Cold and hot integrated activated carbon adsorber for helium purification and use method
Technical Field
The invention relates to the technical field of gas production. In particular to a cold and hot integrated active carbon absorber for helium purification and a use method thereof.
Background
Helium is a rare gas, colorless and odorless, and is inert in chemical properties, and is difficult to react with other substances in a general state, and natural isotopes of helium are two kinds, namely helium-4 and helium-3. Helium has many applications and can be used as a pressure-feed agent and a pressurizing agent for rocket liquid fuels. It has excellent permeability, can be used for nuclear reactor cooling, leak detection of some of the tubes and electronic and electrical devices of rockets and nuclear reactors. Liquid helium can obtain low temperature close to absolute zero, and can be used for superconductor research and other scientific experiments. Helium-3 gas is generally used in the fields of proportional counter tube fabrication, nuclear magnetic resonance and the like. Helium is scarce in reserves and expensive.
Due to the inert chemistry of helium-3 gas, a variety of methods of decontamination can be used, and for small volumes of helium-3 gas, the use of activated carbon for decontamination is a more economical way. The purification principle is as follows:
The activated carbon method is a good adsorbent for various impurity gases, and the adsorption quantity of the adsorbent is related to the adsorption surface area, the adsorption temperature and the gas pressure. The more easily liquefied gas is generally, the more easily it is adsorbed by activated carbon. Because helium isotope critical temperature (-267.9 ℃) is the lowest, it can be said that all other impurity elements are easier to liquefy than helium, so that the adsorption capacity of active carbon to impurity elements is stronger than helium at liquid nitrogen temperature, thereby achieving the purpose of removing impurities. The activated carbon after adsorbing the impurity gas is heated and thoroughly deaerated so as to be convenient for the next use.
In the prior art of helium-3 gas production or purification, the adopted activated carbon purification bed is mainly composed of two types, one type is a straight cylinder type design, the inside is not provided with a flow guiding structure, and the design mode ensures that the gas circulation path is shorter, so that the gas cannot fully contact with the activated carbon, and the purification rate is lower. Another design method adopts a serpentine coil pipe as an active carbon bed shell, and the mode has the advantages that the gas flow path is prolonged, but the manufacturing process is complex, a circular pipe spiral structure can generate a plurality of heating empty areas during heating, the heat uniformity is poor, and a large amount of waste heat is caused. Because the active carbon has better selective adsorption effect at low temperature, the active carbon beds with the two structures are provided with independent cold traps, and the cold traps are used for filling liquid nitrogen and providing a low-temperature environment when the active carbon is required to be adsorbed at low temperature. When the thermal degassing is needed, the independent cold trap is detached, and an electric furnace is sleeved for heating to thermally degas the activated carbon bed. The operation of the activated carbon bed which needs to frequently disassemble and assemble the cold trap and the electric furnace is complicated, the tightness of the electric furnace and the cold trap is poor, and waste heat and liquid nitrogen evaporation amount generated during use are large, so that energy waste is caused.
Therefore, an activated carbon adsorption purifier for helium purification needs to be designed, the operation flow of loading and unloading the cooling and heating device is simplified, and the evaporation amount of liquid nitrogen and waste heat are reduced.
Disclosure of Invention
The invention aims at: a cold and hot integrated active carbon absorber for helium purification is designed, and a use method of the cold and hot integrated active carbon absorber is formulated, so that the cold and hot integrated active carbon absorber can be suitable for a helium impurity removal process. Meanwhile, the method has the characteristics of simplicity in operation and reduction in loss.
The technical scheme of the invention is as follows: a cold and hot integrated active carbon adsorber for helium purification comprises a reaction bed cylinder body, a multi-layer metal heat shield and a double-layer liquid nitrogen heat preservation tank; the reactor cylinder is wrapped by a plurality of layers of metal heat shields which are arranged in the double-layer liquid nitrogen heat preservation tank;
A spiral guide plate is arranged in the reactor cylinder, and activated carbon filler is filled along the spiral guide plate; an armored heater is welded at the middle part of the spiral guide plate; the upper part and the lower part of the reactor cylinder body are respectively provided with a lower filter plate of the reaction bed and an upper filter plate of the reaction bed;
The liquid nitrogen tank evacuation pipe is positioned the top of the double-layer liquid nitrogen heat preservation tank;
the supercharging device is fixed on the double layers a side surface of the liquid nitrogen heat preservation tank;
The liquid nitrogen inlet and outlet pipe is formed by double layers side of liquid nitrogen heat preservation tank introduced into double-layer liquid nitrogen the bottom of the heat preservation tank;
the liquid nitrogen level gauge is inserted into the double-layer liquid nitrogen heat preservation tank;
the gas inlet pipe before purification is introduced from the top of the double-layer liquid nitrogen heat preservation tank, passes through the multi-layer metal heat shield and is welded to the bottom of the reaction bed cylinder;
the armored thermocouple is introduced from the top of the double-layer liquid nitrogen heat-preserving tank, penetrates through the top surface of the multi-layer metal heat shield and goes deep into the reactor cylinder;
the purified gas outlet pipe is led out from the top of the reactor cylinder body, passes through the multi-layer metal heat shield and is led out from the top of the double-layer liquid nitrogen heat preservation tank.
The reactor cylinder is fixed with the top surface of the multilayer metal heat shield through screws; the multi-layer metal heat shield is fixed inside the double-layer liquid nitrogen heat preservation tank through screws.
The application method of the cold and hot integrated activated carbon adsorber for helium purification comprises the following steps:
s1: filling activated carbon particles into a reaction bed cylinder along a spiral guide plate, and compacting to fill the reaction bed cylinder;
s2: measuring the temperature by an armored thermocouple, heating the armored heater to 300-500 ℃, and pumping out the reaction bed cylinder by a purified gas outlet pipe connected to a vacuum pumping system;
S3: the evacuating system which is connected with the evacuating pipe of the liquid nitrogen tank evacuates the air in the double-layer liquid nitrogen heat preservation tank, and liquid nitrogen is injected into the double-layer liquid nitrogen heat preservation tank through the liquid nitrogen inlet and outlet pipe;
S4: the gas to be purified is introduced through the gas inlet pipe before purification, dust in the gas is filtered through the filter plate below the reaction bed, the purified gas is discharged through the gas outlet pipe after purification, and the gas is filtered through the filter plate on the reaction bed again when being discharged from the gas outlet pipe after purification.
In the step S1, the activated carbon particles are high-iodine value activated carbon particles with the particle size of 2-10 mm.
In the step S1, the larger granular activated carbon and the smaller granular activated carbon are mixed and filled during filling, and filler pulverization is prevented in the process.
And in the step S2, continuously evacuating until the vacuum degree is less than 5Pa.
In the step S3, the liquid level in the double-layer liquid nitrogen heat preservation tank is monitored according to a liquid level meter, and the liquid nitrogen is supplemented to a set value.
In the step S4, the flow speed and the gas pressure in the reaction bed cylinder are controlled, and the gas pressure in the reaction bed cylinder is 0.1-0.3MPa.
In S4, the gas is circulated and purified by using a gas circulation pump.
S5, evacuating the liquid nitrogen in the double-layer liquid nitrogen heat preservation tank, filling the vaporized high-pressure nitrogen in the pressurizing device into the double-layer liquid nitrogen heat preservation tank during evacuation, and pressing the liquid nitrogen into the liquid nitrogen recovery tank through the liquid nitrogen inlet and outlet pipe; and then carrying out hot exhaust, heating the armored heater, heating the activated carbon particles to 300-500 ℃, and simultaneously evacuating the heated activated carbon particles from a purified gas outlet pipe by using a vacuum-pumping system, and evacuating the activated carbon particles to a vacuum degree of less than 10Pa.
The invention has the remarkable effects that:
1) The gas adsorption with lower condensation point is realized by utilizing the difference of the adsorption performance of the active carbon on impurity gas in helium at low temperature.
2) The flow guiding type structural design realizes the growth of a gas diffusion path in a limited space without affecting the fluidity of gas, so that the gas to be purified is in more sufficient contact with the activated carbon.
3) And the activated carbon with different specifications is adopted for filling, so that the maximum activated carbon filling amount is realized.
4) The activated carbon purifier is used for a plurality of times, and after the adsorption performance of the activated carbon purifier is reduced, the activated carbon purifier is heated, continuously evacuated and degassed, so that the activated carbon purifier can be recycled.
5) The gas to be purified with the circulation pressure of 1.3-2atm and the flow rate of 1-10L/min is controlled to pass through an active carbon purifier in a liquid nitrogen environment, and helium containing less than 0.5% of oxygen, nitrogen, water vapor, carbon dioxide, argon and other impurity gases can be purified to less than or equal to 0.001% of the impurity gases within 1 h.
Drawings
FIG. 1 is a schematic diagram of a cold and hot integrated activated carbon adsorber for helium purification;
FIG. 2 is a schematic diagram of a thermocouple vacuum gauge for a cold and hot integrated activated carbon adsorber for helium purification;
In the figure: 1-evacuating the liquid nitrogen tank; 2-a supercharging device; 3-a reaction bed cylinder; 4-a multi-layer metal heat shield; 5-a double-layer liquid nitrogen heat preservation tank; 6-a filter plate under the reaction bed; 7-a spiral guide plate; 8-activated carbon particle filler; 9-liquid nitrogen inlet and outlet pipes; 10-a filter plate on the reaction bed; 11-sheathed heater; 12-a liquid level gauge; 13, a gas inlet pipe before purification; 14-thermocouple vacuum gauge; 15-a purified gas outlet pipe.
Detailed Description
In the following description, numerous specific details are set forth in order to provide a thorough understanding of the present application. The present application may be embodied in many other forms than those herein described, and those skilled in the art will readily appreciate that the present application may be similarly embodied without departing from the spirit or essential characteristics thereof, and therefore the present application is not limited to the specific embodiments disclosed below.
The terminology used in the one or more embodiments of the application is for the purpose of describing particular embodiments only and is not intended to be limiting of the one or more embodiments of the application. As used in one or more embodiments of the application and the appended claims, the singular forms "a," "an," and "the" are intended to include the plural forms as well, unless the context clearly indicates otherwise. It should also be understood that the term "and/or" as used in one or more embodiments of the present application refers to and encompasses any or all possible combinations of one or more of the associated listed items.
It should be understood that, although the terms first, second, etc. may be used in one or more embodiments of the application to describe various information, these information should not be limited by these terms. These terms are only used to distinguish one type of information from another. For example, a first may also be referred to as a second, and similarly, a second may also be referred to as a first, without departing from the scope of one or more embodiments of the application.
A cold and hot integrated active carbon adsorber for helium purification comprises a liquid nitrogen tank evacuation pipe 1, a supercharging device 2, a reaction bed cylinder 3, a multi-layer metal heat shield 4, a double-layer liquid nitrogen heat preservation tank 5, a reaction bed lower filter plate 6, a spiral guide plate 7, active carbon particle fillers 8, a liquid nitrogen inlet and outlet pipe 9, a reaction bed upper filter plate 10, an armored heater 11, a liquid level meter 12, a pre-purification gas inlet pipe 13, a thermocouple vacuum gauge 14 and a purified gas outlet pipe 15.
The gas inlet pipe 13 before purification is introduced from the top 5 of the double-layer liquid nitrogen heat preservation tank, passes through the multi-layer metal heat shield 4 and is welded to the bottom of the reaction bed cylinder 3, the filter plate 6 under the reaction bed is welded to the inner bottom of the reactor cylinder 3, so that the gas entering the gas inlet pipe 13 before purification is filtered through the filter plate 6 under the reaction bed, the spiral guide plate 7 is welded in the reactor cylinder 3, and the core part of the spiral guide plate 7 is welded with the armored heater 11 which is used for heating; the armored thermocouple 14 penetrates into the reactor cylinder 3 from the top surface of the multi-layer metal heat shield 4 and is welded to the top surface of the reactor cylinder 3, so that the armored thermocouple 14 measures the temperature of the activated carbon filler 8 in the reactor cylinder 3; the liquid nitrogen level gauge 12 is inserted into the double-layer liquid nitrogen heat preservation tank 5, can output 4-20mA signals, and the signals are connected into the control system to display the liquid level condition in real time; the reactor cylinder 3 is wrapped by a multi-layer metal heat shield 4 and is fixed with the top surface of the multi-layer metal heat shield 4 through screws, the multi-layer metal heat shield 4 is not sealed, and the multi-layer metal heat shield 4 is arranged in a double-layer liquid nitrogen heat preservation tank 5 and is fixed with the double-layer liquid nitrogen heat preservation tank through screws; the purified gas outlet pipe 15 is led out from the top of the reactor cylinder 3, and a filter plate 10 on the reaction bed is arranged on the top of the reactor cylinder 3 and is used for filtering the purified gas. The purified gas outlet pipe 15 is connected to the top of the reactor cylinder 3 in a welding mode and ensures sealing, passes through the multi-layer metal heat shield 4 and is finally led out from the top of the double-layer liquid nitrogen heat preservation tank 5; the activated carbon packing 8 is packed along the spiral guide 7.
The liquid nitrogen inlet and outlet pipe 9 is led into the inner bottom of the double-layer liquid nitrogen heat preservation tank 5 from the side surface of the double-layer liquid nitrogen heat preservation tank and is used for filling and discharging liquid nitrogen; the pressurizing device 2 is fixed on the side surface of the double-layer liquid nitrogen heat preservation tank 5, and can lead out part of liquid nitrogen to be heated and gasified by the environment, and then high-pressure nitrogen is filled into the double-layer liquid nitrogen heat preservation tank 5, so that the liquid nitrogen in the double-layer liquid nitrogen heat preservation tank is extruded by pressure and discharged from the liquid nitrogen inlet and outlet pipe 9, and liquid nitrogen emptying is realized. The liquid nitrogen tank evacuating pipe 1 is positioned at the top of the double-layer liquid nitrogen heat preservation tank 5 and is used for evacuating air in the double-layer liquid nitrogen heat preservation tank 5.
A specific use process of a cold and hot integrated active carbon adsorber for helium purification comprises the following steps:
1. The high-iodine value activated carbon particles 8 with the particle size of 2-10mm are filled into the reaction bed cylinder 3 along the spiral guide plate 7 and are compacted to be full of the reaction bed cylinder 3, the large-particle activated carbon and the small-particle activated carbon are mixed and filled during filling, and the small-particle activated carbon is filled into gaps of the large-particle activated carbon, so that the influence on the gas circulation resistance is reduced as much as possible while the filling amount of the activated carbon is increased. However, in the process, to prevent the filler from being pulverized, activated carbon particles with any shape can be adopted, and spherical particles which are easy to fill are preferably adopted.
2. The whole set of activated carbon adsorption purifier is assembled, connected with a power supply for heating, the thermocouple vacuum gauge 14 measures the temperature and feeds back a signal to a control system, so that the heating temperature is controlled to enable the armored heater 11 to be heated to 300-500 ℃, and the purified gas outlet pipe 15 is connected with a vacuumizing system for vacuumizing, so that impurity gas adsorbed in micropores of activated carbon particles 8 is exhausted, and the vacuumizing is continued until the vacuum degree is less than 5Pa.
3. When the activated carbon bed is used for purification, firstly, the evacuation system connected with the liquid nitrogen tank evacuation pipe 1 evacuates air in the double-layer liquid nitrogen heat preservation tank 5, then liquid nitrogen enters the double-layer liquid nitrogen heat preservation tank 5 through the liquid nitrogen inlet and outlet pipe 9 by controlling the liquid nitrogen supply device valve, the liquid level in the double-layer liquid nitrogen heat preservation tank 5 is monitored according to the signal fed back by the liquid level meter 12, the liquid level is fed back to the control system in real time, and then the signal fed back to the liquid nitrogen automatic filling device by the control system is fed back to enable the liquid nitrogen to be filled to a set value.
4. The purification bed is pre-cooled before use, the purpose of pre-cooling is to make the temperature of the activated carbon particles 8 in the reaction bed cylinder 3 uniform, after the pre-cooling is finished, the gas to be purified is introduced through the gas inlet pipe 13 before purification, the flow rate and the gas pressure in the reaction bed cylinder 3 are controlled, and the gas pressure in the reaction bed cylinder 3 is 0.1-0.3MPa. The gas to be purified is filtered by the filter plate 6 (the aperture of the filter plate is 2-5 μm) under the reaction bed, the purified gas is discharged from the purified gas outlet pipe 15, and the gas is filtered again by the filter plate 10 (the aperture of the filter plate is 0.5-4 μm) on the reaction bed when being discharged from the purified gas outlet pipe 15.
5. In order to achieve better purification effect, a gas circulation pump can be used for circulating and purifying gas (the flow rate is 1-10L/min), and the purification effect is further improved by the gas in the system in a continuous circulation mode.
6. After the purification task is finished, firstly, the liquid nitrogen in the double-layer liquid nitrogen heat preservation tank 5 is emptied, and when the liquid nitrogen is emptied, the vaporized high-pressure nitrogen in the pressurizing device 2 is filled into the double-layer liquid nitrogen heat preservation tank 5, and the liquid nitrogen is pressed into the liquid nitrogen recovery tank through the liquid nitrogen inlet and outlet pipe 9. And then carrying out hot exhaust on the purification bed, namely heating the armored heater 11 to enable the temperature of the activated carbon particles 8 to be raised to 300-500 ℃, and evacuating the purified gas from the gas outlet pipe 15 by using a vacuum pumping system when the activated carbon particles are heated, wherein the vacuum degree is less than 10Pa.
7. After the reaction bed is heated, the reaction bed is kept stand for cooling, or air is introduced into the double-layer liquid nitrogen heat preservation tank 5 for quick cooling, and when the temperature of the filler in the reactor is reduced to below 50 ℃, liquid nitrogen can be introduced for cooling, and the purification work is performed again.
Application instance
According to the test of the steps, the helium-3 gas with the oxygen content of 0.2%, the nitrogen content of 0.6% and the hydrogen content of 0.3% is subjected to the purification test, the traditional separation type active carbon bed and the integrated active carbon bed are respectively used for performance comparison, the purification time is 1h, and therefore, the integrated active carbon bed improves the purification effect and simultaneously reduces the workload and the liquid nitrogen loss
The foregoing description of the preferred embodiment of the present invention is not intended to limit the scope of the present invention, but is intended to cover any modifications, equivalents, improvements or alternatives falling within the spirit and principles of the present invention.
It should be noted that, for the sake of simplicity of description, the foregoing method embodiments are all expressed as a series of combinations of actions, but it should be understood by those skilled in the art that the present application is not limited by the order of actions described, as some steps may be performed in other order or simultaneously in accordance with the present application. Further, those skilled in the art will appreciate that the embodiments described in the specification are all preferred embodiments, and that the acts and modules referred to are not necessarily all required for the present application.
In the foregoing embodiments, the descriptions of the embodiments are emphasized, and for parts of one embodiment that are not described in detail, reference may be made to the related descriptions of other embodiments.
The preferred embodiments of the application disclosed above are intended only to assist in the explanation of the application. Alternative embodiments are not intended to be exhaustive or to limit the application to the precise form disclosed. Obviously, many modifications and variations are possible in light of the above teaching. The embodiments were chosen and described in order to best explain the principles of the application and the practical application, to thereby enable others skilled in the art to best understand and utilize the application.