CA1077457A - Alloy for hydrogen storage - Google Patents
Alloy for hydrogen storageInfo
- Publication number
- CA1077457A CA1077457A CA252,471A CA252471A CA1077457A CA 1077457 A CA1077457 A CA 1077457A CA 252471 A CA252471 A CA 252471A CA 1077457 A CA1077457 A CA 1077457A
- Authority
- CA
- Canada
- Prior art keywords
- hydrogen
- alloy
- percent
- weight
- alloys
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
- Expired
Links
Classifications
-
- C—CHEMISTRY; METALLURGY
- C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
- C22C—ALLOYS
- C22C14/00—Alloys based on titanium
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B3/00—Hydrogen; Gaseous mixtures containing hydrogen; Separation of hydrogen from mixtures containing it; Purification of hydrogen; Reversible storage of hydrogen
- C01B3/0005—Reversible storage of hydrogen, e.g. by hydrogen getters or electrodes
- C01B3/001—Reversible storage of hydrogen, e.g. by hydrogen getters or electrodes characterised by the uptaking media; Treatment thereof
- C01B3/0018—Inorganic elements or compounds, e.g. oxides, nitrides, borohydrides or zeolites; Solutions thereof
- C01B3/0031—Intermetallic compounds; Metal alloys
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B6/00—Hydrides of metals including fully or partially hydrided metals, alloys or intermetallic compounds ; Compounds containing at least one metal-hydrogen bond, e.g. (GeH3)2S, SiH GeH; Monoborane or diborane; Addition complexes thereof
- C01B6/24—Hydrides containing at least two metals; Addition complexes thereof
-
- C—CHEMISTRY; METALLURGY
- C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
- C22C—ALLOYS
- C22C22/00—Alloys based on manganese
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/30—Hydrogen technology
- Y02E60/32—Hydrogen storage
Landscapes
- Chemical & Material Sciences (AREA)
- Organic Chemistry (AREA)
- Engineering & Computer Science (AREA)
- Inorganic Chemistry (AREA)
- Materials Engineering (AREA)
- Mechanical Engineering (AREA)
- Metallurgy (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Combustion & Propulsion (AREA)
- Hydrogen, Water And Hydrids (AREA)
Abstract
ABSTRACT OF THE DISCLOSURE
There is described an alloy metal hydride for storing and releasing hydrogen at predetermined temperatures and pressures intended for storing and transporting said hydrogen and also for use as a hydrogen supply source of a fuel cell and fuel electrode.
The alloy of this invention consisting of 30 to 80 percent by weight Ti and 20 to 70 percent by weight Mn having a high dissoc-iation pressure, easy hydrogen activation, low heat of formation of hydrides and a very fast rate of absorption and desorption, also the alloy is of light weight and of low cost therefore being of great industrial use.
There is described an alloy metal hydride for storing and releasing hydrogen at predetermined temperatures and pressures intended for storing and transporting said hydrogen and also for use as a hydrogen supply source of a fuel cell and fuel electrode.
The alloy of this invention consisting of 30 to 80 percent by weight Ti and 20 to 70 percent by weight Mn having a high dissoc-iation pressure, easy hydrogen activation, low heat of formation of hydrides and a very fast rate of absorption and desorption, also the alloy is of light weight and of low cost therefore being of great industrial use.
Description
~10774S'7 This invention relates to an alloy for storing and ~eleasing hydrogen at predetermined temperatures and pressures respectively. It is already known that metals or alloys con-taining transition metal groups are able to store a large amount of hydrogen by way of forming metal hydrides.
However, these hydrides are, in most cases, thermo-dynamically very stable so that they release hydrogen stored in the crystal lattice only at such high temperatures as 400C
and above.
The following are the requirements which the hydrogen storing material must satisfy.
(1) The hydrogen absorbing capacity must large both for weight and volume.
However, these hydrides are, in most cases, thermo-dynamically very stable so that they release hydrogen stored in the crystal lattice only at such high temperatures as 400C
and above.
The following are the requirements which the hydrogen storing material must satisfy.
(1) The hydrogen absorbing capacity must large both for weight and volume.
(2) It must be stable chemically as well as thermo-synamically at an ambient temperature and have a suitable dissociation pressure of several times atmospheric pressure.
(3) A sufficient absorption and desorption rate of hydrogen under the conditions required for practical use.
(4) Stable characteristics or performance even after ~-having been subjected to repeated absorption and desorptioncycles.
(5) It must be unsusceptible to the influence of impurities entrapped in the hydrogen gas and further can be easily regenerated when the materials are degraded by said impurities.
(6) The density of the hydrides should be as low as possible.
(7) It must be inexpensive.
(8) The heat of formation of the hydride must be as low as possible.
Recently, hydrides of Lantanide alloys have been developed, but they were found to be unsuitable for industrial ~ . .
., . ~ . ~ . ~ . . .
- ., .:, . .. - : , , : . .
~077457 use because, their production costs are extremely high, they are J vc /,~
too heavy and are ~eo sen~itive to impurities in the hydrogen gas to be stored. Also hydrides of conventional Ti-Fe alloys and Ti-Ni alloys do not satisfy the above conditions itemized in (1), (2), (3), (S), (6) and (8) and particularly they have a serious drawback of having comparatively less activation of hydrogen.
This invention aims to provide novel metal hydrides for storage and transportation of hydrogen and also for a hydrogen supply source for a fueI cell and hydrogen electrode.
The inventors of this invention found that some alloy phases of Ti-Mn system, for example, TiMn are able to readily absorb large amounts of hydrogen at room temperature and at a relatively low pressure of only about several times atmospheric pressure, and the hydrides of these alloys phases release the absorbed hydrogen at a suitably fast rate when the hydrides are placed under certain combined conditions of temperature and pressure. In other words, Ti-Mn alloys in solid state containing 30 to 80 weight percent of Ti and 20 to 70 weight percent of Mn, preferably, containing about 45 weight percent of Ti and 55 per-cent of Mn absorb hydrogen equals to 2.5 percent in weight of the alloy used, when they are placed directly in contact with hydrogen gas at several times atmospheric pressure at an ambient temperature, and they also release a large amount of hydrogen thus absorbed reversively and readily at room temperature and at another predetermined pressure.
The alloys of this invention are not required to be crushed before the hydriding step but can be used as in lamp form, while conventional alloys such as Ti-Ni and Ti-Fe systems must be previously crushed prior to their initial hydriding step.
The alloys of this invention in lump form are able to readily absorb hydrogen without being subjected to any pre-treatment `: 10774S7 and thereafter they disintegrate into fine powders without being applied with any external force.
- The alloys of this invention can be obtained by conventional melting technique such as an argon-arc melting .. , process. -~
~r~ Alloy lumps thus obtained are uniform in ~uality and ':' J~ are fairly brittle and thus can be crushed by any mechanical -~ means.
~:.
When a hydrogen gas is introduced and contacted with ~10 these alloy lumps it is absorbed by the alloy lumps at a fairly :
fast rate and as a result, hydrides, such as TiMnH2 5 are formed and eventually take the powder state having a grain size of less than 10 micron.
Thus the present invention provides a method of storing hydrogen comprising contacting gaseous hydrogen with a solid titanium-manganese alloy, said alloy consisting essentially of 30 to 80 percent by weight of titanium and 20 to 70 percent by weight manganese.
.
At room temperature, neither oxide layer nor nitride ; 20 layer is formed on this Ti-Mn alloy, moreover, the inventive alloys readily absorb hydrogen gas and desorb it without being influenced by any impurities entrapped in the hydrogen gas, these alloys are '~ al60 able to purify hydrogen.
`;~ No special container construction is required for absorb-.~
ing hydrogen by using the alloy of this invention, an airtight -~ container for containing alloy hydride powder is satisfactory for ~;. ., utilizing this invention, also no special consideration of temper-~'; ature is needed.
. :.;, , The following is a working example for forming metal hydrides according to this invention.
As starting materials, for example rod-shaped metallic -titanium having a diameter of 8 mm and a length of 10 mm, of 99.9 ; ' .. ~ . . . .
'i~`
;" 1077457 ., ~' percent grade purity, and metallic man~anese plate having 10 mm square and thickness of 1.5 mm of 99.2 percent grade purity were directly melted together in an argon arc furnace into a Ti-Mn alloy.
~- The button shaped Ti-Mn alloys thus prepared were . :
~., broken ;'~i~
~ 10 :'~ ' ~' ' ,'' .
~"., ~ .
, .
,.
, " ,~ ., .
.,:~ . . .
,.. , i , ~ 20 ~:'. .
,;
,,:,...................................................................... .
~,....
'~7'., ~,,~., .;' \ ....
~^
..; 30 .~.
; .
:.
,, .'. ~1 , ~ -3a-.
- : :
~1)774~
; .
~` :
down into several pieces and placed in a hydriding reactor vessel made of stainless steel, and the vessel was evacuated for about , .
' 1 minute by a rotary pump.
~,~ Hydrogen gas of 99.9 percent purity was introduced into the vessel until the internal pressure of the vessel reached about twenty atmospheric pressures, then the alloy began to absorb the ,~ .
hydrogen, the volume of thus absorbed hydrogen amounted to 2 to 5 liters within several minutes, the weight of the used alloy was 10 gr.
As a result, in a powder state hydride of Ti-Mn was .. . .
' formed, while generating heat of formation of hydride which -heated the vessel to some extent.
p~5~r~
'!' ~lg~a~ of the absorbed hydrogen was carried out in j A~ entireIy the same manner as in a conventional hydrogen bomb, and was available for release by merely opening a valve.
r~
Adjustment of the 4~ ~-~tn rate of the hydrogen gas is performed either mechanically by any reducing valve or by controll-` ing the pressure or temperature of the ambient hydrogen .
,,~ Absorption of hydrogen gas is performed again and ~ 20 repeatedly in an entirely similar manner.
: ......................................................... .
' There exists a certain relationship between the compos- ~ -'b.',' ition of the Ti-Mn hydrides and the number of absorbed hydrogen ~ atoms (HX) per one mole of TiMn alloy at room temperature.
~, .
,` Absorbtion and desorption of the hydrogen at room ~,".
~' temperature becomes considerably less thus a superior property of this alloy is lost when the content of Mn in the alloy lies :; . ~ . .. .
in the ranges of less than 20 percent and more than 70 percent .:
~ by weight.
, ~
~ Also the amount of absorbed hydrogen within the range , of 20 to 70 percent by weight Ti increases as the content of Mn increases, on the other hand, amount of hydrogen desorbed shows maximum at about 37 weight percent Ti then begins to decrease as :-.
. . .
_ 4 _ :
, , - ~ , : -: . .
:; - 10'77457 the content of Ti increase above said 37 percent Ti.
: In view of this tendency of desorption, the preferable range of Ti content within which the alloys display a 50 percent . hydrogen desorption ratio of desorbed hydrogen to absorbed hydrogen wàs selected 35 to 50 weight percent Ti.
. ; . .
Also, it was found that the less the Mn content in the alloy is, the lower the equilibrium dissociation pressure of the hydrogen becomes.
~ Distinguishable features of the Ti-Mn hydrides of this invention as described above can be summarized as follows:
; (1) Has an equilibrium dissociation pressure of hydrogen of less than several atmospheric pressures.
(2) Activation of hydrogen is very easy.
(3) Has low heat of formation of hydrides.
.
(4) Rates of absorption and desorption of hydrogen are very fast at room temperature.
I (5) Repeated cycling of absorption and desorption do ',' not change the performance of the alloy.
~ (6) Is very much less susceptible to impurities in j 20 the hydrogen gas.
(7) Comparatively low in cost.
(8) Stable at service condition and guarantee safety.
Recently, hydrides of Lantanide alloys have been developed, but they were found to be unsuitable for industrial ~ . .
., . ~ . ~ . ~ . . .
- ., .:, . .. - : , , : . .
~077457 use because, their production costs are extremely high, they are J vc /,~
too heavy and are ~eo sen~itive to impurities in the hydrogen gas to be stored. Also hydrides of conventional Ti-Fe alloys and Ti-Ni alloys do not satisfy the above conditions itemized in (1), (2), (3), (S), (6) and (8) and particularly they have a serious drawback of having comparatively less activation of hydrogen.
This invention aims to provide novel metal hydrides for storage and transportation of hydrogen and also for a hydrogen supply source for a fueI cell and hydrogen electrode.
The inventors of this invention found that some alloy phases of Ti-Mn system, for example, TiMn are able to readily absorb large amounts of hydrogen at room temperature and at a relatively low pressure of only about several times atmospheric pressure, and the hydrides of these alloys phases release the absorbed hydrogen at a suitably fast rate when the hydrides are placed under certain combined conditions of temperature and pressure. In other words, Ti-Mn alloys in solid state containing 30 to 80 weight percent of Ti and 20 to 70 weight percent of Mn, preferably, containing about 45 weight percent of Ti and 55 per-cent of Mn absorb hydrogen equals to 2.5 percent in weight of the alloy used, when they are placed directly in contact with hydrogen gas at several times atmospheric pressure at an ambient temperature, and they also release a large amount of hydrogen thus absorbed reversively and readily at room temperature and at another predetermined pressure.
The alloys of this invention are not required to be crushed before the hydriding step but can be used as in lamp form, while conventional alloys such as Ti-Ni and Ti-Fe systems must be previously crushed prior to their initial hydriding step.
The alloys of this invention in lump form are able to readily absorb hydrogen without being subjected to any pre-treatment `: 10774S7 and thereafter they disintegrate into fine powders without being applied with any external force.
- The alloys of this invention can be obtained by conventional melting technique such as an argon-arc melting .. , process. -~
~r~ Alloy lumps thus obtained are uniform in ~uality and ':' J~ are fairly brittle and thus can be crushed by any mechanical -~ means.
~:.
When a hydrogen gas is introduced and contacted with ~10 these alloy lumps it is absorbed by the alloy lumps at a fairly :
fast rate and as a result, hydrides, such as TiMnH2 5 are formed and eventually take the powder state having a grain size of less than 10 micron.
Thus the present invention provides a method of storing hydrogen comprising contacting gaseous hydrogen with a solid titanium-manganese alloy, said alloy consisting essentially of 30 to 80 percent by weight of titanium and 20 to 70 percent by weight manganese.
.
At room temperature, neither oxide layer nor nitride ; 20 layer is formed on this Ti-Mn alloy, moreover, the inventive alloys readily absorb hydrogen gas and desorb it without being influenced by any impurities entrapped in the hydrogen gas, these alloys are '~ al60 able to purify hydrogen.
`;~ No special container construction is required for absorb-.~
ing hydrogen by using the alloy of this invention, an airtight -~ container for containing alloy hydride powder is satisfactory for ~;. ., utilizing this invention, also no special consideration of temper-~'; ature is needed.
. :.;, , The following is a working example for forming metal hydrides according to this invention.
As starting materials, for example rod-shaped metallic -titanium having a diameter of 8 mm and a length of 10 mm, of 99.9 ; ' .. ~ . . . .
'i~`
;" 1077457 ., ~' percent grade purity, and metallic man~anese plate having 10 mm square and thickness of 1.5 mm of 99.2 percent grade purity were directly melted together in an argon arc furnace into a Ti-Mn alloy.
~- The button shaped Ti-Mn alloys thus prepared were . :
~., broken ;'~i~
~ 10 :'~ ' ~' ' ,'' .
~"., ~ .
, .
,.
, " ,~ ., .
.,:~ . . .
,.. , i , ~ 20 ~:'. .
,;
,,:,...................................................................... .
~,....
'~7'., ~,,~., .;' \ ....
~^
..; 30 .~.
; .
:.
,, .'. ~1 , ~ -3a-.
- : :
~1)774~
; .
~` :
down into several pieces and placed in a hydriding reactor vessel made of stainless steel, and the vessel was evacuated for about , .
' 1 minute by a rotary pump.
~,~ Hydrogen gas of 99.9 percent purity was introduced into the vessel until the internal pressure of the vessel reached about twenty atmospheric pressures, then the alloy began to absorb the ,~ .
hydrogen, the volume of thus absorbed hydrogen amounted to 2 to 5 liters within several minutes, the weight of the used alloy was 10 gr.
As a result, in a powder state hydride of Ti-Mn was .. . .
' formed, while generating heat of formation of hydride which -heated the vessel to some extent.
p~5~r~
'!' ~lg~a~ of the absorbed hydrogen was carried out in j A~ entireIy the same manner as in a conventional hydrogen bomb, and was available for release by merely opening a valve.
r~
Adjustment of the 4~ ~-~tn rate of the hydrogen gas is performed either mechanically by any reducing valve or by controll-` ing the pressure or temperature of the ambient hydrogen .
,,~ Absorption of hydrogen gas is performed again and ~ 20 repeatedly in an entirely similar manner.
: ......................................................... .
' There exists a certain relationship between the compos- ~ -'b.',' ition of the Ti-Mn hydrides and the number of absorbed hydrogen ~ atoms (HX) per one mole of TiMn alloy at room temperature.
~, .
,` Absorbtion and desorption of the hydrogen at room ~,".
~' temperature becomes considerably less thus a superior property of this alloy is lost when the content of Mn in the alloy lies :; . ~ . .. .
in the ranges of less than 20 percent and more than 70 percent .:
~ by weight.
, ~
~ Also the amount of absorbed hydrogen within the range , of 20 to 70 percent by weight Ti increases as the content of Mn increases, on the other hand, amount of hydrogen desorbed shows maximum at about 37 weight percent Ti then begins to decrease as :-.
. . .
_ 4 _ :
, , - ~ , : -: . .
:; - 10'77457 the content of Ti increase above said 37 percent Ti.
: In view of this tendency of desorption, the preferable range of Ti content within which the alloys display a 50 percent . hydrogen desorption ratio of desorbed hydrogen to absorbed hydrogen wàs selected 35 to 50 weight percent Ti.
. ; . .
Also, it was found that the less the Mn content in the alloy is, the lower the equilibrium dissociation pressure of the hydrogen becomes.
~ Distinguishable features of the Ti-Mn hydrides of this invention as described above can be summarized as follows:
; (1) Has an equilibrium dissociation pressure of hydrogen of less than several atmospheric pressures.
(2) Activation of hydrogen is very easy.
(3) Has low heat of formation of hydrides.
.
(4) Rates of absorption and desorption of hydrogen are very fast at room temperature.
I (5) Repeated cycling of absorption and desorption do ',' not change the performance of the alloy.
~ (6) Is very much less susceptible to impurities in j 20 the hydrogen gas.
(7) Comparatively low in cost.
(8) Stable at service condition and guarantee safety.
(9) Has considerably high amount of hydrogen absorption equal to about 1.5 times that of Fe-Ti system.
Furthermore, Ti-Mn alloys of this invention are not limited to only binary alloys of Ti and Mn but other Ti or Mn base alloys within the above-mentioned Ti and Mn content range and further containing third or fourth alloying elements such as Cu, Ni and Co and so on also display similar superior properties for storaging hydrogen according to this invention.
Furthermore, Ti-Mn alloys of this invention are not limited to only binary alloys of Ti and Mn but other Ti or Mn base alloys within the above-mentioned Ti and Mn content range and further containing third or fourth alloying elements such as Cu, Ni and Co and so on also display similar superior properties for storaging hydrogen according to this invention.
Claims (4)
PROPERTY OR PRIVILEGE IS CLAIMED ARE DEFINED AS FOLLOWS:
1. A method of storing hydrogen comprising contacting gaseous hydrogen with a solid titanium-manganese alloy, said alloy consisting essentially of 30 to 80 percent by weight of titanium and 20 to 70 percent by weight manganese.
2. A method according to Claim 1, wherein the alloy consists essentially of 35 to 50 percent by weight of titanium and 50 to 65 percent by weight of manganese.
3. A method according to Claim 1, wherein the alloy consists essentially of about 45 percent by weight of titanium and about 55 percent by weight of manganese.
4. A method according to Claim 1, wherein the alloy consists essentially of about 37 percent by weight of titanium and the balance being manganese.
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP50056949A JPS51132108A (en) | 1975-05-13 | 1975-05-13 | Alloy for hydrogen storage |
Publications (1)
| Publication Number | Publication Date |
|---|---|
| CA1077457A true CA1077457A (en) | 1980-05-13 |
Family
ID=13041791
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| CA252,471A Expired CA1077457A (en) | 1975-05-13 | 1976-05-13 | Alloy for hydrogen storage |
Country Status (3)
| Country | Link |
|---|---|
| JP (1) | JPS51132108A (en) |
| CA (1) | CA1077457A (en) |
| GB (1) | GB1548581A (en) |
Families Citing this family (7)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPS5288518A (en) * | 1976-01-20 | 1977-07-25 | Matsushita Electric Ind Co Ltd | Metallic material for storing hydrogen |
| JPS536214A (en) * | 1976-07-07 | 1978-01-20 | Matsushita Electric Ind Co Ltd | Hydrogen storing metallic material |
| NL8001314A (en) * | 1980-03-05 | 1981-10-01 | Philips Nv | PROCESS FOR PREPARING A HYDROGEN ABSORBING ALLOY. |
| US4431561A (en) * | 1982-04-28 | 1984-02-14 | Energy Conversion Devices, Inc. | Hydrogen storage materials and method of making same |
| US4505764A (en) * | 1983-03-08 | 1985-03-19 | Howmet Turbine Components Corporation | Microstructural refinement of cast titanium |
| US5814241A (en) * | 1994-12-29 | 1998-09-29 | Tovarischetstvo S Organichennoi Otvetstvennostju "Tekhnovakt" | Non-vaporizing getter and method of obtaining the same |
| RU2073737C1 (en) * | 1994-12-29 | 1997-02-20 | Товарищество с ограниченной ответственностью "Техновак +" | Nondusting tape gas absorber and method of manufacture thereof |
Family Cites Families (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPS5425911B2 (en) * | 1975-03-24 | 1979-08-31 |
-
1975
- 1975-05-13 JP JP50056949A patent/JPS51132108A/en active Granted
-
1976
- 1976-05-13 CA CA252,471A patent/CA1077457A/en not_active Expired
- 1976-05-13 GB GB19809/76A patent/GB1548581A/en not_active Expired
Also Published As
| Publication number | Publication date |
|---|---|
| JPS5527610B2 (en) | 1980-07-22 |
| GB1548581A (en) | 1979-07-18 |
| JPS51132108A (en) | 1976-11-17 |
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Legal Events
| Date | Code | Title | Description |
|---|---|---|---|
| MKEX | Expiry |