CN111137957A - Gas-liquid-solid three-phase pulse discharge electrical characteristic research experimental device and method thereof - Google Patents
Gas-liquid-solid three-phase pulse discharge electrical characteristic research experimental device and method thereof Download PDFInfo
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- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F1/00—Treatment of water, waste water, or sewage
- C02F1/48—Treatment of water, waste water, or sewage with magnetic or electric fields
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- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F1/00—Treatment of water, waste water, or sewage
- C02F1/30—Treatment of water, waste water, or sewage by irradiation
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- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F1/00—Treatment of water, waste water, or sewage
- C02F1/30—Treatment of water, waste water, or sewage by irradiation
- C02F1/32—Treatment of water, waste water, or sewage by irradiation with ultraviolet light
- C02F1/325—Irradiation devices or lamp constructions
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- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F1/00—Treatment of water, waste water, or sewage
- C02F1/72—Treatment of water, waste water, or sewage by oxidation
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- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2201/00—Apparatus for treatment of water, waste water or sewage
- C02F2201/48—Devices for applying magnetic or electric fields
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- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2305/00—Use of specific compounds during water treatment
- C02F2305/02—Specific form of oxidant
- C02F2305/023—Reactive oxygen species, singlet oxygen, OH radical
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Abstract
The invention discloses a gas-liquid-solid three-phase pulse discharge electrical characteristic research experimental device and a method thereof. The invention has a promoting effect on the development of gas-liquid-solid three-phase high-voltage pulse discharge experiments and device design on the wide application of underwater pulse discharge technology in the fields of wastewater treatment and the like.
Description
Technical Field
The invention relates to a gas-liquid-solid three-phase pulse discharge electrical characteristic research experimental device and a method thereof, belonging to the technical field of high-voltage pulse discharge.
Background
The high-voltage pulse discharge has the characteristics of steep front and narrow pulse, can improve the processing capacity of the reactor with wide electrode spacing, increases the discharge stability and enhances the mass transfer efficiency of the discharge plasma reactor.
The underwater pulse discharge technology is to use high voltage pulse power supply to breakdown and discharge in water to generate complex physical processes of plasma chemistry, ultraviolet, shock wave, electron collision and the like and further generate free radicals (OH, O and HO)2H, etc.), ozone (O3) And hydrogen peroxide (H)2O2) And the like. The underwater pulse discharge is beneficial to the mutual diffusion of reactants, and the catalyst is used for assisting to improve the treatment effect. In recent years, underwater pulse discharge has been widely used in the fields of wastewater treatment, underwater sterilization, material surface treatment, biomedicine, and the like.
At present, most of researches on underwater pulse discharge are on discharge of a liquid-electric pulse and gas-liquid two-phase mixture in a single-phase body, and few research reports on three-phase discharge are reported; for a gas-liquid mixture reactor, the electric field in the bubbles near the high-voltage electrode is relatively strong, so that ionization breakdown is easy to occur, but the space-time distribution of the discharge bubbles in a certain voltage range presents larger randomness due to the complex flow state of the bubbles; the large amount of high concentration liquid leads to more frequent electron collisions and lower charge mobility, and the high voltage pulse discharge characteristics are easily affected by the solution conductivity and the water content of the liquid.
The research on the gas-liquid-solid three-phase high-voltage pulse discharge device is less after the data are consulted. In a patent CN201020672259, "an underwater pulsed rf plasma discharge device for wastewater treatment", a part of the power electrode and a part of the grounding electrode of the device are immersed in water in a water collecting tank, and a pulsed rf field is used to instantaneously heat and evaporate the solution to form a local low-density bubble or gas layer area on the surface of the electrode, where the pulsed rf field breaks down the gas, thereby exciting and generating a pulsed rf plasma. In our device, gas is introduced, and loaded TiO is filled between two electrodes2The quartz small ball reduces the discharging difficulty by utilizing the bubbles retained in the small ball gap, and has higher efficiency. In the patent, the glass container of the opposite device as the water collecting tank has a diameter of 100mm, and an electromagnetic shielding box is arranged on the periphery, so that the whole structure is more complex than that of the device. In the patent of contrast, the other side's device can not carry out cyclic utilization to the gas that produces, and this work can realize the cyclic utilization to gas-liquid diphase, and the resource utilization who improves is an environment-friendly experimental apparatus.
Disclosure of Invention
Based on the application and research status of underwater pulse discharge, it is necessary to develop a high-voltage pulse discharge active component generating device under a gas-liquid-solid three-phase environment, and after a solid phase is added into a gas-liquid two-phase body to form three-phase discharge, the solid phase retains bubbles in a discharge area, so that the discharge difficulty of the gas-liquid two-phase body is reduced. Compared with gas-liquid two-phase discharge, the discharge in the gas-liquid-solid three phases not only has the discharge breakdown of gas, but also has the surface discharge and partial discharge of solid particles, and simultaneously, the discharge also exists between the adjacent solid particles, so that the breakdown voltage is further reduced, and the discharge difficulty in the gas-liquid two phases is reduced. Meanwhile, a catalyst can be loaded on the solid phase to cooperate with ultraviolet rays and active ingredients generated by discharge to improve the water treatment efficiency.
The influence of the solutions in different states on the electrical characteristics of high-voltage pulse discharge in a gas-liquid-solid three-phase discharge environment is explored, and the underwater pulse discharge technology has a promoting effect on the wide application in the fields of wastewater treatment and the like. The invention provides a gas-liquid-solid three-phase pulse discharge electrical characteristic research experiment and a method thereof, and the specific technical scheme is as follows:
a gas-liquid-solid three-phase pulse discharge electrical characteristic research experimental device comprises a gas-liquid-solid three-phase discharge reactor, a high-voltage nanosecond pulse power supply, an electrical parameter detection unit, an active ingredient detection unit, a voltage regulating transformer, an isolation transformer, an air pump, a liquid pump, a gas flowmeter, a liquid flowmeter, a gas-liquid separator, a buffer air chamber, a water storage tank A, a water storage tank B and a pressure regulating valve;
the gas-liquid-solid three-phase discharge reactor is provided with an air inlet, an air outlet, a water inlet and a water outlet, a water sample to be treated is connected with an inlet of a water storage tank B, an outlet of the water storage tank B is connected with an inlet of a liquid pump, an outlet of the liquid pump is connected with an inlet of a liquid flow meter, an outlet of the liquid flow meter is connected with a water inlet of the gas-liquid-solid three-phase discharge reactor, a water outlet of the gas-liquid-solid three-phase discharge reactor is connected with an inlet of a water storage;
the gas outlet of the gas-liquid-solid three-phase discharge reactor is connected with the inlet of a gas-liquid separator, the outlet of the gas-liquid separator is respectively connected with the inlet of a buffer gas chamber and the inlet of a water storage tank A, a gas source is connected with the inlet of the buffer gas chamber through a pressure regulating valve, the outlet of the buffer gas chamber is connected with the inlet of a gas pump, the outlet of the gas pump is connected with the inlet of a gas flowmeter, and the outlet of the gas flowmeter is connected with the gas inlet of;
the isolation transformer, the voltage regulating transformer and the high-voltage nanosecond pulse power supply are sequentially connected, the isolation transformer is connected with a mains supply, the high-voltage nanosecond pulse power supply is connected with the gas-liquid-solid three-phase discharge reactor, and the gas-liquid-solid three-phase discharge reactor is connected with the electric parameter detection unit.
The gas-liquid-solid three-phase discharge reactor comprises an upper part, a middle part and a lower part, wherein the middle part is a stainless steel cylinder, and the upper part and the lower part are both made of polytetrafluoroethylene materials. The upper part comprises a water outlet, a gas outlet and an upper insulating baffle, the lower part comprises a gas inlet, a water inlet, a lower insulating baffle and an electrode bracket, and the upper part and the lower part are respectively connected with a middle stainless steel cylinder body through threads. The stainless steel cylinder body comprises a high-voltage electrode and is filled with solid-phase pellets; the upper end of the high-voltage electrode penetrates through the upper insulating baffle, and the lower end of the high-voltage electrode is fixed above the lower insulating baffle through an electrode support.
The high-voltage electrode is provided with threads, and the high-voltage electrode is made of tungsten, molybdenum, titanium, stainless steel, tungsten-molybdenum alloy or titanium alloy.
The material of above-mentioned upper and lower insulating barrier is one in polytetrafluoroethylene, the organic glass material, sets up the aperture of array on the upper and lower insulating barrier, and the array aperture of going up insulating barrier can be so that the aqueous vapor in the reactor that discharges flows, and the array aperture on the lower insulating barrier is used for becoming the bubble with the gas that lets in, further reduces the degree of difficulty of discharging.
The electrode support is made of one of quartz, glass and ceramic.
The solid-phase pellets are made of glass or quartz, and the diameter of the pellets is within the range of 0.50mm-5.00 mm.
The surface of the solid-phase small ball is loaded with a catalyst.
The catalyst is titanium dioxide or the combination of titanium dioxide and graphene oxide.
A gas-liquid-solid three-phase pulse discharge electrical characteristic research experiment method utilizes the device and comprises the following steps:
step 1: opening a valve between a water sample to be treated and the water storage tank B, enabling the water sample to be treated to enter the water storage tank B, and closing the valve after the water storage tank B is full;
step 2: opening a pressure valve and an air pump to enable air to circulate in the gas-liquid-solid three-phase discharge reactor;
step 3: opening a one-way valve between a liquid flowmeter and a water inlet of the gas-liquid-solid three-phase discharge reactor, opening a liquid pump, and turning on a power supply to perform discharge treatment when liquid begins to flow into the gas-liquid-solid three-phase discharge reactor;
step 4: when the water storage tank B is empty, the power supply, the liquid pump, the air pump and the pressure valve are closed;
step 5: opening a valve between the water storage tank A and the water storage tank B to enable all water samples in the water storage tank A to flow into the water storage tank B, then closing the valve, if the water samples are circularly processed, returning the flow to Step2, and after the experiment is finished, closing a power supply, a high-pressure liquid pump system, an air pump and all valves;
if the water sample is not circularly treated, the experimental platform is operated according to Step1, Step2, Step3 and Step 4; after the experiment is completed, the power supply, the high-pressure liquid pump system, the air pump and all the valves are closed.
If the active ingredient content of the processed water sample is detected in the experimental process or after the experiment, a valve between the water storage tank A and the active ingredient detection unit is opened, the processed water sample in the water storage tank A flows to the active ingredient detection unit, and the real-time detection of the active ingredient in the processed water sample is realized.
The liquid phase discharge plasma technology is a novel water treatment advanced oxidation technology, and is an ideal and potential technology for treating biodegradable organic wastewater such as papermaking, pharmacy, printing and dyeing and the like.
In theory, alternating current, direct current and pulse electric fields can be used for liquid phase discharge, but high-voltage pulse discharge has nanosecond-scale rising and falling edges and narrow pulse width, the electric field change rate in a discharge gap is larger, and a medium in a discharge electrode is easier to break down to generate active ingredients. The high-voltage nanosecond pulse power supply can improve the processing capacity of a reactor with a wide electrode distance, increase the discharge stability, enhance the mass transfer efficiency of a discharge plasma reactor, and continuously and stably generate and maintain non-equilibrium plasma, so that pulse discharge in water is widely applied in recent years. The underwater pulse discharge technology can generate plasma in liquid, and the process can simultaneously generate four effects of shock waves, ultraviolet rays, strong oxidation free radicals and strong electric fields.
In order to prolong the retention time of gas in the reactor and reduce the difficulty of discharge reaction, the invention is realized by filling solid-phase pellets between two electrodes. After a solid phase is added into a gas-liquid two-phase body to form three-phase discharge, not only discharge breakdown of gas exists, but also surface discharge and partial discharge of solid particles exist, and discharge also exists between adjacent solid particles. The discharge space-time distribution in the reactor is more uniform, the discharge state is more stable, the amount of the generated active substances is more, and simultaneously, due to the action of the medium particle bed layer, the mass transfer and the chemical action are more favorably realized.
Drawings
FIG. 1 is a block diagram of an embodiment of the apparatus of the present invention;
FIG. 2 is a schematic diagram of an apparatus according to an embodiment;
FIG. 3 is an overall structural view of a gas-liquid-solid three-phase discharge reactor;
FIG. 4 is a longitudinal structural view of the inside of a gas-liquid-solid three-phase discharge reactor;
FIG. 5 is a schematic representation of a solid phase pellet;
FIG. 6 is a schematic structural view of upper and lower insulating barriers;
FIG. 7 is a side view of FIG. 6;
FIG. 8 is a schematic view of a protective sheath;
FIG. 9 is an energy acquisition and calculation flow;
FIG. 10 is a waveform of power supply to the gas-liquid-solid three-phase discharge reactor in the second embodiment;
FIG. 11 is a gas-liquid-solid three-phase discharge reactor power spectrum of example two;
FIG. 12 is the experimental operating flow of example three;
FIG. 13 is a flow chart of finding the critical breakdown voltage for different conductivities of example three;
FIG. 14 is a flowchart of water cut control in the fourth embodiment;
FIG. 15 is a flowchart of finding the critical breakdown voltage for different water cut in the fourth embodiment.
Detailed Description
The invention is further described below with reference to the accompanying drawings. The following examples are only for illustrating the technical solutions of the present invention more clearly, and the protection scope of the present invention is not limited thereby.
As shown in fig. 1, the experimental device for researching gas-liquid-solid three-phase pulse discharge electrical characteristics comprises a gas-liquid-solid three-phase discharge reactor, a high-voltage nanosecond pulse power supply, an electrical parameter detection unit, an active component detection unit, a voltage regulation transformer, an isolation transformer, an air pump, a liquid pump, a gas flowmeter, a liquid flowmeter, a gas-liquid separator, a buffer air chamber, a water storage tank A, a water storage tank B and a pressure regulating valve;
the gas-liquid-solid three-phase discharge reactor is provided with an air inlet, an air outlet, a water inlet and a water outlet, a water sample to be treated is connected with an inlet of a water storage tank B, an outlet of the water storage tank B is connected with an inlet of a liquid pump, an outlet of the liquid pump is connected with an inlet of a liquid flow meter, an outlet of the liquid flow meter is connected with a water inlet of the gas-liquid-solid three-phase discharge reactor, a water outlet of the gas-liquid-solid three-phase discharge reactor is connected with an inlet of a water storage;
the gas outlet of the gas-liquid-solid three-phase discharge reactor is connected with the inlet of a gas-liquid separator, the outlet of the gas-liquid separator is respectively connected with the inlet of a buffer gas chamber and the inlet of a water storage tank A, a gas source is connected with the inlet of the buffer gas chamber through a pressure regulating valve, the outlet of the buffer gas chamber is connected with the inlet of a gas pump, the outlet of the gas pump is connected with the inlet of a gas flowmeter, and the outlet of the gas flowmeter is connected with the gas inlet of;
the isolation transformer, the voltage regulating transformer and the high-voltage nanosecond pulse power supply are sequentially connected, the isolation transformer is connected with a mains supply, the high-voltage nanosecond pulse power supply is connected with the gas-liquid-solid three-phase discharge reactor, and the gas-liquid-solid three-phase discharge reactor is connected with the electric parameter detection unit.
As shown in fig. 3 and 4, the gas-liquid-solid three-phase discharge reactor comprises an upper part, a middle part and a lower part, wherein the middle part is a stainless steel cylinder 1, and the upper part and the lower part are both made of polytetrafluoroethylene materials. The upper part comprises a water outlet, a gas outlet and an upper insulating baffle 3, the lower part comprises a gas inlet, a water inlet, a lower insulating baffle 4 and an electrode bracket 5, and the upper part and the lower part are respectively connected with a middle stainless steel cylinder body through threads. The stainless steel cylinder body comprises a high-voltage electrode 2 and is filled with solid-phase pellets; the upper end of the high-voltage electrode penetrates through the upper insulating baffle 3, and the lower end of the high-voltage electrode is fixed above the lower insulating baffle 4 through the electrode support 5.
The high-voltage electrode 2 is provided with threads, the curvature radius of the surface of the raised threads is smaller, the local electric field is stronger, and the high-voltage electrode is more beneficial to breaking down a medium between the two electrodes compared with a smooth surface. The high voltage electrode 2 is made of tungsten, molybdenum, titanium, stainless steel, tungsten-molybdenum alloy or titanium alloy.
As shown in fig. 6, the upper and lower insulating baffles are made of one of teflon and organic glass, and the upper insulating baffle 3 is provided with small holes in an array, so that water vapor in the discharge reactor can flow out. The array small holes on the lower insulating baffle 4 have the functions of dispersing air introduced into the reactor to generate uniform bubbles so as to reduce the reaction difficulty, and have the functions of fixing the electrodes to prevent toppling; the insulating baffle is embedded with the metal electrode with threads through the electrode bracket and is used for fixing the electrode and preventing the electrode from toppling;
as shown in FIG. 7, the insulating barrier has an outer diameter d2Thickness of h1With a central opening having a diameter d1The light hole is used for placing the electrode bracket; the surface is provided with an array of small holes, andis 3 layers and arranged at equal intervals; diameter of the small hole is d3To make the diameter d4The quartz small balls are put into the reactor and cannot block the small holes to influence the introduction of water and gas, so that the diameter of the small holes and the diameter of the quartz small balls meet the condition that the center distance of any two adjacent small holes is larger than that of any two adjacent quartz small balls, and the following relational expression is met, wherein delta diThe center distance between any two small holes is as follows:
Δdi<d4(1)。
as shown in fig. 8, the electrode holder is made of one of quartz, glass, and ceramic. Because high-voltage discharge can generate local high temperature, the electrode support can prevent the contact point of the metal electrode and the insulating baffle from generating local high-temperature damage. The diameter of the insulating baffle plate of the electrode bracket with the small-diameter cylindrical end inserted into the bottom of the device is d1In the light aperture of (a); the material is glass, quartz or ceramic, which has high insulation property, prevents the high-voltage electrode from discharging to the bottom of the reactor, and has higher melting point, so that the glass, quartz or ceramic is not melted due to high temperature of reaction; the electrode sleeve is of a double-step structure, and the diameter of the upper end cylinder is d5High is h2The diameter of the lower end cylinder is d1High is h3The upper end surface is provided with a diameter d1Depth h4The cylindrical groove is used for fixing the high-voltage electrode.
As shown in FIG. 5, the solid-phase pellets are made of glass or quartz, and the diameter of the pellets is in the range of 0.50mm to 5.00 mm. The surface of the solid-phase pellet may or may not be loaded with a catalyst. Solid-phase pellets are filled in the gap between the two electrodes, and in the process of introducing water and gas, bubbles staying in the gaps of the pellets can provide conditions for reducing the discharge difficulty. If the solid-phase pellets are loaded with the catalyst, the treatment efficiency can be effectively improved in practical application, such as water treatment. The solid-phase pellets are generally made of glass or quartz. The diameter 2R of the small ball is generally designed to be in the range of 0.50mm-5.00mm, if the small ball is too small, the gas introduced into the reactor is not easy to be changed into bubble shape, and the blockage in the reactor is easy to cause; if the small balls are too large, the specific surface area is small, the amount of the surface-loaded catalyst is small, and the effect of degrading organic matters or toxic substances in the wastewater by the synergetic catalysis is reduced.
The catalyst supported on the solid beads is usually titanium dioxide. The titanium dioxide is excited by ultraviolet ray generated by discharge to form superoxide ion free radical (O)2 -) And hydroxyl free radical (. OH), can penetrate the bacterial cell wall adsorbed on the surface of the solid-phase pellet, destroy the cell membranous substance and effectively kill bacteria; under the condition of illumination, the titanium dioxide can lead organic matters in water to generate oxidation-reduction reaction, and finally become harmless substances such as carbon dioxide, water and the like which are harmless to the environment.
The titanium dioxide loading process comprises the following steps: selecting quartz spheres with particle size of 0.50-5.00 mm, sintering to obtain porous quartz spheres, and soaking the spheres in butyl titanate (Ti (OC)4H9)4) And slowly lifting the solution in the alcohol solution, and blowing the solution by using a fan to promote the volatilization of the alcohol so as to enable the solution to generate a titanic acid film on the surface of the quartz pellet. Then placing the porous quartz pellets in a furnace with the temperature of 350-2A film.
The catalyst supported on the solid-phase pellets can also be a combination of titanium dioxide and graphene oxide. Graphene oxide is a single atomic layer that can be extended to tens of microns in lateral dimension at any time. Thus, its structure spans the typical dimensions of general chemistry and material science. Graphene oxide can be considered a non-traditional soft material with properties of polymers, colloids, films, and amphiphilic molecules. After being oxidized, the graphene has more oxygen-containing functional groups, so that the graphene has more active properties than the graphene, and can improve the properties of the graphene through various reactions with the oxygen-containing functional groups.
The invention combines titanium dioxide and graphene oxide and attaches the titanium dioxide and the graphene oxide to the solid-phase pellets together. Firstly, the solid-phase pellets are soaked in a mixed solution of HF (hydrofluoric acid) and NaF (sodium fluoride), then graphene oxide is added in a heating environment, and the process of attaching the graphene oxide to the solid-phase pellets has high requirements on the dosage of the solution, the heating temperature and the time. The graphene oxide is attached to the solid-phase pellets, so that the specific surface area of the titanium dioxide catalyst is further increased, and meanwhile, the efficiency of catalytically degrading organic matters and inorganic matters in water is further improved by utilizing the characteristics of the graphene oxide and cooperating with the graphene oxide and the titanium dioxide.
The present invention detects the amount of active ingredient produced by the absorbance method. Adding a certain amount of liquid to be detected into a chromogenic reagent, fully mixing, standing, fully reacting the chromogenic reagent with the detected active component, detecting by using an ultraviolet-visible spectrophotometer to obtain an absorbance characteristic peak of the reacted generated substance, wherein the wavelength of the characteristic peak is different from that of the original detected substance, and calculating by using the intensity of the characteristic peak to obtain the generation amount of the detected active component. The color reaction can use ozone and nitrite nitrogen color reagent of the giga-swan. In addition, the amount of active ingredient produced can be measured directly by a liquid phase concentration meter, such as a Gieser and Swan ozone meter (GDYS-101SC2), a nitrite nitrogen meter (GDYS-101SX3), and a Kyoritsuchemical-check Lab2O2)。
The first embodiment is as follows:
as shown in FIG. 2, the structure of the experimental platform realizes a gas-liquid-solid three-phase high-voltage pulse discharge water treatment experimental system. The voltage of the output end of the high-voltage nanosecond pulse power supply is in positive correlation with the voltage of the input end, and the voltage of the input end of the high-voltage nanosecond pulse power supply can be changed by rotating a knob of the voltage regulating transformer, so that the voltage of the output end of the high-voltage nanosecond pulse power supply is changed.
As shown in FIG. 2, a high-voltage nanosecond pulse power supply provides high-voltage pulse excitation for a discharge reactor, a high-voltage probe VP (North Star: PVM-5) collects voltage at a gas-liquid-solid three-phase discharge reactor end, a high-frequency current probe CS (Pearson: 6595) collects current at the discharge reactor end, and a mixed domain digital oscilloscope (Tektronix: MDO3054) monitors a supply voltage current waveform at the gas-liquid-solid three-phase discharge end. A water storage tank B for storing the original water sample to be treated, a one-way throttle valve Vl1Controlling the on-off of the water sample to be treated flowing to the water storage tank B. MlThe system is a liquid pump with adjustable flow, and can pump the original water sample in the water storage tank B into the discharge reactor from a water inlet. FlIs a liquid flowmeter for monitoring the liquid flowing to gas-liquid-solid three-phase discharge reactorThe flow rate. One-way throttle valve Vl2The on-off of the water sample in the water storage tank B from the water inlet to the reactor is controlled, and meanwhile, the liquid is prevented from flowing back from the water inlet. The water storage tank A stores the water sample after the discharge treatment and the one-way throttle valve Vl3Controlling the on-off of the water sample in the water storage tank A flowing to the water storage tank B. One-way throttle valve Vl4Controlling the on-off of the water sample in the water storage tank A flowing to the active ingredient detection unit.
MgThe gas in the buffer gas chamber can be pumped into the gas-liquid-solid three-phase discharge reactor from the gas inlet by the gas pump with adjustable flow. FgThe gas flowmeter is used for monitoring the instantaneous flow of gas flowing to the gas-liquid-solid three-phase discharge reactor. One-way throttle valve VgThe on-off of the gas in the buffer gas chamber flowing to the gas-liquid-solid three-phase discharge reactor from the gas inlet is controlled, and meanwhile, liquid is prevented from flowing back to the gas inlet pump from the gas inlet. The gas-liquid separator can separate the wet gas from the gas outlet into gas and liquid, the dry gas is introduced into the buffer gas chamber again, and the liquid flows into the water storage tank A again. The buffer gas chamber stores residual gas and gas generated by the reaction. The pressure valve controls air in the air source to supplement and enter the buffer air chamber, and the air pressure of the internal circulation of the device is kept constant, so that the air circularly flows in the gas-liquid-solid three-phase discharge reactor.
The workflow of the whole application platform is as follows:
step 1: opening valve Vl1Water sample to be treated enters a water storage tank B, and a valve V is closed after the water storage tank B is filledl1。
Step 2: opening the pressure valve and the air pump MgAnd circulating the gas in the gas-liquid-solid three-phase discharge reactor.
Step 3: opening one-way throttle valve Vl2Opening the liquid pump Ml. When liquid begins to flow into the gas-liquid-solid three-phase discharge reactor, a power supply is turned on for discharge treatment.
Step 4: when the water storage tank B is empty, the power supply and the liquid pump M are turned offlAir pump MgAnd a pressure valve.
Step 5: opening valve Vl3The water sample of the water storage tank A flows into the water storage tank B completely, and then V is closedl3. If the water sample is circularly processedThe flow returns to Step 2. After the experiment is completed, the power supply, the high-pressure liquid pump system, the air pump and all the valves are closed.
If the water samples are not circularly treated, the experimental platform is operated according to Step1, Step2, Step3 and Step 4. After the experiment is completed, the power supply, the high-pressure liquid pump system, the air pump and all the valves are closed.
If the active ingredient content of the processed water sample is detected in the experimental process or after the experiment, the Vl4 is opened, the processed water sample in the water storage tank A flows to the active ingredient detection unit, and the real-time detection of the active ingredient in the processed water sample is realized.
Example two: analyzing the correlation characteristics of energy and active ingredients under different breakdown voltages:
breakdown voltage definition:
in a gas-liquid-solid three-phase high-voltage nanosecond pulse discharge reactor, a high-strength electric field can break down a medium between two electrodes to form a discharge channel. Once the discharge channel is formed, the load of the reactor is instantaneously reduced, the current flowing through the discharge reactor is suddenly increased, and the power supply voltage at the end of the discharge reactor is suddenly reduced due to the limited power of the power supply. And (3) judging whether breakdown occurs or not by observing the voltage and current waveforms of the discharge reactor end on the oscilloscope. When the voltage amplitude of the discharge reactor suddenly rises and the current amplitude suddenly falls instantaneously, the dielectric between the two electrodes is considered to be broken down under the high-intensity electric field, and the power supply voltage of the discharge reactor end is called as breakdown voltage.
And (3) defining the water content:
in this embodiment, the water content is changed by fixing the conductivity of the solution and changing the ratio of water to gas introduced into the reactor by controlling the variation method.
Water cut α is defined as the ratio of the volume of a water sample to the total volume of the water sample and gas:
wherein the volume V of the water samplelTotal volume V of water sample and gastCan be expressed by the following formula:
Vl＝svlt (7)
Vt＝svlt+svgt (8)
s represents the cross-sectional area in the water inlet direction of the reactor, vlIs the flow velocity, v, of the water sample in the reactorgThe water cut α can also be expressed by the following equation:
the product of the cross-sectional area and the flow velocity is equal to the flow, and the flow Q of the introduced water samplelThe flow rate of the introduced gas is QgThe unit of flow is LPM (liter per minute), and the total flow Q of the introduced water and the air istThe formula is as follows:
Qt＝Ql+Qg(10)
the water cut α can also be defined as the ratio of the water sample flow to the total flow of water sample and gas:
in this embodiment, by holding QtSetting different water content without changing, and calculating corresponding QlAnd Qg。
Energy acquisition and calculation process:
fig. 7 shows the flow of the power supply energy acquisition and calculation at the end of the discharge reactor. And after the water content and the water sample conductivity are determined, the high-voltage nanosecond pulse power supply starts to excite the discharge reactor. The voltage at the end of the discharge reactor was collected with a high voltage probe (North Star, PVM-5) and the current at the end of the discharge reactor was collected with a high frequency current probe (Pearson, 6595). The supply voltage current waveform at the end of the discharge reactor was monitored with a mixed domain digital oscilloscope (Tektronix, MDO 3054). And if the discharge breakdown condition defined above occurs, storing the voltage and current waveform data displayed on the current oscilloscope, and exporting the data to the USB flash disk. And if the dielectric between the two electrodes is not broken down under the current experimental condition, adjusting the voltage at the front end of the power supply until the voltage current waveform on the oscilloscope changes suddenly.
The obtained voltage and current waveform data are plotted in Origin, and the energy applied to the discharge reactor by a single pulse is calculated by using an instantaneous power method and a full width half maximum method.
The total flow of the fixed water and the gas is QtUnder the condition of certain water content and water sample conductivity, when the breakdown voltage of the end of the discharge reactor is different, the power supply energy and the active ingredient content on the reactor are different.
When the voltage and current waveforms on the load are compared regularly, the instantaneous power method is suitable for calculating the power supply energy, as shown in fig. 10, the voltage and current waveforms are multiplied to obtain the instantaneous power spectrum as shown in fig. 11, and then the full-width-at-half-maximum (FWHM) method is used to obtain the power supply energy. Energy E in a Single Pulse periodspThe expression of (a) is:
Esp＝∑Pi·ti(2)
in equation (2), Pi is the ith power peak, and ti is the time taken by the ith power half-peak.
Total power supply energy E in discharge duration t timetThe expression of (a) is:
Et＝t×f×Esp(3)
wherein f is the pulse repetition frequency of the high-voltage nanosecond pulse power supply.
The experimental data are shown in Table 1
TABLE 1
Example three: experiment for exploring critical breakdown voltage law and active ingredient generation characteristics under different solution conductivities
The solution conductivity is an important factor affecting the critical breakdown voltage and the active ingredient generation characteristics, and therefore, the rule of the critical breakdown voltage and the active ingredient generation characteristics under the condition of not affecting the solution conductivity needs to be researched. Independent variables such as water content, total gas-liquid flow, discharge time and the like are kept unchanged, the conductivity of each solution is changed, and the rule of critical breakdown voltage and the generation characteristic of active ingredients under the condition of not connecting the conductivity of the solution are researched through experiments.
The preparation method of the solution with different conductivities comprises the following steps:
determining the required conductivity range, equally dividing to obtain experiment conductivity numerical value points, and preparing. Firstly, calculating the mass of a conductive solute required to be added when a certain volume of deionized water reaches a certain conductivity, weighing quantitative conductive solute crystals, adding the weighed conductive solute crystals into a water tank filled with deionized water, fully mixing and standing.
The calculation process of the mass of the required conductive solute under a certain solution conductivity is as follows:
the upper formula ismIs molar conductivity, in units of S.m2·mol-1Refers to the conductance achieved when a solution containing 1mol of electrolyte is placed between two parallel electrodes of a conductance cell spaced apart by a unit distance;
the unit of ultimate molar conductivity is the same molar conductivity, which means that the molar conductivity can really reflect the conductivity of the strong electrolyte only by the infinite dilution of the solution due to the interaction of ions of the solution, and is called ultimate molar conductivity, and the ultimate molar conductivity is specific to a specific substance
Is a constant, taking the conductive solute as NaCl for example:
β is a constant related to temperature, electrolyte and solvent oil pipe, c is the mass concentration of solute in mol m-3。
Molar conductivity ΛmWith a conductivity k, the quantity concentration c of solute speciesThe following relationship:
the above formula k is the solution conductivity with the unit of S.m-1Measured by a DDS-11A digital display conductivity meter.
The quantity concentration c of the solute substance can be obtained by combining the two types (4) and (5). And then the mass m of the required conductive solute can be obtained according to the following formula:
m＝c·V·M (6)
m is the mass of the required conductive solute and is g; v is the volume of deionized water and is expressed in L; m is the molar mass of solute in g.mol-1，M(NaCl)＝58.5g·mol-1。
The conductive solute can be selected from strong electrolyte salts such as NaCl, KCl, NaNO3And the analytical purification is adopted, so that the solution conductivity error is reduced. Through the calculation, the solutions with different conductivities can be prepared, and the solution is prepared in situ at present so as to ensure the accuracy of the conductivity of the solution.
Fig. 12 is a flowchart of an experiment for exploring the critical breakdown voltage law and the generation characteristics of active ingredients under different conductivities. The method comprises the following steps:
step 1: solution preparation
And calculating the mass of the solute required under different conductivity experimental points and fully mixing the solute with a certain volume of deionized water to obtain a water sample to be treated.
Step 2: regulating gas-liquid two-phase flow
After the water content is fixed, the liquid flow and the gas flow are respectively calculated, and the gas pump and the liquid pump are adjusted to enable the two-phase flow to reach the budget value.
Step 3: discharge seeking breakdown voltage
And opening an air pump and a liquid pump, starting a power supply output button when gas-liquid two phases at the tail end of a water outlet pipe of the reactor are stably output, starting discharging, observing current and voltage waveforms on an oscilloscope in the discharging period, reducing the voltage until the voltage cannot be punctured if the voltage is punctured, finding out the critical breakdown voltage, recording and collecting data, and increasing the voltage until the voltage is punctured if the voltage is not punctured, and finding out the critical breakdown voltage, recording and collecting the data.
Step 4: detection of amount of active ingredient produced
And after the single test is finished, taking 25.00mL of discharged water sample as a water sample to be detected, and detecting the active ingredients.
Step 5: energy efficiency ratio calculation
And calculating the energy of one discharge cycle by using the collected current and voltage data and a full width at half maximum method, and dividing the generation amount of the active ingredients by the energy of one discharge cycle to obtain the energy efficiency ratio.
Step 6: image rendering
And (3) taking the conductivity of the solution as an abscissa and respectively taking the generation amount of the active ingredient and the critical breakdown voltage as an ordinate to make an image.
The experimental data is reported in table 2 below:
TABLE 2
The method for finding the relation between the solution conductivity and the critical breakdown voltage under the same water content comprises the following steps:
as shown in fig. 13, to explore the critical breakdown voltage and the active component generation correlation characteristics of different solution conductivities, the solution conductivity range required by the experiment is determined first, the experiment conductivity points are obtained by averaging, the voltage is gradually increased from the smaller power input voltage for different solution conductivities, the voltage and current waveforms on the oscilloscope are observed at the same time, whether the voltage is the breakdown voltage or not can be determined according to the shape characteristics of the voltage and current waveforms corresponding to the breakdown voltage, and the breakdown voltage found for the first time is the critical breakdown voltage. And then recording the voltage and current peak value-peak value displayed on the oscilloscope, storing the voltage and current data by using a mobile hard disk through a USB interface on the oscilloscope, and drawing a relation curve of the critical breakdown voltage and the solution conductivity.
Example four: experiment for exploring critical breakdown voltage law and active ingredient generation characteristics under different water contents
And (3) defining the water content:
in this embodiment, the water content is changed by fixing the conductivity of the solution and changing the ratio of water to gas introduced into the reactor by controlling the variation method.
Water cut α is defined as the ratio of the volume of a water sample to the total volume of the water sample and gas:
wherein the volume V of the water samplelTotal volume V of water sample and gastCan be expressed by the following formula:
Vl＝svlt (7)
Vt＝svlt+svgt (8)
s represents the cross-sectional area in the water inlet direction of the reactor, vlIs the flow velocity, v, of the water sample in the reactorgThe water cut α can also be expressed by the following equation:
the product of the cross-sectional area and the flow velocity is equal to the flow, and the flow Q of the introduced water samplelThe flow rate of the introduced gas is QgThe unit of flow is LPM (liter per minute), and the total flow Q of the introduced water and the air istThe formula is as follows:
Qt＝Ql+Qg(10)
the water cut α can also be defined as the ratio of the water sample flow to the total flow of water sample and gas:
in this embodiment, by holding QtSetting different water content without changing, and calculating corresponding QlAnd Qg。
The adjusting method comprises the following steps:
as shown in FIG. 15, in the air pump MgA valve V is additionally arranged between the reactor and the reactorgIn the liquid pump MlA valve V is additionally arranged between the reactor and the reactorl2The gas-liquid flow is controlled by adjusting a valve. VgThe one-way throttle valve enables the gas to flow to the reactor in one way only by the gas pump. Vl2And is also a one-way throttle valve, so that the liquid can only flow to the reactor in one way through the liquid pump.
The gas flowmeter Fg and the liquid flowmeter Fl are used for displaying the current flow rate of the gas and the liquid introduced into the reactor.
FIG. 14 is a flowchart of a method for adjusting the water content. At the beginning of the experiment, the valve Vl1 is opened first, and when the water storage tank B is full, the Vl1 is closed. The liquid pumps Ml, Vl2 were turned on to pump the liquid into the discharge reactor. Ml is adjusted so that the reading of Fg equals Ql.
Opening the pressure valve and the air pump Mg、VgAnd pumping the gas source into the discharge reactor. Regulating MgSo that the gas flowmeter FgThe reading is equal to Qg. Due to pressure disturbances between the incoming liquid and gas, FgAnd FlIndication of and Ql、QgWith slight difference, fine-tuning Ml、MgSo that they are identical. And after the regulation is finished, turning on the power supply to start discharging.
Finding the critical breakdown voltage:
as shown in fig. 15, to explore the critical breakdown voltage and the active component generation correlation characteristics of different fluid water contents, the fluid water content range required by the experiment is determined, the water content points are obtained by averaging, the voltage is gradually increased from the smaller power input voltage for different fluid water contents, the voltage and current waveforms on the oscilloscope are observed, when the voltage waveform suddenly decreases, the instantaneous voltage when the current waveform suddenly increases is the breakdown voltage, and the breakdown voltage found for the first time is the critical breakdown voltage. And then recording the peak value-peak value of the voltage and current displayed on the oscilloscope, storing the group of voltage and current data by using a mobile hard disk through a USB interface on the oscilloscope, and drawing a relation curve of the critical breakdown voltage and the water content of the fluid.
The above description is only a preferred embodiment of the present invention, and it should be noted that, for those skilled in the art, several modifications and variations can be made without departing from the technical principle of the present invention, and these modifications and variations should also be regarded as the protection scope of the present invention.
Claims (9)
1. A gas-liquid-solid three-phase pulse discharge electrical characteristic research experimental device is characterized by comprising a gas-liquid-solid three-phase discharge reactor, a high-voltage nanosecond pulse power supply, an electrical parameter detection unit, an active component detection unit, a voltage regulation transformer, an isolation transformer, an air pump, a liquid pump, a gas flowmeter, a liquid flowmeter, a gas-liquid separator, a buffer air chamber, a water storage tank A, a water storage tank B and a pressure regulating valve;
the gas-liquid-solid three-phase discharge reactor is provided with an air inlet, an air outlet, a water inlet and a water outlet, a water sample to be treated is connected with an inlet of a water storage tank B, an outlet of the water storage tank B is connected with an inlet of a liquid pump, an outlet of the liquid pump is connected with an inlet of a liquid flow meter, an outlet of the liquid flow meter is connected with a water inlet of the gas-liquid-solid three-phase discharge reactor, a water outlet of the gas-liquid-solid three-phase discharge reactor is connected with an inlet of a water storage;
the gas outlet of the gas-liquid-solid three-phase discharge reactor is connected with the inlet of a gas-liquid separator, the outlet of the gas-liquid separator is respectively connected with the inlet of a buffer gas chamber and the inlet of a water storage tank A, a gas source is connected with the inlet of the buffer gas chamber through a pressure regulating valve, the outlet of the buffer gas chamber is connected with the inlet of a gas pump, the outlet of the gas pump is connected with the inlet of a gas flowmeter, and the outlet of the gas flowmeter is connected with the gas inlet of;
the isolation transformer, the voltage regulating transformer and the high-voltage nanosecond pulse power supply are sequentially connected, the isolation transformer is connected with a mains supply, the high-voltage nanosecond pulse power supply is connected with the gas-liquid-solid three-phase discharge reactor, and the gas-liquid-solid three-phase discharge reactor is connected with the electric parameter detection unit.
2. The gas-liquid-solid three-phase pulse discharge electrical characteristic research experimental device of claim 1, characterized in that: the gas-liquid-solid three-phase discharge reactor comprises an upper part, a middle part and a lower part, wherein the middle part is a middle stainless steel cylinder body, the upper part and the lower part are both made of polytetrafluoroethylene materials, the upper part comprises a water outlet, a gas outlet and an upper insulating baffle, the lower part comprises a gas inlet, a water inlet, a lower insulating baffle and an electrode support, and the upper part and the lower part are respectively connected with the middle stainless steel cylinder body through threads; the stainless steel cylinder body comprises a high-voltage electrode and is filled with solid-phase pellets; the upper end of the high-voltage electrode penetrates through the upper insulating baffle, and the lower end of the high-voltage electrode is fixed above the lower insulating baffle through an electrode support.
3. The gas-liquid-solid three-phase pulse discharge electrical characteristic research experimental device of claim 2, characterized in that: the high-voltage electrode is provided with threads, and the high-voltage electrode is made of tungsten, molybdenum, titanium, stainless steel, tungsten-molybdenum alloy or titanium alloy.
4. The gas-liquid-solid three-phase pulse discharge electrical characteristic research experimental device of claim 2, characterized in that: go up insulating baffle, lower insulating baffle's material is one of polytetrafluoroethylene, organic glass material, goes up insulating baffle, sets up the aperture of array on the lower insulating baffle, and the array aperture of going up insulating baffle can be so that the aqueous vapor in the reactor that discharges flows, and the array aperture on the lower insulating baffle is used for becoming the bubble with the gas that lets in, further reduces the degree of difficulty of discharging.
5. The gas-liquid-solid three-phase pulse discharge electrical characteristic research experimental device of claim 2, characterized in that: the electrode support is made of one of quartz, glass and ceramic.
6. The gas-liquid-solid three-phase pulse discharge electrical characteristic research experimental device of claim 2, characterized in that: the solid-phase pellets are made of glass or quartz, and the diameter of the pellets is within the range of 0.50mm-5.00 mm.
7. The gas-liquid-solid three-phase pulse discharge electrical characteristic research experimental device of claim 2, characterized in that: the surface of the solid-phase small ball is loaded with a catalyst.
8. The gas-liquid-solid three-phase pulse discharge electrical characteristic research experiment device of claim 7, wherein: the catalyst is titanium dioxide or a combination of titanium dioxide and graphene oxide.
9. A gas-liquid-solid three-phase pulse discharge electrical characteristic research experiment method is characterized in that the device of claim 1 is utilized, and the method comprises the following steps:
step 1: opening a valve between a water sample to be treated and the water storage tank B, enabling the water sample to be treated to enter the water storage tank B, and closing the valve after the water storage tank B is full;
step 2: opening a pressure valve and an air pump to enable air to circulate in the gas-liquid-solid three-phase discharge reactor;
step 3: opening a one-way valve between a liquid flowmeter and a water inlet of the gas-liquid-solid three-phase discharge reactor, opening a liquid pump, and turning on a power supply to perform discharge treatment when liquid begins to flow into the gas-liquid-solid three-phase discharge reactor;
step 4: when the water storage tank B is empty, the power supply, the liquid pump, the air pump and the pressure valve are closed;
step 5: opening a valve between the water storage tank A and the water storage tank B to enable all water samples in the water storage tank A to flow into the water storage tank B, then closing the valve, if the water samples are circularly processed, returning the flow to Step2, and after the experiment is finished, closing a power supply, a high-pressure liquid pump system, an air pump and all valves;
if the water sample is not circularly treated, the experimental platform is operated according to Step1, Step2, Step3 and Step 4; after the experiment is finished, the power supply, the high-pressure liquid pump system, the air pump and all valves are closed;
if the active ingredient content of the processed water sample is detected in the experimental process or after the experiment, a valve between the water storage tank A and the active ingredient detection unit is opened, the processed water sample in the water storage tank A flows to the active ingredient detection unit, and the real-time detection of the active ingredient in the processed water sample is realized.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
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| CN201911413007.5A CN111137957A (en) | 2019-12-31 | 2019-12-31 | Gas-liquid-solid three-phase pulse discharge electrical characteristic research experimental device and method thereof |
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