ITMI941320A1 - Composizione marcante-denaturante particolarmente adatta per marcare e denaturare combustibili - Google Patents
Composizione marcante-denaturante particolarmente adatta per marcare e denaturare combustibili Download PDFInfo
- Publication number
- ITMI941320A1 ITMI941320A1 IT001320A ITMI941320A ITMI941320A1 IT MI941320 A1 ITMI941320 A1 IT MI941320A1 IT 001320 A IT001320 A IT 001320A IT MI941320 A ITMI941320 A IT MI941320A IT MI941320 A1 ITMI941320 A1 IT MI941320A1
- Authority
- IT
- Italy
- Prior art keywords
- denaturing
- marking
- fuels
- composition according
- liquefiable
- Prior art date
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- 239000000446 fuel Substances 0.000 title claims description 26
- 239000000203 mixture Substances 0.000 title claims description 16
- 239000003915 liquefied petroleum gas Substances 0.000 claims description 12
- YRKCREAYFQTBPV-UHFFFAOYSA-N acetylacetone Chemical compound CC(=O)CC(C)=O YRKCREAYFQTBPV-UHFFFAOYSA-N 0.000 claims description 10
- 239000007788 liquid Substances 0.000 claims description 10
- 230000006835 compression Effects 0.000 claims description 6
- 238000007906 compression Methods 0.000 claims description 6
- HYBBIBNJHNGZAN-UHFFFAOYSA-N furfural Chemical compound O=CC1=CC=CO1 HYBBIBNJHNGZAN-UHFFFAOYSA-N 0.000 claims description 6
- 125000004178 (C1-C4) alkyl group Chemical group 0.000 claims description 5
- 150000001875 compounds Chemical class 0.000 claims description 5
- 229910052736 halogen Chemical group 0.000 claims description 4
- 150000002367 halogens Chemical group 0.000 claims description 4
- 125000003118 aryl group Chemical group 0.000 claims description 2
- 239000000975 dye Substances 0.000 claims description 2
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 claims 1
- 125000000217 alkyl group Chemical group 0.000 claims 1
- 239000002635 aromatic organic solvent Substances 0.000 claims 1
- 239000003153 chemical reaction reagent Substances 0.000 description 11
- 238000012360 testing method Methods 0.000 description 10
- 239000003550 marker Substances 0.000 description 9
- 239000003921 oil Substances 0.000 description 4
- OKKJLVBELUTLKV-UHFFFAOYSA-N Methanol Chemical compound OC OKKJLVBELUTLKV-UHFFFAOYSA-N 0.000 description 3
- 238000000034 method Methods 0.000 description 3
- 239000000243 solution Substances 0.000 description 3
- 239000002904 solvent Substances 0.000 description 3
- 239000000126 substance Substances 0.000 description 3
- VHBSECWYEFJRNV-UHFFFAOYSA-N 2-hydroxybenzoic acid Chemical compound OC(=O)C1=CC=CC=C1O.OC(=O)C1=CC=CC=C1O VHBSECWYEFJRNV-UHFFFAOYSA-N 0.000 description 2
- 230000036425 denaturation Effects 0.000 description 2
- 238000004925 denaturation Methods 0.000 description 2
- 239000002283 diesel fuel Substances 0.000 description 2
- 238000004821 distillation Methods 0.000 description 2
- ZXEKIIBDNHEJCQ-UHFFFAOYSA-N isobutanol Chemical compound CC(C)CO ZXEKIIBDNHEJCQ-UHFFFAOYSA-N 0.000 description 2
- 239000003208 petroleum Substances 0.000 description 2
- VTLYFUHAOXGGBS-UHFFFAOYSA-N Fe3+ Chemical class [Fe+3] VTLYFUHAOXGGBS-UHFFFAOYSA-N 0.000 description 1
- 229910015400 FeC13 Inorganic materials 0.000 description 1
- CTQNGGLPUBDAKN-UHFFFAOYSA-N O-Xylene Chemical compound CC1=CC=CC=C1C CTQNGGLPUBDAKN-UHFFFAOYSA-N 0.000 description 1
- CSCPPACGZOOCGX-UHFFFAOYSA-N acetone Substances CC(C)=O CSCPPACGZOOCGX-UHFFFAOYSA-N 0.000 description 1
- 239000000654 additive Substances 0.000 description 1
- 150000001298 alcohols Chemical class 0.000 description 1
- 239000003849 aromatic solvent Substances 0.000 description 1
- 239000003225 biodiesel Substances 0.000 description 1
- 238000006243 chemical reaction Methods 0.000 description 1
- 239000003398 denaturant Substances 0.000 description 1
- 238000010790 dilution Methods 0.000 description 1
- 239000012895 dilution Substances 0.000 description 1
- 230000008030 elimination Effects 0.000 description 1
- 238000003379 elimination reaction Methods 0.000 description 1
- 238000013095 identification testing Methods 0.000 description 1
- 239000004434 industrial solvent Substances 0.000 description 1
- 238000004519 manufacturing process Methods 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 239000003960 organic solvent Substances 0.000 description 1
- 239000003209 petroleum derivative Substances 0.000 description 1
- 238000000053 physical method Methods 0.000 description 1
- 230000002110 toxicologic effect Effects 0.000 description 1
- 231100000027 toxicology Toxicity 0.000 description 1
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 1
- 239000008096 xylene Substances 0.000 description 1
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- C10L1/1857—Aldehydes; Ketones
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- C10M171/00—Lubricating compositions characterised by purely physical criteria, e.g. containing as base-material, thickener or additive, ingredients which are characterised exclusively by their numerically specified physical properties, i.e. containing ingredients which are physically well-defined but for which the chemical nature is either unspecified or only very vaguely indicated
- C10M171/007—Coloured or dyes-containing lubricant compositions
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- C10L1/1822—Organic compounds containing oxygen containing hydroxy groups; Salts thereof hydroxy group directly attached to (cyclo)aliphatic carbon atoms
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- C10M—LUBRICATING COMPOSITIONS; USE OF CHEMICAL SUBSTANCES EITHER ALONE OR AS LUBRICATING INGREDIENTS IN A LUBRICATING COMPOSITION
- C10M2215/00—Organic non-macromolecular compounds containing nitrogen as ingredients in lubricant compositions
- C10M2215/28—Amides; Imides
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Description
Descrizione del brevetto per invenzione industriale avente per titolo:
"Composizione marcante-denaturante particolarmente adatta per marcare e denaturare prodotti combustibili".
DESCRIZIONE
L'invenzione si riferisce ad una composizione marcante e denaturante particolarmente adatta, alla marcatura e denaturazione di combustibili liquidi o liquefacibili per compressione.
E' noto ai tecnici del ramo che la denaturazione di combustibili liquidi o liquefacibili per compressione consiste nell'aggiungere degli appositi additivi, chiamati denaturanti, la cui presenza in detti combustibili è rivelabile mediante trattamento con opportuni reagenti; inoltre, la loro quantità può essere determinata per mezzo di una semplice reazione colorimetrica.
E' correntemente necessario marcare i prodotti petroliferi (per esempio i combustibili o i solventi industriali) a causa della differenza di prezzo con la quale lo stesso prodotto può essere commercializzato .
Infatti, come conseguenza di diversi rapporti di tassazione, gasoli per scopi agricoli o per industria della pesca, hanno aliquote di tassazione più basse del gasolio per autotrazione, pertanto, questa situazione è soggetta a subire frodi fiscali quando il prodotto viene utilizzato per scopi differenti da quelli previsti dai regolamenti tributari.
Un marcante o una composizione marcante ideali dovrebbero possedere le seguenti caratteristiche;
soddisfacente stabilità nelle normali condizioni d'uso
non alterare le caratteristiche chimico-fisiche del combustibile o del solvente
- sufficiente stabilità per permetterne l'uso in forme di soluzione concentrata
ridottissime possibilità di eliminazione per mezzo di metodi chimici o fisici
- possibilità di uso in piccole quantità - possibilità di identificazione per mezzo di metodi semplici, veloci e sensibili
- assenza di caratteristiche tossicologiche. La richiedente ha ora trovato una nuova famiglia di sostanze marcanti che presenta le caratteristiche chimico-fisiche adatte alla marcatura di una larga serie di prodotti combustibili derivante sia dalla distillazione del petrolio che da altri tipi di produzione (per es. biodiesel) .
Nella sua forma più ampia, l'invenzione consiste in una composizione marcante e denaturante particolarmente adatta per combustibili liquidi o liquefacibili derivanti dalla distillazione del petrolio e altri prodotti equivalenti (ad esempio a combustibili ottenuti da trattamento di vegetali) a base uno o più prodotti organici corrispondenti alle seguenti formule (I) o (II):
O O II II
R1 C CH 2CR2 ( I )
dove
R1 e R2 sono uguali o diversi e rappresentano :
H, (C1-C4) alchile oppure
dove
X = H, N H oppure O, e
Z , Y = CH3, oppure alogeno
M = H, OH oppure (C1-C4) alchile e
L, T = H, OH, (C1-C4) alchile, alogeno, oppure un anello aromatico.
Secondo la presente invenzione, la quantità di prodotto da impiegare come marcante può variare entro ampi limiti e il valore minimo dipende sia dal particolare prodotto impiegato che dal test di identificazione .
Impiegando come marcante il composto con R1=R2=-CH3 (2,4-pentandione) e usando il semplice e rapido test per il riconoscimento qualitativo descritto in seguito possono essere usate concentrazioni fino a 5 ppm.
Con lo stesso metodo, il marcante può successivamente essere dosato in modo quantitativo. In pratica, è opportuno aggiungere quantità maggiori di prodotto marcante, di modo che il test risulti positivo in ogni caso, anche in previsione di una possibile diluizione in caso di frode.
Da un punto di vista pratico, possono essere usate da 10 a 500 ppm (preferibilmente 50-100 ppm) di marcante.
I vantaggi connessi con questo derivato organico sono i seguenti:
- nessuna modificazione delle caratteristiche chimico-fisiche dei carburanti;
nessuna modificazione di colore del carburante ;
- può essere maneggiato sia come composto puro che come soluzione in solventi organici compatibili con i carburanti, come ad esempio solventi aromatici come xilene, oppure paraffinici, oppure alcoli come l'isobutanolo e simili;
compatibilità con altre sostanze denaturanti, eventualmente già presenti nel carburante, quali, per esempio, furfurolo o coloranti organici quale Solvent Red 198.
Secondo la presente invenzione, per l'identificazione del prodotto si può usare un reattivo consistente in una soluzione diluita idro-alcolica o idro-acetonica di sali di Fe (III).
Nel caso di carburanti liquidi, a condizioni ambiente (ad esempio benzina o gasolio) si aggiungono 2 ml di reattivo a 20 ml di carburante marcato, in imbuto separatore. Si agita energeticamente per 15-20 secondi la miscela e poi si lascia stratificare. Si formano 2 fasi. In presenza di marcante la fase sottostante si colora di rosso o di viola-bruno a seconda del composto impiegato .
La quantità di marcante presente può essere dosata quantitativamente eseguendo una lettura spettrofotometrica, nel campo del visibile, operando sul contenuto della fase inferiore.
Nel caso di carburanti gassosi a condizioni ambiente, ma usualmente liquefatti per compressione (ad esempio GPL) il saggio viene eseguito nel seguente modo:
si pongono in una provetta 1-2 ml di reattivo e poi si lascia fuoriuscire dal contenitore del GPL, raccogliendo, nella provetta stessa, una certa quantità di carburante liquefatto.
Si lascia evaporare il GPL e in circa 15-20 secondi, in presenza di marcante, il reattivo si colora analogamente a quanto avviene con i carburanti liquidi.
Gli esempi che seguono servono a meglio illustrare la presente invenzione, senza, tuttavia, limitarla.
Esempio 1
GPL, in bombola, marcato con 2,4-pentandione, ad una concentrazione di 50 ppm. Dal rubinetto della bombola si fa uscire, per 15-20 secondi, del carburante, tenendo la bombola capovolta, (in modo che il carburante esca ancora allo stato liquido) e lo si raccoglie in una provetta contenente 1-2 mi del seguente reattivo:
0,1 g di FeC13 disciolto in
20 ml di acqua e
80 ml di metanolo.
In 15-20 secondi, il GPL evapora completamente e il reattivo si colora di rosso.
Esempio 2 (Confronto)
Questo esempio, è un esempio di confronto per dimostrare l'efficacia e la funzionalità del marcante secondo la presente invenzione. La stessa prova dell'esempio 1 viene eseguita con del GPL non marcato: il reattivo rimane di colore giallo.
Esempio 3
GPL in bombola marcato con acido salicilico (acido 2-idrossibenzoico) ad una concentrazione di 50 ppm. Si ripete il saggio descritto all'esempio 1: il reattivo si colora nettamente di viola.
Esempio 4
20 ml di gasolio marcato ad una concentrazione di 50 ppm con 2,4-pentandione vengono messi in imbuto separatore. Quindi si aggiungono 2 mi del reattivo descritto nell'Esempio 1 e si agita vigorosamente la miscela per 15-20 secondi. Si lascia decantare. Dopo circa 5 minuti si separano due fasi, l'inferiore delle quali risulta nettamente colorata di rosso.
Esempio 5
1 ml di gasolio, marcato come nell'esempio 4, è diluito con 9 ml di gasolio non marcato. Si ripete il saggio descritto all'esempio 4. La fase inferiore risulta ancora debolmente colorata di rosso.
Esemplo 6 (Confronto)
Si esegue il saggio descritto all'esempio 4, su 20 ml di gasolio non marcato: la fase inferiore rimane gialla.
Esempio 7
20 ml di gasolio, marcato ad una concentrazione di 50 ppm con acido salicilico (acido 2-idrossibenzoico), vengono messi in imbuto separatore. Quindi si aggiungono 2 ml di reattivo e si agita vigorosamente la miscela per 15-20
secondi. Si lascia decantare. Dopo circa 5 minuti si separano due fasi, l'inferiore delle quali è nettamente colorata di viola.
Esempi 8-27
Si è sostanzialmente ripetuta la procedura descritta nell'esempio 1, nel caso di combustibili GPL e quella descritta nell'esempio 4 per i gasoli o per le benzine, apportando di volta in volta le modifiche indicate nella Tabella che segue:
(1)contenenteanche 10ppm difurfurolo
(2)coloratacon 20 ppa diSolventRed 198
Claims (1)
- RIVENDICAZIONI 1. Composizione marcante e denaturante, particolarmente adatta per marcare e denaturare prodotti combustibili liquidi, o liquefacibili per compressione, a base di un derivato β-dicarbonilico di formula (I), oppure da un derivato orto-idrossicarbonilico di formula (II): dove R1 e sono uguali o diversi e rappresentano: H, (C1 -C4) alchile oppure dove X - H, N H oppure 0, e Z, Y = CH3, oppure alogeno in cui M = H, OH oppure alchile e L, T = H, OH, (C1-C4) alchile, alogeno, oppure un anello aromatico 2. Composizione marcante e denaturante secondo la rivendicazione 1, contenente anche un solvente organico aromatico oppure un alcool. 3. Composizione marcante e denaturante secondo le rivendicazioni 1 e 2, contenente eventualmente anche furfurolo. 4. Composizione marcante e denaturante secondo le rivendicazioni 1, 2 0 3 contenente eventualmente anche coloranti del tipo comunemente usato nell'industria dei carburanti. 5. Carburanti liquidi o liquefacibili per compressione caratterizzati dal fatto di contenere da 10 a 1000 ppm di una composizione secondo la rivendicazione 1. 6. Carburanti liquidi o liquefacibili caratterizzati dal fatto di contenere da 30 a 500 ppm di una composizione secondo la rivendicazione 1. 7. Carburanti liquidi o liquefacibili per compressione secondo la rivendicazione 4, caratterizzati dal fatto che la composizione secondo la rivendicazione 1 è costituita sostanzialmente dal composto 2,4-pentandione. 8. Gas di petrolio liquefatto (GPL) secondo la rivendicazione 5, caratterizzato dal fatto che la composizione secondo la rivendicazione 1 è costituita sostanzialmente dal composto 2,4-pentandione. 9. Gas di petrolio liquefatto (GPL) secondo la rivendicazione 7, contenente anche furfurolo.
Priority Applications (14)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
ITMI941320A IT1269947B (it) | 1994-06-24 | 1994-06-24 | Composizione marcante-denaturante particolarmente adatta per marcare e denaturare combustibili |
PCT/EP1995/002330 WO1996000271A1 (de) | 1994-06-24 | 1995-06-16 | Verwendung von carbonylverbindungen zum markieren von kohlenwasserstoffen |
AU27928/95A AU2792895A (en) | 1994-06-24 | 1995-06-16 | Use of carbonyl compounds for marking hydrocarbons |
BR9508104A BR9508104A (pt) | 1994-06-24 | 1995-06-16 | Uso de composto de carbonila hidrocarboneto e processo para detectar composto de carbonila |
JP8502759A JPH10502111A (ja) | 1994-06-24 | 1995-06-16 | 炭化水素の標識のためのカルボニル化合物の使用 |
HU9603550A HUT76753A (en) | 1994-06-24 | 1995-06-16 | Use of carbonil compounds for marking hydrocarbons |
CA002193886A CA2193886A1 (en) | 1994-06-24 | 1995-06-16 | Use of carbonyl compounds for marking hydrocarbons |
MX9700119A MX9700119A (es) | 1994-06-24 | 1995-06-16 | Uso de compuestos de carbonilo como marcadores para hidrocarburos. |
EP95923333A EP0766724A1 (de) | 1994-06-24 | 1995-06-16 | Verwendung von carbonylverbindungen zum markieren von kohlenwasserstoffen |
PL95317941A PL317941A1 (en) | 1994-06-24 | 1995-06-16 | Application od carbonyl compounds for labelling hydrocarbons |
CZ963792A CZ379296A3 (en) | 1994-06-24 | 1995-06-16 | Use of carbonyl compounds for labelling hydrocarbons, method of their detection in hydrocarbons and hydrocarbons containing thereof |
IL11419595A IL114195A0 (en) | 1994-06-24 | 1995-06-16 | Use of carbonyl compounds as markers for hydrocarbons |
CO95027629A CO4410389A1 (es) | 1994-06-24 | 1995-06-22 | Hidrocarburos que comprenden uno o mas compuestos de carbo- nilo |
NO965554A NO965554L (no) | 1994-06-24 | 1996-12-23 | Anvendelse av karbonylforbindelser for markering av hydrokarboner |
Applications Claiming Priority (1)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
ITMI941320A IT1269947B (it) | 1994-06-24 | 1994-06-24 | Composizione marcante-denaturante particolarmente adatta per marcare e denaturare combustibili |
Publications (3)
Publication Number | Publication Date |
---|---|
ITMI941320A0 ITMI941320A0 (it) | 1994-06-24 |
ITMI941320A1 true ITMI941320A1 (it) | 1995-12-24 |
IT1269947B IT1269947B (it) | 1997-04-16 |
Family
ID=11369163
Family Applications (1)
Application Number | Title | Priority Date | Filing Date |
---|---|---|---|
ITMI941320A IT1269947B (it) | 1994-06-24 | 1994-06-24 | Composizione marcante-denaturante particolarmente adatta per marcare e denaturare combustibili |
Country Status (14)
Country | Link |
---|---|
EP (1) | EP0766724A1 (it) |
JP (1) | JPH10502111A (it) |
AU (1) | AU2792895A (it) |
BR (1) | BR9508104A (it) |
CA (1) | CA2193886A1 (it) |
CO (1) | CO4410389A1 (it) |
CZ (1) | CZ379296A3 (it) |
HU (1) | HUT76753A (it) |
IL (1) | IL114195A0 (it) |
IT (1) | IT1269947B (it) |
MX (1) | MX9700119A (it) |
NO (1) | NO965554L (it) |
PL (1) | PL317941A1 (it) |
WO (1) | WO1996000271A1 (it) |
Families Citing this family (3)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
FR2787577B1 (fr) * | 1998-12-16 | 2001-03-02 | Total Raffinage Distrib | Indicateur colore pour la mesure de la repartition des familles d'hydrocarbures contenues dans un melange, son procede d'obtention et ses utilisations |
FR2971254B1 (fr) * | 2011-02-08 | 2014-05-30 | Total Raffinage Marketing | Compositions liquides pour marquer les carburants et combustibles hydrocarbones liquides, carburants et combustibles les contenant et procede de detection des marqueurs |
EP2738154A1 (en) * | 2012-11-30 | 2014-06-04 | Inter-Euro Technology Limited | Improved fuel markers |
Family Cites Families (10)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
GB287192A (en) * | 1926-10-25 | 1928-03-22 | British Dyestuffs Corp Ltd | Improvements in and relating to fuels for internal combustion engines |
GB473653A (en) * | 1936-04-15 | 1937-10-15 | Ig Farbenindustrie Ag | Improvements in the manufacture and production of carbon compounds of high molecularweight |
US2205408A (en) * | 1938-08-09 | 1940-06-25 | Gen Aniline & Film Corp | Fluorescent hydrocarbon oil |
US3508875A (en) * | 1967-10-03 | 1970-04-28 | Union Oil Co | Method for tracing the flow of water in subterranean formations |
NL7103060A (it) * | 1970-03-11 | 1971-09-14 | ||
IT1222752B (it) * | 1987-09-28 | 1990-09-12 | Acna Chimica Organica | Metodo di marcatura di prodotti petroliferi e di solventi organici |
GB8802237D0 (en) * | 1988-02-02 | 1988-03-02 | Shell Int Research | Detection of chemicals by immunoassay |
FR2650606B1 (fr) * | 1989-08-07 | 1992-04-30 | Aussedat Rey | Papier de securite infalsifiable et composition aqueuse ou organique utile, notamment pour rendre un papier infalsifiable |
JPH048798A (ja) * | 1990-04-26 | 1992-01-13 | Yoshibi:Kk | 高輝度有色炎発生用液化ガス燃料 |
IT1254456B (it) * | 1992-02-14 | 1995-09-25 | Basf Italia | Composizione marcante-denaturante particolarmente adatta per marcare edenaturare bitumi combustibili o prodotti affini. |
-
1994
- 1994-06-24 IT ITMI941320A patent/IT1269947B/it active IP Right Grant
-
1995
- 1995-06-16 PL PL95317941A patent/PL317941A1/xx unknown
- 1995-06-16 EP EP95923333A patent/EP0766724A1/de not_active Withdrawn
- 1995-06-16 MX MX9700119A patent/MX9700119A/es unknown
- 1995-06-16 CA CA002193886A patent/CA2193886A1/en not_active Abandoned
- 1995-06-16 BR BR9508104A patent/BR9508104A/pt not_active Application Discontinuation
- 1995-06-16 AU AU27928/95A patent/AU2792895A/en not_active Abandoned
- 1995-06-16 JP JP8502759A patent/JPH10502111A/ja active Pending
- 1995-06-16 IL IL11419595A patent/IL114195A0/xx unknown
- 1995-06-16 WO PCT/EP1995/002330 patent/WO1996000271A1/de not_active Application Discontinuation
- 1995-06-16 CZ CZ963792A patent/CZ379296A3/cs unknown
- 1995-06-16 HU HU9603550A patent/HUT76753A/hu unknown
- 1995-06-22 CO CO95027629A patent/CO4410389A1/es unknown
-
1996
- 1996-12-23 NO NO965554A patent/NO965554L/no unknown
Also Published As
Publication number | Publication date |
---|---|
CO4410389A1 (es) | 1997-01-09 |
ITMI941320A0 (it) | 1994-06-24 |
IT1269947B (it) | 1997-04-16 |
CA2193886A1 (en) | 1996-01-04 |
EP0766724A1 (de) | 1997-04-09 |
JPH10502111A (ja) | 1998-02-24 |
HU9603550D0 (en) | 1997-02-28 |
NO965554L (no) | 1997-02-18 |
AU2792895A (en) | 1996-01-19 |
NO965554D0 (no) | 1996-12-23 |
MX9700119A (es) | 1997-04-30 |
CZ379296A3 (en) | 1997-06-11 |
WO1996000271A1 (de) | 1996-01-04 |
BR9508104A (pt) | 1997-08-12 |
HUT76753A (en) | 1997-11-28 |
IL114195A0 (en) | 1995-10-31 |
PL317941A1 (en) | 1997-05-12 |
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