CN112717852B - Device and method for directionally regulating and controlling low-temperature plasma catalytic reaction - Google Patents
Device and method for directionally regulating and controlling low-temperature plasma catalytic reaction Download PDFInfo
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Abstract
The invention discloses a device and a method for directionally regulating and controlling a low-temperature plasma catalytic reaction. The inventor adjusts the spatial distribution of the rod-shaped catalyst in the discharge area of the dielectric barrier reactor to achieve the control of the low-temperature plasma discharge mode and parameters; specifically, the purpose of directionally regulating and controlling the plasma catalytic reaction is realized by regulating one or more of the selection of the type, the filling quantity, the filling interval and the control in specific positions of the rod-shaped catalyst.
Description
Technical Field
The invention relates to the field of low-temperature plasma catalysis, in particular to a method and a device for directionally regulating and controlling low-temperature plasma catalytic reaction.
Background
The packed bed dielectric barrier reactors (PBRs) combine the technical advantages of catalysis and low-temperature plasma, effectively improve the energy density of the low-temperature plasma, the reactive molecular reaction rate and the chemical reaction path of the dielectric barrier reactors (DBDs), and are ideal low-temperature catalytic reaction devices. In recent years, a number of experimental results have demonstrated that the combined action of PBRs plasma and catalyst is central to the impact of plasma-catalyzed reactions. However, this synergy process is complex and requires consideration of both electric field distortion due to catalyst polarization, transition of plasma formation and propagation paths, and surface catalytic reactions between the plasma and the catalytically active species. The catalyst is typically an insulating medium. When the catalyst fills the PBRs discharge gap, the discharge mode changes from filament discharge to streamer discharge, point-to-point discharge and surface discharge-like. Point discharges are more likely to occur at the contact points between the catalysts, while the intensity and propagation path of surface streamer discharges depend on the morphology and dielectric constant of the catalysts. In the case of plasma surface catalyzed reactions, streamer discharges on the surface of the catalyst are of greater interest to researchers. Since it is a very efficient heterogeneous mass transfer means. The plasma active material will form directly on the catalyst surface, which helps the active material, especially with a short lifetime, to participate in the surface catalytic reaction. Therefore, it is necessary to explore methods and mechanisms for fine tuning the discharge behavior of PB-DBDs.
However, in PBRs, the catalyst is mostly filled in the form of particles in the discharge region. Particle filling causes disorder of a discharge channel and uncertainty of gas discharge, and stable, uniform and reliable discharge behavior is difficult to establish on the surface of the catalyst, so that regulation and control of streamer discharge on the surface of the catalyst cannot be realized, and a reaction path and reaction efficiency of low-temperature plasma catalytic reaction cannot be accurately regulated.
Disclosure of Invention
The invention provides a device and a method for directionally regulating and controlling a low-temperature plasma catalytic reaction, which can achieve the purpose of directionally regulating and controlling the plasma catalytic reaction.
The technical scheme of the invention is that the device for directionally regulating and controlling the low-temperature plasma catalytic reaction comprises a dielectric barrier reactor consisting of an excitation power supply, a high-voltage electrode, a ground electrode and a barrier medium, wherein the barrier medium is positioned between the high-voltage electrode and the ground electrode, a rod-shaped catalyst is arranged in a discharge area of the dielectric barrier reactor, and a catalyst support for fixing the rod-shaped catalyst is also arranged outside the discharge area of the dielectric barrier reactor.
Further, the high voltage electrode and the ground electrode in the dielectric barrier reactor are a plate-plate electrode structure and a coaxial electrode structure.
Furthermore, the catalyst supports are positioned at two ends of the rod-shaped catalyst, a plurality of holes are formed in the catalyst supports, the size of each hole is matched with the diameter of the rod-shaped catalyst, and the number of the holes is the same as that of the rod-shaped catalysts.
Furthermore, the dielectric constant of the rod-shaped catalyst is 10-10000, and the support material adopted by the rod-shaped catalyst comprises ZrO 2 、Al 2 O 3 、MgAl 2 O 4 Or BaTiO 3 。
The invention also relates to a method for directionally regulating and controlling the low-temperature plasma catalytic reaction by using the device, which achieves the control of the low-temperature plasma discharge mode and parameters by regulating the spatial distribution of the rod-shaped catalyst in the discharge area of the dielectric barrier reactor; specifically, the directional regulation is realized by one or more of the selection of the type of the rod-shaped catalyst, the filling quantity, the filling distance and the control in the specific position.
Furthermore, when the dielectric constant of the catalyst carrier is 10-100, a single rod-shaped catalyst is arranged in the direction of an electric field in a discharge area, and the diameter of the rod-shaped catalyst is 1/3-1/2 of the discharge gap;
furthermore, when the dielectric constant of the catalyst carrier is 100-10000, 1-3 rod-shaped catalysts are arranged in the direction of the electric field of the discharge area, and the diameter of each rod-shaped catalyst is 1/6-1/2 of the discharge gap.
Furthermore, the rod-shaped catalysts are uniformly arranged along the vertical direction of the electric field, and the gap between the catalysts is 1 to 3 times of the diameter of the catalysts. In PBRs, the plasma discharge characteristic and the catalytic reaction are closely connected, and the plasma discharge characteristic of PBRs can be effectively regulated and controlled by organically combining factors such as the dielectric constant, the shape, the spatial position distribution and the like of the catalyst, so that the aim of enhancing the plasma catalytic reaction is fulfilled.
The invention adopts the rod-shaped catalyst with ordered spatial arrangement as the filling medium of the dielectric barrier reactor, adopts a novel filling mode, has the characteristics of regular shape and controllable spatial arrangement, and realizes the directional optimization of the low-temperature plasma discharge mode and key parameters from the viewpoint of regulating and controlling the discharge characteristic of the low-temperature plasma.
The invention provides a brand new arrangement form of the rod-shaped catalyst in a discharge area according to the influence rule of the electrical parameters of the rod-shaped catalyst on the formation and propagation characteristics of PBRs plasma.
The PBRs discharge form involves streamer discharge at the catalyst surface and point-to-point discharge between the catalyst and the electrode. The intensity of the gas discharge determines the concentration of the plasma active species. Strength, the higher the active ingredient concentration.
When the dielectric constant of the catalyst carrier is 10-100, the surface of the catalyst is completely wrapped by the streamer discharge on the surface of the catalyst, so that the efficiency of surface catalytic reaction is improved. However, as the number of the rod-shaped catalysts increases in the direction of the electric field, the intensity of streamer discharge on the surface of the catalyst and the contact area between the streamer discharge and the catalyst are correspondingly reduced, which is not favorable for the occurrence of surface catalytic reaction. When the diameter of the rod-shaped catalyst is 1/3-1/2 of the discharge gap, the streamer discharge intensity on the surface of the catalyst is the highest. Therefore, when the dielectric constant of the catalyst carrier is 10-100, a single rod-shaped catalyst is arranged in the direction of the electric field in the discharge area, and the diameter of the rod-shaped catalyst is 1/3-1/2 of the discharge gap.
When the dielectric constant of the catalyst carrier is 100-10000, the PBRs discharge form is mainly between the catalyst and the catalyst, and point-point discharge between the catalyst and the electrode. The quantity of the rodlike catalysts in the direction of the electric field is increased, more point-to-point discharge processes on the surface of the catalysts can be generated, and the efficiency of the surface catalytic reaction is improved. However, the rod-shaped catalyst is excessive, the capacitive reactance of the PBRs reactor is increased, and the efficiency of the plasma power supply is reduced. Therefore, when the dielectric constant of the catalyst carrier is 100-1000, 1-3 rod-shaped catalysts are arranged in the direction of the electric field in the discharge region, and the diameter of the rod-shaped catalyst is 1/6-1/2 of the discharge gap.
The PBRs discharge gaps are filled with the rod-shaped catalysts, the number of the rod-shaped catalysts arranged is increased along the vertical direction of the electric field, more plasmas are favorably formed, and the reaction efficiency is improved. However, the distance of the rod-shaped catalyst along the electric field vertical mode is too small, the catalysts can interfere with each other, and the formation and the propagation path of streamer discharge on the surface of the rod-shaped catalyst are influenced. Therefore, the rod-shaped catalysts are uniformly arranged in the vertical direction of the electric field, and the gap between the catalysts is 1 to 3 times of the diameter of the catalysts.
Drawings
Fig. 1 is a schematic structural view of embodiment 1.
FIG. 2 is a top view of the apparatus of example 1.
FIG. 3 is a graph of the effect of media barrier reactor rod catalyst filling on plasma formation characteristics in example 2, where a is the effect of applied voltage and rod catalyst spacing on the plasma formation characteristics and b is the effect of rod catalyst filling quantity on the plasma formation characteristics at an applied voltage of 25.6 kV.
Detailed Description
Embodiments of the present invention will be described in detail below with reference to examples, but it will be understood by those skilled in the art that the following examples are only illustrative of the present invention and should not be construed as limiting the scope of the present invention.
Example 1:
a directional regulation and control device for low-temperature plasma catalytic reaction, which is shown in figures 1 and 2. The dielectric barrier reactor adopts a plate-plate electrode mechanism which consists of an excitation power supply 6, a high-voltage plate electrode 1, a plate ground electrode 3 and a barrier dielectric 2.
In fig. 1, the rod-shaped catalyst 4 is filled in the discharge area of the dielectric barrier reactor, and the catalyst support 5 plays a role of supporting the rod-shaped catalyst 4 and is placed outside the discharge area of the dielectric barrier reactor. The catalyst support 5 is provided with a plurality of holes which are regularly arranged, and the size and the number of the holes are the same as the diameter and the number of the rod-shaped catalysts 4. The arrangement of the catalyst support holes is shown in figure 2.
The spatial arrangement of the rod-shaped catalysts, which is used for two rod-shaped catalysts with different diameters, can be clearly distinguished from fig. 2. The 4 rod-shaped catalysts with smaller diameters are uniformly arranged along the direction of an electric field, and the rod-shaped catalysts with larger diameters are crosswise arranged along the direction vertical to the electric field.
The rod-shaped catalyst carrier with smaller diameter adopts BaTiO with high dielectric constant 3 The polarization discharge intensity of the dielectric barrier reactor is enhanced; the rod-shaped catalyst carrier with larger diameter adopts Al with lower dielectric constant 2 O 3 And is favorable for forming surface discharge on the surface of the rod-shaped catalyst.
Example 2:
a directional regulation and control device for low-temperature plasma catalytic reaction is characterized in that a dielectric barrier reactor adopts a coaxial electrode structure, and specifically, al is filled in the coaxial dielectric barrier reactor 2 O 3 The rod-shaped catalyst is used for regulating and controlling the plasma forming characteristics by changing and adjusting the applied voltage and the filling quantity of the rod-shaped catalyst.
As can be seen from fig. 3 (a), the plasma discharge form changes after the rod-shaped catalyst is filled. Due to the rod-shaped catalyst filling, distortion of the peripheral electric field was caused, and when the applied voltage was 21.8kV, plasma was generated only in the periphery of the rod-shaped catalyst. When the applied voltage is 24.2kV, plasma appears between the rod-shaped catalysts which are far away, and the intensity of plasma discharge is increased along with the increase of the applied voltage; after the distance between the rod-shaped catalysts along the vertical direction of the electric field is reduced, the plasma between the rod-shaped catalysts disappears. As can be seen from fig. 3 (b), after the rod-shaped catalyst is filled, the plasma discharge form changes, and as the filling amount of the rod-shaped catalyst increases, the discharge form of the dielectric barrier reactor gradually transits from filament discharge to polarization discharge and catalyst surface discharge, and the formation of more catalyst surface discharge helps to enhance the contact efficiency between the plasma and the catalyst and improve the reaction characteristics.
Claims (3)
1. A method for directionally regulating and controlling low-temperature plasma catalytic reaction is characterized by comprising the following steps: the device comprises a dielectric barrier reactor consisting of an excitation power supply (6), a high-voltage electrode (1), a ground electrode (3) and a barrier medium (2), wherein the barrier medium (2) is positioned between the high-voltage electrode (1) and the ground electrode (3), a rod-shaped catalyst (4) is arranged in a discharge area of the dielectric barrier reactor, and a catalyst support (5) for fixing the rod-shaped catalyst is also arranged on the outer side of the discharge area of the dielectric barrier reactor; the directional regulation and control are realized by one or more of the selection of the type, the filling quantity, the filling interval and the specific position of the rod-shaped catalyst; the dielectric constant of the rod-shaped catalyst is 10-10000, and the carrier material adopted in the rod-shaped catalyst (4) is ZrO 2 、Al 2 O 3 、MgAl 2 O 4 Or BaTiO 3 (ii) a When the dielectric constant of the catalyst carrier is 10-100, a single rod-shaped catalyst is arranged in the direction of an electric field in a discharge area, and the diameter of the rod-shaped catalyst is 1/3-1/2 of the discharge gap; when the dielectric constant of the catalyst carrier is 100-10000, 1-3 rod-shaped catalysts are arranged in the direction of an electric field of a discharge area, and the diameter of each rod-shaped catalyst is 1/6-1/2 of a discharge gap; the rodlike catalysts are uniformly arranged along the vertical direction of the electric field, and the gap between the catalysts is 1 to 3 times of the diameter of the catalysts.
2. The method of claim 1, wherein: the high-voltage electrode and the ground electrode in the dielectric barrier reactor are in a plate-plate electrode structure or a coaxial electrode structure.
3. The method of claim 1, wherein: the catalyst support (5) is positioned at two ends of the rod-shaped catalyst (4), a plurality of holes are formed in the catalyst support, the size of each hole is matched with the diameter of the rod-shaped catalyst, and the number of the holes is the same as that of the rod-shaped catalysts.
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Citations (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JP2002241774A (en) * | 2001-02-15 | 2002-08-28 | Mitsubishi Heavy Ind Ltd | Apparatus and method for producing gas |
| JP2015189599A (en) * | 2014-03-27 | 2015-11-02 | 株式会社日本触媒 | Method for electric field synthesis of chemicals |
| CN112007486A (en) * | 2020-08-17 | 2020-12-01 | 中国船舶重工集团公司第七0四研究所 | VOCs (volatile organic compounds) line tube reaction unit adopting double-dielectric barrier low-temperature plasma for cooperative catalytic treatment |
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| Publication number | Priority date | Publication date | Assignee | Title |
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| US20030030374A1 (en) * | 2001-08-03 | 2003-02-13 | Deepak Pai | Dielectric barrier discharge plasma reactor cell |
| US9117636B2 (en) * | 2013-02-11 | 2015-08-25 | Colorado State University Research Foundation | Plasma catalyst chemical reaction apparatus |
| CN107051198A (en) * | 2017-03-21 | 2017-08-18 | 复旦大学 | The emission-control equipment of array plasma catalyst synergy |
| CN107333376A (en) * | 2017-04-21 | 2017-11-07 | 南京航空航天大学 | A kind of atomic plasma jet generating device of atmospheric pressure |
| CN111760450A (en) * | 2020-06-12 | 2020-10-13 | 崇左南方水泥有限公司 | Line plate type dielectric barrier discharge cooperative catalysis denitration device |
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| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JP2002241774A (en) * | 2001-02-15 | 2002-08-28 | Mitsubishi Heavy Ind Ltd | Apparatus and method for producing gas |
| JP2015189599A (en) * | 2014-03-27 | 2015-11-02 | 株式会社日本触媒 | Method for electric field synthesis of chemicals |
| CN112007486A (en) * | 2020-08-17 | 2020-12-01 | 中国船舶重工集团公司第七0四研究所 | VOCs (volatile organic compounds) line tube reaction unit adopting double-dielectric barrier low-temperature plasma for cooperative catalytic treatment |
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