CN104630598A - Method for quickly selecting hydrogen isotope separating material - Google Patents
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- CN104630598A CN104630598A CN201510093420.3A CN201510093420A CN104630598A CN 104630598 A CN104630598 A CN 104630598A CN 201510093420 A CN201510093420 A CN 201510093420A CN 104630598 A CN104630598 A CN 104630598A
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Abstract
The invention discloses a method for quickly selecting a hydrogen isotope separating material. The method comprises the following steps: (1) selecting a titanium, vanadium and chromium alloy as the hydrogen isotope separating material and determining the content of vanadium in the selected titanium, vanadium and chromium alloy at 40at%, wherein the purities of titanium, vanadium and chromium are greater than 99.9%; (2) adjusting the contents of titanium and chromium under the condition that e/a=4.4-5.6 in the titanium, vanadium and chromium alloy according to the content of vanadium; and (3) obtaining a molecular formula of the titanium, vanadium and chromium alloy according to the contents of titanium, vanadium and chromium, determined in the step (2), and determining the titanium, vanadium and chromium alloy needed to be selected. The method disclosed by the invention provides a very good concept for searching for the Ti-V-Cr alloy with a remarkable anti-hydrogen isotopic effect, so that the blank is effectively filled, thereby providing guarantee for lowering the technical research cost of hydrogen isotope separation and shortening the research and development period. Therefore, the method disclosed by the invention has high practical and promotional values.
Description
Technical field
The present invention relates to a kind of method that fast selecting goes out hydrogen isotope separation material.
Background technology
In many methods of hydrogen isotope separation, the hydrogen isotope effect of hydrogen storage material is utilized to be wherein a kind of up-and-coming method to carry out separation.The key of this method needs a kind of material simultaneously with remarkable hydrogen isotope effect and excellent hydrogen storage performance.Up to now, palladium metal is the most the superior of over-all properties in all material.But palladium is a kind of very expensive metal, therefore, which has limited its large-scale application in the industry.On the other hand, palladium has positive isotopic effect, and situation when this is very low for hydrogen isotope (as deuterium or the tritium) concentration that process is heavy is disadvantageous.Now, we need the material with antihydrogen isotopic effect to process some special situations.
Vanadium is a kind of metal with larger antihydrogen isotopic effect, but its activation difficulty, and reversible hydrogen storage amount is little, and dynamic performance is too poor, and easily poisons.Other some metal or alloy, or be that hydrogen isotope effect is not remarkable; That hydrogen storage performance is poor.In general, the material that really can be actually used in hydrogen isotope separation at present only has palladium.Therefore, no matter be researchist or slip-stick artist, all urgently wish to find one both to have remarkable antihydrogen isotopic effect, there is again the material of excellent hydrogen storage performance simultaneously, to replace expensive palladium, or be applied to the situation that palladium is not too applicable to.In recent years, Ti-V-Cr(titanium-vanadium-chromium) be that the hydrogen storage performance of solid solution hydrogen-storage alloy obtains very systematic research, substantially understand fully about the relation between the every character of alloy and hydrogen storage performance.These achievements in research show, Ti-V-Cr system alloy is a kind of up-and-coming hydrogen storage material, has both had large hydrogen storage amount, has again excellent dynamic performance, and its level ground platform pressure can also adjust in very wide scope.
Thus, if the Ti-V-Cr alloy determined has significant antihydrogen isotopic effect, just in the very possible process at hydrogen isotope (such as the separation of hydrogen isotope), gather around and have broad application prospects.But, in the face of the processing demands of different hydrogen isotopes, how fast do not see, effectively select the relevant report of the Ti-V-Cr alloy simultaneously with antihydrogen isotopic effect and excellent hydrogen storage performance at present both at home and abroad, usually be all through a large amount of intimate experiment of having no main threads to screen, thus not only extend the cycle of technical research, and significantly add the cost of research and development.
Summary of the invention
For the deficiency of above-mentioned technology, the invention provides a kind of method that fast selecting goes out hydrogen isotope separation material, for obtaining the Ti-V-Cr(titanium-vanadium-chromium simultaneously with remarkable antihydrogen isotopic effect and excellent hydrogen storage performance fast) alloy material, provide the thinking of research and design.
To achieve these goals, the technical solution used in the present invention is as follows:
Fast selecting goes out a method for hydrogen isotope separation material, comprises the following steps:
(1) select titanium vanadium Chrome metal powder as hydrogen isotope separation material, and determine that, in selected titanium vanadium Chrome metal powder, the content of vanadium is 40at%, and meanwhile, the purity of titanium, vanadium and chromium is all greater than 99.9%;
(2) according to the content of the vanadium determined, under the condition of sum total e/a=4.4 ~ 5.6 guaranteeing the outermost s electronics of atoms metal and d electronics number in titanium vanadium Chrome metal powder, the content of titanium and chromium is adjusted according to actual demand;
(3) content of the titanium determined according to step (2), vanadium, chromium, obtains the molecular formula of titanium vanadium Chrome metal powder, determines the titanium vanadium Chrome metal powder needing to choose.
Further, in described step (2), sum total e/a=4.8 ~ 5.2 of the outermost s electronics of atoms metal and d electronics number in titanium vanadium Chrome metal powder, and in step (2), the content of chromium is 20 ~ 40at%.
Again further, in described step (2), the sum total e/a=5 of the outermost s electronics of atoms metal and d electronics number in titanium vanadium Chrome metal powder, and the titanium chrome alloy molecular formula that described step (3) is determined is Ti
30v
40cr
30.
Principle of design of the present invention is, we design each composition according to the flat fare electron density (e/a) of Ti-V-Cr alloy, and the content of vanadium be aided with in alloy adjusts properties, thus select the Ti-V-Cr alloy with remarkable antihydrogen isotopic effect.Because the electronic structure of alloy has significant impact to its thermodynamic property, and equilibrium separation factor-alpha is also a kind of thermodynamic property of alloy, and therefore, the e/a in Ti-V-Cr alloy can have larger impact to α.Theoretically, this has the impact (with regard to antihydrogen isotopic effect) of two aspects, on the one hand, e/a increase can cause interaction between atoms to strengthen, thus cause the lattice parameter of alloy to reduce, resonance model according to shielding proton model and separation factor can be known, this effect can cause the vibrational energy of hydrogen atom in interstitial void to increase, thus increases separation factor alpha; On the other hand, e/a increase can cause hydrogen atom to occupy the increase of octahedral interstice, thus reduces separation factor alpha, and this is because the potential curve of hydrogen in octahedral interstice and tetrahedral interstice determines.Therefore, under the impact of factor both ways, separation factor alpha will increase along with the increase of e/a, and reduce gradually after certain point reaches maximum value, and result shows, is determining that the scope of e/a is 4.4 ~ 5.6, and the content of vanadium is after 40at%, be no matter the content of e/a or vanadium, can cause putting hydrogen difficulty lower than the above-mentioned lower value determined, then can cause inhaling hydrogen difficulty higher than its higher limit.Therefore, according to this principle and thinking, the choosing method determined Ti-V-Cr alloy of the present invention's design will have excellent hydrogen storage performance, can meet the separation demand of different hydrogen isotopes.
Compared with prior art, the present invention has following beneficial effect:
(1) present invention applicant finds and a kind of method can selecting hydrogen isotope separation material fast of research and design, its e/a by Ti-V-Cr alloy and content of vanadium scope choose the parting material with antihydrogen isotopic effect, thus not only can select the Ti-V-Cr alloy simultaneously with larger antihydrogen isotopic effect and excellent hydrogen storage performance, and alloying constituent can be adjusted flexibly with practical requirement according to the separation condition of reality.Thus, only by determining without the need to experiment on a small quantity, even, just need can select required titanium vanadium chromium alloy material, this has greatly saved the cost of research and development undoubtedly, and shortens the cycle of research and development.The present invention finds the Ti-V-Cr alloy with remarkable antihydrogen isotopic effect to provide extraordinary thinking, effectively formulate a kind of standard, fill up the blank of this respect, the research of hydrogen isotope separation technology is made to have risen to a new height, for the R&D costs reducing hydrogen isotope separation technology provide good guarantee.
(2) in the present invention, the preferred scope of e/a is 4.8 ~ 5.2, under the content of vanadium is 40at% and the content of chromium is 20 ~ 40at% condition, in the scope of e/a=4.8 ~ 5.2, the Ti-V-Cr alloy selected all has significant antihydrogen isotopic effect (separation factor alpha >1.3), and within the scope of this, its level ground platform pressure can change several order of magnitude, thus can meet the demand of practical application completely flexibly.
(3) determined best titanium vanadium Chrome metal powder (the molecular formula Ti of the present invention
30v
40cr
30), antihydrogen isotopic effect is obvious, hydrogen storage amount is high (can reach 420ml/g), fast, the antitoxin voltinism of activating velocity can be good, compared with existing antihydrogen isotopic effect material, it (namely considers separation factor and hydrogen storage performance) simultaneously has fairly obvious advantage in over-all properties.
Accompanying drawing explanation
Fig. 1 is realization flow schematic diagram of the present invention.
Fig. 2 is the graph of relation of separation factor and e/a in the present invention.
Fig. 3 is the graph of relation of separation factor and content of vanadium in the present invention.
Embodiment
Below in conjunction with drawings and Examples, the invention will be further described, and embodiments of the present invention include but not limited to the following example.
Embodiment
As shown in Figure 1, the invention provides a kind of method that fast selecting goes out hydrogen isotope separation material, its mainly for be the alloy of Ti-V-Cr series, and can flexibly according to substantial sepn condition design with select required titanium vanadium chromium alloy material.The present invention forms primarily of following steps:
(1) determine that in the titanium vanadium Chrome metal powder that will choose, the content of vanadium is 40at%, and the purity of titanium, vanadium and chromium is all greater than 99.9%;
(2) according to the content of the vanadium determined, under the condition guaranteeing e/a=4.4 ~ 5.6 in titanium vanadium Chrome metal powder, the content of titanium and chromium is adjusted according to actual demand;
(3) according to the content of the titanium determined, vanadium, chromium, determine the molecular formula of titanium vanadium Chrome metal powder, obtain the titanium vanadium Chrome metal powder needing to choose; The titanium vanadium Chrome metal powder that the present invention selects under e/a=4.4 ~ 5.6, V=40at% condition has: Ti
60v
40cr
0(e/a=4.4), Ti
55v
40cr
5(e/a=4.5), Ti
50v
40cr
10(e/a=4.6), Ti
45v
40cr
15(e/a=4.7), Ti
40v
40cr
20(e/a=4.8), Ti
35v
40cr
25(e/a=4.9), Ti
30v
40cr
30(e/a=5), Ti
25v
40cr
35(e/a=5.1), Ti
20v
40cr
40(e/a=5.2), Ti
15v
40cr
45(e/a=5.3), Ti
10v
40cr
50(e/a=5.4), Ti
5v
40cr
55and Ti (e/a=5.5)
0v
40cr
60(e/a=5.6).
Above-mentioned selected titanium vanadium Chrome metal powder all prepares by prior art means, and its main preparation process is: weighed each alloy by proportioning, then load weighted alloy sample is put into sample chamber, is evacuated to 10
-3pa, is filled with argon gas to about 0.6bar, starting the arc melting, after alloy melts completely, then continues melting about 1 minute, can obtain corresponding titanium vanadium Chrome metal powder.
In addition, be necessary to be defined as a detailed explanation to e/a.For transition metal, e/a broadly refers to the flat fare electron density of metal, then refers to the sum total of the outermost s electronics of atoms metal and d electronics number in the narrow sense.Such as, the outermost electron structure of Ti is 3d
24s
2, then the e/a=4 of Ti, in like manner, the e/a=6 of the e/a=5 of V, Cr.The flat fare electron density of alloy is then a weighted mean according to each Elements Atom ratio.Such as, Ti
30v
40cr
30e/a=30% × 4+40% × 5+30% × 6=5.
In above-mentioned steps, in described step (2), the scope of e/a can elect 4.8 ~ 5.2 as.When the content of vanadium is 40at%, 4.8 ~ 5.2 within the scope of this, Ti-V-Cr alloy all has significant antihydrogen isotopic effect (separation factor alpha >1.3), and its level ground platform pressure then can change several order of magnitude.Say further, because separation factor alpha can increase along with the increase of e/a, reduce gradually after certain point reaches maximum value, therefore, in 4.8 ~ 5.2 scopes, what can determine further is, this maximum point is exactly e/a=5, and α=1.47 now, as shown in Figure 2.And can be determined by e/a=5, α=1.47, the alloying constituent at this some place is Ti
30v
40cr
30experiment records, this kind of alloy has good hydrogen storage performance, its hydrogen storage amount can reach 420ml/g, this is also after the comprehensive antihydrogen isotopic effect of the present invention and hydrogen storage performance are considered, the alloy with optimal synthesis performance selected, its more than 80% of hydrogen－sucking amount that can reach capacity within 10min, XRD analysis then shows, the structure mainly body-centered cubic structure (BCC) of this alloy.
Say further, choose mode according to above-mentioned, if wish that the level ground platform pressure of alloy is lower, so can select the alloy that some e/a are less, otherwise then can select the alloy that those e/a are larger.After obtaining great separation factor by e/a adjustment, if also wish to obtain larger separation factor, then can realize by adjusting the content of vanadium of alloy, because along with the increase of content of vanadium, separation factor can present the increase of near-linear, and its rule as shown in Figure 3.
In addition, what deserves to be explained is, contrast the more existing material with anti-isotopic effect, the unique advantage that the present invention chooses and the material determined has can be found.
Following a few class roughly can be divided into for existing, that there is antihydrogen isotopic effect material at present:
1) AB
2type hydrogen storage material, Typical Representative is as TiMn
1.5, ZrMn
2and ZrCr
2deng, they are respectively 1.14,1.27 and 1.37 in the separation factor of near room temperature to protium, deuterium, are all less than the determined best materials of the present invention (i.e. Ti in antihydrogen isotopic effect
30v
40cr
30).In addition, AB
2the hydrogen storage amount of type hydrogen storage material is generally at about 200ml/g, and the determined best materials of the present invention (i.e. Ti
30v
40cr
30) hydrogen storage amount reach 420ml/g, be more than its twice.Therefore, with traditional AB
2type hydrogen storage material is compared, the determined material of the present invention, particularly Ti
30v
40cr
30, advantage is obvious.
2) AB
5type hydrogen storage material, Typical Representative is LaNi
5, this material does not embody antihydrogen isotopic effect substantially near room temperature, only has less antihydrogen isotopic effect when temperature is very low, as being 1.22 when 218K to the separation factor of protium, deuterium, be far inferior to the determined material of the present invention, and its hydrogen storage amount compares AB
2the hydrogen storage material of type is also low.Therefore, the determined material of the present invention, particularly Ti
30v
40cr
30, in contrast, advantage is more obvious.
3) pure metal, Typical Representative is vanadium.Vanadium is 1.77 in the separation factor of near room temperature, will exceed 0.3 than the determined material of the present invention.But the inferior position of vanadium in storage hydrogen is obvious, as activated difficulty, Shuan Pingtai, dynamic performance difference and easily poisoning etc., this is also the reason that it is not applied for many years in hydrogen isotope separation.And the determined material of the present invention, particularly Ti
30v
40cr
30, substantially there is not the problem of activation, it just can effectively need be activated through once vacuumizing, and dynamic performance is fine, and just can reach capacity within 10min more than 80% of hydrogen－sucking amount.In addition, the determined material of the present invention, antitoxin voltinism can be also fine, exposes in atmosphere (proof maximum duration is one week) even if long-time, also not obviously affects its hydrogen storage performance.
In sum, compared with existing antihydrogen isotopic effect material, in over-all properties, (namely consider separation factor and hydrogen storage performance), the present invention determined Ti-V-Cr alloy material, particularly Ti simultaneously
30v
40cr
30, there is fairly obvious advantage.
The present invention, according to the rule embodied between e/a in the hydrogen isotope effect of Ti-V-Cr alloy and alloy and content of vanadium (rule shown in Fig. 2,3), have devised and fast selecting can go out the method for the Ti-V-Cr alloy material simultaneously with remarkable antihydrogen isotopic effect and excellent hydrogen storage performance.And according to this method and rule, and can choose correct Research Thinking is provided with regard to the design of hydrogen isotope separation material, thus lay a solid foundation for saving Innovation Input cost and shortening the R&D cycle, therefore, the present invention has outstanding substantive distinguishing features with significant progressive.
Above-described embodiment is only the preferred embodiments of the present invention; be not construed as limiting the scope of the present invention; in every case principle of design of the present invention being adopted, and the change carried out non-creativeness work on this basis and make, all should belong within protection scope of the present invention.
Claims (3)
1. fast selecting goes out a method for hydrogen isotope separation material, it is characterized in that, comprises the following steps:
(1) select titanium vanadium Chrome metal powder as hydrogen isotope separation material, and determine that, in selected titanium vanadium Chrome metal powder, the content of vanadium is 40at%, and meanwhile, the purity of titanium, vanadium and chromium is all greater than 99.9%;
(2) according to the content of the vanadium determined, under the condition of sum total e/a=4.4 ~ 5.6 guaranteeing the outermost s electronics of atoms metal and d electronics number in titanium vanadium Chrome metal powder, the content of titanium and chromium is adjusted according to actual demand;
(3) content of the titanium determined according to step (2), vanadium, chromium, obtains the molecular formula of titanium vanadium Chrome metal powder, determines the titanium vanadium Chrome metal powder needing to choose.
2. a kind of fast selecting according to claim 1 goes out the method for hydrogen isotope separation material, it is characterized in that, in described step (2), sum total e/a=4.8 ~ 5.2 of the outermost s electronics of atoms metal and d electronics number in titanium vanadium Chrome metal powder, and in step (2), the content of chromium is 20 ~ 40at%.
3. a kind of fast selecting according to claim 2 goes out the method for hydrogen isotope separation material, it is characterized in that, in described step (2), the sum total e/a=5 of the outermost s electronics of atoms metal and d electronics number in titanium vanadium Chrome metal powder, and the titanium chrome alloy molecular formula that described step (3) is determined is Ti
30v
40cr
30.
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Citations (5)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPH08311596A (en) * | 1994-07-22 | 1996-11-26 | Toshiba Corp | Hydrogen storage alloy, surface modifying method for hydrogen storage alloy, battery cathode, and alkali secondary battery |
| US20050113607A1 (en) * | 2002-07-05 | 2005-05-26 | Biocon Limited | Novel halo-substituted active methylene compounds |
| CN1715179A (en) * | 2005-06-07 | 2006-01-04 | 四川材料与工艺研究所 | Hydrogen isotope separating device and method |
| JP2007270209A (en) * | 2006-03-30 | 2007-10-18 | Toshiba Corp | Hydrogen storage alloy, hydrogen storage film and hydrogen storage tank |
| CN101349679A (en) * | 2007-07-19 | 2009-01-21 | 柯香文 | Method for quantitatively measuring hydrogen, deuteration hydrogen and deuterium hydrogen isotope element |
-
2015
- 2015-03-03 CN CN201510093420.3A patent/CN104630598B/en not_active Expired - Fee Related
Patent Citations (5)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPH08311596A (en) * | 1994-07-22 | 1996-11-26 | Toshiba Corp | Hydrogen storage alloy, surface modifying method for hydrogen storage alloy, battery cathode, and alkali secondary battery |
| US20050113607A1 (en) * | 2002-07-05 | 2005-05-26 | Biocon Limited | Novel halo-substituted active methylene compounds |
| CN1715179A (en) * | 2005-06-07 | 2006-01-04 | 四川材料与工艺研究所 | Hydrogen isotope separating device and method |
| JP2007270209A (en) * | 2006-03-30 | 2007-10-18 | Toshiba Corp | Hydrogen storage alloy, hydrogen storage film and hydrogen storage tank |
| CN101349679A (en) * | 2007-07-19 | 2009-01-21 | 柯香文 | Method for quantitatively measuring hydrogen, deuteration hydrogen and deuterium hydrogen isotope element |
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