CN103936110A - Domestic water electrolysis preparation device - Google Patents
Domestic water electrolysis preparation device Download PDFInfo
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- CN103936110A CN103936110A CN201410146256.3A CN201410146256A CN103936110A CN 103936110 A CN103936110 A CN 103936110A CN 201410146256 A CN201410146256 A CN 201410146256A CN 103936110 A CN103936110 A CN 103936110A
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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
- C02F1/46—Treatment of water, waste water, or sewage by electrochemical methods
- C02F1/461—Treatment of water, waste water, or sewage by electrochemical methods by electrolysis
- C02F1/467—Treatment of water, waste water, or sewage by electrochemical methods by electrolysis by electrochemical disinfection; by electrooxydation or by electroreduction
- C02F1/4672—Treatment of water, waste water, or sewage by electrochemical methods by electrolysis by electrochemical disinfection; by electrooxydation or by electroreduction by electrooxydation
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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
- C02F1/46—Treatment of water, waste water, or sewage by electrochemical methods
- C02F1/461—Treatment of water, waste water, or sewage by electrochemical methods by electrolysis
- C02F1/46104—Devices therefor; Their operating or servicing
- C02F1/46109—Electrodes
- C02F1/46114—Electrodes in particulate form or with conductive and/or non conductive particles between them
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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
- C02F1/46—Treatment of water, waste water, or sewage by electrochemical methods
- C02F1/461—Treatment of water, waste water, or sewage by electrochemical methods by electrolysis
- C02F1/46104—Devices therefor; Their operating or servicing
- C02F1/4618—Devices therefor; Their operating or servicing for producing "ionised" acidic or basic water
- C02F2001/46185—Devices therefor; Their operating or servicing for producing "ionised" acidic or basic water only anodic or acidic water, e.g. for oxidizing or sterilizing
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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
- C02F1/46—Treatment of water, waste water, or sewage by electrochemical methods
- C02F1/461—Treatment of water, waste water, or sewage by electrochemical methods by electrolysis
- C02F1/46104—Devices therefor; Their operating or servicing
- C02F1/4618—Devices therefor; Their operating or servicing for producing "ionised" acidic or basic water
- C02F2001/46195—Devices therefor; Their operating or servicing for producing "ionised" acidic or basic water characterised by the oxidation reduction potential [ORP]
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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
- C02F2201/46—Apparatus for electrochemical processes
- C02F2201/461—Electrolysis apparatus
- C02F2201/46105—Details relating to the electrolytic devices
- C02F2201/46115—Electrolytic cell with membranes or diaphragms
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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
- C02F2201/46—Apparatus for electrochemical processes
- C02F2201/461—Electrolysis apparatus
- C02F2201/46105—Details relating to the electrolytic devices
- C02F2201/4616—Power supply
- C02F2201/4617—DC only
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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
- C02F2201/46—Apparatus for electrochemical processes
- C02F2201/461—Electrolysis apparatus
- C02F2201/46105—Details relating to the electrolytic devices
- C02F2201/4616—Power supply
- C02F2201/46175—Electrical pulses
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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
- C02F2307/00—Location of water treatment or water treatment device
- C02F2307/02—Location of water treatment or water treatment device as part of a bottle
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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
- C02F2307/00—Location of water treatment or water treatment device
- C02F2307/04—Location of water treatment or water treatment device as part of a pitcher or jug
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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
- C02F2307/00—Location of water treatment or water treatment device
- C02F2307/10—Location of water treatment or water treatment device as part of a potable water dispenser, e.g. for use in homes or offices
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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
- C02F2307/00—Location of water treatment or water treatment device
- C02F2307/12—Location of water treatment or water treatment device as part of household appliances such as dishwashers, laundry washing machines or vacuum cleaners
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- Chemical Kinetics & Catalysis (AREA)
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- Environmental & Geological Engineering (AREA)
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- Water Treatment By Electricity Or Magnetism (AREA)
- Electrolytic Production Of Non-Metals, Compounds, Apparatuses Therefor (AREA)
Abstract
The invention relates to a domestic water electrolysis preparation device, and belongs to the technical field of water electrolysis equipment. The domestic water electrolysis preparation device comprises a water containing container, at least one pair of negative electrode and positive electrode arranged in the water containing container and an electrolysis power supply for supplying power to the negative electrode and the positive electrode, wherein a water permeable membrane is arranged between the paired negative electrode and positive electrode, and the water permeable hole diameter of the water permeable membrane is less than or equal to 2mm and is greater than or equal to 1 nanometer. When the domestic water electrolysis preparation device is used for electrolyzing water, lots of safe and usable oxidizing factors can be efficiently generated at low consumption, and oxidizing factors in the water can be effectively adjusted, so that the effect of washing and clearing pollutants in the water is intensified, and meanwhile, the requirements of users on the safety, functionality and the like of water are satisfied.
Description
Technical field
The present invention relates to a kind of apparatus for electrolyzing, belong to water electrolysis equipment technical field, do not belong to technical field of sewage.
Background technology
In reality, daily water consumption (not containing sewage) especially domestic water institute is contaminated more and more serious.Existing with medium absorption or adopt the filtering membrane in various apertures the nuisance in water to be tackled to the physics mode treatment process of filtering, because sorbing material is easy to saturated inefficacy, and various filtering membranes are easy to be contaminated by bacterial or organism blocks or breakage, practical situation are to reach the desired effects of purification quality of Design Theory, even the bacterium problem that exceeds standard is all difficult to solve, and is necessary to introduce the potent purification techniques of new water quality.On the other hand, follow social progress, people also propose some functional demands to daily water consumption.For example, expectation can strengthen water washability, remove dirt in washings, with energy-saving and emission-reduction, etc.For the above-mentioned demand to daily water consumption, more suitable is water body plasma discharge technology.
Plasma body is by a large amount of unbound electrons and ion forms and show as on the whole electroneutral material the 4th state.So-called water body plasma discharge technology, is to bring out discharge in water by appropriate ways, impels water molecules ionization to occur and excite.Water body plasma discharge technology specific form has multiple variation, and common trait is in water, to have a large amount of bubbles, and generate a large amount of strong oxidation factor (OH, H, H
2o
2, free oxygen, ozone etc.); Obviously for washing, the ultramicro air bubble in water can rinse dirt to peel off to washes inside by depth of penetration; And strong oxidation factor can be by the various pollutent efficient degradation in water body.Yet existing water body plasma discharge technology exists that initial exciting voltage is higher, erosion of electrode is serious, energy consumption is crossed high deficiency, is still difficult to apply in daily water consumption especially domestic water.
Chinese patent 1(ZL200480007381.0) publicity a kind ofly with so-called " virtual mesh point " discharge in water method, produce technology and the device of ionization sterilized water, for water body plasma discharge technology, for daily life, used water as very good try.Yet, this technology is not only subject to discharge mechanism and Practical manufacturing process technology limit (it is very little that anodic-cathodic spacing can not keep) efficiency to be difficult to improve, especially can not be according to the concrete water demand of the different occasions of daily water consumption, strong oxidation factor type and quantity that discharge in water is generated adjust accordingly; Therefore be of limited application.
As for generate the technology of strong oxidation factor in sewage disposal by electrolysis, due to sewage and daily water consumption gap in water quality very large, and electrolytic sewage processes and to belong to high energy consumption industrial technology, therefore completely different from the civilian technology of daily water consumption electrolysis.
Summary of the invention
Description by above-mentioned background technology can know, existing water technology is only for unitary demand and be difficult to reach, and still do not have at present a kind ofly can meet the water treatment device of people to the safety of daily water consumption and functional demand simultaneously.In daily water consumption field, need to seek a kind of reduce power consumption, micro discharges water body cold plasma efficient and water safety occurs, and the full and uniform release of the cold plasma of generation can be reached to technology or the device fully reacting with water simultaneously; In other words, need a kind of can reduce power consumption, the efficient water treatment device that produce the available oxidation factor of a large amount of safety, to, produce out the water of the suitable washing of strong detergency or there is the water of certain sterilizing ability the safety of daily water consumption or functional different demand according to people.
Therefore, the technical problem to be solved in the present invention is: propose a kind of can reduce power consumption and efficient electrolysis produce the available oxidation factor of a large amount of safety, thereby produce out the water of the suitable washing of strong detergency or there is the device of the water of certain sterilizing ability.
In order to solve the problems of the technologies described above, the disclosed technical scheme of the present patent application is: a kind of daily water consumption Electrowinning device, comprises water container, is located at least one pair of negative electrode in water container and positive electrode, for the electrolysis power to negative electrode and positive electrode power supply; Between paired negative electrode and positive electrode, be provided with water-permeable barrier film, the permeable aperture of described water-permeable barrier film is less than or equal to 2 millimeters and be more than or equal to 1 nanometer.
The barrier film of water-permeable described in technique scheme is also water permeable membrane or water-permeable barrier film, refer to can through-fall molecule barrier film, its permeable aperture permeable barrier film of (it is 2 millimeters of-1 nanometers that the present invention limits permeable pore diameter range) from grade to nano level, comprise the various filtering membranes that daily water treatment is used, as: ultra-filtration membrane (UF), nanofiltration membrane (NF) and microfiltration membrane (MF), etc.
Working mechanism and the beneficial effect of the disclosed daily water consumption Electrowinning of the invention described above device technique scheme are presented below.
The ionic membrane of the barrier film of water-permeable described in apparatus of the present invention unconventional employing, but in water electrolysis field unused a kind of barrier film, the inventor innovates water-permeable barrier film is introduced in apparatus for electrolyzing as the interelectrode barrier film of yin, yang.Reaction process when we think daily water consumption Electrowinning device busy of the present invention thus, except conventional electrolysis reaction process, has produced a new important reaction process, i.e. water body low pressure cold plasma discharge reaction process.Make a concrete analysis of as follows:
1, the equivalent model of eletrode tip diameter curvature and water permeable membrane pore diameter
In water body electric discharge, bringing out the generation of water applying plasma often needs to give an initial high voltage exciting, and affects the parameter that one of initial voltage principal element is discharge electrode.Under equal conditions electrode material, discharging distance, electrode diameter (electrode curvature radius) have impact to initial exciting voltage.Along with reducing of electrode diameter, initial exciting voltage reduces.From another angle, under additional same electrical press strip part, the more little severe degree that is more conducive to strengthen free-radical generating in gas ions passage of electrode diameter.In the present invention, between anodic-cathodic, there is one deck water-permeable barrier film, barrier film has the hole of numerous permeable diameter very little (grade and even nano level), from macroscopic view, sees and can be considered the point discharge that the discharge in water reaction equivalence of electrode is on a large scale decomposed into numerous very shallow curvature radius electrode.And then greatly reduce the initial voltage of activated plasma reaction.
In water, can generate a large amount of ultramicro air bubbles during electrolysis, wherein have bubble hydrogen also to have oxygen bubbles.And the shelf depreciation of bubble can greatly increase the generation of reactive behavior molecule and be easy to produce the free radicals such as hydroxyl, thus the reaction efficiency of raising discharge in water.But produce electric discharge in bubble, need field intensity in bubble higher than in water, require whole electric field more even; In the present invention, water permeable membrane is decomposed into two groups of large electrodes of negative and positive without array sub-electrode, but material, the voltage of all sub-electrodes are all identical.This just guarantees that whole electric field is evenly arranged in macroscopical field, and the bubble that electrolysis produces suffered electric field in uphill process is more even, has guaranteed the high-level efficiency of exoelectrical reaction.
2, enlarge active surface, improves reaction efficiency in water
As everyone knows, the equal object that cumulative volume is identical, more overall the individuality that is divided into specific surface area be larger.In like manner, the present invention with do not add permeable barrier film electrode discharge situation is contrasted, in the situation that producing equivalent gas, the microbubble volume that water electrolysis produces in numerous ultramicropore is far smaller than same homalographic and does not add the bubble volume that permeable barrier film produces electrolysis, and number of bubbles is also far away more than it.This has just effectively increased the specific surface area of gas-liquid two-phase contact.And we know, the various oxidation factor (as: hydroxyl) that plasma body generates mainly occur in the contact surface of gas-liquid two-phase.That is to say: the contact area of gas-liquid two-phase is larger, the generation of oxidation factor is more and reaction is more abundant, and organic degraded in water, microbial disinfection effect are better, have further improved the final efficiency of discharge in water reaction.
Traditional water body plasma discharge technology for producing water body plasma discharge, often imports gas by outside in water, and imposes and add high intensity pulses voltage or hot conditions.The present invention innovates the countless small water storage space that plasma discharge is directed to water-permeable barrier film and carries out, the gas that dependence generates water electrolysis liberation of hydrogen, oxygen evolution reaction, enter and in film, bring out water body self gasification, and then inspire efficient water body plasma discharge with minimum voltage, its meaning is not only the raising of efficiency, has also effectively prevented because of the excessive deterioration that easily causes biological index of current density.
In apparatus of the present invention, if the permeable aperture of water-permeable barrier film excessive (being that micropore space is excessive) is equivalent to the covert electrode diameter (electrode curvature radius) that increased, cause the initial exciting voltage of discharge in water to increase, and make to produce bubble volume and become and to have reduced greatly the catalytic specific surface area of gas-liquid two-phase.And the permeable aperture of water-permeable barrier film too small (being that micropore space is too small), can make electrolysis aerogenesis occur or gas producing efficiency extremely low, littlely can cause to a certain extent in barrier film the point discharge of numerous small curvature radius electrode in each micropore normally to carry out.Therefore,, through contriver's repetition test, determine that permeable pore diameter range is 2 millimeters of-1 nanometers.
The beneficial effect of summarizing the daily water consumption Electrowinning device technique scheme of the invention described above is: the present invention is by being arranged on the water-permeable barrier film with certain pore size between cathode and anode, brought beyond the conventional electrolysis reaction process and in water-permeable barrier film, in micropore, formed the reaction of water body low pressure cold plasma discharge, thereby can in water, generate efficiently the transient state oxidation factor of tool sterilizing ability.Concrete practical function is: the water oxygen factor can be strengthened the washing of water pollutant is removed to effect, meets user for water safety and many-sided demand such as functional simultaneously.
The improvement of the present invention on technique scheme basis is: the spacing of described negative electrode and positive electrode is more than or equal to the thickness of described water-permeable barrier film and is less than or equal to 20 millimeters.
In apparatus of the present invention, under equal voltage condition, in distance less (thickness of the distance=film under extreme case between the anodic-cathodic) water between anodic-cathodic, strength of electric field is larger, and interelectrode plasma channel more easily forms, cold plasma generation efficiency is higher, and the oxidation factor of generation is more.For example, and film can very thin (ultra-filtration membrane can be accomplished 0.1mm～0.3mm), the electrolysis voltage under Condition such as Gong such as Tong Deng can be very low, even only with a 3.7V lithium battery power supply, can form 2 amperes of above working currents, and prior art cannot be accomplished.Otherwise, widen the distance between anodic-cathodic, the corresponding minimizing of oxidation factor of generation, especially the generation probability of ozone class strong oxidizer has declined.We know, ozone results from a large number oxygen and passes through electrical discharge zone with bubble form.Anodic-cathodic spacing increases, and the probability that anode precipitated oxygen enters in the film in plasma discharge state reduces, and contrast ozone has just reduced.The oxidation factor generating in water, shows as hydroxy kind transient state oxidation factor more.This is for example, in some water occasion (cosmetic water) required exactly.But the excessive reduction that brings again efficiency of spacing, even in film, discharge process cannot carry out.Therefore,, through contriver's repetition test, the spacing of daily life water negative electrode and positive electrode is more than or equal to the thickness of described water-permeable barrier film and is less than or equal to 20 millimeters for best.
The further improvement of the present invention on technique scheme basis is: described water-permeable barrier film is dielectric water-permeable barrier film.This is because in most cases, wish that the oxidation factor producing in water is The more the better.The good water-permeable barrier film of electroconductibility easily forms combined electrode with close electrode and affects effect that discharge in water reacts and the kind of resultant when exoelectrical reaction, and uncontrollable factor is more, so preferred dielectric water-permeable barrier film.
The further improvement of the invention described above technical scheme is: in described negative electrode, have the first through hole, the aperture of described the first through hole is more than or equal to 1 millimeter.By such improvement, can be conducive to cathodic reaction and more fully carry out, and the bubble hydrogen that region between negative electrode and barrier film is produced is better derived.
Further improving again of the invention described above technical scheme is: described water-permeable barrier film has the second through hole, and the aperture of described the second through hole is greater than 2 millimeters.The bubble that can be conducive to produce by such improvement is better derived, and especially at anodic-cathodic and water-permeable barrier film spacing, compared with hour its bubble, derives better effects if.The permeable hole difference of the second through hole and water-permeable barrier film is: permeable hole is that the barrier film self of buying is intrinsic, and the second through hole is to make separately in addition.
In the oxidation factor generating in some water occasion is wished water, the composition of hydrogen peroxide can be more, can select carbonaceous material film (active carbon fiber fabrics for example with certain electroconductibility).Now carbonaceous barrier film is equivalent to a target, negative electrode (be equivalent between carbonaceous barrier film and negative electrode a gac anode-metallic cathode to) in the middle of being equivalent to by anode side, and based on activated carbon cathode Fenton, reaction generates more H2O2; Further, we can be by the optimum combination of two-layer above various trait barrier film, controls the generation situation of the water oxygen factor, i.e. effective regulation and control oxidation factor growing amount.Therefore, the invention described above technical scheme is improved one and is: described water-permeable barrier film is individual layer water-permeable barrier film or multilayer water-permeable barrier film.Wherein the concrete selection of water-permeable barrier film is: described individual layer water-permeable barrier film is the individual layer water-permeable barrier film that ultra-filtration membrane or employing carbonaceous material are made.
Improving of the invention described above technical scheme two is: described electrolysis power is direct current or the component pulse-changing power of the narrow pulsewidth of high level.The pulse power of the narrow pulsewidth of employing high level is conducive to the plasma discharge of water body inside between anodic-cathodic more, obtains better water effect processed.
As one of application extension of the invention described above technical scheme, be: the present invention proposes a kind of kitchen cleaning sink, and this kitchen cleaning sink contains the invention described above technical scheme.
As two of the application extension of the invention described above technical scheme, be: the present invention proposes a kind of dishwasher, and this dishwasher contains the invention described above technical scheme.
As three of the application extension of the invention described above technical scheme, be: the present invention proposes a kind of fruit-vegetable clear cleaning device, and this fruit-vegetable clear cleaning device contains the invention described above technical scheme.
As four of the application extension of the invention described above technical scheme, be: the present invention proposes a kind of washing machine, and this washing machine contains the invention described above technical scheme.
As five of the application extension of the invention described above technical scheme, be: the present invention proposes a kind of bathing apparatus, and this bathing apparatus contains the invention described above technical scheme.
As six of the application extension of the invention described above technical scheme, be: the present invention proposes a kind of toothbrush sanitizer, and this toothbrush sanitizer contains the invention described above technical scheme.
As seven of the application extension of the invention described above technical scheme, be: the present invention proposes a kind of nail therapeutic equipment or beri-beri therapeutic instrument, and this nail therapeutic equipment or beri-beri therapeutic instrument contain the invention described above technical scheme.
As eight of the application extension of the invention described above technical scheme, be: the present invention proposes a kind of skin therapeutic equipment, skin-nursing device or portable skin nursing spray bottle, this skin therapeutic equipment, skin-nursing device or portable skin nursing spray bottle contain the invention described above technical scheme.
As nine of the application extension of the invention described above technical scheme, be: the present invention proposes a kind of Medical sausage meat extruder, and this Medical sausage meat extruder contains the invention described above technical scheme.
As ten of the application extension of the invention described above technical scheme, be: the present invention proposes a kind of air humidifier, and this air humidifier contains the invention described above technical scheme.
Accompanying drawing explanation
Below in conjunction with accompanying drawing, daily water consumption Electrowinning device of the present invention is described further.
Fig. 1 is the structural representation of the embodiment of the present invention one daily water consumption Electrowinning device.
Fig. 2 is the structural representation of the embodiment of the present invention two daily water consumption Electrowinning devices.
Fig. 3 is the structural representation of the embodiment of the present invention three daily water consumption Electrowinning devices.
Fig. 4 is the structural representation of the embodiment of the present invention four daily water consumption Electrowinning devices.
Fig. 5 is the partial enlarged drawing at A place in Fig. 4.
Fig. 6 is the structural representation of the embodiment of the present invention five daily water consumption Electrowinning devices.
Fig. 7 is the partial enlarged drawing at B place in Fig. 6.
Fig. 8 is the structural representation of the embodiment of the present invention six daily water consumption Electrowinning devices.
Fig. 9 is the partial enlarged drawing at C place in Fig. 8.
Figure 10 is the structural representation of the embodiment of the present invention seven daily water consumption Electrowinning devices.
Figure 11 is the partial enlarged drawing at D place in Fig. 8
Figure 12 is the structural representation of the embodiment of the present invention eight daily water consumption Electrowinning devices.
Figure 13 is the structural representation of the embodiment of the present invention nine daily water consumption Electrowinning devices.
Figure 14 is the structural representation of the embodiment of the present invention ten daily water consumption Electrowinning devices.
Embodiment
Embodiment mono-
The daily water consumption Electrowinning device of the present embodiment is referring to Fig. 1, comprises water container 1, is located at a pair of negative electrode 2 in water container 1 and positive electrode 3, for the electrolysis power 4 to negative electrode 2 and positive electrode 3 power supplies; The water container 1 of the present embodiment is open container.Between a pair of negative electrode 2 and positive electrode 3, be provided with water-permeable barrier film 5, the water-permeable barrier film 5 of the present embodiment adopts the individual layer PVDF ultra-filtration membrane (PVDF membrane) in 0.03 micron, average permeable aperture; Certainly the ultra-filtration membrane of the present embodiment also can adopt the ultra-filtration membrane of other materials, all can in average permeable aperture between 0.01～0.05 micron.
Water-permeable barrier film 5 is all 1mm with the spacing δ of yin, yang electrode, and to exceed respectively yin, yang electrode a bit of at barrier film 5 two ends.
The negative electrode 2 of the present embodiment and positive electrode 3 all adopt titanium base to cover and are coated with the noble electrode that platinum family oxide compound (coat-thickness is 0.8 millimeter) is made, the rounded sheet of negative electrode 2, positive electrode 3 sheet that is rectangle.All not perforates of surface of negative electrode and positive electrode.
The electrolysis power 4 of the present embodiment adopts the direct current pulse power source of 30 volts of the narrow pulsewidth voltage stabilizings of high level, also can adopt component pulse-changing power.
The negative electrode 2 of the present embodiment and parallel placement in the water of positive electrode 3 in water container 1, negative electrode 2 is positioned at the top of positive electrode 3.
One, experiment 1
Adopt the daily water consumption electrolyzer of the present embodiment to carry out water electrolysis experiment, water container volume is 200 * 80 * 120 millimeters, and source water is the water outlet of RO water purification machine, TDS=3mg/L, approximately 1.5 liters of water container water fillings, electrolysis time is 30 minutes, within every 5 minutes, water sampling is measured once.
Below, in experiment, how many underwater bubble amount (intensity) and water oxygen factors adopt qualitative observation procedure
1. the range estimation classification of underwater bubble amount (intensity):
From underwater bubble, be that zero～experiment, air bubble content is maximum relatively, be divided into 0～5 grade;
2. the mensuration of the water oxygen factor
As previously mentioned, because oxidation factor retention time in water is very of short duration, analysis selectivity and the confidence level of existing detection method (for example chemical reaction method and prize law) are also unsatisfactory.Consider that apparatus of the present invention system is exclusively used in the processing of daily water consumption, what stress to be concerned about is the variation tendency level macroscopic view effect of oxidation factor simultaneously.Therefore for simplifying, repeat cut-and-try work amount, researched and developed specially the titrating solution of qualitative understanding water oxygen factor total amount.After being titrated in water by self-control titrating solution, observe the yellowing degree of water body color, be divided into 5 grades, qualitatively judge water oxygen factor content:
Colourless---the corresponding water oxygen factor is zero substantially, is made as 0 grade;
Color is the most yellow---and the corresponding water oxygen factor is relatively maximum, is made as 5 grades;
From the colourless degree difference to the most yellow middle colour-change of color, be divided into 1,2,3 and 4 grade.
Test 1 result as following table 1:
Table 1
Interpretation
With the increase of electrolysis time, water oxygen factor amount all proportional example increases.
Two, experiment 2
Contrast without film/ionic membrane/water-permeable film
The water-permeable barrier film of the present embodiment 5 and three kinds of situations taking away water-permeable barrier film 5 or be replaced by ionic membrane are carried out respectively to water electrolysis, and contrast experiment's condition is:
1) take away the water-permeable barrier film 5 between negative electrode 2 and anode 3, make to form without barrier film state between negative electrode 2 and anode 3, the spacing between negative electrode 2 and anode 3 is 2.0 millimeters (with insulating washer location, maintenance spacing is constant);
2) water-permeable barrier film 5 makes neutral ion film into, and film 5 is respectively 1 millimeter with cathode and anode spacing δ;
3) the present embodiment adopts the water-permeable barrier film 5 of PVDF ultra-filtration membrane;
4) experiment source water is the water outlet of commercially available RO water purification machine, TDS=3mg/L, and pH=6.8, to approximately 1 liter of container injected water.
Keep Faradaic current in three kinds of situations to be 300 milliamperes, electrolysis 15 minutes, experiment 2 the results are shown in table 2.
Table 2
Three, experiment 3
The impact of spacing δ range on device performance characteristics between test negative electrode and water-permeable barrier film
Spacing δ between the negative electrode of the present embodiment 2 and water-permeable barrier film 5 is adjusted into respectively: δ=10,7,4,1,0 millimeters of five kinds of situations.Other experiment conditions are identical with above-mentioned experiment 2, and experiment 3 the results are shown in table 3.
Table 3
Embodiment bis-
Daily water consumption electrolyzer and the embodiment mono-of the present embodiment are basic identical, and as shown in Figure 2, the variations different from embodiment mono-are: 1) hydrophobic diaphragm 5 is close on negative electrode 2 and positive electrode 3 simultaneously, and barrier film 5 is 0 with the spacing of anode and cathode; 2) barrier film 5 two ends exceed respectively longer one section of yin, yang electrode.
The daily water consumption electrolyzer of the present embodiment is carried out to water electrolysis experiment, and Yuan Shuiwei city supplies tap water, ORP=+320mv, and pH=7.1, TDS=48mg/L, electrolysis time is 20 minutes, within every 5 minutes, water sampling is measured once.Other experiment conditions and detection method are identical with embodiment mono-, and experimental result is as following table 4:
Table 4
Embodiment tri-
Daily water consumption Electrowinning device and the embodiment mono-of the present embodiment are basic identical, and as shown in Figure 3, the variations different from embodiment mono-are: 1) water container 1 is closed container, is provided with water-in 6 and water outlet 7; 2) positive electrode 3 is the noble electrodes (having certain electroconductibility) that adopt the carbonaceous materials such as graphite, gac to make; 3) water-permeable barrier film is the individual layer water-permeable barrier film that adopts the carbonaceous materials such as graphite, gac to make; 4) water-permeable barrier film 5 is 8mm with the spacing δ 1 of positive electrode 3; 5) water-permeable barrier film 5 is 0.5mm with the spacing δ 2 of negative electrode 2.
The daily water consumption electrolyzer of the present embodiment is carried out to water electrolysis experiment, and experiment condition and detection method are identical with embodiment bis-.Increase the mensuration of a hydrogen peroxide, select on the market conventional hydrogen peroxide quick detection reagent, after quick testing reagent is titrated in water, observe the yellowing degree of water body color, be divided into 5 grades, qualitatively judge the content of hydrogen peroxide in water:
Colourless---in corresponding water, hydrogen peroxide is zero substantially, is made as 0 grade;
It is orange that color is---and in corresponding water, hydrogen peroxide is relatively maximum, is made as 5 grades;
From the colourless degree difference to the most yellow middle colour-change of color, be divided into 1,2,3 and 4 grade.
Experimental result is as following table 5:
Table 5
Interpretation
Select carbonaceous material to do after barrier film, with the increase of electrolysis time, water oxygen factor amount all proportional example increases, and the content of the hydrogen peroxide in water is also increasing than the increase of source water much step by step.
Embodiment tetra-
Daily water consumption Electrowinning device and the embodiment bis-of the present embodiment are basic identical, and as shown in Figure 4 and Figure 5, the variations different from embodiment bis-are: 1) in negative electrode 2, have the first through hole 8, through-hole aperture is got 1mm; 2) water-permeable barrier film 5 and negative electrode 2, the same length of positive electrode 3; 3) water-permeable barrier film 5 is close to positive electrode 3 but is separated with negative electrode 2, and water-permeable barrier film 5 is 2mm with the spacing δ of negative electrode 2.
The daily water consumption Electrowinning device of the present embodiment is carried out to water electrolysis experiment, the present embodiment is uniform the first through hole that has 24 diameter phi 3mm in negative electrode, electrolysis time 20 minutes, other experiment conditions and detection method are identical with embodiment mono-, and experimental result is as following table 6:
Table 6
Embodiment five
Daily water consumption Electrowinning device and the embodiment tetra-of the present embodiment are basic identical, as shown in Figure 6 and Figure 7, with the variation of embodiment tetra-be: 1) water-permeable barrier film 5 has the second through hole 9, the second through holes 9 of diameter phi 2.1mm and essentially concentric identical with the first through hole 8 quantity and aligns; 2) water-permeable barrier film 5 is 3mm with the spacing δ of negative electrode 2.
The daily water consumption Electrowinning device of the present embodiment is carried out to water electrolysis experiment, electrolysis time 20 minutes, other experiment conditions and detection method are identical with embodiment tetra-, and experimental result is as following table 7:
Table 7
Embodiment six
The present embodiment as shown in Figure 8 and Figure 9, to develop on embodiment tri-bases, different variations are: 1) water-permeable barrier film 5 is to add by activated carbon fiber film (felt) 5-1 and the folded 5-2 of ultra-filtration membrane two layers of water-permeable barrier film that are composited, activated carbon fiber film 5-1 near positive electrode 3(towards positive electrode 3) and all surfaces of coated positive electrode 3, towards negative electrode 2(, deviate from positive electrode 3) the part surface (positive electrode is towards all surfaces of negative electrode 2 one sides) of the coated positive electrode 3 of ultra-filtration membrane 5-2, and the two ends of ultra-filtration membrane 5-2 exceed positive electrode slightly; 2) water-permeable barrier film 5 is 5mm with the spacing δ of negative electrode 2; 3) the employing titanium base that positive electrode 3 is identical with negative electrode 2 covers and is coated with the noble electrode that platinum family oxide compound (coat-thickness is 0.8 millimeter) is made, rounded sheet.
Embodiment seven
The daily water consumption Electrowinning device of the present embodiment is the variation on embodiment six bases, as shown in Figure 10 and Figure 11, different from embodiment six: 1) towards negative electrode 2(, to deviate from positive electrode 3) ultra-filtration membrane 5-2 also with all surfaces of the equally coated positive electrode 3 of activated carbon fiber film 5-1; 2) in negative electrode 2, have φ 2mm the first through hole 8; 3) at water-permeable barrier film 5(, comprise activated carbon fiber film (felt) 5-1 and ultra-filtration membrane 5-2) on a side of negative electrode 2, have the second through hole 9 of diameter phi 2.5mm.
Embodiment eight
The daily water consumption Electrowinning device of the present embodiment as shown in figure 12, is the variation on embodiment bis-bases, different from embodiment bis-: 1) negative electrode 2 and positive electrode 3 are disk plane electrode, and size is 48 millimeters of diameters, 1 millimeter of thickness; 2) uniform pectination the first through hole 8 that has of negative electrode 2; 3) water-permeable barrier film 5 has following three kinds to select and arrange:
1. individual layer PVDF ultra-filtration membrane (being numbered film 1#), 0.03 micron, average permeable aperture, thickness is 0.5mm, not perforate, is close to anodic-cathodic.
2. two membranes stack combinations (being numbered film 2#+ film 1#): the first layer adopts PVDF ultra-filtration membrane, 0.03 micron, average permeable aperture, thickness is 0.5mm, not perforate, is close to positive electrode; The second layer adopts 0.05 micron, average permeable aperture PVDF ultrafiltration diaphragm, and thickness 0.5mm cuts into negative electrode 2 same sizes and has the disk film of pectination the second through hole 9, is close to negative electrode; Pectination the second through hole 9 is perpendicular with pectination the first through hole 8 localities.
3. trilamellar membrane stack combinations (being numbered film 3#+ film 2#+ film 1#): the first layer adopts active carbon fiber fabrics, specific surface area 1200m2/g, immersion is pressed approximately 1.8 millimeters of rear thickness and is close to positive electrode; The second layer (middle layer) adopts PVDF ultra-filtration membrane, 0.03 micron, average permeable aperture, and thickness is 0.5mm, not perforate; The 3rd layer adopts 0.05 micron, average permeable aperture PVDF ultrafiltration diaphragm, and thickness 0.5mm cuts into negative electrode 2 same sizes and has the disk film of pectination the second through hole 9, is close to negative electrode; Pectination the second through hole 9 is perpendicular with pectination the first through hole 8 localities.
About the combination of water-permeable barrier film single or multiple lift, on the daily water consumption Electrowinning device of experiment the present embodiment of the impact of the present embodiment device performance characteristics, select respectively different water-permeable barrier films 5 to carry out water electrolysis experiment as follows:
1, experiment condition
The volume of 1.1 water containers 1 is 100 * 100 * 300 millimeters
1.2 electrolysis powers 4, adopt D.C. regulated power supply;
1.3 other experiment conditions and detection method are identical with embodiment mono-.
Yuan Shuiwei city supplies tap water, TDS=160mg/L, and pH=7.5, to approximately 1 liter of container injected water.Respectively with above-mentioned single-layer septum and composite membrane, each electrolysis 15 minutes, in electrolytic process, Faradaic current all remains 300 milliamperes, and experimental result is shown in table 9.
Table 9
Embodiment nine
The present embodiment is a kind of aseptic water storage container, referring to Figure 13.The aseptic water storage container of the present embodiment is to develop from embodiment eight, and the variations different from embodiment eight are:
1) diaphragm that water-permeable barrier film 5 adopts carbon fiber to make, average hydrophobic aperture is 150 microns, thick 2 millimeters of diaphragm, diameter D=42 millimeter, uniform the having and orthogonal pectination the second through hole 9 of negative electrode pectination the first through hole 8 locality in surface;
2) positive electrode 3 is arranged on water container 1 bottom, and negative electrode 2 adds insulating sheath through positioning screw 10(overcoat) with one heart through fixing behind water-permeable barrier film 5 and positive electrode 3 and water container 1 bottom surface, also water-permeable barrier film 5 is compressed simultaneously;
3) in positive electrode 3 neighborings, be added with one with screw rod 12 fixing plastics housing 11, for the water-permeable barrier film 5 covering on positive electrode 3 is pressed on to water container 1 bottom surface, to accomplish being reliably coated positive electrode 3, water container 1 bottom surface is close in the bottom surface of the present embodiment positive electrode 3, therefore water-permeable barrier film 5 is coated all surfaces of positive electrode 3 except bottom surface, negative electrode 2, carbon fiber diaphragm and positive electrode 3 gapless stack combinations;
4) in positive electrode 3 bottom surfaces, 90 degree positions relative to negative electrode 2 positioning screws 10 are welded with two anode screw rods 13 of dividing equally, and the positive and negative lead wires of externally fed electrolysis power is connected respectively on positioning screw 10 and anode screw rod 13.
For the sterilising effect of check the present embodiment device, commercially available drummed pure water is filled with to container, and add bacterial concentration in coliform sampling detection receptacle water approximately to reach 9.5 ten thousand/cm3; To anodic-cathodic group power supply, maintaining Faradaic current is 10 milliamperes, electrolysis water sampling detected result again after 25 minutes, and in vessel water, total plate count reduces to zero.
Embodiment ten
A kind of suitable electrolysis cells device of producing bath water of the present embodiment, referring to Figure 14, is to develop from embodiment nine, and the variations different from embodiment nine are:
1) water-permeable barrier film 5 is formed by two tunic stack combinations, the first layer is towards the average permeable aperture of polysulphones hyperfiltration membrane sheet 5-1(of negative electrode 2 0.02 micron, thickness 0.5mm, cut into disk identical with negative electrode 2), the second layer is 0.05 micron, the average permeable aperture of PVDF ultra-filtration membrane 5-2(being close to all standing positive electrode, thickness is 0.5mm, not perforate);
2) pectination first through hole 8 of negative electrode 2 changes uniform φ 3mm circular hole into; The first layer polysulphones hyperfiltration membrane sheet 5-1 of corresponding water-permeable barrier film 5 arranges circle the second through hole 9 with the concentric size of the first through hole 8.
For the water effect processed of check the present embodiment cell arrangement, carried out following test:
1) the present embodiment device is fixed on to plastic containers bottoms (negative electrode upward), injects city for approximately 20 liters, tap water;
2), by appendix A method in GB GB-T4288-2003 domestic electric washer, prepare respectively A, B double, three kinds of pollution sample cloth (carbon black oil pollutes cloth, protein contamination cloth, sebum pollution cloth);
3) by above-mentioned three kinds, pollute sample cloth respectively and put into container, through outside D.C. regulated power supply, embodiment device is provided the electrolysis voltage of 12V, electrolysis 20 minutes, electrolysis is three times respectively.During surveying each electrolysis, Faradaic current is about 2～8A range;
4) stop after electrolysis, hand-launder above-mentioned three kinds of soaking through electrolysis and pollute sample cloth each 5 minutes, with clear water, rinse afterwards; Three kinds of sample cloth after rinsing are labeled as: " carbon black sample cloth A ", " albumen sample cloth A ", " sebum sample cloth A ";
5) in addition, use a commercially available mini washing machine (duckling board), inject city for approximately 20 liters, tap water, add washing powder, by standard wash program, wash respectively three kinds and pollute sample cloth each 20 minutes, after rinsing dries, marking three kinds of sample cloth is: " carbon black sample cloth B ", " albumen sample cloth B ", " sebum sample cloth B ";
6) washability of two kinds of methods of ready visual contrast, result proves, three kinds of category-As pollution sample cloth that clean through apparatus of the present invention, washability all pollutes sample cloth apparently higher than the category-B of washing powder machine washing mode.If the category-B sample cloth wash degree of establishing after washing machine machine washing is 1, A, two kinds of washing effect contrasts of B are about 1.5:1.
Above-mentioned experimental result shows, the water after apparatus of the present invention are processed, and washability greatly improves.
Embodiment 11
The present embodiment is to provide a kind of kitchen cleaning sink, and this tank has adopted the daily water consumption Electrowinning device of above-described embodiment.
Embodiment 12
The present embodiment is to provide a kind of dishwasher, and this dishwasher has adopted the daily water consumption Electrowinning device of above-described embodiment.Embodiment 13
The present embodiment is to provide a kind of fruit-vegetable clear cleaning device, and this fruit-vegetable clear cleaning device has adopted the daily water consumption Electrowinning device of above-described embodiment.
Embodiment 14
The present embodiment is to provide a kind of washing machine, and this washing machine has adopted the daily water consumption Electrowinning device of above-described embodiment.Embodiment 15
The present embodiment is to provide a kind of bathing apparatus, and this bathing apparatus has adopted the daily water consumption Electrowinning device of above-described embodiment.
Embodiment 16
The present embodiment is to provide a kind of toothbrush sanitizer, and this toothbrush sanitizer has adopted the daily water consumption Electrowinning device of above-described embodiment.
Embodiment 17
The present embodiment is to provide a kind of nail therapeutic equipment, and this nail therapeutic equipment has adopted the daily water consumption Electrowinning device of above-described embodiment.
Embodiment 18
The present embodiment is to provide a kind of beri-beri therapeutic instrument, and this beri-beri therapeutic instrument has adopted the daily water consumption Electrowinning device of above-described embodiment.
Embodiment 19
The present embodiment is to provide a kind of skin therapeutic equipment, and this skin therapeutic equipment has adopted the daily water consumption Electrowinning device of above-described embodiment.
Embodiment 20
The present embodiment is to provide a kind of skin-nursing device, and this skin-nursing device has adopted the daily water consumption Electrowinning device of above-described embodiment.
Embodiment 21
The present embodiment is to provide a kind of portable skin nursing spray bottle, and this portable skin nursing spray bottle has adopted the daily water consumption Electrowinning device of above-described embodiment.
Embodiment 22
The present embodiment is to provide a kind of Medical sausage meat extruder, and this Medical sausage meat extruder has adopted the daily water consumption Electrowinning device of above-described embodiment.
Embodiment 23
The present embodiment is to provide a kind of air humidifier, and this air humidifier has adopted the daily water consumption Electrowinning device of above-described embodiment.
Daily water consumption Electrowinning device of the present invention is not limited to the concrete technical scheme described in above-described embodiment, such as: 1) positive electrode 3 and negative electrode 2 can be also two pairs; 2) electrolysis power 4 can be also AC pulse power supply; 3) water-permeable barrier film 4 can be also that the barrier film of three layers or more multi-layered unlike material is formed by stacking; 4) shape of negative electrode 2 and positive electrode 3 can be also except circular and other square different shapes; 5), in embodiment six, the activated carbon fiber film 5-1 of close positive electrode 3 can be also, or the water-permeable barrier film of being made by graphite or other carbon materials; 6) technical scheme of above-mentioned each embodiment of the present invention can combined crosswise form new technical scheme each other; Etc..The technical scheme that all employings are equal to replacement formation is the protection domain that the present invention requires.
Claims (23)
1. a daily water consumption Electrowinning device, comprises water container, is located at least one pair of negative electrode in water container and positive electrode, for the electrolysis power to negative electrode and positive electrode power supply; It is characterized in that: between paired negative electrode and positive electrode, be provided with water-permeable barrier film, the permeable aperture of described water-permeable barrier film is less than or equal to 2 millimeters and be more than or equal to 1 nanometer.
2. daily water consumption Electrowinning device according to claim 1, is characterized in that: the spacing of described negative electrode and positive electrode is more than or equal to the thickness of described water-permeable barrier film and is less than or equal to 20 millimeters.
3. daily water consumption Electrowinning device according to claim 1, is characterized in that: described water-permeable barrier film is dielectric water-permeable barrier film.
4. daily water consumption Electrowinning device according to claim 2, is characterized in that: described water-permeable barrier film is dielectric water-permeable barrier film.
5. daily water consumption Electrowinning device according to claim 4, is characterized in that: in described negative electrode, have the first through hole, the aperture of described the first through hole is more than or equal to 1 millimeter.
6. daily water consumption Electrowinning device according to claim 4, is characterized in that: described water-permeable barrier film has the second through hole, and the aperture of described the second through hole is greater than 2 millimeters.
7. daily water consumption Electrowinning device according to claim 4, is characterized in that: described water-permeable barrier film is individual layer water-permeable barrier film.
8. daily water consumption Electrowinning device according to claim 4, is characterized in that: described water-permeable barrier film is multilayer water-permeable barrier film.
9. daily water consumption Electrowinning device according to claim 7, is characterized in that: described individual layer water-permeable barrier film is ultra-filtration membrane or the individual layer water-permeable barrier film that adopts carbonaceous material to make.
10. daily water consumption Electrowinning device according to claim 4, is characterized in that: described electrolysis power is direct current or the component pulse-changing power of the narrow pulsewidth of high level.
11. 1 kinds of kitchen cleaning sinks, is characterized in that containing the arbitrary described daily water consumption Electrowinning device just like claim 1-10.
12. 1 kinds of dishwashers, is characterized in that containing the arbitrary described daily water consumption Electrowinning device just like claim 1-10.
13. 1 kinds of fruit-vegetable clear cleaning devices, is characterized in that containing the arbitrary described daily water consumption Electrowinning device just like claim 1-10.
14. 1 kinds of washing machines, is characterized in that containing the arbitrary described daily water consumption Electrowinning device just like claim 1-10.
15. 1 kinds of bathing apparatus, is characterized in that containing the arbitrary described daily water consumption Electrowinning device just like claim 1-10.
16. 1 kinds of toothbrush sanitizers, is characterized in that containing the arbitrary described daily water consumption Electrowinning device just like claim 1-10.
17. 1 kinds of nail therapeutic equipments, is characterized in that containing the arbitrary described daily water consumption Electrowinning device just like claim 1-10.
18. 1 kinds of beri-beri therapeutic instruments, is characterized in that containing the arbitrary described daily water consumption Electrowinning device just like claim 1-10.
19. 1 kinds of skin therapeutic equipments, is characterized in that containing the arbitrary described daily water consumption Electrowinning device just like claim 1-10.
20. 1 kinds of skin-nursing devices, is characterized in that containing the arbitrary described daily water consumption Electrowinning device just like claim 1-10.
21. 1 kinds of portable skin nursing spray bottles, is characterized in that containing the arbitrary described daily water consumption Electrowinning device just like claim 1-10.
22. 1 kinds of Medical sausage meat extruders, is characterized in that containing the arbitrary described daily water consumption Electrowinning device just like claim 1-10.
23. 1 kinds of air humidifiers, is characterized in that containing the arbitrary described daily water consumption Electrowinning device just like claim 1-10.
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| CN201410146256.3A CN103936110B (en) | 2014-04-12 | 2014-04-12 | Daily water consumption Electrowinning device |
| PCT/CN2015/076247 WO2015154714A1 (en) | 2014-04-12 | 2015-04-10 | Device for preparing daily water by electrolysis |
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| CN201410146256.3A CN103936110B (en) | 2014-04-12 | 2014-04-12 | Daily water consumption Electrowinning device |
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| WO2015154713A1 (en) * | 2014-04-12 | 2015-10-15 | 大连双迪创新科技研究院有限公司 | Device for preparing drinking water by electrolysis |
| WO2015154708A1 (en) * | 2014-04-12 | 2015-10-15 | 大连双迪科技股份有限公司 | Water electrolysis cup |
| US10294128B2 (en) | 2014-04-12 | 2019-05-21 | Dalian Shuangdi Innovative Technology Research Institute Co., Ltd. | Device for preparing drinking water by electrolysis |
| CN107416950A (en) * | 2017-06-16 | 2017-12-01 | 福州金慧健康科技有限公司 | A kind of free radical generation device and the dish-washing machine with the free radical generation device |
| CN109942059A (en) * | 2019-04-03 | 2019-06-28 | 大连理工大学 | A kind of falling liquid film device for treating aqueous discharge plasma that water distribution is integrated with catalysis |
Also Published As
| Publication number | Publication date |
|---|---|
| WO2015154714A1 (en) | 2015-10-15 |
| CN103936110B (en) | 2017-03-29 |
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