DE1265133B - Process for the anion exchange of hydrogen acids - Google Patents
Process for the anion exchange of hydrogen acidsInfo
- Publication number
- DE1265133B DE1265133B DEC34894A DEC0034894A DE1265133B DE 1265133 B DE1265133 B DE 1265133B DE C34894 A DEC34894 A DE C34894A DE C0034894 A DEC0034894 A DE C0034894A DE 1265133 B DE1265133 B DE 1265133B
- Authority
- DE
- Germany
- Prior art keywords
- exchange
- anion exchange
- anions
- hydrogen acids
- hydroxysodalite
- 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.)
- Pending
Links
- 238000000034 method Methods 0.000 title claims description 10
- 239000002253 acid Substances 0.000 title claims description 9
- -1 hydrogen acids Chemical class 0.000 title claims description 9
- 239000001257 hydrogen Substances 0.000 title claims description 8
- 229910052739 hydrogen Inorganic materials 0.000 title claims description 8
- 238000005349 anion exchange Methods 0.000 title claims description 4
- 150000001450 anions Chemical class 0.000 claims description 16
- BFRXZIMAUMUZJH-UHFFFAOYSA-M [OH-].[Na+].[Na+].[Na+].[Na+].[Al+3].[Al+3].[Al+3].[O-][Si]([O-])([O-])[O-].[O-][Si]([O-])([O-])[O-].[O-][Si]([O-])([O-])[O-] Chemical group [OH-].[Na+].[Na+].[Na+].[Na+].[Al+3].[Al+3].[Al+3].[O-][Si]([O-])([O-])[O-].[O-][Si]([O-])([O-])[O-].[O-][Si]([O-])([O-])[O-] BFRXZIMAUMUZJH-UHFFFAOYSA-M 0.000 claims description 9
- 150000002500 ions Chemical class 0.000 claims description 9
- 239000000243 solution Substances 0.000 claims description 6
- 239000007864 aqueous solution Substances 0.000 claims description 5
- 239000000126 substance Substances 0.000 claims description 3
- 125000002887 hydroxy group Chemical group [H]O* 0.000 claims description 2
- HEMHJVSKTPXQMS-UHFFFAOYSA-M Sodium hydroxide Chemical compound [OH-].[Na+] HEMHJVSKTPXQMS-UHFFFAOYSA-M 0.000 description 9
- 239000000460 chlorine Substances 0.000 description 6
- FAPWRFPIFSIZLT-UHFFFAOYSA-M Sodium chloride Chemical compound [Na+].[Cl-] FAPWRFPIFSIZLT-UHFFFAOYSA-M 0.000 description 4
- 150000001768 cations Chemical class 0.000 description 4
- GUJOJGAPFQRJSV-UHFFFAOYSA-N dialuminum;dioxosilane;oxygen(2-);hydrate Chemical compound O.[O-2].[O-2].[O-2].[Al+3].[Al+3].O=[Si]=O.O=[Si]=O.O=[Si]=O.O=[Si]=O GUJOJGAPFQRJSV-UHFFFAOYSA-N 0.000 description 4
- 229910052901 montmorillonite Inorganic materials 0.000 description 4
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 4
- 239000013078 crystal Substances 0.000 description 3
- 229910052500 inorganic mineral Inorganic materials 0.000 description 3
- 239000011707 mineral Substances 0.000 description 3
- 235000010755 mineral Nutrition 0.000 description 3
- 239000000203 mixture Substances 0.000 description 3
- 235000011121 sodium hydroxide Nutrition 0.000 description 3
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 description 2
- 229910052802 copper Inorganic materials 0.000 description 2
- 239000010949 copper Substances 0.000 description 2
- 239000007788 liquid Substances 0.000 description 2
- 150000003839 salts Chemical class 0.000 description 2
- 239000011780 sodium chloride Substances 0.000 description 2
- IVORCBKUUYGUOL-UHFFFAOYSA-N 1-ethynyl-2,4-dimethoxybenzene Chemical compound COC1=CC=C(C#C)C(OC)=C1 IVORCBKUUYGUOL-UHFFFAOYSA-N 0.000 description 1
- ZSLUVFAKFWKJRC-IGMARMGPSA-N 232Th Chemical compound [232Th] ZSLUVFAKFWKJRC-IGMARMGPSA-N 0.000 description 1
- 229910018072 Al 2 O 3 Inorganic materials 0.000 description 1
- ZAMOUSCENKQFHK-UHFFFAOYSA-N Chlorine atom Chemical compound [Cl] ZAMOUSCENKQFHK-UHFFFAOYSA-N 0.000 description 1
- 229910019142 PO4 Inorganic materials 0.000 description 1
- 229910004298 SiO 2 Inorganic materials 0.000 description 1
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 1
- 229910021607 Silver chloride Inorganic materials 0.000 description 1
- 229910052776 Thorium Inorganic materials 0.000 description 1
- QCWXUUIWCKQGHC-UHFFFAOYSA-N Zirconium Chemical compound [Zr] QCWXUUIWCKQGHC-UHFFFAOYSA-N 0.000 description 1
- 150000007513 acids Chemical class 0.000 description 1
- 239000012670 alkaline solution Substances 0.000 description 1
- WNROFYMDJYEPJX-UHFFFAOYSA-K aluminium hydroxide Chemical compound [OH-].[OH-].[OH-].[Al+3] WNROFYMDJYEPJX-UHFFFAOYSA-K 0.000 description 1
- 230000015556 catabolic process Effects 0.000 description 1
- 229910052801 chlorine Inorganic materials 0.000 description 1
- 238000004140 cleaning Methods 0.000 description 1
- 150000001875 compounds Chemical class 0.000 description 1
- 239000002826 coolant Substances 0.000 description 1
- 238000001816 cooling Methods 0.000 description 1
- 238000005260 corrosion Methods 0.000 description 1
- 230000007797 corrosion Effects 0.000 description 1
- 238000006731 degradation reaction Methods 0.000 description 1
- 238000010612 desalination reaction Methods 0.000 description 1
- 239000012153 distilled water Substances 0.000 description 1
- 238000002474 experimental method Methods 0.000 description 1
- 238000000605 extraction Methods 0.000 description 1
- 150000004679 hydroxides Chemical class 0.000 description 1
- 238000005342 ion exchange Methods 0.000 description 1
- 238000004519 manufacturing process Methods 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 230000007935 neutral effect Effects 0.000 description 1
- 230000035699 permeability Effects 0.000 description 1
- 235000021317 phosphate Nutrition 0.000 description 1
- 150000003013 phosphoric acid derivatives Chemical class 0.000 description 1
- 238000002360 preparation method Methods 0.000 description 1
- 230000005855 radiation Effects 0.000 description 1
- 230000000630 rising effect Effects 0.000 description 1
- 229920006395 saturated elastomer Polymers 0.000 description 1
- HKZLPVFGJNLROG-UHFFFAOYSA-M silver monochloride Chemical compound [Cl-].[Ag+] HKZLPVFGJNLROG-UHFFFAOYSA-M 0.000 description 1
- 229910001415 sodium ion Inorganic materials 0.000 description 1
- SFKTYEXKZXBQRQ-UHFFFAOYSA-J thorium(4+);tetrahydroxide Chemical compound [OH-].[OH-].[OH-].[OH-].[Th+4] SFKTYEXKZXBQRQ-UHFFFAOYSA-J 0.000 description 1
- 229910052726 zirconium Inorganic materials 0.000 description 1
- 229910000166 zirconium phosphate Inorganic materials 0.000 description 1
- LEHFSLREWWMLPU-UHFFFAOYSA-B zirconium(4+);tetraphosphate Chemical compound [Zr+4].[Zr+4].[Zr+4].[O-]P([O-])([O-])=O.[O-]P([O-])([O-])=O.[O-]P([O-])([O-])=O.[O-]P([O-])([O-])=O LEHFSLREWWMLPU-UHFFFAOYSA-B 0.000 description 1
Classifications
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J41/00—Anion exchange; Use of material as anion exchangers; Treatment of material for improving the anion exchange properties
- B01J41/08—Use of material as anion exchangers; Treatment of material for improving the anion exchange properties
- B01J41/10—Inorganic material
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J41/00—Anion exchange; Use of material as anion exchangers; Treatment of material for improving the anion exchange properties
- B01J41/02—Processes using inorganic exchangers
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B39/00—Compounds having molecular sieve and base-exchange properties, e.g. crystalline zeolites; Their preparation; After-treatment, e.g. ion-exchange or dealumination
- C01B39/50—Zeolites wherein inorganic bases or salts occlude channels in the lattice framework, e.g. sodalite, cancrinite, nosean, hauynite
Landscapes
- Chemical & Material Sciences (AREA)
- Organic Chemistry (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Inorganic Chemistry (AREA)
- Life Sciences & Earth Sciences (AREA)
- General Life Sciences & Earth Sciences (AREA)
- Geology (AREA)
- Engineering & Computer Science (AREA)
- Materials Engineering (AREA)
- Organic Low-Molecular-Weight Compounds And Preparation Thereof (AREA)
- Agricultural Chemicals And Associated Chemicals (AREA)
Description
DEUTSCHESGERMAN
PATENTAMTPATENT OFFICE
AUSLEGESCHRIFTEDITORIAL
Int. Cl.: Int. Cl .:
BOIdBOId
Deutsche Kl.: 12 d-1/03 German class: 12 d- 1/03
Nummer: 1 265 133Number: 1 265 133
Aktenzeichen: C 34894IV a/12 dFile number: C 34894IV a / 12 d
Anmeldetag: 19. Januar 1965Filing date: January 19, 1965
Auslegetag: 4. April 1968Open date: April 4, 1968
Die Erfindung betrifft ein Verfahren zum Austausch von Anionen, wodurch man Anionen von Wasserstoffsäuren (sauerstofffreien Säuren) aus einer wäßrigen alkalischen Lösung bei Temperaturen in der Nähe von oder über 2000C unter dem entsprechenden Wasserdampfdruck entfernen kann.The invention relates to a method for exchanging anions, whereby anions of hydrogen acids (oxygen-free acids) can be removed from an aqueous alkaline solution at temperatures close to or above 200 ° C. under the corresponding water vapor pressure.
Es gibt eine große Zahl von Anionenaustauschern organischer Herkunft, die sich dazu eignen, aus einer wäßrigen Lösung Wasserstoffsäurenanionen zu extrahieren, jedoch nur in einem begrenzten Temperaturbereich verwendet werden können, da sie bei Temperaturen über 1000C einen sehr raschen Abbau erfahren. Für bestimmte technische Anwendungszwecke benötigt man Anionenaustauscher, die bei höheren Temperaturen, beispielsweise über 2000C, beständig sind. Ein solches Anwendungsgebiet ist beispielsweise die Reinigung des Kühlmediums eines Kernreaktors, wenn dieses Medium Wasserdampf ist. Ein solcher Austauscher muß außerdem folgende Bedingungen erfüllen: Strahlungsbeständigkeit bei Gewährleistung einer guten Entsalzung der zu behandelnden Flüssigkeit; Austausch nur von OH~-Ionen sowie schließlich leichte Durchlässigkeit für die zu reinigende Flüssigkeit. There are a large number of anion exchangers of organic origin, which are used to extract Wasserstoffsäurenanionen from an aqueous solution, but can be used only in a limited temperature range, as they experience a very rapid degradation at temperatures above 100 0C. Anion exchangers which are stable at higher temperatures, for example above 200 ° C., are required for certain technical purposes. One such area of application is, for example, cleaning the cooling medium of a nuclear reactor when this medium is water vapor. Such an exchanger must also meet the following conditions: resistance to radiation while ensuring good desalination of the liquid to be treated; Exchange only of OH ~ ions and finally slight permeability for the liquid to be cleaned.
Man hat sehr bald das Augenmerk gerichtet auf mineralische Ionenaustauscher, die aus natürlichen Mineralien vom Typ Montmorillonit und synthetischen Mineralien (Salze sehr geringer Löslichkeit, Phosphate und Hydroxide von Zirkonium und Thorium) bestehen.Very soon the focus was on mineral ion exchangers made from natural Minerals of the montmorillonite type and synthetic minerals (salts of very low solubility, Phosphates and hydroxides of zirconium and thorium).
Der Montmorillonit, ein Silikoaluminat, ist zwar kein Anionenaustauscher, kann jedoch nach Sättigung mit Ag+-Kationen bestimmte Salze, d. h. deren Anionen gleichzeitig mit den Kationen, binden, beispielsweise Cl~ und das zugehörige Kation (wie NH4 +) nach dem Schema:Montmorillonite, a silicoaluminate, is not an anion exchanger, but after saturation with Ag + cations it can bind certain salts, i.e. their anions at the same time as the cations, for example Cl ~ and the associated cation (such as NH 4 + ) according to the scheme:
Mt — Ag + NH4Cl -> Mt(AgCl)NH4 Mt - Ag + NH 4 Cl -> Mt (AgCl) NH 4
Seine Bindekapazität beträgt ungefähr 0,6 mäqu. pro Gramm Montmorillonit.Its binding capacity is approximately 0.6 meq. per gram of montmorillonite.
Die Verwendung von mit Kationen gesättigtem Montmorillonit zur Abtrennung von Anionen aus Lösungen ist jedoch auf besondere Fälle beschränkt, und außerdem verliert er seine Wirksamkeit mit steigender Temperatur.The use of montmorillonite saturated with cations to separate anions from However, solutions is limited to special cases, and it also loses its effectiveness rising temperature.
Als Anionenaustauscher mit einer guten Beständigkeit bei erhöhten Temperaturen verwendet man auch
Thoriumhydroxid und eine Mischung von Zirkoniumhydroxid und Zirkoniumphosphat. Diese Austauscher
sind besonders geeignet für den Austausch von Anionen, die in sehr geringer Konzentration in einer
Lösung vorhanden sind; sie besitzen jedoch eine sehr Verfahren zum Anionenaustausch
von WasserstoffsäurenThorium hydroxide and a mixture of zirconium hydroxide and zirconium phosphate are also used as anion exchangers with good resistance to elevated temperatures. These exchangers are particularly suitable for the exchange of anions which are present in a solution in very low concentrations; however, they have a very good anion exchange process
of hydrogen acids
Anmelder:Applicant:
Commissariat ä l'Energie Atomique, ParisCommissariat a l'Energie Atomique, Paris
Vertreter:Representative:
Dr. H. U. May, Patentanwalt,
8000 München 2, Ottostr. 1 aDr. HU May, patent attorney,
8000 Munich 2, Ottostr. 1 a
Als Erfinder benannt:Named as inventor:
Jean Louis Guth,Jean Louis Guth,
Raymond Wey,Raymond Wey,
Mulhouse, Haut-Rhin (Frankreich)Mulhouse, Haut-Rhin (France)
Beanspruchte Priorität:Claimed priority:
Frankreich vom 27. Januar 1964 (961 689)France of January 27, 1964 (961 689)
viel geringere Extraktionskapazität als die organischen Austauscher.much lower extraction capacity than the organic ones Exchanger.
Die Erfindung bezweckt ein Verfahren zum Austausch von Anionen, wodurch aus einer wäßrigen Lösung bei erhöhten Temperaturen Anionen von Wasserstoffsäuren mit guten Ausbeuten entfernt werden können.The invention aims a process for the exchange of anions, whereby from an aqueous Solution removed at elevated temperatures anions of hydrogen acids with good yields can be.
Es wurde gefunden, daß der Hydroxysodalith, eine synthetische Verbindung mit kubischer Struktur und der FormelIt has been found that the hydroxysodalite, a synthetic compound with a cubic structure and the formula
3 (Al2O3, 2 SiO2, Na2O) 2 NaOH3 (Al 2 O 3 , 2 SiO 2 , Na 2 O) 2 NaOH
dessen Herstellung von B a r r e r und White in Journal of the Chemical Society, London, 1952, S. 1566/1567, beschrieben wurde und von dem aus der gleichen Veröffentlichung nur bekannt ist, daß er Nationen des im Kristallgitter enthaltenen NaOH gegen H+-Ionen von gasförmigem HCl austauscht, wobei die Na+-Ionen aus dem Kristall herauswandern, in wäßriger Lösung die OH~-Ionen gegen Anionen von Wasserstoffsäuren, wie Cl~, Br~, J-, unter Erhaltung seiner Struktur austauscht.the preparation of which was described by B arrer and White in Journal of the Chemical Society, London, 1952, p. 1566/1567, and of which it is only known from the same publication that the NaOH contained in the crystal lattice is against H + ions exchanged by gaseous HCl, the Na + ions migrate out of the crystal, exchanging the OH ~ ions in aqueous solution for anions of hydrogen acids, such as Cl ~, Br ~, J-, while maintaining its structure.
Das erfindungsgemäße Verfahren zum Anionenaustausch von Wasserstoffsäuren in wäßriger Lösung bei erhöhten Temperaturen mittels hydroxylgruppenhaltiger anorganischer Austauscher ist dadurch ge-The inventive method for the anion exchange of hydrogen acids in aqueous solution at elevated temperatures using inorganic exchangers containing hydroxyl groups, this
809 537/495809 537/495
kennzeichnet, daß man als Anionenaustauscher Hydroxysodalith in schwach alkalischem Milieu bei einer Temperatur nahe bei oder über 200° C verwendet.indicates that the anion exchanger is hydroxysodalite in a weakly alkaline environment at a Temperature close to or above 200 ° C used.
Nach dem erfindungsgemäßen Verfahren geschieht der Austausch in schwach alkalischem Milieu vorzugsweise bei einer OH~-Ionenkonzentration in der Nähe von n/10. Obgleich der Austausch auch in neutralem Milieu vor sich geht, wählt man ein alkalisches Milieu, um eine gute Stabilität des Hydroxysodaliths zu erhalten.According to the method according to the invention, the exchange preferably takes place in a weakly alkaline medium at an OH ~ ion concentration close to n / 10. Although the exchange is also in neutral milieu is going on, one chooses an alkaline milieu in order to have a good stability of the hydroxysodalite to obtain.
Das Verfahren wird in einer gegen die alkalische Korrosion und den Druck beständigen Apparatur durchgeführt.The process is carried out in an apparatus resistant to alkaline corrosion and pressure carried out.
Im folgenden ist ein Ausführungsbeispiel des erfindungsgemäßen Verfahrens beschrieben, ohne die Erfindung damit zu begrenzen, die im Rahmen der chemischen Äquivalente alle Abwandlungen einschließt. In the following an embodiment of the method according to the invention is described without the invention with it, which includes all modifications within the framework of the chemical equivalents.
IOIO
Der Ionenaustausch wird in geschlossenen Kupferrohren durchgeführt, die sich in einem Autoklav befinden.The ion exchange is carried out in closed copper tubes, which are located in an autoclave are located.
Eine Versuchsreihe wurde in einem Autoklav bei 250° C und bei sehr verschiedenen Werten des pH und der Gh-Ionenkonzentrationen durchgeführt.A series of tests was carried out in an autoclave at 250 ° C. and at very different values of pH and of the Gh ion concentrations.
Proben von 400 mg Hydroxysodalith wurden mit cm3 der die Cl~- und OH~-Ionen enthaltenden Lösung zusammengebracht.Samples of 400 mg hydroxysodalite were brought together with cm 3 of the solution containing the Cl ~ and OH ~ ions.
Die Q--Ionen wurden in der Lösung vor und nach dem Austausch bestimmt. Chlorgehaltsbestimmungen wurden am Hydroxysodalith nach dem Austausch vorgenommen. Die erhaltenen Ergebnisse sind in der folgenden Tabelle zusammengestellt und zeigen die selektive Fixierung von Anionen von Wasserstoffsäuren durch den Hydroxysodalith.The Q ions were determined in the solution before and after the exchange. Chlorine content regulations were made on the hydroxysodalite after the exchange. The results obtained are in the The following table compiled and show the selective fixation of anions of hydrogen acids by the hydroxysodalite.
konzentration
an OH-
(in n/100)At first
concentration
at OH-
(in n / 100)
pro 100 g
Austauscher
(vor Austausch)mäqu. NaCl
per 100 g
Exchanger
(before exchange)
an Q-
(in n/100)Final concentration
at Q-
(in n / 100)
in Lösung
geblieben . 0 / ° .. a ~
in solution
remained
konzentration
an Cl-
(in n/100)At first
concentration
at Cl-
(in n / 100)
in 100 g
Austauscher
(nach dem
Austausch)mäqu. NaCl
in 100 g
Exchanger
(after this
Exchange)
Der für diese Versuche verwendete Hydroxysodaüth wurde auf folgende Weise hergestellt:The Hydroxysodaüth used for these experiments was prepared in the following way:
Eine Mischung von 1 Grammol amorphem Siliciumdioxid, 1 Grammol Aluminiumhydroxid, 5 Grammol Ätznatron und 35 Grammol Wasser wird in einem innen mit Kupfer ausgekleideten Autoklav 5 Tage auf ungefähr 325° C erhitzt. Nach dem Abkühlen wird die Mischung filtriert, und die Hydroxysodalithkristalle werden mit destilliertem Wasser gewaschen und bei 400C getrocknet. Die erhaltenen Kristalle sind kubisch und haben Abmessungen zwischen 10 und 50 μ.A mixture of 1 gramol amorphous silica, 1 gramol aluminum hydroxide, 5 gramol caustic soda, and 35 gramol water is heated to approximately 325 ° C for 5 days in an internally lined copper autoclave. After cooling, the mixture is filtered and the Hydroxysodalithkristalle are washed with distilled water and dried at 40 0 C. The crystals obtained are cubic and have dimensions between 10 and 50 μ.
Für die Herstellung von Hydroxysodalith wird kein Schutz beansprucht.No protection is claimed for the manufacture of hydroxysodalite.
Claims (2)
D'Ans — Lax, »Taschenbuch für Chemiker undConsidered publications:
D'Ans - Lax, »Paperback for chemists and
»Journal of the Chemical Society«, London, 1952,Physicist «, 2nd edition. 1949, p. 306;
"Journal of the Chemical Society", London, 1952,
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| FR961689A FR1393380A (en) | 1964-01-27 | 1964-01-27 | Process for removing anions derived from hydracids from a solution |
Publications (1)
| Publication Number | Publication Date |
|---|---|
| DE1265133B true DE1265133B (en) | 1968-04-04 |
Family
ID=8821803
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| DEC34894A Pending DE1265133B (en) | 1964-01-27 | 1965-01-19 | Process for the anion exchange of hydrogen acids |
Country Status (8)
| Country | Link |
|---|---|
| CH (1) | CH431468A (en) |
| DE (1) | DE1265133B (en) |
| ES (1) | ES308614A1 (en) |
| FR (1) | FR1393380A (en) |
| GB (1) | GB1063259A (en) |
| IL (1) | IL22798A (en) |
| LU (1) | LU47853A1 (en) |
| NL (1) | NL6501021A (en) |
-
1964
- 1964-01-18 IL IL2279864A patent/IL22798A/en unknown
- 1964-01-27 FR FR961689A patent/FR1393380A/en not_active Expired
-
1965
- 1965-01-15 CH CH57365A patent/CH431468A/en unknown
- 1965-01-18 GB GB219365A patent/GB1063259A/en not_active Expired
- 1965-01-19 DE DEC34894A patent/DE1265133B/en active Pending
- 1965-01-26 LU LU47853A patent/LU47853A1/xx unknown
- 1965-01-27 ES ES0308614A patent/ES308614A1/en not_active Expired
- 1965-01-27 NL NL6501021A patent/NL6501021A/xx unknown
Non-Patent Citations (1)
| Title |
|---|
| None * |
Also Published As
| Publication number | Publication date |
|---|---|
| ES308614A1 (en) | 1965-05-16 |
| FR1393380A (en) | 1965-03-26 |
| LU47853A1 (en) | 1965-03-26 |
| CH431468A (en) | 1967-03-15 |
| IL22798A (en) | 1968-09-26 |
| NL6501021A (en) | 1965-07-28 |
| GB1063259A (en) | 1967-03-30 |
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