CN104630598B - A kind of fast selecting goes out the method for hydrogen isotope separation material - Google Patents
A kind of fast selecting goes out the method for hydrogen isotope separation material Download PDFInfo
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Abstract
The invention discloses a kind of method that fast selecting goes out hydrogen isotope separation material, comprise the following steps: (1) selects titanium vanadium evanohm as hydrogen isotope separation material, and determine in selected titanium vanadium evanohm, the content of vanadium is 40at%, meanwhile, the purity of titanium, vanadium and chromium is all greater than 99.9%; (2), according to the content of definite vanadium, guaranteeing under the condition of e/a=4.4～5.6 in titanium vanadium evanohm, adjust the content of titanium and chromium; (3) according to the content of the definite titanium of step (2), vanadium, chromium, obtain the molecular formula of titanium vanadium evanohm, determine the titanium vanadium evanohm that need to choose. The present invention has remarkable antihydrogen isotope effect Ti-V-Cr alloy for finding provides extraordinary thinking, effectively fill up the blank of this respect, provide guarantee for reducing the technical research cost of hydrogen isotope separation and shortening the R&D cycle, therefore, the present invention has very high practical value and promotional value.
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, utilize the hydrogen isotope effect of hydrogen storage material to separate to be wherein a kind of up-and-coming method. The key of this method is to need a kind of material simultaneously with remarkable hydrogen isotope effect and good hydrogen storage performance. Up to now, Metal Palladium is the superior of combination property in all material. But palladium is a kind of very expensive metal, therefore, this has limited its large-scale application in industry. On the other hand, palladium has positive isotope effect, and situation when this is very low for heavy hydrogen isotope (as deuterium or the tritium) concentration of processing is disadvantageous. Now, the material that we need to have an antihydrogen isotope effect is processed some special situations.
Vanadium is a kind of metal with larger antihydrogen isotope effect, but its activation difficulty, 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. The material that in general, really can be actually used in hydrogen isotope separation at present only has palladium. Therefore,, no matter be researcher or engineer, all urgent hope can find one both to have remarkable antihydrogen isotope effect, has again the material of good hydrogen storage performance simultaneously, to replace expensive palladium, or is 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 has obtained very systematic research, substantially understand fully about the relation between the every character of alloy and hydrogen storage performance. These achievements in research show, it is a kind of up-and-coming hydrogen storage material that Ti-V-Cr is associated gold, has both had large hydrogen storage amount, has again good dynamic performance, and its level ground platform pressure can also be adjusted in very wide scope.
Thus, if definite Ti-V-Cr alloy has significant antihydrogen isotope effect, just very possible for example, in the processing (separation of hydrogen isotope) of hydrogen isotope, gather around and have broad application prospects. But, in the face of the processing demands of different hydrogen isotopes, at present how fast do not see, effectively select the relevant report of the Ti-V-Cr alloy simultaneously with antihydrogen isotope effect and good hydrogen storage performance both at home and abroad, conventionally be all to screen through a large amount of intimate experiments of having no main threads, thereby not only extended cycle of technical research, and significantly increase 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 quick acquisition has the Ti-V-Cr(titanium-vanadium-chromium of remarkable antihydrogen isotope effect and good hydrogen storage performance simultaneously) alloy material, the thinking of research and design is provided.
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 evanohm as hydrogen isotope separation material, and determine that in selected titanium vanadium evanohm, the content of vanadium is 40at%, meanwhile, the purity of titanium, vanadium and chromium is all greater than 99.9%;
(2) according to the content of definite vanadium, guaranteeing, under the condition of summation e/a=4.4～5.6 of the outermost s electronics of metallic atom and d electronics number in titanium vanadium evanohm, to adjust the content of titanium and chromium according to actual demand;
(3) determine the titanium vanadium evanohm that need to choose; In this step, the titanium vanadium evanohm of choosing has: Ti60V40Cr0（e/a=4.4）、Ti55V40Cr5（e/a=4.5）、Ti50V40Cr10（e/a=4.6）、Ti45V40Cr15（e/a=4.7）、Ti40V40Cr20（e/a=4.8）、Ti35V40Cr25（e/a=4.9）、Ti30V40Cr30（e/a=5）、Ti25V40Cr35（e/a=5.1）、Ti20V40Cr40（e/a=5.2）、Ti15V40Cr45（e/a=5.3）、Ti10V40Cr50（e/a=5.4）、Ti5V40Cr55And Ti (e/a=5.5)0V40Cr60（e/a=5.6）。
Further, in described step (2), summation e/a=4.8～5.2 of the outermost s electronics of metallic atom and d electronics number in titanium vanadium evanohm, and in step (2), the content of chromium is 20～40at%.
Again further, in described step (2), the summation e/a=5 of the outermost s electronics of metallic atom and d electronics number in titanium vanadium evanohm, and the definite titanium chrome alloy molecular formula of described step (3) is Ti30V40Cr30。
Design principle of the present invention is, we design each composition according to the flat fare electron concentration (e/a) of Ti-V-Cr alloy, and the content of vanadium being aided with in alloy adjusts properties, thereby select the Ti-V-Cr alloy with remarkable antihydrogen isotope effect. Because the electronic structure of alloy has significant impact to its macroscopic property, and equilibrium separation factor-alpha is also a kind of macroscopic 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 isotope effect) of two aspects, on the one hand, e/a increase can cause interaction between atoms to strengthen, thereby cause the lattice paprmeter of alloy to reduce, can know according to the resonance model of shielding proton model and separation factor, this effect can cause the vibrational energy of hydrogen atom in interstitial void to increase, thereby increases separation factor alpha; On the other hand, e/a increase can cause hydrogen atom to occupy the increase of octahedral interstice, thereby reduces separation factor alpha, and this is because the potential energy curve of hydrogen in octahedral interstice and tetrahedral interstice determines. Therefore, both ways under the impact of factor, separation factor alpha will increase along with the increase of e/a, and reduce gradually after certain point reaches maximum, and result shows, is 4.4～5.6 in the scope of determining e/a, and after the content of vanadium is 40at%, no matter be e/a or the content of vanadium, can cause putting hydrogen difficulty lower than above-mentioned definite lower limit, can cause inhaling hydrogen difficulty higher than its higher limit. Therefore,, according to this principle and thinking, the determined Ti-V-Cr alloy of choosing method of the present invention's design will have good hydrogen storage performance, can meet the separation demand of different hydrogen isotopes.
Compared with prior art, the present invention has following beneficial effect:
(1) the present patent application people find and research and design a kind of method that can select fast hydrogen isotope separation material, its e/a by Ti-V-Cr alloy and content of vanadium scope are chosen the parting material with antihydrogen isotope effect, thereby not only can select the Ti-V-Cr alloy simultaneously with larger antihydrogen isotope effect and good hydrogen storage performance, and can adjust flexibly alloying component with practical requirement according to actual separation condition. Thus, only need to pass through on a small quantity, even determine without experiment, just can select needed titanium vanadium chromium alloy material, this has greatly saved the cost of research and development undoubtedly, and has shortened the cycle of research and development. The present invention has remarkable antihydrogen isotope effect Ti-V-Cr alloy for finding provides extraordinary thinking, effectively formulate a kind of standard, fill up the blank of this respect, make the research of hydrogen isotope separation technology rise to a new height, for the R&D costs that reduce hydrogen isotope separation technology provide good guarantee.
(2) in the present invention, the preferred scope of e/a is 4.8～5.2, the content that is 40at% and chromium at the content of vanadium is under 20～40at% condition, in the scope of e/a=4.8～5.2, the Ti-V-Cr alloy of selecting all has significant antihydrogen isotope effect (separation factor alpha > 1.3), and within the scope of this, its level ground platform pressure can change several orders of magnitude, thereby can meet flexibly the demand of practical application completely.
(3) determined best titanium vanadium evanohm (the molecular formula Ti of the present invention30V40Cr30), antihydrogen isotope 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 isotope effect material, it (considers separation factor and hydrogen storage performance) simultaneously has fairly obvious advantage aspect combination property.
Brief description of the drawings
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.
Detailed description of the invention
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 fast selecting and go out the method for hydrogen isotope separation material, its mainly for be the alloy of Ti-V-Cr series, and can be flexibly according to the design of actual separation condition with select required titanium vanadium chromium alloy material. The present invention is mainly made up of following steps:
(1) determine that in the titanium vanadium evanohm 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 definite vanadium, guaranteeing under the condition of e/a=4.4～5.6 in titanium vanadium evanohm, adjust the content of titanium and chromium according to actual demand;
(3) according to the content of definite titanium, vanadium, chromium, determine the molecular formula of titanium vanadium evanohm, obtain the titanium vanadium evanohm that need to choose; The titanium vanadium evanohm that the present invention selects under e/a=4.4～5.6, V=40at% condition has: Ti60V40Cr0（e/a=4.4）、Ti55V40Cr5（e/a=4.5）、Ti50V40Cr10（e/a=4.6）、Ti45V40Cr15（e/a=4.7）、Ti40V40Cr20（e/a=4.8）、Ti35V40Cr25（e/a=4.9）、Ti30V40Cr30（e/a=5）、Ti25V40Cr35（e/a=5.1）、Ti20V40Cr40（e/a=5.2）、Ti15V40Cr45（e/a=5.3）、Ti10V40Cr50（e/a=5.4）、Ti5V40Cr55And Ti (e/a=5.5)0V40Cr60（e/a=5.6）。
Above-mentioned selected titanium vanadium evanohm all can prepare by prior art means, and its main preparation process is: weighed each alloy by proportioning, then load weighted alloy sample has been put into sample room, be evacuated to 10-3Pa, is filled with argon gas to 0.6bar left and right, and starting the arc melting after alloy melts completely, then continues melting about 1 minute, can obtain corresponding titanium vanadium evanohm.
In addition, be necessary the detailed explanation that is defined as to e/a. For transition metal, e/a broadly refers to the flat fare electron concentration of metal, refers to narrowly the summation of the outermost s electronics of metallic atom and d electronics number. For example, the outermost electron structure of Ti is 3d24s2, the e/a=4 of Ti, in like manner, the e/a=5 of V, the e/a=6 of Cr. The flat fare electron concentration of alloy is according to each element atomic ratio weighted average. For example, Ti30V40Cr30E/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. In the time that the content of vanadium is 40at%, 4.8～5.2 within the scope of this, Ti-V-Cr alloy all has significant antihydrogen isotope effect (separation factor alpha > 1.3), and its level ground platform pressure can change several orders of magnitude. Say further, because separation factor alpha can increase along with the increase of e/a, after certain point reaches maximum, reduce gradually, therefore,, in 4.8～5.2 scopes, what can further determine is, this maximum point is exactly e/a=5, and α=1.47 now, as shown in Figure 2. And by determining in e/a=5, α=1.47, the alloying component at this some place is Ti30V40Cr30Experiment 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 isotope effect of the present invention and hydrogen storage performance are considered, the alloy with optimal synthesis performance selecting, its more than 80% of hydrogen-sucking amount that can reach capacity in 10min, XRD analysis shows, the structure of this alloy is mainly body-centered cubic structure (BCC).
Say further, according to the above-mentioned mode of choosing, if wish that the level ground platform pressure of alloy is lower, can select so the alloy that some e/a are less, otherwise can select the alloy that those e/a are larger. Adjusting by e/a after the great separation factor of acquisition, if also wish to obtain larger separation factor, can realize by the content of vanadium of adjusting alloy, because along with the increase of content of vanadium, separation factor can present intimate linear increase, and its rule as shown in Figure 3.
In addition, what deserves to be explained is, contrast the more existing material with anti-isotope effect, can find the unique advantage that the present invention chooses and definite material has.
Roughly can be divided into following a few class for material existing, that there is antihydrogen isotope effect at present:
1）AB2Type hydrogen storage material, Typical Representative is as TiMn1.5、ZrMn2And ZrCr2Deng, they are respectively 1.14,1.27 and 1.37 near room temperature to the separation factor of protium, deuterium, (are Ti being all less than the determined optimal material of the present invention aspect antihydrogen isotope effect30V40Cr30). In addition, AB2The hydrogen storage amount of type hydrogen storage material is generally in 200ml/g left and right, and the determined optimal material of the present invention (is Ti30V40Cr30) hydrogen storage amount reached 420ml/g, be that it is more than twice. Therefore, with traditional AB2Type hydrogen storage material is compared, the present invention determined material, particularly Ti30V40Cr30, advantage is obvious.
2）AB5Type hydrogen storage material, Typical Representative is LaNi5, this material does not embody antihydrogen isotope effect substantially near room temperature, only in the time that temperature is very low, has less antihydrogen isotope effect, as being 1.22 to the separation factor of protium, deuterium when the 218K, be far inferior to the determined material of the present invention, and its hydrogen storage amount compares AB2The hydrogen storage material of type is also low. Therefore, the present invention determined material, particularly Ti30V40Cr30, in contrast, advantage is more obvious.
3) simple 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 vanadium is in storage, the inferior position aspect hydrogen is significantly, as it is poor and easy to be poisoning etc. to activate difficulty, Shuan Pingtai, dynamic performance, and this is also its reason not being applied aspect hydrogen isotope separation for many years. And the present invention determined material, particularly Ti30V40Cr30, substantially there is not the problem of activation, it need can effectively be activated through just once vacuumizing, and dynamic performance is fine, and 10min is with interior the more than 80% of hydrogen-sucking amount that just can reach capacity. In addition, the determined material of the present invention, antitoxin voltinism can be also fine, even if be exposed to for a long time (proof maximum duration is one week) in air, also not obvious its hydrogen storage performance that affects.
In sum, compared with existing antihydrogen isotope effect material, aspect combination property, (consider separation factor and hydrogen storage performance), the present invention determined Ti-V-Cr alloy material, particularly Ti simultaneously30V40Cr30, there is fairly obvious advantage.
The present invention is according to the rule embodying between e/a and content of vanadium in the hydrogen isotope effect of Ti-V-Cr alloy and alloy (rule shown in Fig. 2,3), designed the method that can fast selecting goes out simultaneously to have the Ti-V-Cr alloy material of remarkable antihydrogen isotope effect and good hydrogen storage performance. And according to this method and rule, can and choose the Research Thinking that provides correct with regard to the design of hydrogen isotope separation material, thereby for saving research and development input cost and shortening the R&D cycle and lay a solid foundation, therefore, the present invention has outstanding substantive distinguishing features and 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 adopt design principle of the present invention, and carry out non-creativeness work on this basis and the variation made, within all should belonging to 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 evanohm as hydrogen isotope separation material, and determine that in selected titanium vanadium evanohm, the content of vanadium is 40at%, meanwhile, the purity of titanium, vanadium and chromium is all greater than 99.9%;
(2) according to the content of definite vanadium, guaranteeing, under the condition of summation e/a=4.4～5.6 of the outermost s electronics of metallic atom and d electronics number in titanium vanadium evanohm, to adjust the content of titanium and chromium according to actual demand;
(3) determine the titanium vanadium evanohm that need to choose; In this step, the titanium vanadium evanohm of choosing has: Ti60V40Cr0（e/a=4.4）、Ti55V40Cr5（e/a=4.5）、Ti50V40Cr10（e/a=4.6）、Ti45V40Cr15（e/a=4.7）、Ti40V40Cr20（e/a=4.8）、Ti35V40Cr25（e/a=4.9）、Ti30V40Cr30（e/a=5）、Ti25V40Cr35（e/a=5.1）、Ti20V40Cr40（e/a=5.2）、Ti15V40Cr45（e/a=5.3）、Ti10V40Cr50（e/a=5.4）、Ti5V40Cr55And Ti (e/a=5.5)0V40Cr60（e/a=5.6）。
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), summation e/a=4.8～5.2 of the outermost s electronics of metallic atom and d electronics number in titanium vanadium evanohm, 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 summation e/a=5 of the outermost s electronics of metallic atom and d electronics number in titanium vanadium evanohm, and the definite titanium chrome alloy molecular formula of described step (3) is Ti30V40Cr30。
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Citations (4)
| Publication number | Priority date | Publication date | Assignee | Title |
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| 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 |
| CN1715179A (en) * | 2005-06-07 | 2006-01-04 | 四川材料与工艺研究所 | Hydrogen isotope separation 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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| US7179942B2 (en) * | 2002-07-05 | 2007-02-20 | Bicon Limited | Halo-substituted active methylene compounds |
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| 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 |
| CN1715179A (en) * | 2005-06-07 | 2006-01-04 | 四川材料与工艺研究所 | Hydrogen isotope separation 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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