阅读说明：本技术 一种利用水下鼓泡多模式放电合成过氧化氢的装置 (Device for synthesizing hydrogen peroxide by using underwater bubbling multi-mode discharge ) 是由 方志 卢旭 王森 于 2021-08-02 设计创作，主要内容包括：本发明公开了一种利用水下鼓泡多模式放电合成过氧化氢的装置,包括通气室、绝缘体密封塞、金属长针电极、顶盖、反应瓶、底部地电极、高压电源,所述通气室的顶部设置有开口并与绝缘体密封塞连接,所述金属长针电极贯穿绝缘体密封塞并插入通气室内,且通气室顶端侧壁设置有进气口,所述进气口固定连接通气管,所述通气管的另一端固定连接质量流量控制器,通气室贯穿顶盖并插入反应瓶内部,所述底部地电极位于反应瓶底部,本发明的有益效果：本发明可实现单一辉光放电模式和混合放电模式的双模式放电,利用气压在内部形成气相空间,放电产生的等离子体由气泡带入液相中,能够有效降低传质损耗,提高等离子体利用率,能够迅速制取过氧化氢溶液。(The invention discloses a device for synthesizing hydrogen peroxide by utilizing underwater bubbling multi-mode discharge, which comprises an air vent, an insulator sealing plug, a metal long needle electrode, a top cover, a reaction bottle, a bottom ground electrode and a high-voltage power supply, wherein the top of the air vent is provided with an opening and is connected with the insulator sealing plug, the metal long needle electrode penetrates through the insulator sealing plug and is inserted into the air vent, the side wall of the top end of the air vent is provided with an air inlet, the air inlet is fixedly connected with an air pipe, the other end of the air pipe is fixedly connected with a mass flow controller, the air vent penetrates through the top cover and is inserted into the reaction bottle, and the bottom ground electrode is positioned at the bottom of the reaction bottle. The invention can realize dual-mode discharge in a single glow discharge mode and a mixed discharge mode, a gas phase space is formed inside by utilizing air pressure, and plasma generated by discharge is brought into a liquid phase by air bubbles, so that the mass transfer loss can be effectively reduced, the utilization rate of the plasma is improved, and the hydrogen peroxide solution can be quickly prepared.)

1. The utility model provides an utilize device of synthetic hydrogen peroxide of bubbling multi-mode discharge under water, includes breather chamber (1), insulator sealing plug (2), metal long needle electrode (3), top cap (4), reaction flask (5), bottom ground electrode (6) and high voltage power supply (7), its characterized in that: the top of air vent (1) is provided with the opening and is connected with insulator sealing plug (2), metal long needle electrode (3) run through insulator sealing plug (2) and insert in air vent (1), and air vent (1) top lateral wall is provided with air inlet (8), air inlet (8) fixed connection breather pipe (9), other end fixed connection mass flow controller (10) of breather pipe (9), inside air vent (1) run through top cap (4) and insert reaction bottle (5), bottom ground electrode (6) are located reaction bottle (5) bottom, the top electric connection high voltage power supply (7) of metal long needle electrode (3).

2. The device for synthesizing hydrogen peroxide by using underwater bubbling multi-mode discharge according to claim 1, wherein: a removable medium pipe (14) is movably sleeved on the surface of the metal long needle electrode (3).

3. The device for synthesizing hydrogen peroxide by using underwater bubbling multi-mode discharge according to claim 1, wherein: the horizontal height of the bottom of the metal long needle electrode (3) is higher than that of the bottom of the ventilation chamber (1), and the edge of the bottom of the ventilation chamber (1) is provided with an exhaust hole (13).

4. The device for synthesizing hydrogen peroxide by using underwater bubbling multi-mode discharge according to claim 1, wherein: the top cover (4) is divided into an upper layer and a lower layer, wherein the diameter of the upper layer is the same as the outer diameter of the reaction bottle (5), and the outer diameter of the lower layer is the same as the inner diameter of the reaction bottle (5).

5. The device for synthesizing hydrogen peroxide by using underwater bubbling multi-mode discharge according to claim 1, wherein: the reaction bottle (5) comprises a water inlet (11) and a water outlet (12), the water inlet (11) is located on the side wall of the top end of the reaction bottle (5), and the water outlet (12) is located on the side wall of the bottom end of the reaction bottle (5).

Technical Field

The invention relates to the technical field of hydrogen peroxide preparation, in particular to a device for synthesizing hydrogen peroxide by utilizing underwater bubbling multi-mode discharge.

Background

As an important industrial necessity, the capacity and efficiency of hydrogen peroxide production will affect the subsequent processAll industrial production processes. The traditional preparation method of hydrogen peroxide comprises anthraquinone method and H₂/O₂Noble metal catalytic process H₂/O₂Fuel cell method, etc., but these methods all have certain limitations, such as anthraquinone method equipment investment is large, energy consumption is high, only suitable for large-scale production, and there is organic matter pollution; h₂/O₂Noble metal catalytic process requires H₂And O₂Direct contact, explosion risk and a series of side reactions exist; and H₂/O₂H produced by fuel cell process₂O₂Low concentration and high electrode cost. Plasma is an efficient means of molecular activation, and many physicochemical reactions that are difficult to perform under conventional conditions can occur in a plasma environment. Gas-liquid discharge is a common mode for generating low-temperature plasma, and is widely applied to the fields of sewage treatment, sterilization, disinfection, chemical synthesis and the like.

The existing devices for preparing hydrogen peroxide by using plasma can be divided into H according to different production raw materials₂And O₂As raw material and with H₂O is two kinds of raw materials.

With H₂And O₂The synthesis of hydrogen peroxide as a raw material is the most ideal synthetic route from the standpoint of atom economy. With H₂And O₂Apparatus for synthesizing hydrogen peroxide from raw material, such as one using H as proposed in patent CN 101759154A₂And O₂The device and the method for synthesizing the hydrogen peroxide improve the safety of the preparation process by additionally arranging a cooling area, separating a hydrogen area from an oxygen area and carrying out step-by-step reaction. However, the hydrogen gas is ionized and the active hydrogen plasma is sprayed into the oxygen region by pressure difference, which cannot ensure the reaction to be fully carried out, and the utilization rate of the plasma is low. At the same time, the increase in complexity of the apparatus brings about a considerable increase in production costs.

With H₂The raw material for synthesizing the hydrogen peroxide by taking the O as the raw material has low cost, no explosion risk and high reaction safety. An apparatus and method for synthesizing hydrogen peroxide by corona discharge as described in patents CN 108147371a and CN 108212047a, wherein water is atomized by an ultrasonic atomizer and passed upwardCorona discharge is generated between the positive electrode layer and the negative electrode layer which are arranged in parallel and overlapped, and hydrogen peroxide is obtained after gas-liquid separation and condensation of products. Although atomized water droplets are easier to discharge than pure liquid, corona discharge is lower in intensity, less hydrogen peroxide can be synthesized by discharge, and water mist condenses on the electrode layer to form water droplets, which greatly affects discharge. Meanwhile, the use and condensation process of the ultrasonic atomizer lead the production process to be complicated, and the production cost is greatly increased.

Moreover, because of the difficulty of discharging pure liquid phase water, H is currently used₂Production of H by using O as raw material₂O₂The device adopts the discharge form mainly discharging atomized water drops or discharging water vapor. For example, patent CN 205603215U proposes a device for preparing hydrogen peroxide by discharging atomized water, which utilizes an ultrasonic atomizer to generate water mist, and utilizes an air inlet, an air outlet guiding fan and an integrally enclosed structure of the device to form an air flow from bottom to top, and generates plasma by dielectric barrier discharge between electrodes. However, the discharge uniformity in the water mist is poor, and the use of the ultrasonic atomizer and the guide fan increases the complexity of the device and the production cost. Patent CN 107207253B proposes a device for synthesizing hydrogen peroxide by discharging air-liquid flow or steam, which utilizes a hollow rotor to generate cold steam, and improves the discharge stability and uniformity. However, the corona discharge strength is weak, the hydrogen peroxide yield is low, the device cost is high, and the application scene is limited.

Disclosure of Invention

The invention aims to provide a device for synthesizing hydrogen peroxide by using underwater bubbling multi-mode discharge, which solves the defects in the background technology.

In order to achieve the purpose, the invention provides the following technical scheme: the utility model provides an utilize synthetic hydrogen peroxide's of bubbling multi-mode discharge device under water, includes breather chamber, insulator sealing plug, metal long needle electrode, top cap, reaction flask, bottom ground electrode and high voltage power supply, the top of breather chamber is provided with the opening and is connected with the insulator sealing plug, metal long needle electrode runs through the insulator sealing plug and inserts in the breather chamber, and breather chamber top lateral wall is provided with the air inlet, air inlet fixed connection breather pipe, the other end fixed connection quality flow controller of breather pipe, the breather chamber runs through inside the top cap and inserts the reaction flask, the bottom ground electrode is located the reaction flask bottom, the top electric connection high voltage power supply of metal long needle electrode.

As a further scheme of the invention: and a removable medium pipe is movably sleeved on the surface of the metal long needle electrode.

As a further scheme of the invention: the horizontal height of the bottom of the metal long needle electrode is higher than that of the bottom of the ventilation chamber, and the edge of the bottom of the ventilation chamber is provided with an exhaust hole.

As a further scheme of the invention: the top cap is divided into an upper layer and a lower layer, wherein the diameter of the upper layer is the same as the outer diameter of the reaction bottle, and the outer diameter of the lower layer is the same as the inner diameter of the reaction bottle.

As a further scheme of the invention: the reaction bottle comprises a water inlet and a water outlet, the water inlet is located on the side wall of the top end of the reaction bottle, and the water outlet is located on the side wall of the bottom end of the reaction bottle.

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

1. the electrode structure is asymmetrical, the discharge difficulty can be effectively reduced due to extremely uneven electric field distribution, two discharge modes of glow discharge and glow + spark mixed mode discharge can be realized according to whether the dielectric tube is sleeved outside the long needle electrode, different working modes can be selected according to different use requirements, and the electrode structure has the advantages of low energy consumption and high production efficiency;

2. the long needle electrode and the glass ventilation chamber are coaxially integrated, so that the failure rate is low, the maintenance is easy, a long and narrow air gap between the long needle electrode and the glass ventilation chamber can effectively enlarge a discharge area, prolong the gas reaction time and improve the gas utilization rate;

3. the gas phase space is formed in the ventilation chamber by utilizing the air pressure through the vent hole at the bottom of the ventilation chamber, and the plasma generated by discharge is transferred into the liquid in a form of bubbles through the vent hole, so that the utilization rate of the plasma can be effectively improved;

4. compared with the method using hydrogen/oxygen as raw materials, the method has the advantages of high safety, low energy consumption, and no pollution by-product.

Drawings

In order to more clearly illustrate the technical solutions of the embodiments of the present invention, the drawings used in the description of the embodiments will be briefly introduced below, and it is obvious that the drawings in the following description are only some embodiments of the present invention, and it is obvious for those skilled in the art that other drawings can be obtained according to the drawings without creative efforts.

FIG. 1 is a schematic diagram of a hybrid discharge mode structure according to the present invention;

FIG. 2 is a schematic view of a glow discharge mode structure according to the present invention;

FIG. 3 is a schematic view of a plasma reaction region according to the present invention;

FIG. 4 is a graph of the discharge in the single glow discharge mode of the present invention;

FIG. 5 is a discharge image in a mixed mode according to the present invention;

FIG. 6 shows the hydrogen peroxide yield in two discharge modes according to the present invention.

In the figure: 1. a breather chamber; 2. An insulator sealing plug; 3, a metal long needle electrode; 4. a top cover; 5. a reaction bottle; 6. a bottom ground electrode; 7. a high voltage power supply; 8. an air inlet; 9. a breather pipe; 10. a mass flow controller; 11. a water inlet; 12. a water outlet; 13. an exhaust hole; 14. a medium pipe.

Detailed Description

The technical solutions in the embodiments of the present invention will be clearly and completely described below with reference to the drawings in the embodiments of the present invention, and it is obvious that the described embodiments are only a part of the embodiments of the present invention, and not all of the embodiments. All other embodiments, which can be derived by a person skilled in the art from the embodiments given herein without making any creative effort, shall fall within the protection scope of the present invention.

Referring to fig. 1-6, in an embodiment of the present invention, an apparatus for synthesizing hydrogen peroxide by underwater bubbling multi-mode discharge includes a vent chamber 1, an insulator sealing plug 2, a metal long needle electrode 3, a top cover 4, a reaction flask 5, a bottom ground electrode 6, and a high voltage power supply 7, an opening is disposed at a top of the vent chamber 1 and connected to the insulator sealing plug 2, the metal long needle electrode 3 penetrates through the insulator sealing plug 2 and is inserted into the vent chamber 1, an air inlet 8 is disposed on a sidewall of a top end of the vent chamber 1, the air inlet 8 is fixedly connected to a vent pipe 9, another end of the vent pipe 9 is fixedly connected to a mass flow controller 10, the vent chamber 1 penetrates through the top cover 4 and is inserted into the reaction flask 5, the bottom ground electrode 6 is located at a bottom of the reaction flask 5, and a top of the metal long needle electrode 3 is electrically connected to the high voltage power supply 7.

It is worth noting that the horizontal height of the bottom of the metal long needle electrode 3 is higher than that of the bottom of the vent chamber 1, a removable medium pipe 14 is sleeved on the outer side of the metal long needle electrode, and the bottom edge of the vent chamber 1 is provided with an exhaust hole 13.

It should be noted that the top cap 4 is divided into an upper layer and a lower layer, wherein the diameter of the upper layer is the same as the outer diameter of the reaction flask 5, and the outer diameter of the lower layer is the same as the inner diameter of the reaction flask 5.

It is noted that the reaction flask 5 comprises a water inlet 11 and a water outlet 12, the water inlet 11 is located on the top side wall of the reaction flask 5, and the water outlet 12 is located on the bottom side wall of the reaction flask 5.

The first embodiment is as follows:

combined with fig. 1 and 5, hybrid discharge mode: the mixed discharge mode is a combination of a glow discharge mode and a spark discharge mode, at the moment, a medium tube 14 on the surface of the metal long needle electrode 3 is removed, the needle point area of the metal long needle electrode 3 is in the spark discharge mode, the rest part of the metal long needle electrode is in the glow discharge mode, in the mixed mode, the gold needle long needle electrode 3 is in a bare leakage state, and a small-caliber reaction bottle 5 is matched to quickly generate a high-concentration hydrogen peroxide solution, so that the device is suitable for preparing an emergency hydrogen peroxide solution;

example two:

with reference to fig. 2 and 4, in the single glow discharge mode, the medium tube 14 is additionally arranged outside the metal long needle electrode 3 to realize a uniform and stable single glow discharge mode, and the continuous production of the hydrogen peroxide solution can be realized by matching with the large-caliber reaction bottle 5 in the single glow discharge mode, and meanwhile, the medium tube 14 can play a role in protecting the metal long needle electrode 3, so that the service life of the metal long needle electrode 3 is effectively prolonged, and the method is suitable for preparing the reserved hydrogen peroxide.

Example three:

120ml of water is added, microsecond pulse power supply is adopted for driving, and hydrogen peroxide is prepared by two discharge modes respectively, and a change curve of the concentration of the generated hydrogen peroxide along with discharge time is shown in figure 6. As can be seen from FIG. 6, the mixed mode discharge produced 56.458mg/L of hydrogen peroxide at 40 minutes after discharge with an energy yield of 520mg/kWh, and the glow discharge produced 724mg/kWh of hydrogen peroxide at 6.55 mg/L.

The preparation process and the principle thereof are as follows:

firstly, a proper amount of water is introduced from the water inlet 11, then the gas is connected and the aeration chamber 1 is put into the water, then the circuit is connected, and after the circuit is connected, the breakdown discharge of the gas is firstly generated in the gas phase, and the plasma consisting of high-energy electrons and metastable-state particles is generated. The water molecules react with the high-energy electrons and the metastable-state particles to generate hydroxyl, and the hydroxyl undergoes a composite reaction to generate hydrogen peroxide, so that a hydrogen peroxide solution is finally formed.

The asymmetric electrode structure forms a very uneven electric field, so that in mixed mode discharge, a spark discharge is firstly generated at the bottom tip of the metal long needle electrode 3, and a uniform and stable glow discharge is generated in the middle of the metal long needle electrode 3. The aeration chamber 1 is directly inserted into water, a gas-phase discharge space is formed inside by using air pressure, and plasma generated by discharge is brought into a liquid phase by bubbles, so that the mass transfer loss can be effectively reduced, and the utilization rate of the plasma is improved.

It will be evident to those skilled in the art that the invention is not limited to the details of the foregoing illustrative embodiments, and that the present invention may be embodied in other specific forms without departing from the spirit or essential attributes thereof. The present embodiments are therefore to be considered in all respects as illustrative and not restrictive, the scope of the invention being indicated by the appended claims rather than by the foregoing description, and all changes which come within the meaning and range of equivalency of the claims are therefore intended to be embraced therein. Any reference sign in a claim should not be construed as limiting the claim concerned.

Furthermore, it should be understood that although the present description refers to embodiments, not every embodiment may contain only a single embodiment, and such description is for clarity only, and those skilled in the art should integrate the description, and the embodiments may be combined as appropriate to form other embodiments understood by those skilled in the art.