DE1642944C3 - Process for the preparation of cobalt salt solutions from the oxo synthesis - Google Patents
Process for the preparation of cobalt salt solutions from the oxo synthesisInfo
- Publication number
- DE1642944C3 DE1642944C3 DE19671642944 DE1642944A DE1642944C3 DE 1642944 C3 DE1642944 C3 DE 1642944C3 DE 19671642944 DE19671642944 DE 19671642944 DE 1642944 A DE1642944 A DE 1642944A DE 1642944 C3 DE1642944 C3 DE 1642944C3
- Authority
- DE
- Germany
- Prior art keywords
- cobalt
- aqueous
- solution
- cobalt salt
- acid
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
- Expired
Links
- 239000012266 salt solution Substances 0.000 title claims description 29
- XCGBFXNVKPHVEQ-UHFFFAOYSA-N cobalt;2,3-dihydroxybutanedioic acid;ethane-1,2-diamine Chemical compound [Co].NCCN.NCCN.NCCN.OC(=O)C(O)C(O)C(O)=O XCGBFXNVKPHVEQ-UHFFFAOYSA-N 0.000 title claims description 28
- 125000004043 oxo group Chemical group O=* 0.000 title claims description 11
- 238000000034 method Methods 0.000 title claims description 10
- 238000002360 preparation method Methods 0.000 title claims 3
- 230000015572 biosynthetic process Effects 0.000 title 1
- 238000003786 synthesis reaction Methods 0.000 title 1
- 230000002194 synthesizing Effects 0.000 title 1
- 239000000243 solution Substances 0.000 claims description 25
- GUTLYIVDDKVIGB-UHFFFAOYSA-N cobalt Chemical compound [Co] GUTLYIVDDKVIGB-UHFFFAOYSA-N 0.000 claims description 23
- 229910052803 cobalt Inorganic materials 0.000 claims description 23
- 239000010941 cobalt Substances 0.000 claims description 23
- 229910052751 metal Inorganic materials 0.000 claims description 14
- 239000002184 metal Substances 0.000 claims description 14
- KDLHZDBZIXYQEI-UHFFFAOYSA-N palladium Chemical compound [Pd] KDLHZDBZIXYQEI-UHFFFAOYSA-N 0.000 claims description 9
- 150000001735 carboxylic acids Chemical class 0.000 claims description 8
- 238000006243 chemical reaction Methods 0.000 claims description 8
- 150000001869 cobalt compounds Chemical class 0.000 claims description 8
- 239000003054 catalyst Substances 0.000 claims description 7
- 239000008346 aqueous phase Substances 0.000 claims description 6
- 239000011541 reaction mixture Substances 0.000 claims description 6
- 239000001301 oxygen Substances 0.000 claims description 5
- MYMOFIZGZYHOMD-UHFFFAOYSA-N oxygen Chemical compound O=O MYMOFIZGZYHOMD-UHFFFAOYSA-N 0.000 claims description 5
- 229910052760 oxygen Inorganic materials 0.000 claims description 5
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 5
- 229910052763 palladium Inorganic materials 0.000 claims description 4
- PNEYBMLMFCGWSK-UHFFFAOYSA-N al2o3 Chemical compound [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 claims description 3
- 230000000875 corresponding Effects 0.000 claims description 2
- 239000007789 gas Substances 0.000 claims description 2
- 238000000926 separation method Methods 0.000 claims description 2
- 238000010626 work up procedure Methods 0.000 claims description 2
- 239000000969 carrier Substances 0.000 claims 6
- 239000002253 acid Substances 0.000 claims 4
- OKTJSMMVPCPJKN-UHFFFAOYSA-N carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims 4
- 150000002739 metals Chemical class 0.000 claims 4
- 230000001590 oxidative Effects 0.000 claims 4
- 230000002378 acidificating Effects 0.000 claims 3
- 125000004432 carbon atoms Chemical group C* 0.000 claims 3
- 239000000203 mixture Substances 0.000 claims 3
- XBDQKXXYIPTUBI-UHFFFAOYSA-N propionic acid Chemical compound CCC(O)=O XBDQKXXYIPTUBI-UHFFFAOYSA-N 0.000 claims 3
- FUZZWVXGSFPDMH-UHFFFAOYSA-N Hexanoic acid Chemical compound CCCCCC(O)=O FUZZWVXGSFPDMH-UHFFFAOYSA-N 0.000 claims 2
- KQNPFQTWMSNSAP-UHFFFAOYSA-N Isobutyric acid Chemical compound CC(C)C(O)=O KQNPFQTWMSNSAP-UHFFFAOYSA-N 0.000 claims 2
- 125000001931 aliphatic group Chemical group 0.000 claims 2
- 229910052799 carbon Inorganic materials 0.000 claims 2
- 239000007800 oxidant agent Substances 0.000 claims 2
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical compound [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 claims 2
- 239000010970 precious metal Substances 0.000 claims 2
- 150000003839 salts Chemical class 0.000 claims 2
- 239000011780 sodium chloride Substances 0.000 claims 2
- ODIGIKRIUKFKHP-UHFFFAOYSA-N (N-propan-2-yloxycarbonylanilino) acetate Chemical compound CC(C)OC(=O)N(OC(C)=O)C1=CC=CC=C1 ODIGIKRIUKFKHP-UHFFFAOYSA-N 0.000 claims 1
- SKYGTJFKXUWZMD-UHFFFAOYSA-N AC1L2N4H Chemical compound [Co].[Co] SKYGTJFKXUWZMD-UHFFFAOYSA-N 0.000 claims 1
- FERIUCNNQQJTOY-UHFFFAOYSA-N Butanoic acid Chemical compound CCCC(O)=O FERIUCNNQQJTOY-UHFFFAOYSA-N 0.000 claims 1
- 239000005977 Ethylene Substances 0.000 claims 1
- ZGEGCLOFRBLKSE-UHFFFAOYSA-N Heptene Chemical compound CCCCCC=C ZGEGCLOFRBLKSE-UHFFFAOYSA-N 0.000 claims 1
- JRZJOMJEPLMPRA-UHFFFAOYSA-N Nonene Chemical compound CCCCCCCC=C JRZJOMJEPLMPRA-UHFFFAOYSA-N 0.000 claims 1
- 150000001298 alcohols Chemical class 0.000 claims 1
- 150000001299 aldehydes Chemical class 0.000 claims 1
- 150000007933 aliphatic carboxylic acids Chemical class 0.000 claims 1
- 150000001336 alkenes Chemical class 0.000 claims 1
- 239000000956 alloy Substances 0.000 claims 1
- 229910045601 alloy Inorganic materials 0.000 claims 1
- UGFAIRIUMAVXCW-UHFFFAOYSA-N carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 claims 1
- 239000003795 chemical substances by application Substances 0.000 claims 1
- WHWBTOCNUBAGRL-UHFFFAOYSA-N cobalt;formaldehyde Chemical group [Co].O=C WHWBTOCNUBAGRL-UHFFFAOYSA-N 0.000 claims 1
- 150000001875 compounds Chemical class 0.000 claims 1
- 239000012043 crude product Substances 0.000 claims 1
- 230000000694 effects Effects 0.000 claims 1
- VGGSQFUCUMXWEO-UHFFFAOYSA-N ethene Chemical compound C=C VGGSQFUCUMXWEO-UHFFFAOYSA-N 0.000 claims 1
- 239000001257 hydrogen Substances 0.000 claims 1
- UFHFLCQGNIYNRP-UHFFFAOYSA-N hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 claims 1
- 229910052739 hydrogen Inorganic materials 0.000 claims 1
- 238000004519 manufacturing process Methods 0.000 claims 1
- 229910000510 noble metal Inorganic materials 0.000 claims 1
- 230000000737 periodic Effects 0.000 claims 1
- 229910052697 platinum Inorganic materials 0.000 claims 1
- 235000019260 propionic acid Nutrition 0.000 claims 1
- 239000002965 rope Substances 0.000 claims 1
- 239000000741 silica gel Substances 0.000 claims 1
- 229910002027 silica gel Inorganic materials 0.000 claims 1
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 claims 1
- 125000000383 tetramethylene group Chemical group [H]C([H])([*:1])C([H])([H])C([H])([H])C([H])([H])[*:2] 0.000 claims 1
- QTBSBXVTEAMEQO-UHFFFAOYSA-N acetic acid Chemical compound CC(O)=O QTBSBXVTEAMEQO-UHFFFAOYSA-N 0.000 description 18
- 239000002244 precipitate Substances 0.000 description 3
- 239000003610 charcoal Substances 0.000 description 2
- 239000011521 glass Substances 0.000 description 2
- IJGRMHOSHXDMSA-UHFFFAOYSA-N nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 2
- 125000004805 propylene group Chemical group [H]C([H])([H])C([H])([*:1])C([H])([H])[*:2] 0.000 description 2
- 239000011552 falling film Substances 0.000 description 1
- 238000010438 heat treatment Methods 0.000 description 1
- 229910052757 nitrogen Inorganic materials 0.000 description 1
- 239000000047 product Substances 0.000 description 1
- 230000002035 prolonged Effects 0.000 description 1
- 238000000746 purification Methods 0.000 description 1
- 239000003247 radioactive fallout Substances 0.000 description 1
- 238000004904 shortening Methods 0.000 description 1
Description
an der nach dem Verfahren der Erfindung zu verwendenden Carbonsäure, die bereits für die Entkobaltung zugefügt worden ist, so daß sich in diesem Falle eine weitere Zugabe an Carbonsäure erübrigt.on the carboxylic acid to be used according to the process of the invention, which is already used for cobalt removal has been added, so that in this case no further addition of carboxylic acid is necessary.
Es ist vorteilhaft, während der Behandlung der verdünnten Kobaltsalziösungen mit dem erfindungsgemäß zu verwendenden Metall Sauerstoff oder sauerstoffhaltige Gase, insbesondere Luft, durch die Lösung hindurchzuleiten, wodurch die Behandlungsdauer verkürzt werden kann.It is beneficial while treating the diluted Cobalt salt solutions with the metal to be used according to the invention, oxygen or oxygen-containing Passing gases, especially air, through the solution, thereby shortening the treatment time can be.
Man leitet zweckmäßig je Liter der verdünnten wäßrigen Kobaltsalzlösung etwa 0,5 bis 10 Normalliter Sauerstoff ein. It is expedient to introduce about 0.5 to 10 normal liters of oxygen per liter of the dilute aqueous cobalt salt solution.
Die nach der Behandlung mit dem Metall erhaltene Kobaltsalzlösung wird anschließend, zweckmäßig nach Abtrennen des Metalls, in üblicher Weise in. eine höherkonzentrierte Kobaltsalzlösung übergeführt. Dies kann z. B. unier Verwendung eines Fallstromverdampfers durchgeführt werden. Man destilliert zweckmäßig so viel Wasser ab, daß das Kobaltsalz der entsprechenden Carbonsäure gerade noch bei Raumtemperatur in Lösung bleibt. Man erhält so je nach der verwendeten Carbonsäure Kobaltsalzlösungen mit einem Kobaltgehalt von etwa 3 bis 8 Gewichtsprozent, die der Oxo-Reaktion in dieser Form als Katalysatorlösung wiederzugeführt werden.The cobalt salt solution obtained after the treatment with the metal is then, expediently, after Separation of the metal, converted in the usual way into a more highly concentrated cobalt salt solution. This can z. B. can be carried out using a falling film evaporator. It is expedient to distill in this way a lot of water so that the cobalt salt of the corresponding carboxylic acid is still in at room temperature Solution remains. Depending on the carboxylic acid used, cobalt salt solutions with a cobalt content are obtained from about 3 to 8 percent by weight, which is fed back to the oxo reaction in this form as a catalyst solution will.
Die in den Beispielen angegebenenTeile sind Gewichtsteile. Sie verhalten sich zu den Volumenteilen wie g zu 1.The parts given in the examples are parts by weight. They are related to parts by volume like g to 1.
Eine wäßrige Kobaltsalzlösung, welche erhalten wird, indem man ein aus Propylen erhaltenes Oxoreaktionsgemisch bei 1150C in Gegenwart von verdünnter wäßriger Essigsäure mit Luft behandelt und anschließend die wäßrige Phase abtrennt, enthält 1,14 Gewichtsprozent Kobalt. 100 Teile dieser Lösung werden nach Zugabe von 3 Teilen 99gewichtsprozentiger Essigsäure unter Durchleiten von 3 Volumenteilen Luft mit 3 Teilen Palladium-Tierkohle 30 min bei 95 bis 100° C gerührt. Nach dem Absaugen von Palladium-Tierkohle wird aus der erhaltenen Lösung durch Abdestillieren von Wasser eine 7 gewichtsprozentige Kobalt enthaltende Lösung hergestellt, aus der auch nach längerem Stehen bei 200C keine Kobaltverbindung ausfällt. Bei der Palladium-Tierkohle wird auch nach 5facher Wiederverwendung keine Abnahme der Wirksamkeit bei der Aufarbeitung der verdünnten wäßrigen Kobaltsalzlösung beobachtet.An aqueous cobalt salt solution, which is obtained by treating a product obtained from propylene Oxoreaktionsgemisch at 115 0 C in the presence of dilute aqueous acetic acid with air and subsequently separating the aqueous phase containing 1.14 weight percent cobalt. 100 parts of this solution are, after addition of 3 parts of 99% strength by weight acetic acid, stirred with 3 parts of palladium-animal charcoal for 30 minutes at 95 to 100 ° C. while 3 parts by volume of air are passed through. After the palladium charcoal has been suctioned off, a solution containing 7 percent by weight cobalt is produced from the solution obtained by distilling off water, from which no cobalt compound precipitates even after prolonged standing at 20 ° C. In the case of palladium animal charcoal, even after being reused five times, no decrease in the effectiveness of the work-up of the dilute aqueous cobalt salt solution is observed.
Versucht man dagegen die ursprüngliche verdünnte wäßrige Kobaltsalzlösung in eine höherkonzentrierte Lösung überzuführen, so fallen bei 200C bereits ab einer Kobalt-Konzentration von etwa 1,5 Gewichtsprozent Kobaltverbindungen aus.If, on the other hand, an attempt is made to convert the original dilute aqueous cobalt salt solution into a more highly concentrated solution, cobalt compounds precipitate at 20 ° C. from a cobalt concentration of about 1.5 percent by weight.
Eine wäßrige Kobaltsalzlösung, welche erhalten wird, indem man ein aus isomeren Heptenen erhaltenes Oxoreaktionsgemisch bei 115° C in Gegenwart vonAn aqueous cobalt salt solution which is obtained by mixing an isomeric heptene Oxo reaction mixture at 115 ° C in the presence of
xo verdünnter wäßriger Essigsäure mit Luft behandelt und anschließend die wäßrige Phase abtrennt, enthält 0,95 Gewichtsprozent Kobalt. 0,3 l/h dieser Lösung werden ohne weitere Reinigung nach Zugabe von 2,5 g 99gewichtsprozentiger Essigsäure je 100 ml Lösung von oben durch ein Glasrohr von 55 cm Länge und 3 cm Durchmesser geleitet, welches mit 210 g (300 ml) eines Katalysators aus 1 Gewichtsprozent Palladium auf Aluminiumoxid gefüllt ist, wobei im Inneren des Glasrohrs eine Temperatur zwischen 85 und 900C durch Heizung von außen aufrechterhalten wird. Außerdem werden vom unteren Ende des Rohres her 3 l/h Luft eingeleitet. Die am unteren Ende des Rohres abfließende Konaltsalzlösung wird auf einen Gehalt von 4,52 Gewichtsprozent Kobalt einge-Treated xo dilute aqueous acetic acid with air and then separating off the aqueous phase, contains 0.95 percent by weight cobalt. 0.3 l / h of this solution are passed without further purification after adding 2.5 g of 99 weight percent acetic acid per 100 ml of solution from above through a glass tube 55 cm in length and 3 cm in diameter, which is filled with 210 g (300 ml) of a catalyst is filled from 1 percent by weight palladium on aluminum oxide, with a temperature between 85 and 90 0 C being maintained inside the glass tube by heating from the outside. In addition, 3 l / h of air are introduced from the lower end of the pipe. The conalt salt solution flowing off at the lower end of the pipe is brought to a cobalt content of 4.52 percent by weight.
a5 engt. Aus der erhaltenen Lösung fallen auch nach lOtägigem Stehen bei 2O0C keine Kobaltverbindungen aus. Engt man dagegen die ursprüngliche Lösung ein, so fallen bereits bei einer Kobaltkonzentration von 1,9 Gewichtsprozent Kobaltverbindungen aus. a 5 narrows. No cobalt compounds fall out even after lOtägigem standing at 2O 0 C from the resulting solution. If, on the other hand, the original solution is concentrated, cobalt compounds precipitate at a cobalt concentration of 1.9 percent by weight.
Eine wäßrige Kobaltsalzlösung, welche erhalten wird, indem man ein aus Propylen erhaltenes Oxoreaktionsgemisch bei 115° C in Gegenwart von verdünnter Essigsäure mit Luft behandelt und anschließend die wäßrige Phase abtrennt, enthält 0,93 Gewichtsprozent Kobalt. 100 Teile dieser Lösung werden mit 2,37 Teilen 99 gewichtsprozentiger Essigsäure versetzt. Wie in Beispiel 2 beschrieben, leitet man stündlich 0,2 1 dieser Lösung über einen Katalysator aus Palladium auf Aluminiumoxid und führt von unten anstatt Luft stündlich 3 1 Stickstoff zu.An aqueous cobalt salt solution obtained by adding an oxo reaction mixture obtained from propylene at 115 ° C in the presence of dilute Treated acetic acid with air and then separating off the aqueous phase, contains 0.93 percent by weight Cobalt. 100 parts of this solution are combined with 2.37 parts of 99 percent strength by weight acetic acid offset. As described in Example 2, 0.2 l of this solution is passed over a catalyst every hour made of palladium on aluminum oxide and feeds 3 liters of nitrogen per hour from below instead of air.
Die am unteren Ende des Rohres abschließende Kobaltsalzlösung wird auf einen Gehalt von 4,65 Gewichtsprozent Kobalt eingeengt. Aus der erhaltenen Lösung fallen auch nach lOtägigem Stehen bei 20°C keine K obaltverbindungen aus. Engt man dagegen die ursprüngliche Lösung ein, so fallen bereits bei einerThe cobalt salt solution at the bottom of the pipe is reduced to a content of 4.65 percent by weight Cobalt concentrated. The solution obtained also falls after standing at 20 ° C. for 10 days no cold connections. If, on the other hand, you narrow down the original solution, one already falls
Konzentration von 1,4 Gewichtsprozent Kobaltverbindungen aus.Concentration of 1.4 percent by weight of cobalt compounds.
Claims (2)
Priority Applications (1)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
US781636A US3607786A (en) | 1967-12-07 | 1968-12-05 | Production of a concentrated aqueous cobalt salt solution |
Applications Claiming Priority (2)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
DEB0095731 | 1967-12-07 | ||
DEB0095731 | 1967-12-07 |
Publications (3)
Publication Number | Publication Date |
---|---|
DE1642944A1 DE1642944A1 (en) | 1971-05-19 |
DE1642944B2 DE1642944B2 (en) | 1975-06-12 |
DE1642944C3 true DE1642944C3 (en) | 1976-02-19 |
Family
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