US1160811A - Method for producing nitrogen compounds. - Google Patents

Description

C. E. ACKER.

METHOD FOR PROOUCING NHROGEN COMPOUNDS.

APPLICATION HLED SEPT. 2, 1910.

Patented Nov. 16, 1915.

2 SHEETS-SHEET 1.

MOOOM.

C. E. ACKER.

METHOD FOR PRODUCING NITROGEN COMPOUNDS.

APPLICATION FILED SEPT. 2. IBIO.

latented Nov. 16, 1915.

2 SHEETS-SHEET 2.

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LIIULII.

pounds, of which the following is a f\1lll clear, and exact escription.

`rIhis invention relates to a process for the manufacture of alkali metal cyanids, cyanav mids and the like, and more particularly to certain improvements in the processes de scribed in my United States applications,- Serial No. 485,344, filed March 23, 1909, and Serial No. 579,763, filed August 30, v19101. The processes therein disclosed consist in initially 4reacting on a particularly reactive metal such as barium, lithium, strontium, manganese, etc., with carbon or a carbonaa carbid of such metal, e. g., barium carbid; in then treating this carbid with nitrogen or a nitrogenous reagent, for the purpose'of producing the cyanidV of such metal, and in nnally reacting on the barium cyanid or the like with an alkali metal e. g., sodium, with the consequent production of sodium cyanid -and metallic barium. In the first application, the reactions involved occur within the body or mass of a molten alloy, such alloy preferably comprising the alkali metal, the

reactive metal and a vrelatively inactive diluent metal; while in the second case thel reactions resulting in the formation of carbid were confirmed principally to the surface of the alloy, the subsequent reaction of the carbid so formed with a nitrogenous reagent occurring in the body of a mass of sup'erposed fused salt. As I stated in the second of the applications aforesaid, the formation of the final product was expedited and the process made more eficient by bringing about the reaction between the carbon and nitrogen compounds entirely outside of the body of alloy, and I have sincefound that a still greater increase in efficiency may be obtained by causing4 all of the reactions to occur in the body of fused salt. This application therefore relates to a process of this descrition, and covers the feature of electro# lytic y both thu reactiva etal Specification of Letters Patent.

- contact with the liberated metals.

reactive metal c anid, e.

be similarly' decom` ceous reagent for the purpose of producingposed by metallic sodium. As stated in the t. ns is. acaror ossrn'rna, NEW Yo, ass'ron'o o irnnnrrnoenn coa a conronafrron or row: y s

It THOD FOB. PRODUCING NITOGEN COO'UNDS.

ratentoa not. ic, rara;

Application med September 2, 1910. Serial No. M1190.

and the alkali metal on a suitable cathodel from the molten alloy, using a suitable electrolyte, such for example, as sodium cyanid; and 1n lntroducing nitrogenous and carbonaceous reagents into the electrolyte in such manner that the same may come directly into As stated 1n applicatlon 485,344, some portion of the reactive metal e. g., barium, might combine directly with nitrogen to' forml barium 'nitrid which would then react with carbonv to form barium cyanld; and that this cyanid would in turn be decomposed bvsodium as above, with formation of sodium cyanidand metallic barium. I stated, furthermore, that 'I both carbid and nitrid might be formed -under the conditions of theprocesses, and

that they might then react together to form g., vbarium cyanid, which 'wou/l second application, by far the greater part of the initial formation of reactive metal carbid, e.' g., barium carbid, 1n what seems to be a particularly favorable physical con.

dition for the absorption of nitrogen at a low temperature; and that a comparatively small proportion' of the final product is obtained as a result of the initial formation of reactive metal 7 nitrid which afterward combines with carbon. etc.

The chemical reactions involved in the present case,l when suicient free carbon is present, are substantially similar to those described in my applications above referred to, and may be represented as follows:

.It will be observed by considering reac-' tions No. 1 to No.4representing the principal steps of the process) that the reactive metal, e.' g., barium, passes from the nie` tellin ttate to carbid, carbid to cyanld, and

As stated inv my other applications the..

reactive metal` e. g., barium, and the alkali metal, e. g., sodium, may each be employed in the pure state, in the form of an alloy with each other, or in the form of an alloy with certain heavy and relatively inert metals such as lead, tin, etc.; the nitrogen may be employed in the form of pure or diluted gas, ammonia, or other nitrogenous reagent; and the carbon may be employed in the form of finely divided, granular, or lump charcoal, coal, coke, hydrocarbon gas, fuel oil, lamp black, a cyanid, cyanamid or other carbonaceous reagent. By the term carbonaceous reagent as used in the appended claims, I mean therefore, carbon or any compound thereof capable of yielding carbon under the conditions vof the process; While the term nitrogenous reagent correspondingly refers to and includes nitrogen or any compound including nitrogen as an ingredient thereof, which will yield that element under such conditions.

If the source of carbon is a gas, fuel oil, or lamp black, the resultant carbid, produced by the combination of the reactive metal .with carbon (as pointed out in application No. 485,844) is found to be present in finely divided form.

As stated in application 579,7 63 filed August 30, 1910, the carbid produced in the process, is in peculiarly favorable physical condition for the absorption of nitrogen, being apparently amorphous and impalpable and quite unlike the ordinary hard, iridescent, impure commercial crystalline carbids known to commerce. The former is produced at a very low temperature {generally below 900o C.) and under radically different conditions from the later, which is produced in electric smelting furnaces at a very high temperature,generally overl When both barium and sodium are alloyed with a heavy metal such as lead, and so utilized in the process,v-some of the reactions in which barium, sodium, carbon, etc., are concerned must obviously take place in the actual presence of the alloy-either at the surface thereof or in contact with some -(reaction #3) must come into actual con-l tact with sodium as contained in the alloy. In my latter application, also, I called attention to the fact that the presence of a considerable. body of molten sodium cyanid on the surface of the alloyl was an advantage. in that the barium carbid became suspended, diffused, orv dissolved in the: cyanid and could there be more advantageously reacted upon by the nitrogenous reagent, the product ofthe reaction bein barium cyanid, which fusedreadily anldissolved in the sodium cyanid and thus came into contact with the metallic sodium contained in the alloy, at the surfacethereof, whereby the barium in the barium cyanid was set free at the sur-face of the alloy, and sodium cyanid was formed; `and further that the metallic barium thus liberated at the surface of the alloypromptly combined with carbon to form more carbid, which then became disseminated throughout the molten cyanid as before.

' When metallic barium is liberated at the surface of the alloy, it may renter the alloy, if only momentarily, and then afterward combine with carbon in contact with the surface of the alloy at4 that particular point to form barium carbid; at any -rate the decomposition of the barium cyanid is effected by the sodium at the surface of the alloy, and not elsewhere inthe mass of molten cyanid. It thus transpires that some of the intermediate reactions of the lprocess as carried out in the apparatus described in application Serial No. 579,763 .take place at the surface of the alloy only and that they are effected by certain metals While diluted with other metals, and which are therefore to some extent less effective in bringing about such reactions than they would be if in the pure state, and not diluted, so to speak, with yother relatively inert metals.

Il have found it desirable in carrying out these reactions at the surface of the alloy to have a comparatively high percentage of both reactive metal and alkali metal present in the alloy, so that they will not be unduly diluted in which case the process proceeds smoothly and rapidly,-but I have also found that it is possible and convenient to liberate from the alloy-and within the mass -of the molten cyanid itself-both reactive metal and alkali metal in the pure state, that is to say, not in the least diluted with an inert metal such as lead, (although the two metals actually concerned in the reactions, e. g., barium and sodium, when simultaneously liberated in the interior of the molten cyanid maybe momentarily alloyed with each other) by passing a current of electricity from the surface of the molten alloy constituting an anode, through the molten lcyanid constituting an electrolyte, to a solid carbon, iron or other metal disk or grid, partly submerged in the cyanid, and constituting the cathode of an electrolytic cell. The metallic barium thus' liberated Within the mass of the molten cyanid `in stantly combines with carbon-either vthe carbon of the cathode, if the cathode ,be `of carbon, freecarbon disseminated throughout nieolai'i itself-the latter according to the following equation llr employing a solid iron or metal catli ode, as l prefer, and in case there is no free carbon disseminated or didused throughout the molten cyanid, the above reaction (#5) will always take place when bariumis the reactive metal used. x

llllhe same reaction will take place when lithium, or some other reactive metal is employed instead of barium. 'Jlhe products oit the reduction of the sodiumcyanid are thus, sodium cyanamid (dialkali cyanamiol) and barium carbid, and if no freecarbon is present or afterward supplied, the reduction of the cyanid to cyan mid will proceed until the entire mass of cyaanid is converted into cyanamid, and the process may be used accordingly for the production of alkali cyanamids. When, however, free carbon is present in the molten mass at the time the barium is liberated in a free state, or whenever it is afterward supplied, the c anamid which is probably always formed within the molten mass is quickly reconverted intocyanid. When metallic barium, or other reactive metal is set free at the surface of fthe solid cathode, and within the mass of molten sodiumcyanid it probably does not preserve its metallic character for more than a brief moment, but combines with carbon practi-y cally at the moment of its liberation.

lI regard it as likely, in view of the 'fact that barium does reduce molten sodium cyanid to sodium cyanamid by combining with some of its combined carbon, and in view ofv the fact that molten sodium cyanid is in intimate and close contact with the barium at the moment of its liberatiom-pressed against it in fact by the weight of the supernatant fluid cyanid, and in view of the impalpable and amorphous character of the barium carbid produced in the process at so low a temperature (below 900 C.) that the greater part of the barium carbid, which is concerned in the synthesis of sodium cyanid by this process is produced by barium combining with one element of carbon in the cyanid itself,-it being understood, of course, that but a very small proportion of the whole mass of cyanid would be thus momentarily reduced--and that the free carbon ioating around therein quickly recouverts the reduced portion back to cyanid.

The barium carbid, produced in accordance with reaction #l or reaction #5, remains suspended in the molten cyanid by reason of the agitation of the molten mass.

rl`he entire mass of cvanid is practically saturated with im alpable carbid, and if a sample ot the me ten cyanid taken during? this process is moist'ene'd with water, the presence of carbid is very'evident from the odor of the evolved. acetylene,-although no lumps or crystals of carbid may be visible. The carbid 1s present in a very fine stae of division.' (Some carbid may also possibly be 1n .actual solution.) When the cyanid is examined under the microscope the npure colorless crystals of cyanid loom up very large and clear, and squeezed in between the crystals is the dark gray or black carbid apparently in the form of a film. The moisture 1n the air attacks this film of carbid between the crystals at the exposed edges of the film and minute bubbles of gas are constantly given oil all along the exposed edges. E videntlythe carbid is in very soft condition since it is squeezed into the thin spaces between the crystals of the cvanid iii the manner described; but it is impossible to examine it directly in the open air on account of the minute bubbles of gas which instantly cover its surface.

The specific gravity of barium carbid is4 con s1derably greater than that of molten sodium cvanid, but owing to the fact that the carbid. is apparently in amorphous condition, a little agitation suflices to maintain 1t in suspension. y

he gaseous nitrogen or ammonia, or a little fuel oil, inJec'ted into the alloy, or into the molten cyanid, and used primarily as a source of carbon, produces all the agitationV required to maintain both the carbon and amorphous carbid in suspension in the molten cyanid. Meanwhile, nitrogen or ammonia 1s continuously or intermittently introduced into the mass of molten cyanid in such manner as to come into contact with the suspended carbid with which it then combines to form barium cyanid, which v fuses easily, and being perfectly miscible with the sodium cyanid, diffuses throughout the entire molten mass. Barium cyanid is thus constantly present throughout the moltenelectrolyte and at the very surface of the solid cathode where metallic sodium is liberated. It may be liberated simultaneously with the barium. -As soon as pure sodium is liberated at the cathode it enters into reconsiderabh7 greater than that'of the molten electrolyte it cannot settle through the electrolyte without comingr in contact with carbon, either free or combined, and uniting therewith to form barium carbid. It thus transpires that as long as there is any barium cyanid in the meltfunder normal workin@ conditions it alioiild always be' present until the charge is to be inished-the liberfree at the solid cathode and therefore does not accumulate as such within nor on the surface of the melt. If the residual lead alloy should contain a suflicient percentage of sodium to react with barium cyanid in the electrolyte, then such al'loyed sodium when reacting With barium cyanid at the surface of the alloy, will liberate the barium' at the surface of the alloy, and it may then combine in whole or in part with the heavy, inert metal of the alloy; but by far the greater part of the final product will bc produced as a result of intermediate and nal reactions taking place within the mass of the molten cyanid at the surface of the solid cathode, or in the vicinity thereof.

The present process may be conducted in a double `compartment electrolytic furnace similar to the sodium furnace described in application Serial No. 575,189, tiled August 5, 1910, except that the solid cathode has a hole in its shank for introducing nitrogen (and fuel oil, if desired), and that the iron cover is preferably fitted with a hopper.

Referring therefore to the accompanying drawings, which illustrate one form of apparatus which may be used: Figure 1 is a vertical cross section of an apparatus adapted for the carrying out of my improved process taken on the line I-I. Fig. 2 is a horizontal section through the said apparatus taken on the line II--II of Fig. 1. Fig. 3 is a transverse vertical section of said apparatus taken on the line III-IIIof Fig. 2. Fig. 4 is a fragmentary section taken on line IV-IV of Fig. 3.

Like parts are designated by the same reference sign throughout the respective views.

Referring now to the drawings, the furnace or inner container 1 should preferably be made of cast iron or cast steel,'and the inner walls of such chamber should preferably be lined with refractory material 2, such as alumina or magnesia. The furnace casting is inclosed at the bottom and on all sides by heat insulating material 3, preferably brick or the like. The furnace comprises two principal chambers, a primary electrolytic chamber 4 and a secondary chamber 5, these chambers being separated by a septum or wall 6, the bottom flanges 7' of which serve to support the adjacent side lining 2. A set of anodes 8 extend into the primary chamber and are preferably made of some form of carbon. The primary chamber 4 is covered with a slab 9 of refractory material; and the gases liberated at the anodes are conducted away through fiues 10 A The secondary chamber 5 it fitted with a spout 11 for conducting off the final product, such compartment having a cover 12 spaced from the container b y an an: tight gasket to prevent the admission of air into the reaction chamber. An iron, nickel or carbon electrode 13 yprojects through the cover into the mass of electrolyte 14 disl posed in the secondary.chamber; the electro- 'the alloy may be effected either intermittently or continuously by mechanicalmeans or otherwise; a centrifugal pump 17 being shown in the drawings; and suitable means, such as a hopper 18, .may be provided for permitting the continuous or intermittent introduction of the salt'required in the electrolytic chamber. The secondary cathode 13 is adjustable in the air tight cover 12 and has a hole extending through its shank, the upper part of which is fitted with a valved pipe 19 for introducing nitrogen or ammonia into the molten mass in the reaction chamber; and is also fitted with an oil feed device 20, through which fuel oil or other hydrocarbon may be introduced in carefully regulated quantities into the reactive chamber. An auxiliary supply pipe 21 extends through the side of the reaction chamber; its lower end being below the surface of the alloy, and such pipe may be used to introduce nitrogen or hydrocarbon, or both, directly into the mass of molten metal, when desired, thus affording a means of preheating the nitrogen when desired. The cover 12 is also fitted with a specially constructed hopper 22, which has an air ti ht cover and is so arranged that it may be lled with charcoal and then subjected to the'action of a vacuum pump for the purpose of exhausting the air from the hopper and the charcoal contained therein, before it is charged into the reaction chamber.

The molten cyanid is produced in the secondary chamber and normally rises to the level of the outlet before it is permitted to run off through spout 11; this spout may be temporarily closed, however, to permit the cyanid to accumulate in the chamber to a much greater depth, before being tapped off.

The primary electrolyte may consist largely, at the beginning of the operation, of molten barium chlorid-with a small proportion of sodium chlorid.

The electrolyte in the secondary chamber consists preferably of pure molten sodium cyanid, (although it may contain any proportion of pure barium carbid, cyanid, or other barium salt from which barium may be set free by sodium at the temperature of the operation). Both electrolytes rest on the surface of the molten lead in their rethe surface of the'lead land turned on.

s ectivecompartmenta. 4 rllhe anodesv vSand t e cathode 13 are thenraised slightly- .ebiqw I theicurrentis The current densitydinbth primaryoand. secondary is4 determined by the; electrode surface and the aniram and thavolteais detelzmind by? :the length iaith@ fblumunf electrolyte,,through- 'which the current'. must ,pass in eachhcell; .the currentdensity. and

voltage in each cell -being* regulatedat ,will

toy ymaintain the electroly tesv in molten y con- ,dtiomand to decom osethem. The current liberatesbarium an sodium. atthe surface of the lead in the primary cell, therebyA producing an ,alloy of barium-leadfsodium, which isthenonducted into or circulated through the l secondary chamber ,bv means of the centrifugal pump,-and soonbecomes practically homogeneous and Vof uniform temperature throughout the entire The current thenpasses from the surface of the alloy in the secondary chamber (constituting the secondary anode) through the molten cyanid to the solid cathode; the liberated anions (CN) combining with barium at the surface of the alloy to form barium cyanid, which accumulates in the electrolyte. The liberated anions (CN) may also combine with sodium at the surface of the alloy, `but this is of no consequence since the electrolyte consists of molten sodium cyanid. V

The liberated anions cannot :combine with thei heavy'metal of the alloy, e. g., to form "a cyanid which would contaminate the sec-` ondary electrolyte or the product, and which would then yield, by electrolysis, lead at the solid cathode,-for reasons set forth in application 575,819 ;-none of4 the heavy metals combining with carbon and nitrogenl or. cyanogen to vform cyanids or cyanamids which are stable at the temperature of the operation. This feature is of great importance in this process.

Metallic sodium is liberatedat the cathode but as soon as an appreciable roportion of barium cyanid is present,whic may be purposely introduced at theve'ry start, the me-v tallic lsodium displaces the barium which latter then immediatelycombines with carbon, free or combined, to form amorphous barium carbid; and this substance remains suspendedyin the cyanid. Nitrogen may then be introduced through pipe 21 andwill pass' down through the hollow shank ofthe cathode 13 to the'lower surface thereof, and there spread out in the form of a thin layer between the face of the cathode, or plunger, since it may be sol termed, and the molten alloy, and thus come into effective reactive Contact with the suspended barium carbid with which it combines to produce barium cyanid. rll`he barium in the barium cyanid isv then displaced by the metallic sodium at the cathode, with the consequent production of sodium .cyanidland metallic barium which latter again becomes available for the production of more carbid. If there 4,is no free carbon present the barium will seize upon one elementv` of combined carbon yin. the sodiumv cyanid to form sodium cyanamid which is'perfectly stable; but this latter substance is vromptly reconverted v'into sodium cyanidJ as soon-.as free carbon is added. f Carbon in theform of' charcoal, from which the'air and moisture-have been re'- moved by heat and vacuum may be introduced through the hopper into the reactive chamber. Fuel oil may be introduced through the oilfeed device under pressure,

and will thencome into contact with the and thence by electrolysis into the secondary electrolyte', it becomes unnecessary to supply more,-for the reason that the reactive metal is used over and over again, and therefore no more barium chlorid need be added to the primary electrolyte, which may thereafter consist substantially' of sodium chlorid. lf there is any loss, however, of available barium in the alloy, or ofvbarium carbid or kcyanid in the melt, through any unavoidable or inadvertent circumstance or by being withdrawn in the finished product, or for any other reason, the deficiency may be supplied from time to time by adding barium chlorid to the electrolyte in the primary cell, or by supplying'it in any other manner.

The temperature of the lower end of the secondary cathode or plunger if submerged in the red hot alloy would be, of course, substantially equal to that of the molten metal itself; but when the face of the plunger is raised slightly above this eiiicient metallic heatconductor, Il nd that suicient heat may be conducted away through the shankv of the -plunger to the heavycopper conductors on the outside of the furnace to mit ' the carbid, whereas if the ammonia is firstintroduced into the red hot alloy it is there partly decomposed into its elements, nitrogen (in the atomic state) and hydrogen, but

th1s atomic nitrogen, unless instantly absorbed, passes into the molecular state, (N2). When molecular nitrogen rises into the molten cyanid it does not combine with the suspended -carbid with such avidity, as does the atomic nitrogen.' The absorption of' molecular nitrogen, in other words, is efvfected somewhat more slowly than the absorption of atomic nitrogen. While it is disadvantageous for this reason to first introduce ammonia into the red hot alloy and then permit the nitrogen to rise into thc cyanid, this objection does not hold with nitrogen obtained from the air,-z'. e., molecular nitrogen, which may advantageously be first introduced into the molten metal for the purpose of preheating it before it comes into contact with the carbid. The auxiliary nitrogen pipe 21 may be used for this purose. p When the reaction vessel is suliciently full of cyanid it becomes necessary to vfinish or clarify the charge. The flow of gas should be stopped, and the sodium liberated a short time longer in order to insure the decomposition of all of the barium cyanid by sodium-which should be in excess in the alloy-after which the suspended materials in the mass should be allowed to settle.

Barium carbid has a specific gravity somewhat greater than that of molten cyanid, and it, together with the excess carbon, will settle in the course of time through the tranquil, undisturbed melt to the surface of the alloy after which the clear molten cyanid, or any part of it, may be tapped off at one of the spouts above the surface of the alloy. Another method of finishing a charge of cyanid consists in limiting or withdrawing the supply of sodium in the bath and in the alloy so that all of the residual suspended carbon and carbid may be permanently converted into barium cyanid, and the melt will consist of a clear molten mixture of substantially pure sodium cyanid and barium cyanid which may be drawn oil" and utilized as such.

The respective proportions of the two cyanids may be controlled at will; but in general the sodium cyanid shouldbe greatly in excess.

It will be apparent from a consideration of the above reactions that a free reactive metal must be employed at some point in the cycle, or in lieu thereof a compound which will yielda free reactive metal at some point in the cycle, and that the use of any salt or compound which when introduced into the. molten mass or employed under any of the conditions of the process will yieldsuch reactive metal, is within the scope of my invention. It will be apparent, also, that a' carbid, nitrid, cyana mid, or cyanid of the reactive metal 1f of sufficient purity and in suitable physical condition may be employed at the outset instead of the reactive metal itself, and that this is possible by reason of the fact that the initial carbid or nitrid, under the condi-` tions of the process, will be converted into either cyanamid or cyanid of the reactive metal, and that the alkali metal,-sodium or potassium will thereupon liberate-and set free the reactive metal-in metallic form. Other reactive metal salts may be similarly introduced and decomposed with consequent liberation of a free reactive metal but the method is slightly objectionable for the reason that it introduces an impurity or diluent, e. g., sodium chlorid into the final cyanid. Thus barium chlorid, lithium chlorid, etc., if introduced into the molten cyanid will'melt and dissolve therein and come into contact with the liberated sodium or potassium or that contained in the alloy, which will then decompose such chlorids with the formation of sodium or potassium chlorids, and metallic barium, or metallic lithium will be liberated, according to the following equation:

(6) LiCl+Na=NaCl+Li (free metal).

Other reactive metals may be employed instead of barium,notably, lithium, strontium, and calcium, in which event the reactions will be quite similar to those indicated for barium.

The reactive metals chromium, titanium, vanadium, etc., will also bring about the synthesis of sodium` cyanid under this process, although the mechanism of the intermediate reactions is not the same inall cases, Aand the process is somewhat slower.

What I claim, is:

l. In a process of producing alkali-metalcyanogen compounds and the like, th'e steps whlch comprise separatingr alkali-metal from a molten metallic bath and reacting on the separated metal with a nitrogen-carbon compound.

2. In a process of producing alkali-metalcyanogen compounds and the like, the steps which consist in electrolytically separating manganese, cerium,

alkali-metal from a molten metallic bath and cyanogen compounds and the like, the steps which consist in electrolytically depositing alkali metal of the compound to be produced, and similarly depositing a reactive metal,7 reacting on the reactive metal with carbonaceous and nitrogenous reagents to form a nitrogen-carbon compound of such metal and substituting the alkali-metal aforesaid for the reactive metal in said compound.

5. ln a process of producing cyanogen compounds and the like. the steps which consist in effecting a reaction between electrolytically liberated reactive metal and acarbonaceous reagent within a bath of fused mixed salts and reacting on the compound so formed with a nitrogenous reagent.

6. ln a process of producing cyanogen compounds and the like the step which comprises edecting a chemical reaction between a carbonaceous reagent and an electrolytically liberated metal within a. bath of fused salt to form an amorphous carbon compound of said metal.

7. In a process of producing cyanogen compounds and the like, the steps which comprise effecting a chemical reaction vbetween a carbonaceous reagent and an electrolytically liberated metal within a 'bath of fused salt to vform an amorphous carbon compound of said metal, and reacting on said carbon compound with a nitrogenous reagent.

8. ln a process of producing cyancgen compounds and the like, the steps which comprise effecting a chemical reaction between a carbonaceous reagent and an elec-A trolytically liberated metal to form an amorphous carbon compound of said metal, and reacting on said carbon compound with a nitrogenous reagent to form a carbon-nitrogen compound of said metal,-the reactions taking place within a bath 'of fused salt.

9. In a process of producing cyanogen compounds and the like the steps which comprise electrolytically depositing a metal from a bath of fused salt and reacting on such metal with a carbonaceous reagent to form a carbon compound, said compound being held in suspension in the salt, and re acting on the suspended carbon compound with a nitrogenous reagent.

10. ln a process of producing cyanogen compounds and the like the steps which comprise electrolytically depositing a metal from a bath of mixed fused cyanogen compounds, the radical forming constituents of one at least of which are the same as those of the compound to be produced, one of said fused compounds including an alkaline metal and another a metal belonging to a dierent group of metals, and reacting on such metal with carbonaceousreagent.

11. lin a process of producing cyano en compounds and the like the steps which comprise electroytically depositing a metal from a bath of mixed fused alkali and alkaline earth cyanogen compounds, and react-` ing thereon in such bath with carbonaceous and nitrogenous reagents to form a nitrogen-carbon compound of the metal.

12. ln a process of producing a compound consisting of a metal and a combination of elements capable of forming a radical the steps which consist in electrolytically depositing a metal from a bath which comprises the said combination of elements and reacting on said metal with a reagent to form a substance which is held in suspension in said bath.

13. The process of producing alkali-metal cyanogen compounds and the like, which includes liberating alkali-metal by passing a current of electricity through a fused bath from a substance which contains such alkalimetal as one of the constituents thereof, forming a carbon-nitrogen compound in sail.-I bath and reacting on the liberated alkalimetal with said compound.

14. The process of producing alkali-metal cyanogen compounds and the like, which includes liberating an alkali-metal and a reactive metal by passing a current of electricity through a fused bath from a body of alloy which contains said metals, forming a carbon-nitrogen compound of the reactive metal in said bath and reacting on the liberated alkali-metal with said compound.

15. In a process of producing cyanogen compounds and the like, the steps which consist in electrolytically liberating a reactive metal, reacting thereon with a molten carbonaceous reagent to form a carbid, at a temperature below that at which such carbid will fuse, and edecting a reaction between said carbid and a nitrogenous reagent.

16.'The process of forming a carbonaiitrogen compound which comprises electrolytically depositing a plurality of metals in the presence of nitrogenous and carbonaceous reagents, one of said metals forming a nitrogenrarbon compound with constituents of said reagents and another of said metals being thereafter substituted in said compound for the first.

17. The process of producing alkali-metal cyanogen compounds and the like, which involves reacting with a carbonaceous reagent on free reactive-metal to form a carbon compound thereof, reacting on said compound with a nitrogenous reagent to form a carbon-nitrogen compound, electrolytically dissociating an alkali-metal from a mass of molten alloy, and reacting onthe free alkali-metal with said carbon-nitrogen compound.

18.. The process of producing a carbonnitrogen compound which includes forming a carbon compound within a mass'of electrolyte through which an electric current is owing, said electrolyte being in contact with a fluid body of relatively high density which supplies at l'ea'st one of the ingredients of the compound aforesaid, and reacting on said compound with a nitrogenous reagent.

19. The process of roducin'g a carbonnitrogen compound which includes forming a carbon compound Within a mass of electrolyte through which an velectric current is flowing said electrolyte being in contact with 1o a fluid body of relatively high density which supplies at least one of' the ingredients of the compound aforesaid, and reacting on said compound while in said electrolyte, with a nitrogenous reagent.

In witness whereof, I subscribe my signa- 15 ture, in the presence of two Witnesses.

CHARLES E.4 ACKER.

lVitnesses:

WALDo M. CHAPIN, WILLIAM C. LANG.

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