CS271982B1 - 2,2,6,6-Tetramethyl-4-piperidinoideneacetone and its preparation - Google Patents

2,2,6,6-Tetramethyl-4-piperidinoideneacetone and its preparation Download PDF

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CS271982B1
CS271982B1 CS888115A CS811588A CS271982B1 CS 271982 B1 CS271982 B1 CS 271982B1 CS 888115 A CS888115 A CS 888115A CS 811588 A CS811588 A CS 811588A CS 271982 B1 CS271982 B1 CS 271982B1
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tetramethyl
piperidylideneacetone
pentanone
methyl
preparation
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CS888115A
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Czech (cs)
Slovak (sk)
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CS811588A1 (en
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Peter Rndr Danko
Alojz Balogh
Julius Ing Csc Durmis
Milan Ing Csc Karvas
Marcela Rndr Csc Goghova
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Danko Peter
Alojz Balogh
Durmis Julius
Karvas Milan
Goghova Marcela
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Publication of CS271982B1 publication Critical patent/CS271982B1/en

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Abstract

Riešenie sa týká 2,2,6,6-tetrametyl- -4-pipéridylidénacetónu a sposobu jeho přípravy reakciou zmesi acetonu a amoniaku samotnej alebo s přidáním mezityloxidu, 2,2,4,6,6-pentamety1-1,2,5,6-tetrahydropyrimidínu, 4-metyl-4-hydroxy-2-pentanónu, 4-metyl-4-amíno-2-pentanónu alebo 2,2,6,6- -tetrametyi-4-piperidónu počas 1 až 12 h při teplote 20 0 až 120 °C, tlaku 0,1 až 5 MPa, v prítomnosti^kyslého katexu. Proces je možné uskutočňovat diskontinuitne alebo kontinuitne. 2^2,6,6-Tetramety1- -4-piperidylidénaceton je medziproduktom na výrobu světelných stábilizátorov a biologicky účinných látokThe solution concerns 2,2,6,6-tetramethyl-4-piperidylideneacetone and the method of its preparation by reacting a mixture of acetone and ammonia alone or with the addition of mesityl oxide, 2,2,4,6,6-pentamethyl-1,2,5,6-tetrahydropyrimidine, 4-methyl-4-hydroxy-2-pentanone, 4-methyl-4-amino-2-pentanone or 2,2,6,6- -tetramethyl-4-piperidone for 1 to 12 h at a temperature of 20 0 to 120 °C, a pressure of 0.1 to 5 MPa, in the presence of an acid cation. The process can be carried out discontinuously or continuously. 2^2,6,6-Tetramethyl-4-piperidylideneacetone is an intermediate for the production of light stabilizers and biologically active substances

Description

CS 271982 B1

Vynález sa týká 2,2,6,6-tetrametyl-4-piperidylidénacetónu vzorca I

a sposobu jeho přípravy. 2,2,6,6-Tetrametyl-4-piperidylidénacetón je medziproduktom napřípravu vysokoúčinných avetelných stabilizátorov polymérov a biologicky účinných lá-tok vrátane liečiv a pesticídov.

Hlavným východiskovým produktom na priemyselnú výrobu světelných etabilizátorovpolymérov ako aj celého radu liečiv na báze polyalkylpiperidínov je 2,2,6,6-tetrame-tyl-4-piperidon /triacetónamín/. Jeho syntéza reakciou acetonu s amoniakom, medzipro-duktqm ktorej je 2,2,4,6,6-pentametyl-l,2,5,6-tetrahydropyrimidín /acetonín/ je v lite-ra túře ,/J. Am.-Chem. Soc. 79, 5444, 1957? 5U52O 357? DE 3525 385? SU 891 548/ podrobnéopísaná. Pri syntéze 2,2,6,6-tetrametyl-4-piperidonu je možné vychádzať aj zo 4-metyl--4-hydroxy-2-pentanonu /diacetonalkohol/ a amoniaku /Helv. Chim. Acta 30, H14. 1947? JP 1627 /1972//, 4-metyl-4-amino-2-pentanonu /diacetónamín/ a acetonu /Nippon KagakuZasshi 90, 296, 1969/ alebo 2,6-dimetyl-4-oxo-2,5-heptadiénu /foron/ a amoniaku /Bull.Soc. Chim. Pr. 1950, 345/. Uvedené reakcie sa uskutočňujú v přítomnosti kyslých kataly-zátorov najma zo skupiny karboxylových kyselin a Lewisových báz, ktoré usmerňujú ichpriebeh v prospěch tvorby 2,2,6,6-tetrametyl-4-piperidónu.

Teraz sa zietil nový derivát tetrametylpiperidínu, 2,2,6,6-tetrametyl-4-piperidyli-dénacetón vzorca i a spSsob jeho přípravy reakciou zmesi acetónu a amoniaku samotnej ale-bo s přidáním mezityloxidu, 2,2,4,6,6-pentametyl-l,2,5,6-tetrahydropyrimidínu, 4-metyl--4-hydroxy-2-pentanónu, 4-metyl-4-amíno-2-pentanónu alebo 2,2,6,6-tetrametyl-4-piperi-dónu počas 1 až 12 h pri teplote 20 0 až 120 °C, tlaku 0,1 až 5 MPa, v přítomnostikyslého katexu. Proces je možné uskutočňovaí diskontinuitne v uzavretej reakčnej zóněalebo kontinuitne v prietokovom reaktore pri době kontaktu reagujúcich zložiek 1 až 9 h.Ako kyslé katexy je možné použit polykondenzované katexy napr. typu sulfónovaných kopoly-mérov styrénu s divinylbenzénom /Ostion KS, Wofatit OK 80, připadne aalšie/. 2,2,6,6-Tetrametyl-4-piperidylidénacetón vzorca i podlá vynálezu je možné použitako medziprodukt na výrobu světelných stabilizátorov vhodných pre termoplastické sub-stráty ako sú polyolefíny, polyestery, polyétery, polyuretány, polystyrény a připadne3alšie, Je vhodným medziproduktom aj na výrobu biologicky účinných látok vrátane liečiva pesticídov.

Nasledujúce příklady ilustrujú, ale neobmedzujú predmet vynálezu. Příklad 1

Do autoklávu o objeme 600 ml sa vnieslo 348 g /6 molov/ acetonu, 25,5 g /1,5 molu/ amoniaku a 150 g katalyzátore Ostion KS a reakčná zmes sa za intenzívneho miešania za- hrievala počas 6 h pri teplote 90 °c, pričom tlak v autokláve nepřevýšil hodnotu 0,5 MPa. Po ochladení reakčnej zmesi sa katalyzátor odfiltroval, získaná hnedožltá kvapalina CS 271982 B1 sa rektifikovala najprv za atmosférického tlaku, potom ve vákuu 400 Pa, pričom sa akokonečný produkt zachytila frakcia s teplotou varu 49,5 °C až 50 °C pri tlaku 400 Pavo formě svetložltej kvapaliny, ktorá představuje 2,2,6,6-tetrametyl-4-piperidylidén-acetón.

Elementárna analýza pre C12H21 N0 !

vypočítané : 73,79 % C, 10,84 % H, 7,18 % N

Nájdené : 73,72 % C, 10,80 % H, 7,20 % N

Hmotnostná spektroskopie :

Molekulový ión M+ « 195. 1H - NMR spektrum v CCl^, 10 %-ný roztok : ppmy skupina I Multiplicita 5,41 2,92 2,00 1,58 • CH - co - 1 - ch2- kruh 2 - CO - CH3 3 - c”2 - kruh 2 s s s s 1,08 1,03 0,58

:nh IČ spektrum v CCl4 : /0 = 0/ - 1625 cm-1 *, λ) /0 = 0/ - 1725 cm"1 J \)/N-H/ - 3425 cm"1 . 13·

Uvedené štruktúru potvrdilo i C - NMR spektrum. příklad 2

Do vsádzkového reaktora sa umiestnilo 154 g /1 mol/ 2,2,4,6,6 - pentametyl --1,2,5,6-tetrahydropyrimidínu, 174 g /3 moly/ acetonu, 8,5 g /0,5 molu/ amoniaku a 150 gkatalyzátore Ostion KS, reakčná zmes sa za miešania zahrievala 6 h pri teplote 70 °Ca tlaku 0,1 MPa a po ochladení sa spracovala rovnako ako v příklade 1. Získaný produktbol identifikovaný ako 2,2,6,6-tetrametyl-4-piperidylidénacetón.

Elementárna analýza pre C12H21 NO :

Vypočítané : 73,79 % C, 10,84 % H, 7,18 % N

Nájdené : 73,82 % C, 10,79 % H, 7,19 % N

Hmotnostně spektrum : molekulový ión M+ = 195.

CS 271982 B1

The invention relates to 2,2,6,6-tetramethyl-4-piperidylideneacetone of the formula I

and the method of its preparation. 2,2,6,6-Tetramethyl-4-piperidylideneacetone is an intermediate for the preparation of high performance avionic polymer stabilizers and biologically active substances including drugs and pesticides.

The main starting product for the industrial production of light stabilizer polymers as well as a variety of polyalkylpiperidine based drugs is 2,2,6,6-tetramethyl-4-piperidone / triacetone amine. Its synthesis by the reaction of acetone with ammonia, the intermediate of which is 2,2,4,6,6-pentamethyl-1,2,5,6-tetrahydropyrimidine (acetonine), is in the lithium titration. Am.-Chem. Soc. 79, 5444 (1957)? 5U52O 357? DE 3525 385? SU 891 548 / detailed. In the synthesis of 2,2,6,6-tetramethyl-4-piperidone, it is also possible to start from 4-methyl-4-hydroxy-2-pentanone (diacetone alcohol) and ammonia / Helv. Chim. Acta 30, H14. 1947? JP 1627 (1972), 4-methyl-4-amino-2-pentanone (diacetone amine) and acetone (Nippon KagakuZasshi 90, 296, 1969) or 2,6-dimethyl-4-oxo-2,5-heptadiene / foron / and ammonia /Bull.Soc. Chim. Pr. 1950, 345. The reactions are carried out in the presence of acidic catalysts, especially carboxylic acids and Lewis bases, which direct their course in favor of 2,2,6,6-tetramethyl-4-piperidone formation.

The novel tetramethylpiperidine derivative, 2,2,6,6-tetramethyl-4-piperidylideneacetone of formula (I) and its preparation by reaction of acetone / ammonia alone or with the addition of mesityloxide, 2,2,4,6,6- pentamethyl-1,2,5,6-tetrahydropyrimidine, 4-methyl-4-hydroxy-2-pentanone, 4-methyl-4-amino-2-pentanone or 2,2,6,6-tetramethyl-4-piperidine -done for 1 to 12 h at 20 to 120 ° C, 0.1 to 5 MPa in the presence of an acid cation exchanger. The process can be carried out discontinuously in a closed reaction zone or continuously in a flow reactor at a contact time of the reactants of 1 to 9 h. As acid cation exchangers, polycondensed cation exchangers of, for example, sulfonated styrene copolymers with divinylbenzene / Ostion KS, Wofatit OK 80 can be used; aalšie /. The 2,2,6,6-tetramethyl-4-piperidylideneacetone of the formula (I) according to the invention can be used as an intermediate for the production of light stabilizers suitable for thermoplastic substrates such as polyolefins, polyesters, polyethers, polyurethanes, polystyrenes and possibly other. production of biologically active substances including pesticide drug.

The following examples illustrate, but do not limit the invention. Example 1

348 g (6 moles / acetone, 25.5 g / 1.5 moles / ammonia) and 150 g of Ostion KS catalyst were added to a 600 ml autoclave and the mixture was heated to 90 ° C for 6 h with vigorous stirring. c, wherein the pressure in the autoclave does not exceed 0.5 MPa. After cooling the reaction mixture, the catalyst was filtered off, the brownish-yellow liquid CS 271982 B1 obtained was rectified first at atmospheric pressure, then under a vacuum of 400 Pa, and the final product was collected by a fraction having a boiling point of 49.5 ° C to 50 ° C under a pressure of 400 µmol. a pale yellow liquid which is 2,2,6,6-tetramethyl-4-piperidylidene acetone.

Elemental analysis for C 12 H 21 NO!

N, 7.18. Found: C, 73.79; H, 10.84;

Found: C, 73.72; H, 10.80; N, 7.20

Mass Spectroscopy:

Molecular ion M + «195. 1 H-NMR spectrum in CCl 3, 10% solution: ppmy group I Multiplicity 5.41 2.92 2.00 1.58 • CH - co - 1 - ch 2 - ring 2 - CO - CH3 3 - c ”2 - ring 2 ssss 1.08 1.03 0.58

: nh IR spectrum in CCl4: 0 = 0 / - 1625 cm @ -1, λ) / 0 = 0 / - 1725 cm @ -1 J / NH / - 3425 cm @ -1. 13·

This structure was confirmed by the C-NMR spectrum. Example 2

154 g (1 mol) of 2,2,4,6,6-pentamethyl-1,2,5,6-tetrahydropyrimidine, 174 g (3 moles / acetone), 8.5 g / 0.5 were placed in a batch reactor. mole / ammonia and 150 g of Ostion KS catalyst, the reaction mixture was heated with stirring for 6 hours at 70 ° C and a pressure of 1 MPa and, after cooling, treated as in Example 1. The product obtained was identified as 2,2,6,6- tetramethyl-4-piperidylideneacetone.

Elemental analysis for C 12 H 21 NO:

% C, 73.79;% H, 10.84; N, 7.18

Found: C, 73.82; H, 10.79; N, 7.19

Mass spectrum: molecular ion M + = 195.

Claims (4)

PREDMET VYNÁLEZUOBJECT OF THE INVENTION 1. 2,2,6,6-Tetrametyl-4-piperidylidénacetón vzorca I c - c - ch3 (I)2,2,6,6-Tetramethyl-4-piperidylideneacetone of formula I c - c - ch 3 (I) CS 271982 BlCS 271982 Bl 2. Sposob přípravy 2,2,6,6-tetrametyl-4-piperidylidénacetónu podia bodu 1, vyznačujúci sa tým, že sa nechá reagovat zmes acetonu a amoniaku samotná alebo s přidáním mezityloxidu, 2,2,4,6,6-pentametyl-l,2,5,6-tetrahydropyrimidínu, 4-metyl-4-hydroxy~2~pentanónu, 4-metyl-4-amino-2-pentanónu alebo 2,2,6,6-tetrametyl-4-piperidónu, počas 1 až 12 h pri teplote 20 0 až 120 °C, tlaku 0,1 až 5 MPa, v přítomnosti kyslého katexu.2. A process for the preparation of 2,2,6,6-tetramethyl-4-piperidylideneacetone according to item 1, characterized in that a mixture of acetone and ammonia is reacted alone or with the addition of mesityl oxide, 2,2,4,6,6-pentamethyl -1,2,5,6-tetrahydropyrimidine, 4-methyl-4-hydroxy-2-pentanone, 4-methyl-4-amino-2-pentanone or 2,2,6,6-tetramethyl-4-piperidone, during 1 to 12 h at 20 0 and 120 DEG C., a pressure of 0.1 to 5 MPa, in the presence of an acid cation exchanger. 3. Spósob podlá bodu 2, vyznačujúci sa tým, že reakcia sa uskutečňuje diskontinuitne v uzavretej reakčnej zóně.3. The process according to item 2, characterized in that the reaction is carried out batchwise in a closed reaction zone. 4. Sposob podlá bodu 2, vyznačujúci sa tým, že reakcia sa uskutočňuje kontinuitne v prietokovom reaktore pri době kontaktu reagujúcich zložiek 1 až 9 h.4. The process according to item 2, characterized in that the reaction is carried out continuously in a flow reactor with a contact time of the reactants of 1 to 9 hours.
CS888115A 1988-12-08 1988-12-08 2,2,6,6-Tetramethyl-4-piperidinoideneacetone and its preparation CS271982B1 (en)

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