US2064260A

US2064260A - Method and apparatus for synthesizing nitrogen compounds

Info

Publication number: US2064260A
Application number: US520923A
Authority: US
Inventors: Herrmann Ludwig
Original assignee: KURT ADAMCZICK AND WILLY LIST
Current assignee: KURT ADAMCZICK AND WILLY LIST
Priority date: 1930-03-08
Filing date: 1931-03-17
Publication date: 1936-12-15
Anticipated expiration: 1953-12-15

Description

Dec; 15, 1936. HERRMANN 2,064,260

METHOD AND APPARATUS FOR SYNTHESIZING NITROGEN COMPOUNDS Filed March '7, 1951 to be a vacuum-tube which permits the exit of Patented .Dec. 15, 1936 UNITED STATES,

METHOD APPARATUS FOR SYNTHESIZ- I ING NITROGEN COMPOUNDS Ludwig Herrmann, Frankfort-on-the-Main, Ger- -many, assignor to Kurt Adamczick and Willy List, both 0! Frankfort-on-the-Main, Germany Application March I, 1931, Serial No. 520,923

In Germany March 8, 1930 I 23 Claims.

duction of certain nitrogen compounds and means serving therefor.

In making my experiments I started from the so-called Lenard-tube. A Lenard-tube is known theelectrons or cathode-rays produced therein. For this purpose the vacuum-tube or vessel is provided with a window consisting of a thin metahfoil. Such tubes or vessels had been already used for influencing chemical reactions by the electrons or cathode-rays emitted therefrom.

In such a vacuum-tube X-rays also are produced in larger or smaller quantities.

My invention is based upon the observation that new and unexpected effects are produced if the tube is so constructed that positive rays also strike against its window. Positive rays are understood to be both the canal-rays or diacathode-rays discovered by Goldstein and the anode-rays discovered by Gehrcke and Reichenheim. I have ascertained the unexpected fact that the efiects I had observed are not produced if two vacuum-tubes are joined to a common reaction chamber, one of which tubes emits only cathode-rays through its window into the reaction chamber whereas in the other tube only canal-rays are directed against the window separating the last mentioned tube from the reaction chamber. It is on the contrary necessary for obtaining the effects characterizing my invention to produce in the same vacuum-tube or bulb both the cathode-rays and the positive rays and to direct them both against a window provided at the tube.

In the accompanying drawing some embodiments of apparatus constructed according to my invention are, illustrated which I used in carry ing out chemical syntheses.

Figure 1 is a plan view of one embodiment partly in section.

Figure 2 is a section on line A-B of Fig. 1.

Figure 3 shows schematically a reactionchamber for the production of ammonia sulphate.

Figure 4 shows a further embodiment of an apparatus for the production of positive and negative rays, partly in section.

Figure 5 shows a side elevation of the apparatus according to Fig. 4 partly in section.

As illustrated in Figures 1 and 2 the tube I is provided with five tubular extensions 2a, -2b, 3, 4 and 5 for introducing electrodes. In the upper extension 4 the leading-in conductor for the cathode 6 is arranged. The cathode 6 has a pocket 6a in which a heating-coil for heating the cathode is inserted. A circular cathodedisc id is fixed by an arm 6c to the cathodebody 6. This disc forms the cathode for the a anode I or target serving for the production of X-rays and shaped in such a manner as the anticathodes or targets of X-ray tubes for medical purposes. The bushing of the anode 1 passes the tubular extension 5; The anode l is cooled by w the cooling-coil 8. In the oblique tubular ex tension 3 is arranged the leading-in conductor 9a of a second cathode 9 which is a piercedcathode. This has a large aperture 8b in its center and small openings towards its pe- 15 riphery. The large aperture 9b serves for letting pass the electrons or cathode-rays emitted by the cathode 6. These electrons are accelerated by the two auxiliary electrodes lOa, Illb having a positive potential. The leading- 20 in conductors for these two auxiliary electrodes are arranged in the

tubular extensions

2a, 2b. Canal-rays pass through the small openings of the pierced electrode 9. The bulb l is provided with a window H which is formed by a thin 25 metal-foil for instance of an aluminium-alloy. Because of the rays passing through the window H excessive heating of the window would tend to occur. For preventing this it is cooled by a cooling-device with liquid-circuit. The cooling 3o effect of the coil I2 is sufllcient for preventing the temperature of the window II from rising to an unpermissible degree. This window iscovered by a pierced metal can I 3 cemented to a circular flange of the reaction-chamber 14. This chamber is provided with an inlet pipe I 4a and an outlet pipe Mb. A nozzle I5 is introduced into the reaction-chamber H with its mouth l6 opened against the direction of the gas-current and serving for the injection of o liquids.

The tube I being in operation and air being conducted to the reaction-chamber through the inlet pipe Ha a highly explosive gas is produced in the reaction-chamber which leaves this cham- 45 her by the outlet. pipe llb, Preferably water or hydrogen'peroxlde is injected through the nozzle I6.

I have not yet analyzed exactly the chemical combination of the gas produced by these experimerits. I was able, however, to determine with certainty that this combination is a compound or a mixture of compounds of nitrogen. This gas has been found to be an excellent fuel for interu nal combustion engines, Before feeding the combustion chamber of the engine with the gas it should be admixed with air.

If the gas produced in the reaction-chamber. It by irradiating air with positive and negative rays is led according to the Figure 3 into a second reaction-chamber Il provided with a leading-out pipe Ilo and containing ferrous sulphide (res) and water acidifled with sulphuric acid, ammonia sulphate is produced.

' For producing anode-rays in addition to canalrays the anticathode or target 'I is provided with a recess fllled with a salt causing the generation of anode-rays. Such salts are known to be salts such as sodium-, potassiumor'strontium-salts.

I cannot give an explanation of the kind of chemical influence the positive rays exert, but I presume that the cathode-rays preactivate the gases flowing through the reaction chamber I4 and that the positive rays act as a catalyst. I do not desire to limit the invention-by this theory. It may be imagined that the rays themselves exercise no direct influence upon the chemical reaction but produce accompanying secondary phenomena.

Moreover it is not at all necessary to provide in the tube I a special anticathode I for producing X-rays. In each vacuum-tubeX-rays are produced to larger or smaller extent by the cathoderays of the tube. These X-rays are sufllcient for the carrying-out of the syntheses according to my invention. In view of this I suppose that X-rays are of less importance as to the scope of my invention. On the other hand, the addition of positive rays to the cathode-rays is an essential feature of my invention whether the positive rays be merely canalor diacathode-rays or such rays and anode-rays. In making my experiments I have evacuated the bulb or vessel I-to an extremely high degree, e. g. to 10- mm. Hg, and for this purpose I leave the pump permanently joined to the bulb.

The bulb I shown in Figures 4 and 5 has two lateral tubular extensions 20., 2b provided with re-entrant portions, to which the auxiliary electrodes I00, III!) are hermetically sealed. Metal bolts I80, I81) serving as conductors are screwed to the electrodes IIIa, "lb. The upper part of the glass bulb I has two oblique tubular extensions I9 and 20. An incandescent cathode 2| surrounded by a metal cap 22 is arranged within the upper part of the extension It. An anode 23 with an opening 231: for the passage of the electrons or cathode-rays emitted from the incandescent cathode 2I is sealed to a circular re-entrant portion of the under part of the tubular extension It. These electrons are deflected by means of the auxiliary electrodes Illa, ID!) in such a manner that they strike the window II. The extension I 9 carries a small tubular extension Isa containing the leading-in conductor 23b for the anode 23. An anode 24 is sealed to the re-entrant portion of the tubular extension 20, the lower part of this extension carrying the pierced cathode 25. The openings 25a in this cathode are of small diameter, but they are many in number. The cathode 25 is put under tension by means of a leading-in conductor 25b, traversing the small tubular extension 201: of the inclined extension 20. v

A third extension 26 is arranged between the extensions I9 and 20 having a globular shape and two

tubular ends

26a, 26b. The extension 26 is cathode rays emitted from the cathode 2I and accelerated by the field of the auxiliary electrodes I0a, lob also the canal or diacathode rays leaving the openings 25a of the pierced cathode 25 are directed against this window. The cooling coil cools the window II. A similar cooling device may be provided for the target 21. A metal cap I3 is arranged below the window II, said cap having a large number of small openings. The reaction chamber I4 is shaped in. the same manner as the reaction chamber according to the embodiment of the invention shown in Figures 1 and 2. It has a leading-in pipe Ila and a leading-out pipe Mb. A nozzle I5 traverses the wall of the reaction chamber I4 the opening of which is directed against the leading-in pipe Ila, i, e. against the direction of the gas current.

Experiments carried out with canal-rays and anode rays only showed no change of irradiated air or other irradiated substances within the limits of 10- to 2 l0- mm. Hg and anode tensions between the limits of 1.5)(10 to 3.5X10 volts. In all experiments I chose the tensions for the heating of filaments of the cathodes to be about 4 to 6 volts.

In other experiments made under the same conditions I investigated the influence of X-rays on atmospheric .air and other substances but I could not ascertain any chemical change of the substances irradiated only by X-rays. They had been only ionized by the x-rays.

Further experiments I carried out with cathode rays only, but'with these experiments the occurrence of X-rays naturally could not be prevented. They showed a yellow flash up of the irradiated air i. e. its nitrogen, continuing about thirty seconds after irradiation and then disappearing. This phenomenon could be ascertained with a vacuum of 8.3x 10- mm. Hg and a tension of 1.5 (10 volts.

After canal rays and/or anode rays were added to the cathode rays and X-rays the flashing up disappeared and the substances irradiated pro-' duced a chemical compound, the constitution of which I have not yet been able to determine but which is characterized by a great explosive force.

Although I have referred to the electrodes in the apparatus herein-before described as anode and cathode I wish to state that this has been done only for the sake of simplicity. In fact some of the electrodes are entitled to have a multiple function. For avoiding any misunderstanding I have inserted in the following schedules the voltages that might be by way of example applied to the electrodes:

Embodiment according to Figs. 1 and 2 Embodiment according to Figs. 4 and 5 Electrode Tension 21,22 0 volt 23 150 volts 24 0 volt 25 200 kv. 10m 200 kv. 100 200 kv. 27 200 kv. 28 0 volt common evacuated bulb, and means ,for subjecting the said gas to the action of all of said rays.

2. In an apparatus-for carrying out chemical reactions, in combination, a reaction chamber, means for driving gas through this chamber, means for producing X-rays, means for producing cathode rays, means for producing canal rays, all said ray producing means being included in a common evacuated bulb, and means for subjecting the said gas to the action of all of said rays.

3. In an apparatus for carrying out chemical reactions, in combination, a reaction chamber, means for driving gas through this chamber, means for producing X-rays, means for producing cathode rays, means for producing canal rays, means for producing anode rays, all said ray producing means being included in a common evacuated bulb, and means for subjecting the said gas to the action of all of said rays.

4. In an apparatus for carrying out chemical reactions, in combination, a reaction chamber, means for driving gas through this chamber, an evacuated bulb, a window of sheet metal between the bulb and the reaction chamber, electrodes enclosed in said bulb and adapted to produce -rays, cathode rays and positive rays, .all the said rays being directed to the metal window.

5. In an apparatus for carrying out chemical reactions, in combination, a reaction chamber, means for driving gas through this chamber, an evacuated bulb, a window consisting of a thin metal foil separating the bulb from the reaction chamber, and electrodes in said bulb including a plurality of anodes and cathodes adapted to emit X-rays, cathode rays and positive rays to-said" window.

' 6. In an apparatus for carrying out chemical reactions, in combination, a reaction chamber, means for driving gas through this chamber, an evacuated bulb, a Window consisting of a thin metal foil separating this bulb from-the reaction chamber, cathodes and anodes in the said bulb adapted to direct a beam of X-rays, cathode rays and positive rays to the said window, one of said cathodes being pierced for the passage of canal rays, and auxiliary electrodes in the said bulb adapted to accelerate the electrons striking the said window. w

7. In an apparatus for carrying out chemical reactions, in combination, a

evacuated. bulb, a window consisting of a. thin.

aoe aeo produced in a common reaction chamber} means for drivinggas through this chamber, an.

metal foil separating this bulb from the reaction chamber, electrodes within this bulb, adapted to direct a beam of cathode. rays to thev said window, auxiliary electrodes adapted to accelerate the said electrons and a pierced cathode, the apertures of which, opposite the electrode in said bulb which acts as the cooperating anode, are facing the said window.

. 8. In an apparatus for carrying out chemical reactions, in combination, a reaction chamber, means for driving gas through this chamber, an evacuated bulb, a window consisting of a thin metal foil separating this bulb from the reaction chamber, meansfor cooling this window and electrodes within this bulb adapted to emit X-rays, cathode rays and positive rays to said window. I a I 9. In an apparatus for carrying out the chemical reactions, in combination, a reaction chamber, means for driving gas through this chamber, an evacuated vessel, a window consisting of 'a thin metal ioil'separating this vessel from the reaction chamber, means for cooling this windew and electrodes within this vessel adapted to emit electrons, canal rays and anode rays to the said window.

10. A method of. synthesizing nitrogen compounds which consists-in influencing nitrogen o1 atmospheric air in presence 01' water by X-rays, cathode rays and positive rays produced in a common evacuated vessel.

11. A method of synthesizing nitrogen compounds which consists in influencing nitrogen of atmospheric air in presence of water by X-rays, cathode rays, canal rays and anode rays evacuated bulb.

12. As an explosive gas the product obtained by influencing the nitrogen of atmospheric air in presence of water by X-rays, cathode rays and positive rays produced in the same evacuated bulb.

13. In a fuel generator for internal combustion machines, in combination, a reaction chamber, means for driving atmospheric air through this chamber, means for producing X-ra'ys, means for producing cathode rays, means for producing positive rays, all said means being enclosed in the same evacuated bulb, said bulb.

being separated from the reaction chamber by a window consisting of a metal foil.

14. Apparatus for carrying out chemical reactions consisting of an evacuated vessel, electrodes therein for the production of cathode rays and canal, rays so arranged that the rays cooperate to produce a radiation which is able to penetrate parts opaque to canal rays, and means outside the vessel the tube at which the radiation produced by cooperation of the cathode and canal rays emerges from the vessel.

15. Apparatus for the production of strongly active rays consisting of an evacuated vessel,- anode and cathode arranged therein for the for directing a stream, of gas past the portion of production of an electron current, an anode trodes therein for the production of cathode rays 75 I and canal rays, one or said electrodes being an incandescent cathode and another of said electrodes being a pierced cathode, a reaction chamber associated with said evacuated vessel and means for driving gases through said chamber so that said gases are subjected to the action of said rays.

17. Apparatus for carrying out chemical reactions consisting of an evacuated vessel, electrodes therein for the production of negative and positive rays, one of said electrodes being an incandescent cathode and another of said electrodes being an anode containing a substance adapted to produce anode rays, a reaction chamber associated with said evacuated vessel and means for driving gases through said chamber so that said gases are subjected to the action of said rays.

18. The method preparing an explosive gas comprising the activation of the nitrogen of atmospheric air in presence of water by X-rays, cathode rays and positive rays produced in the same evacuated vessel and mixing the irradiated gas with atmospheric air.

19. A method of synthesizing nitrogen compounds which consists in influencing nitrogen and another substance capable of reacting therewith by X-rays, cathode rays and positive rays produced in a common bulb, said substance being one of a group consisting of H20 and H202.

20. A method of synthesizing nitrogen compounds which consists in influencing nitrogen of atmospheric air and another substance capable of reacting therewith by X-grays, cathode rays and positive rays produced in a common bulb, said substance being one of a group consisting of H20 and H202.

21. A method of synthesizing ammonia sulphate which consists in influencing nitrogen in presence or another substance by X-rays, cathode rays and positive rays produced in the same evacuated container, said other substance bein one or a group consisting of water and hydrogen peroxide, and bringing the irradiated gas into contact with ierrous sulphide and water acidifled-with sulphuric acid.

22. A method of synthesizing ammonia sulphate which consists in influencing nitrogen of atmospheric air in presence of another substance by X-rays, cathode rays and positive rays produced in the same evacuated container, said other substance being one of a group consisting of water and hydrogen peroxide and bringing the irradiated gas into contact with ferrous sulphide and water acidified with sulphuric acid.

23. As an explosive gas the product obtained by influencing the nitrogen of atmospheric air in presence of another substance selected from a group of compounds consisting of H20 and H20: by X-rays, cathode rays and positive rays produced in a common bulb.

LUDWIG HERRMANN.