July 24, 1923.

1,462,987
w. SIEBERT
PROCESS FOR PRODUCING NITRIC ACID BY MEANS OF THE ELECTRIC ARC

Filed May 13. 1922

 . Patented July 24, 1923. 1,462,9d?
U arse stares PATENT
WERNER SIEBERT, OF LAUFENBURG, AARGAU, SWITZERLAND, ASSIGNOB TO NI'I‘BUM
AKTIENGESELLSCHAFT, OF ZURICH, SWITZERLAND, A CORPORATION OF SWITZER
LAND.

PROCESS FOR PRODUCING NITRIC ACID BY MEANS OF THE ELECTRIC ARC.

Application ?led Kay 13, 1922. Serial No. 580,731.
To all whom it may concern: below 0° C., so that the content of moisture
Be it known that I, \VERNER SIEBERT, a in the gases leaving the absorption system is
citizen of the Republic of Germany, residing so low that these gases can be conducted
at Laufenburg, Aargau, Switzerland, have back to the electric furnace without any
invented certain new and useful Improve danger of causing corrosion of the iron ipes
ments in a Process for Producing Nitric or other apparatus. As the gases intro ucecl
- Acid by Means of the Electric Arc, of which into this circuit, being derived from atmos
the followin is a speci?cation, reference pheric air, always contain small portions of 60
being had t erein ‘to the accompanying argon, which does not take any part in the
10 drawing. reaction of the electric arc and with which
It is a known fact based on chemical laws therefore the gases performing the cycle are
that the oxidation of nitrogen in electric continuously enriched, it is necessary to re
arcs gives a yield which is higher by 25%, new the gas mixture, from time to time, as
if instead of atmospheric air a gas mixture a higher concentration of argon reduces the
15 of 50% oxygen and 50% nitrogen is sub ef?ciency of the combustion in the electric
jected to the action of the arc. Besides this furnaces. Therefore the process has been
a higher concentration of the nitric fumes improved by letting continuously a certain
is obtained, which facilitates absorption and amount of gas escape corresponding to about 70
the production of nitric acid. one-fourth of the gas uantity, which is
20 Nevertheless the existing plants for pro introduced into the circuit as pure nitrogen
ducing nitric acid operate on atmospheric and oxygen. If for instance 400 cubic
air and only the rocess described herein meters of nitrogen and oxygen containing
after, which has een thoroughly worked 0.7% argon i. e. 2.8 cubic meters argon are
on a commercial scale allows the utilization introduced into the circuit per hour, and 100
25 of a 50% mixture of oxygen and nitrogen cubic meters of the gas mixture are led oil‘
and the attainment of the above mentioned ‘at another point of the circuit, it is possible
advantages. According to the present proc to maintain the concentration of argon at
ess the atmospheric air is lique?ed and about 2.8%, i. e. a'concentration which has 80
separated by evaporation into oxygen and no harmful effect on the formation of
30 nitrogen. These gases are introduced into nitric oxides. In the drawings Fig. 1 is a
the gas-current, which is led through the diagrammatic sketch of an installation for
electric furnaces, in such quantities that the carrying out the invention; and Fig. 2 illus
gas mixture treated is maintained continu trates a modi?ed form of an installation. 85
ously at a concentration of 50% oxygen and Referring to Figure 1, the gases coming
35 50% nitrogen. The gases leaving the elec out of the absorption system are led through
tric furnace are cooled down in a steam a conduit to the rotary blower 1, by which
whereby
generatorthe
to aheat
temperature
containedofinabout
the gases
200° is they are raised to the desired pressure and
delivered to the electric furnace 5. 2 and 3 90
conserved. Thereafter the gases are further are gas meters of the nozzle type, through
40 cooled in heat interchange apparatus in which the pure oxy en and nitrogen pass
?uenced by cooling water to a temperature into the conduit leadging to the, electric fur
of about 30° C. ‘The gases are then led to nace 5. 4 denotes a valve, which allows
absorption towers, which are fed with nitric regulation of the gas-current. 6 are the 95
acid. The gases coming out of the absorp— electrodes of the furnace between which the
45 tion system, which are saturated with mois arc is generated. 7 is a jacketed cooling
ture, are-dried b means of sulfuric acid pipe, which allows the abrupt cooling of the
and are led to a b ower, which returns them gases as they leave the furnace in order to
to the electric furnaces for repeated treat avoid the decomposition of the obtained ni 100
ment in a cycle. tric oxid. 8 is a steam generator, in which
50 The rocess can be so modi?ed that the the ases are cooled down to about 200° C.
absorption of the itric fumes in the nitric and in which the heat contained in the gases
acid towers is per ormed at a temperature is conserved in the generation of a large
 1,462,987
amount of steam, which can be utilized for ?ows through a cooling coil 13, which is
the concentration of dilute nitric acid or for placed in a tank 13‘, in which brine at a tem
other purposes. 9 denotes a water cooler perature of —25° C. circulates. Thence‘ the
adapted to further cool the gases. 10 is a nitric acid ?ows back through valve 14 into
chamber, in which the nitrogen monoxide the absorption towers 11. The portion of 70
(NO) is oxidized into nitrogen peroxide this acid however, which is small in compar
(N02). 11 are the absorption towers, which ison with the amount of acid produced from.
are fed from the tank 12 with dilute nitric nitric gases in the tower 11, is led through ‘
acid or with water. 20 denotes an absorp ‘valve 16 to the followingabsorption tower
tion tower of iron, in which the gases are 11. In this tower 11 the process is repeated 75
brought into contact with sulphuric acid and as is also the case in the third tower shown
in which the moisture contained in the gases in Fig. 2. The nitric acid obtained in this
is absorbed by this acid. This drying of the last tower, through which the nitric gases
gases is necessary to prevent the formation of highest concentration are led, has the
of nitric acid in the electric furnace, which highest concentration, for instance 60% 80
would take place ‘if the moisture should HNOS. The nitric acid formed in the ab
come into‘ contact with the nitric fumes sorption system can be drawn off from valve
formed in the electric furnaces, the so formed 17. The great advanta e of the above de
nitric acid would corrode the ap aratus sit scribed process is, that t e whole circuit can
uated between the furnace 5 and) the oxida be kept under pressure or under slight vacu 85
tion chamber 10. 18 is a conduit leading um as desired by regulating the blower 1.
the gases from the sulphuric acid tower 20 Losses of any kind of nitric gases are abso
to the blower 1. 19 denotes a valve allowing lutely impossible. Not only are by this
the escape of a portion of the gases from process all nitric gases, formed by the elec
25 the system and the maintenance of the con tric arc, absorbed and recovered, but also 90
tents of argon at a low percentage. It is nitric oxides of a higher concentration are
seen‘ from the above, that the gases are led obtained in using the oxygen-nitrogen gas
in a closed circuit through the furnace, the mixture. Further the oxidation of NO into .
steam generator, the water cooler, the oxidiz HNO3 takes place very rapidly, owing to 95
30 ing chamber, the absorption towers, the dry the high percentage of oxygen in the gas
ing tower and back to the furnace. The mixture which is not the case when air alone
nitric fumes produced in the furnace are ab is utilized. It is therefore possible to draw
sorbed in the absorption towers to form from the absorption tower,'through which
nitric acid and through the gas meters 2 and the nitric gases areHpassed through ?rst, a
00
35 3, an amount of oxygen and nitrogen is intro nitric acid of 60% N03, whereas with the
duced ‘into the circuit corresponding to the process known and applied up to the present,
amount that has been taken out from the a‘ nitric acid of only 35% has been obtained.
apparatus in form of nitric acid and that The result is, that with the present inven
has escape'dthroufh the‘ valve 19. It is ad tion it is possible to get a yield of 80
40 vantageous to» lea the gas escaping through 105
rammes of I-INO8 per kilowatt-hour or 700
the valve 19 into the nitrogen and oxygen ilogram of HNO3 per kilowatt year.
separating, apparatus, as this gas contains ' ‘~I claim: , -

already 50% oxygen and it is therefore Y. The cyclical process of producing nitric
easier and chea er to gain out of this gas acid by means of the electric are which con- ‘ 110
45 pure our gen, t an if oxygen has to be ‘ sists in treating a hitrogen~oxygen mixture
gained rom atmospheric air. in an electric arc furnace, cooling abruptly
In the modi?ed system, illustrated in Fig the gases leavin said electric arc furnace and
ure 2 the gases are dried in a different man conserving the eat contained in said gases,
ner to that described above. In this modi absorbing the nitric oxides thus formed by 15
50 ?ed installation the gases leaving the oxida nitric acid in absorption towers, leading the
tion- chamber 10fare ,led to similar absorp non-absorbed portion of the gases after a
tion ‘towers 11 as in the previously de~ treatment adapted to keep their content of
scribed installation. These towers are fed moisture below a determined limit back into
in contradistinction to the installation shown the. electric arc furnace, and feeding pure 120
55 in Figure 1 with dilute nitric acid, which is oxygen ‘and nitrogen continuously in such
cooled down to such a low temperature, that uantities to the returned gas-mixture that
the gases coming out of the last absorption t e gas-mixture treated in the furnace con
; tower are dried to such a degree, that the, tains 50% of oxygen and 50% of nitrogen.
gases can be led back to the electric furnace 2. The cyclical process of producing nitric 25
60 5 without affecting the intermedial appara acid by means of the electric arc which con
tus in any harmful manner. To arrive at sists in treating a nitrogen-ox gen mixture
this cooling e?ect, a nitric acid pump 15 is in an electric'arc furnace, cooling abruptly
connected to each absorption tower 11, which the gases leaving saidvelectric arc furnace
pump lifts the acid leaving the towers into and conserving the heat contained in said 30
66 a tank 12. From this tank the nitric acid gases, absorbing the nitric oxides thus formed
 1,462,987

by means of nitric acid in absorption towers, lation in the s stem and adapted to return
subjecting the non-absorbed gases to a treat said nonabsor gases for a repeated
ment causing their content of moisture to be treatment to said furnace,and means adapt
below a determined limit and returning said ed to introduce pure oxygen/and nitrogen
gases for a repeated treatment to the elec in such quantities into said returned gases 70
tric furnace, feeding pure oxygen and nitro that the gas-mixture treated in said furnace
gen continuously in such quantities to the contains 50% of oxygen and 50% of ni-.
returned gas-mixture that the gas-mixture trogen.
treated in the furnace contains 50% of 6. An‘ installation for producing nitric
10 oxygen and 50% of nitrogen, and maintain acid by means of the electric arc comprising 75
ing a pressure slightly below atmospheric 1n combination an electric arc furnace,
in the system to prevent any loss of nitric means to force a nitrogen-oxygen mixture
oxid gases. through said furnace, heat interchange
3. The cyclical process of producing nitric means adapted to abruptly cool the gas-mix
15 acid by means of the electric are which con ture leaving said furnace and to conserve 80
sists in treating a nitrogen-o gen mixture the heat contained in said gases, absorption
in an electric arc furnace, coo 'ng abruptly towers adapted to absorb nitric oxides
the‘ gases leaving said electric arc furnace formed, means adapted to keep the content
and conserving the heat contained in said of moisture in the non-absorbed gases below
20 gases, absorbing the nitric oxides thus formed a determined limit, means to maintain a 85
bymeans of nitric acid in absorption towers, circulation in the system and adapted to re
and maintainin a lowtemperature in the turn said nonabsorbed gases for a repeated
latter to'keep t e moisturg in the non-ab treatment to said furnace means adapted to
sorbed gases below a determined limit, re‘ introduce pure oxygen and nitrogen in such
25 turning said non-absorbed gases for a re quantities into said returned gases that the no
peated treatment to the electric arc furnace,
gas-mixture treated in said furnace contains
and feeding pure oxygen and nitrogen con— 50% of oxygen and 50% of nitrogen, and
tinuously in such uantities to the returned means adapted to maintain a pressure slight
gas-mixture that t e gas-mixture treated in ly below atmos heric in the system to pre
'30 the furnace contains 50% of oxygen and vent any loss 0 nitric oxid gases. 95
50% of nitrogen.‘ 7. An installation for producing nitric
4. The cyclical process of producing nitric acid by means of the electric arc compris
acid by means of the electric arc which con ing in combination an electric arc furnace,
s'sts in treating a nitrogen-oxygen mixture means to force a nitrogen-oxygen mixture
35 in an electric arc furnace, cooling abruptly through said furnace, heat interchange 100
the gases leaving said electric arc furnace means adapted to abruptly cool the gas-mix
and conserving the heat contained in said ture leaving said furnace and to conserve
gases, absorbing the nitric oxides thus formed the heat contained in said gases, absorption
by means of nitric acid inv absorption towers, towers adapted to absorb nitric oxides
40 and maintainin a low temperature in the formed, means adapted to maintain in said
latter to keep t e moisture in the non-ab absorption towers a temperature below 0° C.
sorbed gases below a determined limit, re to keep the content of moisture in the non
turning said, non-absorbed gases for a re absorbed gases below a determined limit,
peated treatment to the electric arc furnace, means to maintain a circulation in the sys
'45 and feeding pure oxygen and nitrogen con tem and adapted to return said nonabsorbed 110
tinuously in such uantities to the returned gases for a repeated treatment to said fur
gas-mixture that t e gas-mixture treated in nace, and means adapted to introduce pure
the furnace contains 50% of oxygen and oxygen and nitrogen in such quantities into
50% of nitrogen and that one quarter of the said returned gases that the gas-mixture
50 gas-mixture passing through the furnace can treated in said furnace contains 50% of oxy 116
continuously be discharged to avoid an ac gen and 50% of nitrogen.
cumulation of argon that exceeds a deter 8. An installation for producing nitric
mined percentage. acid by means of the electric arc comprising
5. An installation for producing nitric in combination an electric arc furnace,
55 acid by means of the electrlc arc comprising means to force a nitrogen-oxygen mix 120
in combination an electric arc furnace, means ture through said furnace, heat inter
to force a nitrogen-oxygen mixture through change means adapted to abruptly cool
said furnace, heat interchange means adapt the gas-mixture leaving said furnace and to
ed to abruptly cool the gas-mixture leaving conserve the heat contained in said gases,
60 said furnace and to conserve the heat con absorption towers adapted to absorb nitric 156
tained in said gases, absorption towers oxides formed, means ‘adapted to main
adapted to absorb nitric oxides formed, tain in said absorption towers a temper
means adapted to kee the content of mois ature below 0° C. to keep the content of
ture in the non-absor ed gases below a de moisture in the non-absorbed gases below a
65 termined limit, means to maintain a circu determined limit, means to maintain a circu
 4, _ - 1,462,987

lation in the system and adapted to return\ and means to permit of a continuous dis;
said non-absorbed gases fora re ated treat$°charge ofone quarter of the gas mixture _
ment to said furnace, means a apted to in- passing through the furnace to avoid an W
troduce pure nitrogen and oxygen in such accumulation of argon that exceeds a de
5 quantities into said returned gases that the termined percentage.
gas-mixture treated in said. furnace con- In testimony whereof I a?ix my signature.
tains 50% of oxygen and 50% of nitrogen, - DR. ‘WERNER SIEBERT.