Container for storage of hydrogen

FIELD: hydrogenous power engineering; containers for storage of hydrogen.

SUBSTANCE: the invention is pertaining to the field of hydrogenous power engineering, in particular, to containers for storage of hydrogen. The container for storage of hydrogen consists of a hermetic body, production process branch-pipes, a heater and a hydrogen filler-accumulator located in the body. The hydrogen filler-accumulator represents the hollow microspheres fixed to each other in an unified rigid structure formed layerwise out of microspheres of different diameter. Diameter of the microspheres is diminishing from the central layer to the peripheral one. On the outer surface of the rigid structure there may be a coating out of metal, which is effectively absorbing hydrogen, for example, palladium or nickel or an alloy of lanthanum with nickel. In the capacity of the material of the microsphere use steel or titanium, either lanthanum, or nickel, either zirconium or alloys on the basis of these metals or black lead, or compositions on the basis of black lead. The microspheres out of a metal may be fixed to each other by a diffusion welding. The invention is intended for creation of a container for a safe storage of hydrogen ensuring an increase of the mass contents of hydrogen above 6 %.

EFFECT: the invention ensures creation of a container for a safe storage of hydrogen and an increase of the mass contents of hydrogen above 6 %.

 

The invention relates to the field of hydrogen energy - accumulation and storage of hydrogen, which is currently used in the chemical, transportation and other industries.

Known devices for hydrogen storage based on the binding of hydrogen in the solid material (for example, metal hydrides or sorption on the surface of dispersed nanomaterials), (RF patents №2037737, 2038525, IPC F 17 5/04), these devices for the accumulation and storage of hydrogen are the most explosion-existing, since hydrogen has no pressure, but such systems are slow and require a certain time (about several minutes) to get started, the uptake and release of hydrogen occurs with significant thermal effects, in addition, the mass content of hydrogen is the ratio of the weight of hydrogen, contained in the battery to the weight of the battery of 4.5% is very low. Mass content depends on the number of hydrogen accumulating material, and the specific weight of the storage material.

Known capacity for hydrogen storage (patent No. 2222749, IPC F 17 C 5/04), representing a sealed casing with an inner vessel for storing liquefied hydrogen, the system gattapone made so that you will reduce the loss of hydrogen, to reduce the time of reservoir filling. This reservoir is used for hydrogen car (Schwartz A. the Car of the future. J. Bulletin, No. 10 (347), p.1-5, 12.05.2004,), it is made of durable composite relatively light materials. Last modification has a volume of 90 liters, weight 40 kg, a hydrogen pressure of 400 ATM. Estimates show that in this case the containers can be stored 3.2 kg of hydrogen, therefore, the mass content of hydrogen is a 3.2/40×100%=8%. The disadvantages of capacity is the explosiveness and low hydrogen content per unit volume, up to 400 liters of hydrogen per 1 liter, loss of gas from the container.

It is known that it is possible to store hydrogen in hollow microspheres made of glass with a diameter of 5-200 μm with a wall thickness of 0.5-5 μm (S. p. Malyshenko, Nazarova O. Accumulation of hydrogen. In the collection of articles: "Atomic-hydrogen energy and technology", VIP, page 155-205. 1988). At a temperature of 200-400°under the pressure of the hydrogen actively diffundere through the walls, filling the microspheres and after cooling remains in them under pressure. So when the hydrogen pressure of 500 atmospheres and heating of the microspheres up to these temperatures were obtained bulk hydrogen content in the microspheres 5.5 to 6.0%. At lower pressures the mass of the hydrogen content in the microspheres will be reduced. When heated to 200°receive about 55% stored in Mick is Asherah hydrogen and about 75% when heated up to 250° C. When storing hydrogen in a glass microspheres loss by diffusion through the walls comprise about 0.5% per day. In the case of the coating of the microspheres metal films diffusive loss of hydrogen at room temperature is reduced by 10-100 times. A significant drawback is that the charging of the battery with the microspheres is carried out at relatively low hydrogen pressures, since the tensile strength of glass under tension has a low value and is within up to 20 kg/mm2. It does not allow for bulk hydrogen content in the microspheres substantially in excess of 6 wt.%.

Known capacity for hydrogen storage, consisting of a sealed enclosure, process pipes, the internal heat transfer surfaces and filler-hydrogen battery, a powder of intermetallic (RF patent No. 2037737, IPC F 17 5/04 - prototype). The disadvantages of the invention is that the absorption and release of hydrogen occurs with significant thermal effects, in addition, the mass content of hydrogen is the ratio of the weight of the hydrogen contained in the vessel, the weight capacity of 4.5% is very low.

The technical result, which aims invention is to provide a container for safe storage of hydrogen, which increases the mass containing the Oia hydrogen above 6%.

To do this, the offered capacity for hydrogen storage, consisting of a sealed enclosure, process pipes, heater and filler-hydrogen battery, accommodated in the housing, the filler-hydrogen battery is a hollow microspheres fastened together into a single, rigid structure formed of layers of microspheres of different diameters, the diameter of the microspheres decreases from the Central layer to the peripheral.

In addition, on the outer surface of the rigid structure can be performed floor.

The coating is made of metal, effectively absorbing hydrogen, such as palladium, or Nickel, or an alloy of lanthanum and Nickel.

As the material of the microspheres used steel, or titanium, or lanthanum, or Nickel, or zirconium, or alloys based on these metals, or graphite, or a composition based on graphite.

Metal microspheres can be fixed between a diffusion welding.

In this capacity hydrogen is filled in the space inside the microspheres, and all the space between them. In addition, changes in the diameter of the microspheres from the center of the body to the periphery will allow you to create a tightly Packed structure that more effectively will allow you to use the space enclosed inside the tank. At saturation the entire structure of the s hydrogen pressure can be increased to several thousand atmospheres, because it allows you to make as running microspheres of high-strength material, so that the walls of the microspheres in such a stiffening structure will be unloaded, because the pressure of hydrogen in the neighboring microspheres will be almost identical, and microspheres with a small diameter on the periphery can withstand large pressure hydrogen. As the material of the microspheres should be used high-strength materials with low diffusion coefficients of hydrogen at temperatures up to 100-150°to leakage of hydrogen storage was minimal. These materials include primarily steel, or titanium, or zirconium, or alloys based on these metals, or graphite, or composite materials. To increase the guarantee retention of hydrogen in voids between the spheres on the outer surface of the rigid structure consisting of microspheres, coated.

Figure 1 gives a General view of capacity for hydrogen storage, where 1 - body, 2 - heater, 3 - microspheres, 4 - technological socket.

Figure 2 shows the cross-section capacity for hydrogen storage, the option with the coating on the outer surface of the rigid structure of microspheres, where 5 is the rigid structure of the microspheres, consisting of three zones 6, 7, 8 with microspheres of different diameters, 9 - sealing coating.

In table 1-4 summarizes the estimated data is on the strength parameters and mass content of hydrogen storage-hydrogen accumulators, made of microspheres of different sizes. In the table - σϕ - tangential stress on the outer shell of the microsphere, kg/mm2that σRradial tension on the shell of the microspheres, kg/mm2.

Microspheres with a diameter of 200 mm, a shell thickness of 1 μm.

The weight of the shell per volume of the battery - 124,3 g/l, the volume of the shell in a liter of battery - 0,0155375 l/l, the amount of hydrogen in the chip - 0,5077875 l/l, the amount of hydrogen in the chips and between the microspheres is 0,9844625 l/L. Microspheres made of steel and titanium. The specific weight of steel is 8 kg/l Specific weight of the titanium - 4.5 kg/L.

Table 1
Pressure, MPaThe content of hydrogen in the battery when filling microspheres, wt.% steel/titanium (weight GN2/l battery)The content of hydrogen in the battery when filling the microspheres and the space between them, wt.% steel/titanium (weight GN2/l battery)The content of hydrogen in the battery when filling microspheres, l/lThe content of hydrogen in the battery when filling the microspheres and the space between them, l/lσϕ-σRkg/mm (option for filling hydrogen only microspheres)
12345
100the 3.5/6.1(4,54)6.6/11,2 (8,79)50,898,450,25
1505,2/ 8,9 (6,8)9,6/15,1 (13,2)76,2a 147.775,375
2006,8/11,5 (9,1)12,4/20,1 (17,6)101,6196,8100,5
3009,8/16,3(13,6)17,5/27,4 (26,4)shall be 152.3295,3150,75
40012,7/20,5 (18,1)22,1/33,5 (35,2)203,1393,8201,0
50015,3/24,2 (22,4)26,1/8,5 (43,9)251,2492,2251,25
60017,7/27,7 (26,8)29,8/43,0 (52,7)300,5590,6301,5
70020,3/31,2 (31,7)33,1/46,8 (61,5)355,5689,1351,75
80022,6/34,1 (36,3)36,1/50,1 (70,3)406,2787,5402,0
90024,7/36,8 (40,8)38,9/53,1 (79,1)457,0886,0452,25
100026,7/39,3 (45,3)41,4/55,7 (87,9)507,8984,4502,5
200042,2/is 56.4 (90,6)58,6/71,5 (175,8)1015.61968,81005,0
1000078,5/86,6 (453,4)87,6/92,6 (878,9)5077,99844,05025,0
2000087,9/92,8 (906,8)93,4/96,2 (1757,9)10155,819688,010050,0

Microspheres with a diameter of 100 mm, a shell thickness of 1 μm.

The weight of the shell per volume of the battery - 0,246208 g/l, the volume of the shell in a liter of battery - 0,030776 l/l, the amount of hydrogen microspheres - 0,492557 l/l, the amount of hydrogen in the microspheres and microspheres - 0,969232 l/L. Microspheres made of steel. The specific weight of steel is 8 kg/L.

Table 2
Pressure, MPaThe content of hydrogen in the battery when filling microspheres, wt.% (weightGH2/l battery)The content of hydrogen in the battery when filling the microspheres and the space between them, wt.% (weight GN2/l battery)The content of hydrogen in the battery when filling microspheres, l/lThe content of hydrogen in the battery when filling the microspheres and the space between them, l/lσϕ-σRkg/mm2(for options : size is in hydrogen only microspheres)
12345
1001,76 (4,4)3,4 (8,65)to 49.396,929,75
1502,6 (6,6)5,0 (13,0)73,9145,437,875
2003,5 (8,8)6,6 (17,3)98,5193,8a 50.5
3005,1 (13,2)9,6 (26,0)147,8290,876,40
4006,7 (17,6)12,3 (34,6)197,0387,7101,0
5008,2 (22,0)15,0 (43,3)246,3484,6126.25 area
6009,7 (26,4)17,4 (51,9)295,5581,5151,5
70011,1 (30,8)19,3 (58,7)345,5657,6176,75
80012,5 (35,2)21,9 (69,2)394,0775,4202,0
90013,9 (39,6)24,0 (77,9)443,30872,3227,25
100015,2 (44,0)26,0 (86,5)492,6252,5
200026,3 (88,0)58,6 (173,1)985,11938,5505,0
1000064,1 (453,4)77,9 (865,4)4925,69692,32525,0
2000078,1 (879,6)87,5 (1730,8)9851,119384,65050,0

Microspheres with a diameter of 10 mm, a shell thickness of 1 μm.

The weight of the shell per volume of the battery - 1,13488 g/l, the volume of the shell in a liter of battery - 0,14186 l/l, the amount of hydrogen microspheres - 0,38151 l/l, the amount of hydrogen in the microspheres and microspheres - 0,858135 l/L. Microspheres made of steel and titanium. The specific weight of steel is 8 kg/l Specific weight of the titanium - 4.5 kg/L.

Table 3
Pressure, MPaThe content of hydrogen in the battery when filling microspheres, wt.%, steel/titanium (weight GN2/l battery)The content of hydrogen in the battery when filling the microspheres and the space between them, the wt.%, steel/titanium (weight GN2/l battery)The content of hydrogen in the battery when filling microspheres, l/lThe content of hydrogen in the battery when filling the microspheres and the space between them, l/l σϕ-σRkg/mm2. (for option of filling hydrogen only microspheres)
12345
1000,3/0,53 (3,4)0,67/1,2 (7,66)38,1585,82,5
1500,45/0,79 (5,1)1,0/1,8 (11,5)57,2128,74,125
2000,6/1,0 (6,8)1,3/2,3 (15,3)76,3171,65,5
3000,9/1,6 (10,2)2,0/3,5 (23,0)114,5257,48,25
4001,2/2,1 (13,6)2,6/4,6 (30,6)152,6343,211,0
5001,5/2,6 (17,0)3,3/5,7 (38,3)190,8429,1of 13.75
6001,8/3,1 (20,4)3,9/6,7 (46,0)228,9514,916,5
7004,5/3,6 (23,8)4,5/7,7 (53,6)267,0600,719,25
8002,3/4,1 (27,2)5,1/8,8 (61,3)305,2686,522,0
9002,6 /4,6 (30,6)5,7/9,8 (69,0)the 33.4 772,327,0
10002,9/5,1 (34,0)6,3/10,7 (76,6)381,5858,127,5
20005,7/9,6 (68,1)11,9/19,4 (153,2)763,01716,355,0
1000023,1/34,8 (340)40,3/54,5 (766,2)3815,18581,35275,0
2000037,/551,6 (681)57,5/70,6 (1532,4)7630,217162,7550,0

Microspheres with a diameter of 3 mm, a shell thickness of 1 μm.

The weight of the shell per volume of the battery - 3992 g/l, the volume of the shell in a liter of battery - 0,499 l/l, the amount of hydrogen microspheres - 0,019 l/l, the amount of hydrogen in the microspheres and microspheres - 0,501 l/L. Microspheres made of steel. The specific weight of steel is 8 kg/L.

Table 4
Pressure, MPaThe content of hydrogen in the battery when filling microspheres, wt.%, steel/titanium (weight GN2/l battery)The content of hydrogen in the battery when filling the microspheres and the space between them, the wt.%, steel/titanium (weight GN2/l battery)The content of hydrogen in the battery when filling microspheres, l/lthe contents of hydrogen in the battery when filling the microspheres and the space between them, l/lσϕ-σRkg/mm2(for the option of filling hydrogen only microspheres)
12345
10000for 0.4/0.75 in (17,0)10,0/16,6 (447,0)190,05010,0100,0

As can be seen from table 1, for example, by saturation with hydrogen at a pressure of 1000 MPa rigid structure created from microspheres with a diameter of 200 μm, the resulting hydrogen weight content 41,4 wt.%. The shell of the microspheres inside the rigid structure is unloaded, because on both sides of the membrane affects the same pressure up to 1000 MPa. But the shell of the microspheres on the surface of the rigid structure are under enormous pressure - 502,5 kg/mm2(see table 1).

Such pressure shell will not sustain and will be broken. To provide the necessary strength characteristics of the surface of a rigid structure, the periphery of this structure is made of microspheres with a diameter of 10 μm, the weight content of hydrogen of 6.3 wt.% (table 3). The voltage envelope of these microspheres at a pressure of 1000 MPa 27.5 kg/mm2such pressure can withstand a wide class of steels and other materials (table 3). Thus, the rigid structure of the microspheres with an unloaded shells in the volume of the structure, as in the sun the x shells with a diameter of 200 μm and a diameter of 10 microns pressure equal to 1000 MPa, and microspheres on the surface with a diameter of 10 microns pressure on the shell of 27.5 kg/mm2. The presence of a rigid structure of small microspheres reduces the mass content of hydrogen (200 μm is 41.4 wt.%, 10 μm to 6.3 wt.%). So for rigid structure consisting of 80% of the microspheres with a diameter of 200 μm and 20% of the microspheres with a diameter of 10 μm, saturated with hydrogen at 1000 MPa, the weight content of hydrogen is 34,38 wt.%.

When saturation of the microspheres with a diameter of 200 μm at a pressure of 10000 MPa (weight content in the rigid structure of 87.6 wt.%) the periphery should be done of small spheres, for example with a diameter of 3 μm. In this case, the pressure on the membrane in the surface layer is 100 kg/mm (table 4), which will produce such a rigid structure of high-strength materials.

For rigid structures composed of 80% of the microspheres with a diameter of 200 μm and 20% of the microspheres with a diameter of 3 μm, saturated with hydrogen at 10,000 MPa the weight content of hydrogen is 72,08%by weight.

Creating a rigid structure of microspheres containing layers of microspheres inside the rigid structure are microspheres with a large diameter, and moving to the periphery with decreasing diameter, you can create a battery with a high gravimetric hydrogen content and high strength characteristics.

In the performance of microspheres of titanium weight content of bodoro is but significantly increases in comparison with its weight content in the steel as the proportion of titanium is less than 1.8 times, (table 1, 2-4). So for rigid structure created from microspheres with a diameter of 200 μm, saturated at 300 MPa hydrogen weight content of hydrogen in the case of steel 17.5 wt.%, and in the case of titanium 27,4% wt. (table 1).

This solution allows you to create batteries with a mass content of hydrogen exceeding 6 wt.%.

We will show the possibility of implementing the invention.

Of hollow microspheres of 3 different diameters, for example, D1D2D3form three layers 6, 7, 8 filler-hydrogen battery, after which the microspheres are rigidly fastened to each other. Metal microspheres can be bonded, for example, by diffusion welding. Microspheres of composites, ceramics and other materials can be secured between them, for example by sintering.

This produces a single rigid structure 5 with decreasing diameter of the microspheres from the center to the periphery. To improve retention of hydrogen can be sealing the outer surface of this structure, for example, apply a coating 9 of the metal, effectively absorbing hydrogen, such as palladium, or Nickel, or an alloy of lanthanum and Nickel of a thickness of 5-8 μm. Then the filler-hydrogen battery is saturated with hydrogen. This rigid structure of the microspheres was placed in an autoclave capable of withstanding high pressure and has a heating system. The autoclave HAC is wmiroot booster pump to remove air, then it serves hydrogen to a slight excess pressure of the order of 1-10 MPa. Next, the autoclave is heated to 300-500°With (depending on the material of the microspheres), then, depending on what the weight content of hydrogen in the rigid structure we want to receive in accordance with tables 1-4 (or, in General, for different materials create the same table), slowly generate a corresponding excess pressure of hydrogen in the autoclave. Rigid structure to withstand these settings to equalize the pressure of hydrogen in the autoclave and in the cavities of the rigid structure due to the diffusion of hydrogen. After that, when the same pressure, the system is cooled to room temperature. Hydrogen at room temperature of the hard structures are not diffused. Reset the hydrogen pressure in the autoclave and remove rigid structure. After this, the hydrogen-filled accumulator is loaded into the housing 1. When turning on the heater 2, the hydrogen stored in the battery will start to stand out and be submitted to the consumer through the process tube 4. The saturation with hydrogen can be produced as the rigid structure and the capacity installed in her rigid structure.

Example 1. Microspheres made of steel with a diameter of 200 μm was filled in a cylinder of quartz with a diameter of 11 mm and a height of 8.0 cm, is crosfire were welded by diffusion welding. Then the cylinder is made of microspheres were placed in a cylinder made of quartz with a diameter of 13 mm, the bottom of which was previously filled microspheres with a diameter of 100 μm, the layer height of 1 mm Microspheres with a diameter of 100 μm was filled in between the wall of the quartz cylinder and the cylinder of microspheres with a diameter of 200 μm. The same layer of microspheres with a diameter of 100 μm was filled to the top of the cylinder of microspheres with a diameter of 200 μm. Spent diffusion welding. Got a hard microstructure of the microspheres. The weight of the cylinder of the hard structure is equal to the Estimated 1,541 weight 1.48 g (table 1, 2). The hydrogen saturation of this structure was performed in an autoclave according to the method described above. The process was carried out at a hydrogen pressure of 150 MPa, the temperature of the process 450°C. To ensure saturation of the rigid structure of the hydrogen process lasted 2 hours. The weight of the rigid structure after hydrogen saturation equal 1,677 g, i.e. the content of hydrogen in it 0,136 g, which is 8.1 wt.%. The estimated value - 8,68 wt.%

Example 2. Established rigid structure of microspheres with a diameter of 100 microns with a shell thickness of 1 μm. The structure created by diffusion welding microspheres with each other. The outer layer structure consisted of microspheres with a diameter of 5 μm. In the ampoule at a temperature of 300°and a hydrogen pressure of 1000 MPa for 2.5 hours was its saturation. After that, the rate the temperature was decreased to 20° With the same excess pressure of hydrogen. The weight of the structure to hydrogen saturation was equal to 1.24 g, after saturation 1.42 g, i.e. the mass content of hydrogen amounted to 12.7 wt.%.

Example 3. On the surface similar rigid structure according to example 2 was deposited Nickel coating, sealing the entire structure. The coating thickness of 5-8 μm. We then conducted a saturation patterns hydrogen as in example 1. Mass content of hydrogen amounted to 18.6%.

Thus, the proposed capacity for hydrogen storage will allow a high degree of security to store hydrogen, the contents in the tank will allow you to use this capacity for vehicles, as well as in other industries.

1. Capacity for hydrogen storage, consisting of a sealed enclosure, process pipes, heater and filler-hydrogen battery, accommodated in the housing, characterized in that the filler-hydrogen battery is a hollow microspheres fastened together into a single rigid structure formed of layers of microspheres of different diameters, the diameter of the microspheres decreases from the Central layer to the peripheral.

2. The container according to claim 1, characterized in that on the outer surface of the rigid structure made floor.

3. The container according to claim 2, characterized in that the coating is being made of metal, effectively absorbing hydrogen, such as palladium, or Nickel, or an alloy of lanthanum and Nickel.

4. The container according to claim 1, characterized in that the material of the microspheres used steel, or titanium, or lanthanum, or Nickel, or zirconium, or alloys based on these metals, or graphite, or a composition based on graphite.

5. The container according to claim 1, characterized in that the microspheres made of metal is fixed between a diffusion welding.



 

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FIELD: hydrogen power engineering.

SUBSTANCE: tank comprises two-layer structure made of a sorbent provided with a coating. The sorbent is made of a metal with positive activation energy and low hydrogen absorption and liberates hydrogen completely at low temperatures. The coating is made of metals with negative activation energy and liberates hydrogen only at high temperatures.

EFFECT: reduced losses and enhanced safety.

2 cl, 2 dwg

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