JP6861550B2 - Hydrogen mixed gas generator and hydrogen mixed gas generation method - Google Patents

Description

The present invention relates to a hydrogen mixed gas generator and a method for producing a hydrogen mixed gas.

In recent years, in the industrial field such as pharmaceuticals, attention has been paid to the function of hydrogen gas such as neutralizing hydroxyl radical in the living body. Therefore, in order to utilize such a function of hydrogen gas, an apparatus for generating and supplying a hydrogen mixed gas in which hydrogen gas and oxygen are mixed has been proposed (Patent Document 1).

In Patent Document 1, the inside and the outside of the electrolytic cell are separated by a diaphragm, and the gas phase in the electrolytic cell is airtight between the gas phase on the anode side and the gas phase on the cathode side by a pair of electrode plates. A hydrogen gas supply device for a living body having an electrolytic cell separated into the above is disclosed. This biological hydrogen gas supply device ensures safety when using the device in medical settings, etc. by always maintaining the hydrogen gas concentration in a predetermined space region in the gas phase of the electrolytic cell at less than 4% by volume. ing.

Japanese Patent No. 5091364

However, in the hydrogen gas supply device for living organisms of Patent Document 1, the structure of the electrolytic cell is such that the gas phase on the anode side and the gas phase on the cathode side are airtightly separated by a diaphragm, and hydrogen generated on the cathode side. Since the oxygen gas is separately supplied and mixed after the gas is diluted, it is not a device that can efficiently supply the hydrogen mixed gas. That is, the biological hydrogen gas supply device of Patent Document 1 cannot directly mix the hydrogen gas generated on the cathode side with the oxygen gas generated on the anode side in the gas phase of the electrolytic cell, and is efficient. It is not a device that can supply hydrogen mixed gas.

The present invention has been made in view of the above circumstances, and provides a hydrogen mixed gas generator capable of safely and efficiently generating a hydrogen mixed gas in a medical field or the like, and a hydrogen gas generation method. The task is to do.

In order to solve the above problems, the present invention has the following configurations.
[1] A hydrogen-mixed gas generator that produces a hydrogen-mixed gas by mixing hydrogen gas generated by electrolyzing raw electrolyzed water with a diluted gas, and is provided with a single-tank type electrolytic cell. A hydrogen mixed gas generator in which at least a pair of electrode plates are immersed in a liquid phase in an electrolytic cell.
[2] The electrolytic cell has a diluting gas introduction port for introducing a diluting gas into the gas phase in the electrolytic cell and a hydrogen mixed gas outlet for drawing out a hydrogen mixed gas from the gas phase in the electrolytic cell. The hydrogen mixed gas generator according to [1].
[3] The hydrogen mixed gas generator according to [2], wherein the diluted gas introduction port is provided closer to the interface between the gas phase and the liquid phase in the electrolytic cell than the hydrogen mixed gas outlet.
[4] A method for producing a hydrogen mixed gas using the hydrogen mixed gas generating apparatus according to any one of [1] to [3].

According to the hydrogen mixed gas generator of the present invention and the method for producing a hydrogen mixed gas, the hydrogen mixed gas can be produced safely and efficiently.

It is a schematic diagram which shows an example of the structure of the hydrogen mixed gas generation apparatus which concerns on embodiment to which this invention is applied. FIG. 1 is an enlarged view showing a portion of the hydrogen mixed gas generation mechanism 20. It is a figure which showed an example of the modification of the hydrogen mixed gas generation mechanism 20. It is a figure which showed an example of the modification of the hydrogen mixed gas generation mechanism 20. It is a figure which shows the first part of the example of the flowchart of the method of generating the hydrogen mixed gas which concerns on embodiment to which this invention is applied. It is a figure which shows the latter part of an example of the flowchart of the method of generating the hydrogen mixed gas which concerns on embodiment to which this invention was applied. It is a schematic diagram which shows an example of the structure of the modification of the hydrogen mixed gas generation apparatus which concerns on embodiment to which this invention is applied.

Hereinafter, a hydrogen mixed gas generating apparatus according to an embodiment to which the present invention is applied and a method for generating a hydrogen mixed gas will be described in detail with reference to the drawings. In addition, in the drawings used in the following description, in order to make the features easy to understand, the featured parts may be enlarged for convenience, and the dimensional ratios of each component may not be the same as the actual ones. Absent.

[Hydrogen mixed gas generator]
First, the configuration of the hydrogen mixed gas generation device 1 which is an embodiment to which the present invention is applied will be described.
FIG. 1 is a schematic view showing an example of the configuration of the hydrogen mixed gas generation device 1. As shown in FIG. 1, the hydrogen mixed gas generation device 1 includes a dilution gas introduction mechanism 10, a hydrogen mixed gas generation mechanism 20, a concentration measuring mechanism 30, a control mechanism 40, and a hydrogen mixed gas supply mechanism 50. It is roughly configured.
Each component of the hydrogen mixed gas generator 1 will be described in detail below.

The oxygen gas cylinder (oxygen gas supply means) 11 included in the dilution gas introduction mechanism 10 is an example of the oxygen gas supply means, and other oxygen gas supply means may be adopted. For example, it may be a device that generates oxygen gas at any time. In that case, a liquid gas vaporizer, a PSA oxygen gas generator, a membrane oxygen gas generator, or the like can be adopted. When using an oxygen gas generator, it is preferable to select one having a small amount of by-produced gas other than oxygen gas. Since the oxygen gas concentration in the air is about 21%, air pressurized by a compressor or the like may be used as the oxygen gas supply means.

Similarly, the nitrogen gas cylinder (nitrogen gas supply means) 12 is an example of the nitrogen gas supply means, and may adopt other nitrogen gas supply means. For example, a device that generates nitrogen gas at any time may be used, in which case a liquid gas vaporizer, a PSA type nitrogen gas generator, a membrane type nitrogen gas generator, or the like can be adopted. When using these devices, it is preferable to select one having a small amount of by-produced gas other than nitrogen gas.
Instead of nitrogen gas, carbon dioxide gas, argon gas, helium gas, xenon gas and the like can be used. Further, when air pressurized by a compressor or the like is used as the oxygen gas supply means as described above, the nitrogen gas supply means can be omitted.

From the viewpoint of use in the medical field, it is desirable that the hydrogen mixed gas generator 1 is lightweight and movable. In this case, the form of the oxygen gas supply means and the nitrogen gas supply means is preferably a cylinder, and each of these cylinders is more preferably composed of a container of 10 L or less. From the viewpoint of miniaturization of the apparatus, a mixed gas cylinder containing two types of gases, nitrogen gas and oxygen gas whose concentration has been adjusted in advance, may be used as a supply source of the dilution gas.
Mass flow controllers 14a and 14b are provided in the pipes 13a and 13b, which are the gas supply paths, respectively.

In this embodiment, the mass flow controllers 14a and 14b are electrically connected to the control mechanism 40. Therefore, the mass flow controllers 14a and 14b can appropriately adjust the flow rates of the gases supplied from the oxygen gas cylinder 11 and the nitrogen gas cylinder 12.

The dilution gas introduction mechanism 10 has a dilution gas mixer 15. The dilution gas mixer 15 is provided at a position where the pipe 13a, which is a path for supplying oxygen gas, and the pipe 13b, which is a path for supplying nitrogen gas, meet. The dilution gas mixer 15 mixes each gas supplied from the oxygen gas cylinder 11 and the nitrogen gas cylinder 12 to generate a dilution gas.
Specific examples of the dilution gas mixer 15 include, but are not limited to, a plate type mixer, an aspirator type mixer, a static mixer, and a mixing tank. A T-shaped joint or the like may be used as the dilution gas mixer 15.

The pipe 13c, which is the introduction route from the dilution gas mixer 15 to the introduction target of the dilution gas, is connected to the hydrogen mixing gas generation mechanism 20.
The pipes 13a, 13b, and 13c are preferably gas-tight, lightweight, and high-strength. Examples of the base material that can be used for the pipes 13a, 13b, 13c include, but are not limited to, austenitic stainless steel, polytetrafluoroethylene, and polyamide.
The dilution gas mixer 15 may be configured as one of the components of the hydrogen mixed gas generation mechanism 20 described later. That is, the dilution gas mixer 15 may be provided in the hydrogen mixed gas generation mechanism 20. In this case, the pipe 13c is omitted, and oxygen gas and nitrogen gas are introduced into the hydrogen mixed gas generation mechanism 20 via the pipes 13a and 13b.

FIG. 2A is an enlarged view of a portion of the hydrogen mixed gas generation mechanism 20 in FIG. As shown in FIG. 2A, the hydrogen mixed gas generation mechanism 20 includes a single-tank type electrolytic cell 21 and a current control device 22, and at least a pair of electrode plates 23 and 24 are immersed in the liquid phase in the electrolytic cell. Has been done. Further, in the electrolytic cell 21, a diluting gas introduction port 25 for introducing a diluting gas into the gas phase in the electrolytic cell and a hydrogen mixed gas outlet 26 for drawing out a hydrogen mixed gas from the gas phase in the electrolytic cell are provided. It is provided.

The hydrogen mixing gas generation mechanism 20 mixes the hydrogen gas generated from the liquid phase in the electrolytic cell 21 by electrolyzing the electrolytic raw water 27 with the diluting gas introduced from the diluting gas introduction mechanism 10 to mix hydrogen. Produces gas. The electrolytic raw water 27 is a liquid capable of generating oxygen gas from the vicinity of the anode and hydrogen gas from the vicinity of the cathode by electrolysis. Examples of the electrolytic raw water 27 include tap water, purified water, purified water, distilled water and the like. Among these, purified water and distilled water are preferable from the viewpoint of preventing impurities from being mixed in the generated hydrogen gas.

Electrolyzed raw water 27 is introduced into the electrolytic cell 21 in order to electrolyze water. A gas phase is formed in the upper part of the electrolytic cell 21, and a liquid phase composed of the electrolytic raw water 27 is formed in the lower part of the electrolytic cell 21. The gas phase in the electrolytic cell 21 is shielded from the outside air, and the airtightness is maintained.

The electrolytic cell 21 has a dilution gas introduction port 25 that introduces a dilution gas into the gas phase in the electrolytic cell 21, and a hydrogen mixture gas outlet 26 that derives a hydrogen mixture gas from the gas phase in the electrolytic cell 21. The dilution gas is introduced from the dilution gas mixer 15 into the gas phase in the electrolytic cell 21 via the pipe 13c and the dilution gas introduction port 25. The introduced diluting gas is mixed with hydrogen gas and oxygen gas generated by electrolysis in the gas phase in the electrolytic cell 21.
From the viewpoint of ensuring safety, it is preferable that the dilution gas introduction port 25 is provided closer to the interface between the gas phase and the liquid phase in the electrolytic cell 21 than the hydrogen mixed gas outlet port 26.

The electrolytic cell 21 is provided with a hydrogen mixed gas outlet 26 for deriving the hydrogen mixed gas from the gas phase in the electrolytic cell 21. The hydrogen mixed gas is led out from the gas phase in the electrolytic cell 21 via the outlet pipe 28 connected to the hydrogen mixed gas outlet 26.

A pair of electrode plates 23 and 24 are immersed in the electrolytic raw water 27 in the electrolytic cell 21.
As the electrode plates 23 and 24, those in which the surface of a base material such as a titanium plate is coated with at least one noble metal selected from the group consisting of platinum, iridium, and palladium can be used, but the electrode plates are not limited to this. ..
A solid electrolyte membrane 29 sandwiched between a pair of electrode plates 23, 24 and electrode plates 23, 24 is immersed in the electrolytic raw water 27 in the electrolytic cell 21. If the solid electrolyte film 29 is sandwiched between the electrode plates 23 and 24, H ⁺ ions can move inside the solid electrolyte 29, the efficiency of electrolysis is easy to be excellent, and even if the electrolytic raw water is pure water. Can be electrolyzed.
Examples of the solid electrolyte membrane 29 include, but are not limited to, a proton conductive fluororesin-based ion exchange membrane, and known materials used in electrolysis for the purpose of generating hydrogen gas can be used.

The electrolytic cell 21 provided in the hydrogen mixed gas generation mechanism 20 is a single-tank type electrolytic cell. In the single-tank type electrolytic cell, the gas phase on the anode side and the gas phase on the cathode side are not airtightly separated, and oxygen gas generated at the anode and hydrogen gas generated at the cathode can be mixed. It is an electrolytic cell.
In a conventional hydrogen mixing gas generator having a multi-tank electrolytic cell, the gas phase on the anode side and the gas phase on the cathode side are airtightly separated, and the oxygen gas generated at the anode is the atmosphere or the like. Only the hydrogen gas released to the cathode and generated at the cathode is used.
If a single-tank type electrolytic cell is adopted as the electrolytic cell 21 as in the present embodiment, the oxygen gas generated at the anode can be effectively used. Further, the cost for manufacturing and maintaining the electrolytic cell is reduced.

The shape of the single-tank type electrolytic tank 21 is a bottomed cylinder such as a cylinder or an elliptical cylinder, a polygonal prism such as a quadrangular prism or a hexagonal prism, a cone, an elliptical pyramid, a polygonal pyramid, etc. A frustum-shaped, tubular or polygonal prism shape whose upper inner diameter is smaller than the lower inner diameter, and a cylindrical or polygonal prism shape whose bottom surface or ceiling surface is bent at least one of them. Etc., but are not limited to these.
Among these, from the viewpoint of dilution efficiency when diluting the concentration of hydrogen gas generated from the liquid phase with a diluting gas, the shape of the electrolytic cell 21 is a frustum shape, a tubular shape, or a polygonal prism shape, and the inner diameter of the upper portion thereof. Is preferably smaller than the inner diameter of the lower part. When the electrolytic cell 21 has these shapes, the surface area of the liquid surface formed in the electrolytic cell 21 can be easily reduced, and the concentration of hydrogen gas generated from the liquid surface is efficiently diluted. Therefore, the hydrogen gas concentration in the electrolytic cell 21 is likely to be maintained at less than 4% by volume. The example given as the shape of the electrolytic cell 21 is only an example. The shape of the electrolytic cell 21 may be a cylindrical container, and may be a gourd shape designed so that the thickness of the cylinder becomes thinner from the upper part and the lower part to the central part thereof.
The electrolytic cell 21 may be provided with a baffle plate or the like in the gas phase portion to increase the mixing efficiency of the hydrogen mixed gas.

In the present embodiment, as shown in FIG. 2B, the volume of the gas phase in the electrolytic cell 21b may be smaller than the volume of the liquid phase. Further, in the present embodiment, as shown in FIG. 2C, from the viewpoint of effectively diluting the concentration of hydrogen gas in the gas phase, the pipe 13c extends to the vicinity of the liquid level in the central portion of the gas phase in the electrolytic cell 21c. It may be inserted and extended. In this case, it is preferable because the safety when using the apparatus is ensured, the generated hydrogen mixed gas is uniformly mixed, dilution unevenness can be prevented, and the quality of the hydrogen mixed gas is improved.

The current control device 22 controls the current flowing through the electrode plates 23 and 24. In this embodiment, the current control device 22 is electrically connected to the control mechanism 40. Therefore, the current value flowing through the electrode plates 23 and 24 can be appropriately controlled.
The current control device 22 is not particularly limited as long as it has a function of controlling the current value flowing through the electrode plates 23 and 24 to an arbitrary value, and specifically, a regulated power supply, a current transformer, and a constant current. Examples include generators.
Although not shown in FIG. 1, the hydrogen mixing gas generation mechanism 20 uses a water level gauge for measuring the water level of the electrolytic cell 21, a water temperature gauge for measuring the temperature of the electrolytic raw water 27, and an electrolytic cell 27 as needed. 21 may have a tank for electrolytic raw water to be replenished.

The concentration measuring mechanism 30 includes a hydrogen concentration meter 31, an oxygen concentration meter 32, and a gas-liquid separator 33. The hydrogen concentration meter 31 and the oxygen concentration meter 32 described above measure the hydrogen gas concentration and the oxygen gas concentration in the hydrogen mixed gas containing the hydrogen gas and the oxygen gas, respectively. The hydrogen mixed gas is introduced into each concentration measuring device from the outlet pipe 28 via the pipe 34a.
In the present embodiment, the hydrogen concentration meter 31 and the oxygen concentration meter 32 are electrically connected to the control mechanism 40. Therefore, the concentration value of each gas measured by each densitometer is transmitted to the control mechanism 40. The hydrogen mixed gas after the measurement by each densitometer is redistributed to the outlet pipe 28 via the pipe 34b.

The hydrogen concentration meter 31 may be any as long as it can measure the concentration of hydrogen gas, and is an ultrasonic hydrogen concentration meter, a contact combustion type hydrogen concentration meter, a FID type hydrogen concentration meter, a semiconductor sensor type hydrogen concentration meter, and a light wave interference type. A hydrogen concentration meter or the like can be used. Further, the oxygen concentration meter 32 may be any as long as it can measure the concentration of oxygen gas, and is an ultrasonic hydrogen concentration meter, a galvanized battery type oxygen concentration meter, a zirconia type oxygen concentration meter, a light wave interference type oxygen concentration meter, and a diaphragm. A galvanized oxygen gas concentration meter or the like can be used.
A gas analyzer may be used assuming that the hydrogen concentration meter 31 and the oxygen concentration meter 32 are integrated. As the gas analyzer, a thermal conductivity detector type gas chromatograph (GC-TCD) using an adsorbent such as molecular sieves can be used.

The gas-liquid separator 33 removes the water contained in the hydrogen mixed gas. Moisture derived from electrolytic raw water may be mixed in the hydrogen mixed gas generated by the hydrogen mixed gas generator 1. When a hydrogen mixed gas mixed with water is introduced into each densitometer and measured, deterioration of the sensor in each densitometer tends to progress. For example, a contact combustion type hydrogen concentration meter, a FID type hydrogen concentration meter, a semiconductor sensor type hydrogen concentration meter, or a light wave interference type hydrogen concentration meter is used as the hydrogen concentration meter 31, and a galvanized battery type oxygen concentration meter or a zirconia type is used as the oxygen concentration meter 32. The above-mentioned deterioration problem occurs when an oxygen concentration meter, a light wave interference type oxygen concentration meter, or a diaphragm galvanized battery type oxygen concentration meter is used. Therefore, if the gas-liquid separator 33 is installed on the primary side of each densitometer, water can be removed and deterioration of each densitometer can be prevented.
The gas-liquid separator 33 is not particularly limited as long as it can remove the water content in the hydrogen mixed gas, and examples thereof include a drain trap, a mist separator, a water separator, a heating type dryer, and an activated carbon type air dryer. From the viewpoint of production cost, the gas-liquid separator 33 may be configured to be able to supply the removed water to the electrolytic cell 21 for reuse.

The control mechanism 40 outputs a control signal to the mass flow controllers 14a and 14b and the current control device 22 based on the measured values of the hydrogen gas concentration and the oxygen gas concentration measured by the concentration measuring mechanism 30, and the generated hydrogen. Control the hydrogen gas concentration and oxygen gas concentration in the mixed gas. The control mechanism 40 outputs a control signal to the mass flow controllers 14a and 14b based on the flow rate of the hydrogen mixed gas measured by the mass flow meter 51 described later, and controls the flow rate of each diluted gas to control the flow rate of the hydrogen mixed gas. Control.
The control mechanism 40 is not particularly specified as long as it is a control device having an arithmetic function, and examples thereof include a sequencer and a CPU. The control mechanism 40 may be divided into a signal receiving unit for receiving the measured value of each electrically connected device and an output unit for outputting the control signal to each device.

The hydrogen mixed gas supply mechanism 50 administers the hydrogen mixed gas to the supply target.
The hydrogen mixed gas supply mechanism 50 includes a mass flow meter 51 and a supply pipe 52. The primary side of the mass flow meter 51 is connected to the lead-out pipe 28, and the secondary side thereof is connected to the supply pipe 52.
The mass flow meter 51 measures the flow rate of the hydrogen mixed gas flowing in the lead-out pipe 28. The mass flow meter 51 is electrically connected to the control mechanism 40. The mass flow meter 51 is not particularly limited as long as it has a function of measuring the flow rate of the mixed gas. For example, a float type flow meter, a positive displacement type flow meter, or the like having a function of measuring the flow rate of the hydrogen mixed gas can be used. Instead of the mass flow meter 51, a mass flow controller having a function of adjusting the flow rate of the hydrogen mixed gas may be used.
Although not shown in FIG. 1, the hydrogen mixed gas supply mechanism 50 is provided with a discharge line for discharging excess gas, a pressure gauge for measuring the pressure in the circuit, a thermometer for measuring the gas temperature to be administered to the patient, and the like. You may. Further, although not shown in FIG. 1, a pressure gauge or the like for measuring the pressure of the hydrogen mixed gas may be provided in the pipe 28 or the pipe 52.

[Hydrogen mixed gas generation method]
Next, an example of the method for generating the hydrogen mixed gas of the present embodiment using the hydrogen mixed gas generating device 1 described above will be described.
The method for producing a hydrogen mixed gas of the present embodiment is a method for generating a hydrogen mixed gas using the hydrogen mixed gas generating device 1 having the above-described configuration. Hereinafter, the method for producing the hydrogen mixed gas of the present embodiment will be specifically described with reference to FIGS. 3 and 4. In FIG. 3, the circled A shown after step S9 is the same symbol as the circled A shown before step S10 in FIG. 4, and from step S9 to step S10, A series of operations indicates that they are continuous.

(Step S1, Step S2, and Step S3)
The power of the hydrogen mixed gas generator 1 is turned on (step S1), and the control mechanism 40 sets the hydrogen gas concentration, the oxygen gas concentration, and the flow rate at the time of supply of the desired hydrogen mixed gas (step S2). After the setting, the operation of the hydrogen mixed gas generator 1 is started, and the supply of oxygen gas and nitrogen gas is started (step S3). The set value of the hydrogen gas concentration is set to less than 4% by volume.

(Step S4)
The concentration measuring mechanism 30 measures the oxygen gas concentration contained in the diluted gas that has been mixed by the dilution gas mixer 15 and has passed through the electrolytic cell 21 and is led out to the lead-out pipe 28 by the oxygen concentration meter 32.

(Step S5)
The control mechanism 40 determines whether the oxygen gas concentration measured in step S4 is the set value. Here, when the control mechanism 40 determines that the oxygen gas concentration is the set value (step S5; YES), the process proceeds to step S6. On the other hand, when the control mechanism 40 determines that the oxygen gas concentration has not reached the set value (step S5; NO), the process returns to step S4 via the process of step S51.

(Step S51)
The control mechanism 40 gives a signal to the mass flow controller 14a based on the oxygen gas concentration measured in step S4 and the determination result in step S5, and controls the flow rate of oxygen gas flowing in the pipe 13a. After controlling the flow rate of the oxygen gas, the control mechanism 40 returns the process to step S4.

(Step S6)
The hydrogen mixed gas supply mechanism 50 measures the flow rate of the diluted gas processed in step S5 with the mass flow meter 51.

(Step S7)
The control mechanism 40 determines whether the flow rate of the diluted gas measured in step S6 is a set value. Here, when the control mechanism 40 determines that the flow rate of the diluted gas is the set value (step S7; YES), the process proceeds to step S8. On the other hand, when the control mechanism 40 determines that the flow rate of the hydrogen mixed gas has not reached the set value (step S7; NO), the process returns to step S4 via the process of step S71.

(Step S71)
The control mechanism 40 gives a signal to the mass flow controller 14b based on the flow rate of the diluted gas measured in step S6 and the determination result in step S7, and controls the flow rate of nitrogen gas flowing in the pipe 13b. After controlling the flow rate of the nitrogen gas, the control mechanism 40 returns the process to step S4.

(Step S8)
The concentration measuring mechanism 30 measures the concentration of hydrogen gas contained in the diluted gas that has been mixed by the diluent gas mixer 15 and passed through the electrolytic cell 21 and led out to the lead-out pipe 28 by the hydrogen concentration meter 31.

(Step S9)
The control mechanism 40 determines whether or not the hydrogen gas concentration measured in step S8 is 0, or whether or not the hydrogen gas concentration is equal to or less than a specified value. The specified value here is a value that ensures safety when electrolyzing in the electrolytic cell 21 in step S10 described later.
When the control mechanism 40 determines that the hydrogen gas concentration is 0 or equal to or lower than the specified value (step S9; YES), the process proceeds to step S10. On the other hand, when the control mechanism 40 determines that the hydrogen gas concentration is not 0 (step S9; NO), the process returns to step S4.

(Step S10)
The control mechanism 40 gives a signal to the current control device 22, starts energizing the electrode plates 23 and 24, and starts electrolysis of the electrolytic raw water 27. The hydrogen gas generated by electrolysis is mixed in the electrolytic cell 21 with the diluting gas whose oxygen gas concentration is controlled to a set value. The hydrogen mixed gas generated in the electrolytic cell 21 is supplied to the concentration measuring mechanism 30 via the lead-out pipe 28. Which of the electrode plates 23 and 24 is used as the anode (cathode) is arbitrarily selected.

(Step S11)
The concentration measuring mechanism 30 measures the concentration of hydrogen gas contained in the hydrogen mixed gas generated in step S10 by the hydrogen concentration meter 31.

(Step S12)
The control mechanism 40 determines whether the hydrogen gas concentration measured in step S11 is a set value. Here, when the control mechanism 40 determines that the hydrogen gas concentration is the set value (step S12; YES), the process proceeds to step S13. On the other hand, when the control mechanism 40 determines that the hydrogen gas concentration has not reached the set value (step S12; NO), the process returns to step S11 via the process of step S121.

(Step S121)
The control mechanism 40 gives a signal to the current control device 22 based on the hydrogen gas concentration measured in step S11 and the determination result in step S12, and controls the current values flowing through the electrode plates 23 and 24. After controlling the current value, the control mechanism 40 returns the process to step S11.

More specifically, when the measured hydrogen gas concentration is lower than the set value, the control mechanism 40 gives a signal to the current control device 22 to increase the current value flowing through the electrode plates 23 and 24. On the other hand, when the measured hydrogen gas concentration is higher than the set value, the control mechanism 40 gives a signal to the current control device 22 to reduce the current value flowing through the electrode plates 23 and 24.

(Step S13)
The concentration measuring mechanism 30 measures the oxygen gas concentration contained in the hydrogen mixed gas processed in step S12 by the oxygen concentration meter 32.

(Step S14)
The control mechanism 40 determines whether the oxygen gas concentration measured in step S13 is the set value. Here, when the control mechanism 40 determines that the oxygen gas concentration is the set value (step S14; YES), the process proceeds to step S15. On the other hand, when the control mechanism 40 determines that the oxygen gas concentration has not reached the set value (step S14; NO), the process returns to step S11 via the process of step S141.

(Step S141)
The control mechanism 40 gives a signal to the mass flow controller 14a based on the oxygen gas concentration measured in step S13 and the determination result in step S14, and controls the flow rate of oxygen gas flowing in the pipe 13a. After controlling the flow rate of the oxygen gas, the control mechanism 40 returns the process to step S11.

The control mechanism 40 adjusts the flow rate of oxygen gas through the mass flow controller 14a while calculating the amount of oxygen gas generated on the anode side in the electrolytic cell 21. If the amount of oxygen gas generated in the electrolytic tank 21 is calculated in this way, and the oxygen gas obtained by subtracting that amount from the desired oxygen gas concentration by back calculation is supplied from the oxygen gas cylinder 11, the oxygen in the hydrogen mixed gas is supplied. It is possible to control the gas concentration accurately and finely.
The amount of oxygen gas generated in the electrolytic cell 21 is estimated from the concentration of hydrogen gas generated. The flow rate of oxygen gas is theoretically derived from the following formula from the measured hydrogen gas concentration, the desired oxygen gas concentration, and the desired mixed gas flow rate.
(Oxygen gas flow rate) [L / min] = (desired oxygen concentration) [%]-(measured hydrogen gas concentration) [%] / 2) × 100 × (desired hydrogen mixed gas flow rate) [ L / min] ・ ・ ・ (Equation 1)

More specifically, when the measured oxygen gas concentration is lower than the set oxygen gas concentration, the control mechanism 40 sends a signal to the mass flow controller 14a to increase the flow rate of the oxygen gas flowing in the pipe 13a. give away. On the other hand, when the measured oxygen gas concentration is higher than the set oxygen gas concentration, the control mechanism 40 gives a signal to the mass flow controller 14a to reduce the flow rate of the oxygen gas flowing in the pipe 13a.

(Step S15)
The hydrogen mixed gas supply mechanism 50 measures the flow rate of the hydrogen mixed gas processed in step S14 by the mass flow meter 51.

(Step S16)
The control mechanism 40 determines whether the flow rate of the hydrogen mixed gas measured in step S15 is a set value. Here, when the control mechanism 40 determines that the flow rate of the hydrogen mixed gas is the set value (step S16; YES), the control mechanism 40 sends a signal to the hydrogen mixed gas supply mechanism 50 to supply the hydrogen mixed gas. give away. On the other hand, when the control mechanism 40 determines that the flow rate of the hydrogen mixed gas has not reached the set value (step S16; NO), the process returns to step S11 via the process of step S161.

(Step S161)
The control mechanism 40 gives a signal to the mass flow controller 14b based on the flow rate of the hydrogen mixed gas measured in step S15 and the determination result in step S16, and controls the flow rate of the nitrogen gas flowing in the pipe 13b.

More specifically, when the flow rate of the hydrogen mixed gas measured in step S15 is lower than the set value, the control mechanism 40 causes the mass flow controller 14b to increase the flow rate of the nitrogen gas flowing in the pipe 13b. Give a signal. By increasing the flow rate of the nitrogen gas, the shortage with respect to the set flow rate of the hydrogen mixed gas is compensated. The control mechanism 40 returns the process to step S11 after increasing the flow rate of the nitrogen gas.

On the other hand, when the flow rate of the hydrogen mixed gas measured in step S15 is higher than the set value, the control mechanism 40 causes the mass flow controller 14b to reduce the flow rate of the nitrogen gas flowing in the pipe 13b. Give a signal. By reducing the flow rate of the nitrogen gas, the amount exceeding the set flow rate of the hydrogen mixed gas is reduced. The control mechanism 40 returns the process to step S11 after reducing the flow rate of the nitrogen gas.

As described above, by measuring the flow rate of the hydrogen mixed gas, the hydrogen gas concentration in the hydrogen mixed gas, and the oxygen gas concentration as in the present embodiment, the current flowing through the electrode plates 23 and 24, the oxygen gas flow rate, and the nitrogen gas flow rate. By controlling each parameter such as, complicated calculation can be left to the control mechanism 40, and each gas concentration can be set and changed.

In this embodiment, carbon dioxide gas, argon gas, helium gas, xenon gas and the like can be used instead of the nitrogen gas used to generate the diluted gas. Further, as described above, when air pressurized by a compressor or the like is used as an oxygen gas supply source instead of the oxygen gas cylinder used in the present embodiment, the nitrogen gas supply means can be omitted.

(Action effect)
According to the hydrogen mixing gas generator 1 having the above configuration, the structure of the electrolytic cell is generated on the anode side because the gas phase on the anode side and the gas phase on the cathode side of the electrode plate are not separated by the diaphragm. Oxygen gas can be directly mixed in the gas phase of the electrolytic cell, and hydrogen mixed gas can be efficiently supplied.

Further, according to the hydrogen mixed gas generator 1, a high concentration region of hydrogen gas is less likely to be formed in the electrolytic cell, and safety can be further improved. Therefore, according to the hydrogen mixed gas generator 1, the high concentration region of hydrogen gas can be reduced and the safety can be further improved while maintaining the hydrogen gas generation efficiency by electrolysis at a level that can withstand practical use.

Although the embodiments of the present invention have been described in detail above, the present invention is not limited to such specific embodiments. In addition, the present invention may be added, omitted, replaced, or otherwise modified within the scope of the gist of the present invention described in the claims. For example, as in the hydrogen mixing gas generating device 1a according to the modified example of the embodiment shown in FIG. 5, oxygen gas and nitrogen gas, which are diluting gases, are introduced into the electrolytic cell 21 via independent pipes 13a and 13b, respectively. The configuration, that is, the oxygen gas introduction port and the nitrogen gas introduction port may be open to the gas phase portion in the electrolytic cell 21, respectively.

The hydrogen mixed gas generator and the hydrogen mixed gas generation method of the present invention are particularly highly useful when applied to medical equipment or the like in which it is required to optimize each component ratio and flow rate.

1 ... Hydrogen mixed gas generator, 10 ... Diluted gas introduction mechanism, 20 ... Hydrogen mixed gas generation mechanism, 30 ... Concentration measurement mechanism, 40 ... Control mechanism, 50 ... Hydrogen mixed gas supply mechanism

Claims (4)

A hydrogen mixed gas generator that produces a hydrogen mixed gas by mixing hydrogen gas generated by electrolyzing raw electrolytic water with a diluted gas containing at least oxygen gas.
A dilution gas introduction mechanism that introduces the dilution gas into the hydrogen gas,
A hydrogen mixed gas generation mechanism that mixes the hydrogen gas and the diluted gas to generate the hydrogen mixed gas, and
A concentration measuring mechanism having a hydrogen concentration meter for measuring the hydrogen gas concentration in the hydrogen mixed gas; and an oxygen concentration meter for measuring the oxygen gas concentration in the hydrogen mixed gas;
A hydrogen mixed gas supply mechanism that administers the hydrogen mixed gas to the supply target, and
A control mechanism that calculates the concentration of oxygen gas generated by electrolyzing the electrolytic raw water from the hydrogen gas concentration and adjusts the flow rate of oxygen gas in the diluted gas using the following formula (1).
With
The diluted gas introduction mechanism is supplied from an oxygen gas supply means; a nitrogen gas supply means; a first mass flow controller that regulates the flow rate of the oxygen gas supplied from the oxygen gas supply means; and the nitrogen gas supply means. Has a second mass flow controller that regulates the flow rate of nitrogen gas;
Have electrolyzer of hydrogen mixed gas generating mechanism is a single tank type, at least a pair of electrode plates is immersed in the liquid phase of the interior of the electrolytic cell,
The hydrogen mixed gas supply mechanism has a mass flow meter for measuring the flow rate of the hydrogen mixed gas or a third mass flow controller having a flow rate adjusting function.
Hydrogen mixing in which the control mechanism is electrically connected to the mass flow meter or the third mass flow controller, the first mass flow controller, the second mass flow controller, the hydrogen concentration meter, and the oxygen concentration meter. Gas generator.
(Flow rate of oxygen gas in diluted gas) [L / min] = ((desired oxygen concentration) [%]-(measured hydrogen gas concentration) [%] / 2) / 100 × (desired hydrogen mixed gas) Flow rate) [L / min] ・ ・ ・ Equation (1) Claim 1 The electrolytic cell has a dilution gas introduction port for introducing a dilution gas into the gas phase in the electrolytic cell and a hydrogen mixture gas outlet for deriving a hydrogen mixture gas from the gas phase in the electrolytic cell. The hydrogen mixed gas generator according to. The hydrogen mixed gas generating apparatus according to claim 2, wherein the diluted gas introduction port is provided closer to the interface between the gas phase and the liquid phase in the electrolytic cell than the hydrogen mixed gas outlet. A method for producing a hydrogen mixed gas using the hydrogen mixed gas generating apparatus according to any one of claims 1 to 3.

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