WO2012113877A1 - Method and device for transporting metal elements in the gas phase - Google Patents

Abstract

The invention relates to a device and method for producing, providing, and transporting metal elements in the gaseous phase, wherein the carrier gas contains carbon monoxide and the carrier gas and the metal elements are brought together in a reaction volume and the metal elements and carbon monoxide combine to synthesize metal-element carbonyl complexes.

Description

 Method and device for

 Gas phase transport of metal elements

description

Field of the invention

 The invention relates to a method and a device for transporting metal elements in gaseous phase.

Background of the invention

 The observation of the chemical-physical properties of various elements is done first by observing their molecular properties. Especially for the synthesis of novel chemical classes of compounds

Transactinoids and other elements of the periodic table, such as transition metals and elements of the d and p groups, it is usually not possible to use a macroscopic

Solid or liquid body to observe, but one observes the behavior of individual atoms and molecules under certain circumstances.

To produce these elements of the periodic table, it is a useful way to use a body of a material, in particular a solid as a target and to activate this target with radiation. Depending on the available radiation source and the

Element to be generated mainly, the target material is selected and exposed to the radiation, by nuclear reactions finally the desired elements arise. For example, thermal

Used neutrons and a neutron-induced Nuclear fission are caused, as for example on

Research Reactor TRIGA Mainz at the Johannes Gutenberg University in Mainz, Germany. Accelerator devices, for example those of the GSI Helmholtz Center for heavy ion research GmbH in

Darmstadt, Germany (hereafter GSI) can also be used. For generating elements with

different mass, for example for the production of metal elements, for example of transition metals, an ion beam of a linear accelerator, a

Synchrotrons, such as the heavy ion beam of the GSI, or a cyclotron are shot at a selected target.

The measurement, use and utilization of the

Physicochemical properties of the metal elements is extremely difficult because the metal elements

sometimes very short-lived. Furthermore, some tend

Metal elements strong at all physical

 Objects, such as a transformation,

for example, to adhere by adsorption.

In addition, it is due to the often extreme

Radiation stress due to running in the production of the metal elements core processes, difficult to impossible to measure or use their properties at the site of formation of the metal elements. Therefore, it is useful if the metal elements from their place

Origin can be removed. In particular, it may be of interest to refractory

To transport metal elements from one place to another, without adsorption, for example, on a wall of a chamber, such as a

Reaction chamber or vacuum chamber in which the

Metal elements are generated, or at one

Lost transport line during the transport process.

Previous methods involving a transport of

Enable metal elements that need for their

 Feasibility partly extreme environmental conditions in pressure and temperature. The mastery of these conditions is often so difficult in addition to the already extreme production conditions of the metal elements that thereby

Yield is low, so that a measuring or

 Application procedure is not feasible, is more difficult or at least takes longer.

In a widely used method, a cluster Gasj et is used, wherein an inert gas aerosol cluster of solid or liquid materials such as

Potassium chloride, lead iodide, carbon or molybdenum trioxide, latex, oil or water, with the refractory elements attaching to the aerosol clusters and thus being transported with the aerosol particles in the gas flow. The disadvantage of this method is that it does not work selectively and also does not have a constant

Yield from the cluster gas et can be ensured. This may be due to the fact that during operation, the aerosol particles accumulate in some places in the system and thereby the system properties can be adversely affected. For another use would be a separation of the refractory elements from the clusters necessary. This is difficult, energy intensive and

time consuming. In another known method for

selective transport of the metal elements ruthenium, osmium, rhenium, molybdenum and technetium are these as

transported non-refractory oxides, oxychlorides or hydroxides in a gas stream by the oxygen and / or water or chlorinating media are added to the gas stream. However, this requires high temperatures of several hundred degrees Celsius to start the process.

Another possibility is in selected cases in the synthesis of non-reactive fluorides. For example, fission zircon can be generated in the induced nuclear fission of uranium-235. For this UF _{3 is used} as target material

used and heated to over 400 ° C. In this way, nonreactive ZrF4 can be generated in these experiments and transported at a pressure of 10 ^-7 bar. This method also requires extreme environmental conditions.

General description of the invention

 The invention therefore has the task of providing a method which makes it possible

Metal elements, especially for moderate

 Ambient conditions to transport from a place to a remote location in order to detect there the metal elements per se, but also to measure their physicochemical properties or the

Metal elements can be used elsewhere. The object of the invention is solved by the subject matters of the independent claims. Advantageous developments of the invention are defined in the subclaims. According to the invention metal elements by means of the synthesis of metal element carbonyl complexes in a

transportable state and can thus be transported over longer distances in the gaseous phase with a carrier gas.

The transport of the metal elements in the gaseous phase proves to be particularly advantageous. On the one hand, this process does not require a phase transition to another, for example solid, phase for the transport, so that the metal elements are not complicated from the other phase into the gaseous phase for a first

Re-use must be returned. This forced phase transition back into the gaseous phase is possible in the prior art only with high loss rates and high energy input. On the other hand, however, by the invention and described below

Carbonyl formation ensures that the metal elements are essentially not attached to physical objects on the body

Adhere to the transport route and are thus no longer available for the transport process.

According to the invention, the carrier gas contains carbon monoxide. The carrier gas is preferably combined with the metal elements in a reaction volume, wherein the

Metal elements and the carbon monoxide molecules of the

Carrier gases can synthesize directly to metal element carbonyl complexes. Metal element carbonyl complexes are Complex compounds of metal elements with

Carbon monoxide ligand. The complex compounds have the general structure d _m (C0) _n . Under the term

 "Carbonyl complex" will be referred to hereinafter as well

simple carbonyl complexes with only one

 Carbon monoxide ligands as well as those with multiple carbon monoxide ligands understood. Further, the term "carbonyl complex" herein means both mononuclear carbonyl complexes (m = 1) and polynuclear carbonyl complexes (m> 1).

In other words, the metal elements are directly synthesized in the gaseous phase to metal element carbonyl complexes and are thereby stably transportable in the gaseous phase. Thus, in the present invention, the metal element carbonyl complexes themselves are gaseous.

The metal elements are thus dissolved out of the target and go into the gaseous phase. Subsequently, the gaseous metal elements synthesize in the

Reaction volume with the molecular carbon monoxide to the gaseous metal element-carbonyl complexes. That it synthesizes an (exothermic) chemical

Reaction remains in the gaseous phase between the metal elements and the molecular carbon monoxide to form the gaseous metal element carbonyl complexes. A physical phase transition of the metal elements, for example a simple freezing on aerosol clusters, as described in the prior art, is with all its Disadvantages are not necessary. In contrast, in a surprising way, the conditions for a

direct synthesis of the metal element carbonyl complexes and thus for a direct gas phase transport of the metal elements are created.

Based on the three exemplary reaction equations listed below, the processes for

Synthesis of the metal element carbonyl complexes according to the invention, which in consequence as carbonyl complex synthesis

will be described.

u ^ Mo + 6 CO -> ^IJ ^ Mo (CO) ₆

l ⁰⁸ u + 5 CO -> ¹⁰⁸ Ru (CO) ₅

m ^x d + n CO -> ^x d _m (CO)

For example, a generated metal element

Molybdenum-104 preferably with six

Synthesize carbon monoxide molecules to form an octahedral Mo (CO) ₆ - carbonyl complex. A metal element ruthenium-108, also formed, may preferably react with five carbon monoxide molecules to form a trigonal bipyramidal Ru (CO) ₅ carbonyl complex compound

synthesize. Optionally, this can also be synthesized in the further course to the metal element carbonyl complex Ru ₃ (CO) i ₂ . In general, a metal element can with charge number X with n carbon monoxide molecules

connect so that the 18-electron rule is satisfied. The synthesized metal element carbonyl complex may be in the form ^x dm (CO) ", where x is the mass number of the respective isotope, m is the number of the respective isotopes

 Metal element atoms (d) in the metal element carbonyl complex and n represents the number of carbon monoxide ligands (CO) in the metal element carbonyl complex. The number m of the respective metal element atoms and the number n of the carbon monoxide ligands may each be any natural number including "one".

In the case of m> 1, a polynuclear metal element carbonyl complex is present. Examples of metal elements which typically preferentially form polynuclear metal element carbonyl complexes are in particular

Metal elements from the 7. Group of the Periodic Table, so in particular rhenium and technetium, for example in the form of the isotopes rhenium-188 ( ¹⁸⁸ Re) or technetium-99 ( ⁹⁹ Tc).

For example, in the case of rhenium, preferably 2 rhenium nuclei with 10 carbon monoxide molecules synthesize a ¹⁸⁸ Re ₂ (CO) 10, with two square-pyramidal ¹⁸⁸ Re (CO) ₅ sub-nuclei joined together via a metal-metal compound. In the case of

Technetiums synthesize preferably 2 technetium nuclei and 10 carbon monoxide ligands to ⁹⁹ Το ₂ (00) ιο, with a similar to the rhenium geometric design.

In general, metal elements of the 6. and 8. Group of the Periodic Table preferably mononuclear Metal element carbonyl complexes, whereas metal elements of the 7th group have an odd number

Valence electrons preferably form polynuclear metal element carbonyl complexes. The number of cores (metal elements) per metal element carbonyl complex which is preferred for a respective element usually results in compliance with the 18-electron rule for the respective metal element.

The synthesized metal element carbonyl complexes, for example, do not adhere or only briefly adhere to surfaces, and therefore have a high volatility. As a result, the metal element carbonyl complexes are suitable for transport and can also be used over greater distances, e.g. by

Transporting utilities such as hoses or pipes are transported.

Of great advantage with this procedure is that the

Synthesis of the metal element carbonyl complexes directly from molecular carbon monoxide gas and the metal elements can proceed successfully at moderate conditions without intermediate reaction. The method can be carried out at a temperature in the interval between 50 and 600 K and at one pressure

be realized between 0.00005 to 200 bar. A special feature, however, is that the procedure at a

Temperature in the interval between 200 and 400 K and

particularly preferably at a temperature in the interval between 250 to 310 K can be performed. Also preferably, the process can be carried out at a pressure in the interval between 0.005 to 20 bar and more preferably at a pressure in the interval between 0.1 to 10 bar. The carbonyl complex synthesis can also take place in ordinary room conditions, ie at a Temperature of about 290 K ± 10K and at one

Total gas pressure of about 1 bar + 0.5 bar, the

Atmospheric pressure accordingly. In the synthesis chamber, the carrier gas can be next to the

Carbon monoxide contain a non-reactive and thus inert gas component. The proportion of non-reactive gas may vary depending on the structure of a device used. Preferably, the inert gas

For example, be helium or N ₂ . Essentially, the non-reactive gas constituent serves for moderation of the metal elements to be transported in the reaction volume of the synthesis apparatus. As a result, the metal elements of higher kinetic energies, these after their

Generation can be decelerated to a carrier gas adapted energy. This allows the

Probability of synthesizing the

Metal element carbonyl complexes are increased. This allows the emitted from a target

 Metal elements are moderated by the carrier gas particles. The efficiency of moderation depends in particular on the mass ratio of the particles involved. In this case, by selecting the carrier gas particles, the proportion of carbon monoxide to the carrier gas, the

Adjustment of pressure and / or setting of

Temperature of the carrier gas, the moderation targeted

to be influenced. Thus, the yield and the

Selectivity of carbonyl complex synthesis targeted

to be influenced. In particular, in the cases where it is apparent from the production conditions that the metal elements produced are already thermalized, or can be thermalized by the carbon monoxide alone, the carrier gas may also consist entirely or at least substantially of carbon monoxide. By thermalizing is meant that the energy of the metal elements of the kinetic energy of the

 Carrier gas particles substantially corresponds. But it is also possible a high proportion of carbon monoxide with, for example, a minimum proportion of preferably 95%,

particularly preferably provide 99% in the carrier gas.

Depending on the geometry chosen, the ion beam, the energy of the repulsive nuclei, and the nature of the other gases in the carrier gas, a lesser amount of carbon monoxide may be sufficient to form the complexes. The proportion of carbon monoxide here can be well below 50%.

The carbon monoxide-containing carrier gas may be in addition to

Carbon monoxide also has another reactive

Gas component contained in the synthesis chamber.

Metal elements, carbon monoxide and constituents of the further reactive gas may optionally be added

Synthesize carbonyl complexes or compounds containing carbonyl complexes. By adjusting the further reactive gas component may preferably the

Moderation and / or the selectivity of the carbonyl complex synthesis can be influenced.

The reaction volume can be in the synthesis chamber

to be provided. In addition to shielding purposes, the synthesis chamber can allow a targeted gas flow of the carrier gas. By means of a supply line, so for example a hose made of polyethylene or a pipe made of copper, can the gas into the synthesis chamber and that in it

be housed reaction volume. With simple hose connections or pipe flanges in addition to the

Lead also a transport line to a

Outlet opening, in particular a gas outlet of the

 Be attached to the synthesis chamber. At this outlet then the carrier gas can flow out. With the carrier gas can

also the metal element carbonyl complexes leave the synthesis or reaction chamber and by means of a gas transport line connected to the reaction chamber to a location remote from the place of production of the metal elements

be transported. At the remote location, the metal elements (in carbonyl complex form) can be detected, assayed, and / or further used. A transport of atomic

 Metal elements, ie those not in the form of

Carbonyl complexes, however, so far, except for mercury (Hg), has not been detected and is very unlikely, in particular almost not feasible. This therefore, since they are less volatile and if they do not already adhere to the wall of the synthesis chamber, will adhere to the gas transport line within a very short time and thus can not be carried along with the gas stream.

The provision and transport of the metal element carbonyl complexes is thus carried out in a gas phase flow-through process. Thus, advantageously, only the transfer of the generated in the reaction chamber

Metal elements in metal element carbonyl complexes one

Transport this allow. The material selection of the gas transport line used can have an influence on the transport of the

Metal element carbonyl complexes have achieved yield. There are generally a variety of simple materials for use as a gas transport line conceivable. In particular, simple plastics such as polyethylene (PE) or polytetrafluoroethylene (PTFE) can be used as a material for a gas transport line. In some cases, the choice of the material of the gas transport line can be dependent on the radiation resistance of the respective material, since it can be guided at least partially in a region in which a greatly increased

 Radiation exposure may be present. At the place of use of the generated elements, in particular the radioactive

Elements can thus have little or even none

additional radiation exposure is present. The length of the gas transport line may therefore preferably be just selected in such a way by a

 Radiation shielding device, for example, a sufficiently thick concrete wall to be able to be passed through.

The gas flow through the respective lines can be adjusted by various settings. In particular, the delivery rate of the carrier gas may be the

 Can directly influence flow velocity,

be set. The flow rate of the individual

Carrier gas components can be adjusted individually at each gas source. As a gas source for each component of the carrier gas may typically serve a compressed gas cylinder to which a pressure reducer may be connected. This can be an individual mass flow control guarantee. The adjustment of the flow rate can be adapted to the structural geometry, such as the diameter or the length of the installed cables, on the one hand. On the other hand, the flow rate adjustment can also be adapted to the average life of the metal elements. This can be radioactive in terms of their

Decay probability, very short lived metal elements may be transported at higher flow rates than less short lived metal elements to reach the transport destination, the remote location. Furthermore, the flow rate to be set can also be dependent on which

Flow rate optimal capture of the

Metal elements is ensured by the carrier gas. In general, the flow rate can be set in a range between 1 ml / min and 10 1 / min in order to adjust the gas flow to these conditions.

It can be used to produce the metal elements

physical reaction can be used. Here, for example, an object called Target, from a

Radiation source irradiated, thereby activated and in a reaction, in particular a nuclear reaction, the

Metal elements are generated. A nuclear reaction can be, for example, a nuclear fission, a nuclear fusion process or a nuclear decay.

In the case of nuclear fission, this can be induced in particular by neutrons. For example, the neutrons can be generated in a nuclear reactor. In this case, thermal neutrons can preferably be used. These conditions may be, for example, on Research Reactor TRIGA Mainz at the Johannes Gutenberg University in Mainz.

Furthermore, the metal elements may be fused by using particle beams, in particular a

 Particle or ion accelerator can be generated. A particle accelerator is especially one

Linear accelerator, a synchrotron or a cyclotron. The particle or ion beams, for example, in facilities such as the GSI Helmholtz Center for

 Schwerionenforschung GmbH in Darmstadt / Germany. The special requirements for the radiation needed to produce the desired

Lead metal elements are known per se. The target is thus with, for example, hadron-containing

 Radiation, i. with hadrons themselves (e.g., neutrons) or hadrons-containing particles (e.g., ions). For example, it is also possible to use photons or

To use electron-induced radiation.

The material of the target is preferably selected according to which metal elements are to be produced. As a material, for example, actinides, in particular the

various fissile elements such as uranium, plutonium or Californium or objects containing these materials can be used. The materials uranium,

Plutonium or Californium have one in each

the material's own likelihood of a particular element, including the desired metal element such as

For example, molybdenum, technetium, rhenium, rhodium or

To produce ruthenium. Since the ranges of the metal elements produced are relatively short, the area in which the generated metal elements are expected to be flooded directly with the carrier gas. Especially since the

Individual particles in contact with a physical

Object with high probability can adhere directly to this, so they can not be picked up and / or transported by a carrier gas. In particular, the target can be lapped directly by the carrier gas, in order to avoid contact of the elements produced, in particular the refractory metal elements, for example, with the outer skin of the synthesis chamber, before this with the

Carbon monoxide molecules can be synthesized to metal element carbonyl complexes. This can be the

Increase the yield of the synthesis of the metal element carbonyl complexes.

The range of the metal elements produced can

in particular as a function of the energy of the radiation, by selection of the target and by pressure and

 Composition of the carrier gas can be influenced.

The conditions (in particular gas type, gas mixture, temperature, pressure and / or size of the

Synthesis chamber) chosen so that the range of

Metal elements such that at least 5% of

produced metal elements in the synthesis chamber by means of the carrier gas moderated, so slowed down, are. More preferred, however, more metal elements by means of

Carrier gases moderated as by too long range

get lost. Particularly preferred is the range of

Metal elements influenced such that at least 98% of the metal elements in the synthesis chamber by means of Carrier gases can be moderated to allow the highest possible yield for the subsequent transport of the metal elements. Preference is given to the production of metal elements which are for the most part short-lived, and those which are extremely short-lived, for example from the group of transactinoids. The

Half-lives of the short-lived refractory metal elements are typically less than 10 minutes, those of the extremely short-lived in the range below 100 milliseconds. When the metal elements decay, they emit radioactive radiation. This radioactive radiation of the radioactively decomposing metal elements can be measured by means of a radiation detector in a detection device. If the detector is connected downstream to the transport line connected to the synthesis chamber, the existence of the metal elements, in particular in the form of the metal element carbonyl complexes at the point of decomposition, can prove beyond doubt the transport location by means of the carrier gas.

The metal elements are preferably radioactive

Properties. For example, the presence of a well-defined half-life allows for different ones

Method of verification, to which the

Description will be received, as well as various applications for metal element transport. Thus, applications for the metal element transport according to the invention can be found, for example, in tribology, in radiochemistry and in nuclear medicine. The place of use may then be, for example, a room in which people can stay, for example a treatment or therapy room. The metal elements can then be in the room or the therapy room of her

Use be supplied.

For example, in the field of nuclear medicine, for example in a scintigraphic examination, for example of the skeleton, lung, thyroid, kidneys, heart and tumors, it may be of considerable advantage to use as short-lived radioactive materials as so-called

radioactive "markers" (tracers)

Carbonyl complex formation are brought over the Gastransportiertung in the vicinity of the patient, the lowest possible radiation exposure of the patient can be achieved. It can therefore be used exactly to the purpose of the investigation tuned radioactive isotopes.

At the same time can radiation exposure of the patient

be significantly reduced.

Preference is given to metal elements, in particular refractory metal elements by means of the above-described

Transfer process into the gaseous phase. Thus, it is preferably possible metal elements, in particular

to transport refractory metal elements. The metal elements to be transported are preferably elements from the Nebengrup s, ie the d groups of

Periodic Table. However, it may also be metal elements from the range of the main groups of the periodic table, which can be transported in the gaseous phase by means of the described method. This can be, for example Indium, tallium or germanium. Furthermore, the elements of the actinides and lanthanides can be transported by the described method. Refractory metal elements from the d-groups of the Periodic Table may in particular be ruthenium, iridium, rhodium, osmium, rhenium, molybdenum, tungsten or technetium, in particular radioactively decomposing isotopes of these elements.

The method shown preferably operates selectively. The selection of a particular metal element from a number of generated or existing metal elements is done depending on various process parameters. For example, by setting the

Carbon monoxide content of the carrier gas and / or the

Delivery rate of the carrier gas can the selectivity of the

 Transport process can be influenced. Furthermore, the particle number resulting from the probability of generation of the chosen target material can also have an influence on the selectivity of the metal element carbonyl complex synthesis. This can already prefer the emergence of a selected metal element with the right choice.

For generating and providing metal elements in gaseous phase, a reaction volume is defined in which the metal elements with the carbon monoxide of the carrier gas to metal element carbonyl complexes

can synthesize. In the case of the carbonyl complexes formed, the synergistic sigma-donor / pi-acceptor interactions of the carbon monoxide with the carbon monoxide

Metal element can be achieved a special stability. These interactions make electrons of the filled sigma orbital of carbon monoxide in

 symmetry-equivalent orbitals of the metal element and filled orbitals of the metal element are shifted into empty pi orbitals of the carbon monoxide multiple bond. This electron delocalization calls for an energetic

 Stabilization. This is also called "nephelauxetic effect".

The structure of the synthesized metal-element carbonyl complex is predicted primarily by the VSEPR model and the 18-electron rule. Carbonyl complexes with several or even different metal elements are due to the density of the metal element particles in the

Reaction volume unlikely, but should not be excluded. The resulting carbonyl

Depending on the metal element, for example, complex symmetry may be tetrahedral, trigonal-bipyramidal,

octahedral. In the case of the synthesis of two

However, metal element particles in a metal element carbonyl complex may also have symmetry, for example

double trigonal-bipyramidal staggered or staggered octahedrally twice. The metal elements

For example, the 6th group preferably form hexacarbonyl complex compounds, those of the 8th group, due to the 18-electron rule

Pentacarbonyl complexes. The molybdenum metal element of the 6th group forms, for example, a high probability of hexacarbonyl complex compound in the form of ¹⁰⁴ Mo (CO). ₆ Here, six carbon monoxide molecules synthesize with a ¹⁰⁴ Mo to form a metal element-carbonyl complex in

Form of a Mo carbonyl complex with octahedral

Symmetry. The reaction volume can be accommodated in a device in a synthesis chamber, which also has a supply line for providing and initiating the

carbon monoxide-containing carrier gas to the carrier gas and the generated in the synthesis chamber or introduced into the synthesis chamber metal elements in

Combine reaction volume. The synthesized metal element carbonyl complexes are thus in the

Synthesis chamber provided by the carrier gas provided for transport and can be discharged via an outlet with the carrier gas from the synthesis chamber. Since the production of the metal elements is often high

Radiation pollution may accompany the removal of the metal elements from the place of origin to a

Radiation-proof place of use appropriate.

The reaction volume is in particular always with

rinsed inflowing carrier gas, so that a steady

Flow can be generated with which the metal element carbonyl complexes can be carried. In particular, with a suitable choice of the synthesis chamber geometry, in such a flow mode, the entire reaction volume can be continuously rinsed with the fresh incoming carrier gas in order to avoid stationary flow areas.

The production of the metal elements is done in particular by a target of fissile material, which is irradiated by a radiation source and activated. The metal elements can therefore be directly in the process

or directly before the carbonyl synthesis and the transport process are generated, in particular in or near the synthesis chamber. In an induced

Nuclear fission reactions can give rise to many different core fragments and thus, and through their further decay processes, an additional nuclear fragment

Radiation exposure present. Accordingly, it is also possible to transport or use primary nuclear reaction products, in particular fission products. Due to the usually short ranges of the metal elements, it is still appropriate to use the target directly in the

Synthesis chamber to install. The target can also be attached outside the synthesis chamber.

To shield other, especially heavier

Core fragments that do not correspond to the desired metal element may preferably have a target

Target cover be attached, which of the

Metal elements can be penetrated without too much loss of yield. The target coverage can be selected so that it can retain heavier fission fragments than the metal elements. Accordingly, through

Selecting the target cover material and / or adjusting the thickness of the target cover increases the selectivity of the target cover penetrating metal elements from the resulting core fragments.

For the passage of the target activating radiation, the synthesis chamber can be provided with an entrance window. This can be constructed in such a way that the respectively used radiation directed to the target, in particular thermal neutrons or accelerated ions, can pass. For example, the entrance window can be a Mylar film, which in particular only a few

Microns has thickness. For detecting the metal elements, the

provided metal element carbonyl complexes are passed through a Transportieitung and fed to a detection device. The detection device can

For example, a catcher for filtering and collecting the metal element carbonyl complexes from the

Carrier gas stream, in which the metal elements

decay radioactively. Furthermore, the detection device may comprise a detector which detects the decay of the

 Detects metal elements resulting radioactive radiation.

To determine the adsorption enthalpy of the metal element carbonyl complexes, the provided

Metal element carbonyl complexes also by a

Directed transport line and then a

Gas Chromatograph be supplied. A per se known gas chromatograph comprises a gas chromatography column through which the gas stream is passed with the metal elements. The gas chromatography column may further include a

Have cooling device.

In the following the invention is based on

 Embodiments and explained in more detail with reference to the figures, wherein the same and similar elements are partially provided with the same reference numerals and the features of the various embodiments can be combined. Independent of

In the summary of the patent claims, further features, details and / or advantages can be derived from the exemplary embodiments. Brief description of the figures

 Shown schematically are: FIG. 1 a basic structure of a schematic

 represented synthesis chamber for synthesizing the metal element Carbony1-Kom 1exe;

Fig. 2 shows another exemplary construction of a

 Device with a radiation source; Fig. 3 shows a further device structure with

 bending magnets;

 4 shows an exemplary device structure with a

 Radiation source of the research reactor TRIGA Mainz for the proof of the synthesis of the

 Metal element carbonyl complex synthesis after yours

Transport;

 5 shows another exemplary construction of a

 Device with the radiation source of the research reactor TRIGA Mainz for determining the adsorption enthalpy of the metal elements-carbonyl-

Complexes after their transport;

 6 shows an exemplary construction of a synthesis chamber for synthesizing the metal element carbonyl complexes;

Fig. 7 is a flow chart for the inventive

 Process for providing and transporting metal element carbonyl complexes in gaseous phase;

 Fig. 8 is a gas flow diagram with a closed

Gas loop; 9 shows a relative transport yield of refractory metal elements as a function of

 Carbon monoxide content in the carrier gas;

 Fig. 10 shows a relative transport yield of refractory

 Metal elements depending on the

Delivery rate of the carrier gas;

 11 shows a dependence of the transport yield on the pressure in the target chamber for a pressure range in the approximate range of the normal conditions;

Detailed description of the figures

 FIG. 1 shows an embodiment of a synthesis chamber 14. In the embodiment shown in FIG. 1, the synthesis chamber 14 has two inlet openings 46 which can each be connected to a supply line 10. The carrier gas may consist of those not shown in FIG

Compressed gas cylinders 2, 4 are mixed and is connected via the with the inlet 46 of the synthesis chamber 14

Supply line 10 of these supplied. The synthesis chamber 14

includes a reaction volume 58 in which the carrier gas and metal elements 55 are combined to facilitate the synthesis of the metal element carbonyl complexes

enable. The carbon monoxide gas is in the

Embodiment of the invention with "CO" symbols

clarified. To produce the metal elements 55, the synthesis chamber 14 comprises a target 54. The target 54 preferably contains fissile material, in particular uranium, plutonium or californium, in order to produce metal elements 55 during a nuclear reaction, for example an induced nuclear fission. In use, when the synthesis chamber 14 is attached to, for example, a measuring station 64, the

Synthesis chamber 14 and in particular the target 54 are irradiated with a radiation 60. In the shown

Embodiment, the target 54 is placed in the synthesis chamber 14. The radiation 60 penetrates the wall 52 of the synthesis chamber 14 at a location provided for this purpose, the inlet window 53. The flow path of the carrier gas at the inlet 46 is symbolized by the arrow 40. The arrow 42 shows the

Flow of the carrier gas at the outlet 48th

The synthesis of the metal elements is briefly described below. The metal elements generated and emitted by the target 54 are defined by the components of the

Carrier gas in the synthesis chamber 14 thermalizes, which increases the likelihood of synthesizing

Metal element carbonyl complexes enlarged. The

Metal elements synthesize in reaction volume 58 with the carrier gas to metal element carbonyl complexes. The synthesized metal element carbonyl complexes are entrained to the outlet 48 by the gas flow of the carrier gas, appearing in the direction shown by the arrow 42

Flow direction from the synthesis chamber 14 and flow with the carrier gas into the transport line 12 connected to the outlet 48. Thus, the metal elements in the form of the metal element carbonyl complexes at the outlet 48 of the synthesis chamber 14 for transport and then for use away from the synthesis chamber 14

provided. The place of use may be so far away due to the created transport that he is not or at least considerably less radiated. A pressure sensor 51 is attached to the synthesis chamber 14 for measuring the pressure in the reaction volume.

Due to the cross section for the metal element carbonyl complex synthesis in the reaction volume 58, individual metal elements can pass through the carrier gas without being synthesized into metal element carbonyl complexes. These are usually adsorbed by the wall 52 of the synthesis chamber 14. Otherwise, these are adsorbed at the latest in the transport line 12.

FIG. 2 shows a further embodiment of a

Transport device for the gas phase transport of

 Metal elements, wherein the target 54 is disposed outside of the synthesis chamber 14. The production of

Metal elements 55 outside the synthesis chamber 14th

optionally allows a separation of

Primary radiation 60 from the metal element "radiation" 55 generated from the target 54. Also, separation of the metal element "radiation" 55 of others is also involved

Nuclear reactions resulting particles can be achieved. The entrance window 53 allows in this

Embodiment, the passage of the metal elements 55 in the synthesis chamber 14 and the housed therein

Reaction volume 58. The further construction of the apparatus is in accordance with the synthesis chamber 14 described with reference to FIG.

FIG. 3 shows a further embodiment of a

Device for transporting metal elements in the Gas phase with an arrangement of the synthesis chamber 14. The target 54 is arranged as in the structure described with Figure 2 outside the synthesis chamber 14 and can be irradiated with the radiation 60, in particular particle radiation. Ablenkmagnete 61 act on the location of the target 54 with a deflecting force.

Particles moving in the magnetic field of the deflecting magnets 61 are deflected by their deflecting force depending on various particle parameters such as mass and charge number.

By means of the radiation 60, for example radiation 60 having thermal neutrons or ions, the target 54 is irradiated, wherein the radiation 60 at least partially penetrates the target 54. This penetrating radiation is shown as "primary radiation" 60 with a little curved arrow in Figure 3. This radiation 60 is little influenced by the deflection magnets 61 in their direction, it does not strike the synthesis chamber 14. The metal elements 55 produced in the target 54, on the other hand, become is deflected by means of the magnetic field in the direction of the synthesis chamber 14. The magnetic field of the deflection magnets 61 is preferably matched to the desired metal elements 55

Field strength set. This leads to a separation of the generated metal elements 55 from the radiation 60.

FIG. 4 schematically shows an exemplary structure of a device for generating, providing, transporting and measuring refractory metal elements. This is at a nuclear reactor 18, in this example the

Research reactor TRIGA Mainz of Johannes Gutenberg University in Mainz, which is shown in a longitudinal section, grown to use the thermal neutrons generated there for the neutron-induced cleavage of a target 54.

The reactor core 16 generates and thermalises the neutrons, which are then made available to four different measurement sites 64, in the case shown. The synthesis chamber 14 shown in more detail in FIG. 4 is installed at one of the four measuring stations 64.

A carrier gas is in the case shown by a

Carrier gas source 3 delivered. The carrier gas source comprises a carbon monoxide gas bottle 2 and a

Inert gas bottle 4. In this example, the

Inert gas cylinder 4 N ₂ gas as an inert gas. The

 Mixing ratio between the carbon monoxide gas and the inert gas can be adjusted to the gas cylinders 2 and 4, respectively, by means of the mass flow controllers 6 and 8. Via a supply line 10, the carrier gas mixture for

 Synthesis chamber 14 out. The process within the

Synthesis chamber 14 is explained in more detail in particular with reference to FIG 4. Optionally, depending on the requirement in the

Substantially pure carbon monoxide gas from the

Carbon monoxide gas cylinder 2 or so a mixture of carbon monoxide gas and inert gas from the

Carbon monoxide gas cylinder 2 and the inert gas cylinder 4, are fed into the supply line 10. About one with an outlet 48 of the synthesis chamber 14th

connected transport line 12 may be the carrier gas which contains the synthesized in the synthesis chamber 14 Metallelement- Carbonyl complexes containing a remote from the place of production of the metal elements in the synthesis chamber 14 structure 15 in the form of a detection or measuring device to the side facing away from the synthesis chamber 14 end 13 of

Transport line 12 are supplied.

An exemplary structure 15 in the form of a

Detection device is in Figure 1 to that of the

Synthesis chamber 14 remote end 13 of the transport line 12 is connected. At the end 13, a filter 34 is arranged, by means of the filter 34, the metal element carbonyl complexes produced are filtered from the carrier gas stream. The filter 34 consists for example of a simple

Collecting tube, which is filled with activated carbon. A detector 20 is in this embodiment above the

Filters 34 arranged. The detector 20 may be a germanium gamma detector. By means of the detector, the

radioactive decay radiation of short-lived

Metal elements are measured. This can be a

Decay frequency can be obtained. With a

 Evaluation system 62, the transport yield can be determined. A gas pump 30 is in the flow direction of the

Carrier gas seen behind the filter 34.

By means of the gas pump 30, a controlled removal of the carrier gas can take place in order to prevent a possible gas flow and to keep the gas flow constant. Of the

Downstream of the gas pump 30, the carrier gas is led to the exhaust air 31. A further embodiment of the invention for the structure 15 'connected to the end 13 of the transport line 12 facing away from the synthesis chamber 14 in the form of a Measuring device, in this example a gas chromatograph

21, is shown in FIG. The used

 System components are up to the end 13 of the transport line

12 identical to the system described in Figure 1. At the end 13 then the structure 15 ', here a

 Gas Chromatograph 21, connected. This comprises a gas chromatography column 22 with a cooling device 24 and a coolant reservoir 26. Ein mit dem

Gas chromatograph connected furnace 32 allows a more accurate setting of a temperature gradient along the gas chromatography column 22. A detector 20 'is arranged longitudinally displaceable on the gas chromatography column 22. The detector 20 'may be, for example, a germanium gamma detector. In principle, any detector that detects a radioactive radiation is suitable. The detector 20 'measures the decay frequency distribution of the radioactive metal element decays along the gas chromatography column

22. The one end of the cooling device 24, which from the end

13 facing away from the transport line, is connected to the

Coolant reservoir 2 6 connected. The other end of the cooling device 24, which the end 13 of the

If necessary, with an oven 32. Along the gas chromatography column 22 forms during operation of the gas chromatograph 21, a temperature gradient from. This corresponds to a thermochromatography apparatus.

The structure 15 ', viewed in the direction of flow of the carrier gas behind the structure 15', in particular the

Gas chromatography column 22, a throttle valve 28 and a gas pump 30 on. The throttle valve 28 regulates the pressure of the carrier gas, a gas pump 30 carries the remaining carrier gas to an unspecified exhaust device 31st Optionally, both structures 15, 15 'can also be constructed serially, by referring to the aforementioned

Thermochromatograph 21 of Figure 3 the

Detection device 15 from Figure 1 connects. If a plurality of detectors 20, 20 'is used, those in the gas chromatography column 22 may not

adhering metal elements in the downstream filter 34 are detected.

The structures 15, 15 'shown in FIGS. 4 and 5 in the form of detection or measuring devices are exemplary. It may there also a different kind used as evidence or measuring apparatus used construction or apparatus for further use of the metal elements produced or be integrated and connected to the end 13 of the transport line 12 to the

to detect, experimentally investigate or otherwise use metal elements provided and transported.

FIG. 6 shows a further embodiment of the

Synthesis chamber 14 in a cross section. The reference numbers used correspond to those of the previous ones

Embodiments match.

Under the target 54 is a ring distributor 43 for the

Carrier gas arranged, which the carrier gas around the target 54 distributed around in the synthesis chamber 14 admits. The flow path of the carrier gas at the inlet 46 is symbolized by the arrow 40. The arrows 44 symbolize a rotationally symmetrical distribution of the carrier gas around the synthesis chamber 14 and the entry of the carrier gas in the reaction volume 58th

On the target 54 in this example is a

Target cover 56 attached. The target cover 56 may comprise further, in particular heavier, fission products, which may be formed in the target 54 in the case of nuclear reactions such as induced nuclear fission, from the reaction volume 58

hold back. The material of which the target cover 56 consists, or which has the target cover 56, will be based on the target material and the desired

Selected metal elements. For example, the

Target cover 56 made of aluminum. A pressure sensor 51 is connected to a port 50 in this embodiment. The pressure sensor 51 allows the adjustment of the gas pressure in the synthesis chamber 14. Also, the synthesis chamber 14 shown in Fig. 6 can

For example, in the devices of Figures 4 and 5 are used. The synthesis chamber 14 has an inlet 46 which is connected to a supply line 10 and with a

Carrier gas source 3 can be connected. The carrier gas may be introduced via the inlet 46 into the synthesis chamber. The synthesis chamber 14 also has a reaction volume 58 in which the carrier gas and the metal elements in

Operation of the synthesis chamber 14 are merged to the synthesis of the metal element carbonyl complexes

enable. In order to produce the metal elements, the synthesis chamber 14 likewise comprises a target 54. The target 54 is in the synthesis chamber 14 in the example shown

arranged. It can also be outside the synthesis chamber 14, preferably in the direction of the source of the radiation 60, be arranged.

The flow path of the carrier gas is symbolized by arrows, wherein at the inlet 46 of the arrow 40

 Inflowing of the carrier gas in and at the outlet 48 of the arrow 42 symbolizes the outflow of the carrier gas with metal element carbonyl complexes from the synthesis chamber 14. The carrier gas passes between the inlet 46 and outlet 48, the reaction volume 58th

In particular, when the synthesis chamber 14 is attached to a measurement site 64, or other irradiation site for hadron-containing radiation 60, the target 54 may be irradiated with the radiation 60. As a result, metal elements can be generated and released. The process parameters of the device preferably allow the release of the metal elements to take place directly in the gaseous phase. On the target 54 of the embodiment shown in Figure 6, a target cover 56 is attached.

In particular, the target 54 may also be configured such that the target cover 56 is included in the target 54. Also, use of the entrance window 53 as

Target cover 56, especially in the case of a

Attachment of the target 54 outside the synthesis chamber 14 is possible.

FIG. 7 shows a flow chart for the method according to the invention for providing and transporting

Metal element carbonyl complexes in gaseous phase. FIG. 8 shows a flow chart of the gas flow. In the embodiment shown, this is a closed circuit, so that the carrier gas circulates between feed line 10, the synthesis chamber 14 and transport line 12.

The carrier gas taken from the carrier gas bottles 2, 4 and adjusted by means of the mass flow controllers 6, 8 is supplied to the circuit in order to fill the circuit and / or to compensate for gas loss. By means of the mass flow controller 7, the mass flow is measured with the pressure regulator 9, the pressure in the circuit and / or adjusted.

The optionally produced in the synthesis chamber 14

Carbonyl complexes are eliminated by means of the filter device 34, the carrier gas then dried in a dryer 11, whereby a multiple use of the

same amount of gas can be made possible. The carrier gas is therefore recirculated. By means of valves 29, the desired gas flow path is adjustable. Thus, for example by means of a gas pump 30, the carrier gas can be sucked and / or the supply and transport lines 10, 12 before

Use be evacuated. After evacuation, the gas pump 30 can be separated from the gas flow path by means of the valve 29. It is also possible in the supply line by means of a valve 29 further, possibly other carrier gas supplied to the gas flow path.

FIG. 9 shows that with the one shown in FIG

Arrangement measured yield of metal element transport depending on the mixing ratio of the

Carbon monoxide with the inert gas N ₂ . There were those with Counting rates measured by the detector 20, 20 'and the

Settings of Massenflussregier 6 and 8 recorded and evaluated with the evaluation device 62. The decay frequency measured by the detector 20, 20 'is plotted in FIG. 7 via the mixing ratio, ie the quotient of the values of the two mass flow controllers 6, 8. The total delivery rate of the gas mixture is for each

Measuring point 500 ml / min. The ratio of the indicated on the abscissa carbon monoxide flow with the

Total delivery gives the proportionate mixture size of the carbon monoxide gas. The ordinate shows a corresponding transport of metal elements normalized to such a corresponding metal element transport by potassium chloride. As can be seen from FIG. 9, the yield obtained is a multiple of the yield obtained when using

 Potassium chloride would have been expected. FIG. 9 shows the results for four refractory metal elements with two measurement series each. Two each for technetium, molybdenum, ruthenium and rhodium.

FIG. 10 shows the yield of metal element transport as a function of the delivery rate of the carrier gas. Again, a structure has been used which corresponds to that shown in Figure 4. For the data acquisition, the detector 20, 20 'and the mass flow controllers 6, 8 are recorded and the data are evaluated by the evaluation device 62. The abscissa here shows the carrier gas flow in ml / min, the ordinate on a transport with potassium chloride

standardized transport yield of the carbon monoxide-containing carrier gas. As the delivery rate depends on the

Construction geometry is, is a suitable for each structure setting the flow rate for maximization adjusted the yield. FIG. 10 shows the results for four refractory metal elements technetium, molybdenum, ruthenium and rhodium. FIG. 11 shows the yield of the metal element transport as a function of the set pressure of the carrier gas in the range from 1000 to 1500 mbar. The ordinate is again normalized to a conventional transport with

Potassium chloride. Here are results for four

Refractory metal elements technetium, molybdenum, ruthenium and rhodium shown.

It will be apparent to those skilled in the art that the above-described embodiments are to be understood by way of example, and that the invention is not limited to them, but that they can be varied in many ways without departing from the invention. Furthermore, it will be understood that the features, independently as they are disclosed in the specification, claims, figures or otherwise, also individually define essential components of the invention, even if described together with other features.

LIST OF REFERENCE NUMBERS

 2 carbon monoxide gas pocket

 3 carrier gas source

 4 inert gas bottle

 6 mass flow regulator of carbon monoxide gas cylinder

7 mass flow controller

 8 mass flow controller of the inert gas bottle

 9 pressure regulator

 10 supply line

 11 dryers

 12 transport line

 13 Far end of the transport line

 14 synthesis chamber

 15 construction

 15 'construction

 16 radiation source (e.g., reactor core)

 18 nuclear reactor

 20 detector

 20 'detector

 21 gas chromatograph

 22 gas chromatography column

 24 cooling device

 26 Cooling reservoir

 28 throttle valve

 29 valve

 30 gas pump

 31 exhaust air

 32 oven

 34 filters

 40 flow direction arrow at the inlet

42 Flow direction arrow at the outlet 43 ring distributor

 44 Flow direction arrow when flowing into the reaction chamber

 46 inlet

48 outlet

 50 connection

 51 pressure sensor

 52 conversion

 53 entrance window

54 Target

 55 metal elements

 56 Target coverage

58 reaction volume

 60 radiation (e.g., neutrons, ions)

61 magnet

 62 evaluation device

 64 measuring station

Claims

Claims: A method of providing gaseous metal elements in a carrier gas,  wherein the carrier gas contains carbon monoxide, wherein the carrier gas and the metal elements are combined in a reaction volume (58), and  wherein the metal elements and the carbon monoxide synthesize Meta11e1ement-Carbony1 Kom 1exen. 2. The method of claim 1, wherein the metal elements in the 4th to 10th groups of the periodic table or the d-groups of the periodic table are included. 3. The method according to claim 1 or 2,  wherein the carrier gas is a mixture of Contains carbon monoxide gas and at least one non-reactive gas component. 4. The method according to claim 1 or 2,  wherein the carrier gas consists essentially of Carbon monoxide gas exists. 5. The method according to any one of the preceding claims,  wherein the reaction volume (58) for the synthesis of Metal element carbonyl complexes in a synthesis chamber (14) is housed,  wherein the carrier gas is conducted by means of a feed line (10) into the synthesis chamber (14) and  wherein the metal element carbonyl complexes with the Carrier gas at an outlet (48) of the synthesis chamber (14) for be provided further use. 6. Method according to the preceding claim,  wherein the metal element carbonyl complex synthesis in the synthesis chamber (14) at a temperature in the interval between 50 to 500 K and a pressure in the interval between 0.00005 to 200 bar is performed. 7. The method according to any one of the preceding claims  wherein the synthesized metal element carbonyl Complexes by means of a transport line (12) of the Reaction volume to one of the reaction volume distant location or structure (15) at the end (13) of Transport line (12) are guided. 8. The method according to any one of claims 5 or 6,  wherein the flow velocity of the carrier gas at Outlet (48) of the synthesis chamber (14) is dependent on its flow rate, which is set in a range between 1 ml / min to 10 1 / min, to transport the metal element carbonyl complexes over with the outlet (48) of the Synthesis chamber (14) to accomplish associated transport line. 9. The method according to any one of the preceding claims,  wherein the metal elements are produced by means of a target (54) and  wherein the target (54) for generating the metal elements is activated by a radiation source (60). 10. Method according to the preceding claim, wherein the target (54) is for producing the metal elements Contains actinide and / or  the target (54) is irradiated with a hadron-containing beam (60), in particular with thermalized neutrons or accelerated ions. 11. The method according to any one of claims 9 or 10,  wherein the target (54) in the synthesis chamber (14) is arranged and is washed by the carrier gas to directly receive the metal elements and the metal element carbonyl complexes of the metal elements and the To synthesize carbon monoxide molecules. 12. The method according to any one of the preceding claims,  the metal elements are short lived and  the short-lived, metal elements in their  Decay emit radioactive radiation. 13. The method according to any one of the preceding claims,  the metal elements ruthenium, osmium, rhenium, Molybdenum, tungsten, iridium, rhodium or technetium. 14. The method according to any one of claims 9 to 13,  wherein in the reaction volume (58) consists of several At least one specific element for synthesis is selected for different metal elements by selecting or adjusting at least one of the following process parameters depending on the metal element to be selected:  Proportion of carbon monoxide in the carrier gas,  Delivery rate of the carrier gas,  Carrier gas pressure in the synthesis chamber (14), - inert gas, - target material,  Target cover material,  - Target cover thickness. 15. Apparatus for generating and providing Metal elements in the form of metal element-carbonyl complexes in gaseous phase in particular to Implementation of the method according to one of the preceding claims, comprising:  a synthesis chamber (14) containing a reaction volume (58) defines  a source of metal elements (55), in particular a target (54) for producing the metal elements or produced metal elements (55),  a carrier gas source (3) with a feed line (10) for Introduction of the carbon monoxide-containing carrier gas into the synthesis chamber (14) to the carrier gas and the Metal elements (55) in the synthesis chamber (14) to synthesize and synthesize metal element carbonyl complexes from the metal elements (55) and the carbon monoxide of the carrier gas,  an outlet (48) for providing the carrier gas with the synthesized metal-element carbonyl complexes for further use. 16. Device according to the preceding claim,  wherein a direct contact of the target (54) with the carrier gas is made possible by the target (54) is lapped by the carrier gas. 17. Device according to one of claims 15 or 16, wherein the target (54) contains actinides and / or to Generation of the metal elements with hadron-containing radiation, in particular with thermalized neutrons or accelerated ions, is activated. 18. Device according to the preceding claim, further comprising a target cover (56) disposed on the side of the target (54) remote from the hadron-containing radiation (60) and having a material and thickness adapted to retain heavier fission fragments. 19. Device according to one of claims 17 to 18, further comprising an entrance window (53) for entering the radiation (60) used for activating the target (54) from the radiation source into the synthesis chamber (14),  the one used to activate the target (54) Radiation (60) contains thermal neutrons or accelerated ions and  wherein the radiation (60) is directed to the target. 20. Device according to one of claims 15 to 19, further comprising a transport line (12) for transporting the metal element carbonyl complexes to one of the Synthesis chamber (14) remote location or structure (15). 21. Use of the method according to one of claims 1 to 14 or the device according to one of claims 15 to 20 for providing metal elements for the Scintigraphy, nuclear medicine, tribology, radiochemistry or radiopharmacology.