entrance 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 described tubular, described tubular outer electrode is sleeved on the tubular block media layer.
Particularly, described tubular block media layer is 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 described tubular.Like this, it is simple and practical, by end cover stop with guide functions under, the reaction bed import that can make described 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 described 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 described chemical catalysis reaction bed.Like this, can monitor the temperature in the chemical catalysis reaction bed, and in time temperature of reaction be regulated accordingly, make heat energy utilization reach best.
The preparation method that the present invention is designed is that the hydrocarbon fuel atomizing is imported in the toroidal plasma region of discharge, makes the hydrocarbon fuel molecule be subjected to the impact of high-energy electron, and the chemical bond that wherein contains ruptures, and forms H, OH, CH
3, C
2H
5, CH
2OH, CH
3CHOH, CH
2CH
2The free radical that OH etc. are bigger, these free radicals fragment into littler free radical after being subjected to further impacting.Directly enter into the chemical catalysis reaction bed through the hydrocarbon fuel droplet after the Cement Composite Treated by Plasma, wherein a large amount of active particles also together enter 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 is 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 for catalyzed reaction, overall reformation efficient and capacity usage ratio are improved.
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, designed simple and compact equipment structure, lightweight and portable in volume are small and exquisite, 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
The present invention is described in further detail below in conjunction with the drawings and specific embodiments.
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 the 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.Tubular block media layer 3 adopts 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%.Tubular outer electrode 1 is sleeved on the tubular block media layer 3, forms the toroidal plasma region of discharge 4 of dielectric impedance structure thus in tubular 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 entrances 8 with toroidal plasma region of discharge 4 of 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 end is fixed on the end cover 6.12 of temperature sensors link to each other with extraneous pilot circuit by signal wire, in order to regulate the temperature of reaction of chemical catalysis reaction bed 5.
The specific design parameter of equipment that the compound reformation of above-mentioned plasma body and chemical catalysis prepares hydrogen-rich combustion gas is as follows:
Embodiment 1:
Be that 122mm, thickness are that the alumina-ceramic of the height insulation of 0.5mm is 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 nickel-base catalyst.Electric heating tubular heater 7 and the 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 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 copper-based catalysts.Be provided with electric heating tubular heater 7 and the 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:
In the toroidal plasma region of discharge 4 that electrode 2 and tubular outer electrode 1 constitute in the tubular of the hydrocarbon fuel droplet importing coaxial arrangement that 1) will handle through atomizing, make the hydrocarbon fuel droplet under the effect of impact of high-energy electron, take place to react based on the reforming plasma of free radical, 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 produces 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 on the surface of chemical catalyst rapid catalyzed reaction take place, produce more and littler small-molecule mixture, the heat of interior electrode 2 generations of tubular simultaneously can be chemical catalysis reaction bed 5 and adds thermal utilization;
3) at last the small-molecule mixture that produces 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 than single chemical catalysis reforming process and reforming plasma method height.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 (9)
1. a plasma body and the compound reformation of chemical catalysis prepare the method for hydrogen-rich combustion gas, comprise the steps:
In the toroidal plasma region of discharge that electrode and tubular outer electrode constitute in the tubular of the hydrocarbon fuel droplet importing coaxial arrangement that 1) will handle through atomizing, the voltage that applies of described toroidal plasma region of discharge is that 5 ~ 20KV, frequency are that 7 ~ 15KHz, electrode discharge spacing are 0.5 ~ 4mm, make the hydrocarbon fuel droplet under the effect of impact of high-energy electron, take place to react based on the reforming plasma of free radical, 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 produces 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 on the surface of chemical catalyst rapid catalyzed reaction take place, produce more and littler small-molecule mixture, the heat that electrode produces in the tubular adds thermal utilization for the chemical catalysis reaction bed simultaneously;
3) at last the small-molecule mixture that produces is derived, can obtain the hydrogen-rich combustion gas of high density.
2. the compound reformation of plasma body according to claim 1 and chemical catalysis prepares the method for hydrogen-rich combustion gas, it is characterized in that: described hydrocarbon fuel is aqueous ethanol, methane, methyl alcohol or petroleum naphtha.
3. the compound reformation of plasma body according to claim 1 and 2 and chemical catalysis prepares the method for hydrogen-rich combustion gas, it is characterized in that: described chemical catalyst is nickel-base catalyst or copper-based catalysts, and the temperature of described chemical catalysis reaction is 320 ~ 400 ℃.
4. a plasma body and the compound reformation of chemical catalysis prepare the equipment of hydrogen-rich combustion gas, the interior electrode (2) of tubular and the tubular outer electrode (1) that comprise coaxial arrangement, form toroidal plasma region of discharge (4) in the described tubular between electrode (2) and the tubular outer electrode (1), one end of described toroidal plasma region of discharge (4) is region of discharge import (8), the other end of described 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 described tubular, the reaction bed import (11) of described 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 described chemical catalysis reaction bed (5) is positioned at the same side also separately with the region of discharge entrance (8) of toroidal plasma region of discharge (4).
5. the compound reformation of plasma body according to claim 4 and chemical catalysis prepares 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 described tubular, described tubular outer electrode (1) is sleeved on the tubular block media layer (3).
6. the compound reformation of plasma body according to claim 5 and chemical catalysis prepares the equipment of hydrogen-rich combustion gas, it is characterized in that: described 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%.
7. the equipment for preparing hydrogen-rich combustion gas according to claim 4 or 5 or 6 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 described tubular, the reaction bed import (11) of described 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.
8. prepare the equipment of hydrogen-rich combustion gas according to claim 4 or 5 or 6 described plasma bodys and the compound reformation of chemical catalysis, it is characterized in that: be provided with well heater (7) in the described chemical catalysis reaction bed (5).
9. prepare the equipment of hydrogen-rich combustion gas according to claim 4 or 5 or 6 described plasma bodys and the compound reformation of chemical catalysis, it is characterized in that: be provided with temperature sensor (12) in the described chemical catalysis reaction bed (5).
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| CN103216336B (en) * | 2013-03-22 | 2015-06-24 | 哈尔滨工程大学 | Chemical heat regenerator |
| CN105056858B (en) * | 2015-07-20 | 2016-11-30 | 浙江工商大学 | Reactor and the method for synthesis gas is prepared in a kind of greenhouse gases reformation |
| 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 |
| CN111320134B (en) * | 2018-12-17 | 2023-03-21 | 中国科学院大连化学物理研究所 | Fuel reaction device for producing hydrogen |
| CN110255496B (en) * | 2019-06-27 | 2022-03-25 | 大连民族大学 | Array type non-equilibrium plasma reformer |
| CN110296025B (en) * | 2019-06-27 | 2021-08-13 | 大连民族大学 | Control method of array type reforming reactor |
| CN112322317B (en) * | 2020-09-29 | 2022-10-21 | 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 |
| CN114623468B (en) * | 2022-03-02 | 2023-07-25 | 中国人民解放军空军航空大学 | DBD plasma combustion chamber head nozzle with round table structure |
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| CN1837029A (en) * | 2005-03-23 | 2006-09-27 | 王绪炀 | Spontaneous recombinant system for hydrogen conversion and separation from methanol aqueous solution particulates |
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| CN202131085U (en) * | 2011-06-27 | 2012-02-01 | 武汉理工大学 | Equipment for preparing hydrogen-rich gas by composite reformation of plasma and chemical catalysis |
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| US20040216378A1 (en) * | 2003-04-29 | 2004-11-04 | Smaling Rudolf M | Plasma fuel reformer having a shaped catalytic substrate positioned in the reaction chamber thereof and method for operating the same |
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| CN1837029A (en) * | 2005-03-23 | 2006-09-27 | 王绪炀 | Spontaneous recombinant system for hydrogen conversion and separation from methanol aqueous solution particulates |
| CN101734620A (en) * | 2009-12-15 | 2010-06-16 | 太原理工大学 | Method for producing hydrogen gas by methane-rich plasma |
| CN202131085U (en) * | 2011-06-27 | 2012-02-01 | 武汉理工大学 | Equipment for preparing hydrogen-rich gas by composite reformation of plasma and chemical catalysis |
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