CA2010850C - Process for separating volatile components from reaction mixtures obtained through high-pressure polymerization - Google Patents

Process for separating volatile components from reaction mixtures obtained through high-pressure polymerization

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Publication number
CA2010850C
CA2010850C CA002010850A CA2010850A CA2010850C CA 2010850 C CA2010850 C CA 2010850C CA 002010850 A CA002010850 A CA 002010850A CA 2010850 A CA2010850 A CA 2010850A CA 2010850 C CA2010850 C CA 2010850C
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CA
Canada
Prior art keywords
ethylene
pressure
melt
mpa
polymer
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 - Fee Related
Application number
CA002010850A
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French (fr)
Other versions
CA2010850A1 (en
Inventor
Heinz Beckemeier
Heinz-Dieter Buhnen
Herbert Mercamp
Wilhelm Zoller
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Hoechst AG
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Hoechst AG
Priority date (The priority date 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 date listed.)
Filing date
Publication date
Priority to DE3844180A priority Critical patent/DE3844180A1/en
Priority to ES90102255T priority patent/ES2057200T3/en
Priority to EP90102255A priority patent/EP0440838B1/en
Priority to AU49395/90A priority patent/AU622278B2/en
Priority to JP3642190A priority patent/JP2904846B2/en
Application filed by Hoechst AG filed Critical Hoechst AG
Priority to CA002010850A priority patent/CA2010850C/en
Publication of CA2010850A1 publication Critical patent/CA2010850A1/en
Priority to US07/790,126 priority patent/US5200486A/en
Application granted granted Critical
Publication of CA2010850C publication Critical patent/CA2010850C/en
Anticipated expiration legal-status Critical
Expired - Fee Related legal-status Critical Current

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    • CCHEMISTRY; METALLURGY
    • C08ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08FMACROMOLECULAR COMPOUNDS OBTAINED BY REACTIONS ONLY INVOLVING CARBON-TO-CARBON UNSATURATED BONDS
    • C08F6/00Post-polymerisation treatments
    • C08F6/26Treatment of polymers prepared in bulk also solid polymers or polymer melts
    • C08F6/28Purification

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  • Chemical & Material Sciences (AREA)
  • Health & Medical Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Medicinal Chemistry (AREA)
  • Polymers & Plastics (AREA)
  • Organic Chemistry (AREA)
  • Addition Polymer Or Copolymer, Post-Treatments, Or Chemical Modifications (AREA)
  • Organic Low-Molecular-Weight Compounds And Preparation Thereof (AREA)

Abstract

Separation of volatile components from the polymer melts formed during the homopolymerization of ethylene or the copolymerization of ethylene with other copolymerizable compounds at elevated pressures and elevated temperatures by countercurrent treatment with ethylene. Superior separations are obtained by the process.

Description

2~

A Process for Separating Volatile Components from Reaction Mixtures Obtained through High~pressure Polymerization The invention relates to a process for separating volatile components from polymer melts which are obtained from the polymerization of ethylene and the copolymerization of ethylene with other copolymerizable compounds under high pressure.

BAC~GROUND OF THE INVENTION

The radical high~pressure polymerization of ethylene alone or together with comonomers is performed on a commercial scale in tubular reactors or in autoclaves with agitation at pressures of 50 to 400 MPa, in particular 140 to 250 MPa, and temperatures of 100 to 400C.

A diagram of the process is shown in Figure 1.
Fresh ethylene is first fed into low~pressure compressor 8 via line 9, compressed to 10 to 35 MPa and then, together with the unreacted ethylene from the polymerization stage and which is recycled, it is raised to the reaction pressure in a high~pressure compressor 5. With the aid of suitable pumping equipment, e.g, piston pumps, the initiators present in solution are mixed into the compressed ethylene or metered into the reactor directly.

2 20~850 Comonomers such as vinyl esters, olefinically unsaturated carboxylic acids, or alpha~olefins are also fed into the high~pressure compressor 5 via feed line 10.
In reactor 1 between 10 and 45 % by weight of the monomers entering the reactor are reacted in one run. The polymer is precipitated in high-pressure separator 3 by reducing the pressure on the mixture to 5 to 50 MPa, preferably 10 to 35 MPa, after optional cooling in cooler 2. During pressure~relief, the gaseous components released are returned to the high~pressure compressor 5 via high~pressure return gas system 4. The polymer, which contains dissolved unreacted monomers, is pressure~relieved via a system consisting of low~pressure separator 6 and low~pressure cooler 7. The low-molecular weight compounds released are returned via the low~pressure compressor g to the high~pressure compressor 5. The polymer precipitated in the low-pressure separator 6 contains not only residual amounts of ethylene and comonomers but also oligomers.

Even when the polymerization products are separated carefully, it is impossible to avoid volatile admixtures such as comonomers, their decomposition products, and other low~molecular weight compounds being retained in the polymers. During storage and processing of the polymers, these residues lead to undesirable emissions and odors; in addition, the flame point of the polymers is considerably reduced. Therefore, efforts are made to insure that the products are free of volatile compounds by taldng suitable measures during the plessule-relieving process and by subjecting the polymer to an additional tre~tm~-nt Further difficulties are caused by the fact that the ethylene liberated in the low-ple~ulc sepal~or contains comonomers, oligomers, and other compounds which 5 condense out when the sepal~ed ethylene is recycled, forming deposits in the colllplcssors and pumps which can lead to clogging.

According to a process described in DD-PS 131 824, issued July 26, 1978, either the reaction ~ lure is brought into contact intensively with the ethylene downstream of the polymP.ri7~tion reactor or the polymer melt is brought into contact 10 intensively with the ethylene after separation of the majority of the unreacted gas llli~lurc in a pressure stage and the llli~lure is then sep~ t-0A in a stabilizing zone.
According to an al)pr~liate embodiment of this process, the reaction l~ lurc is fed c~unlel-;ullelllly into a widening tube, ethylene also being ~im~llt~n~ously introduced and the Illi~lurc thus formed is separated in the low-pressure sepal~tor.

Another procedure for high-plcs~ulc polymeri7~tion of ethylene is disclosed in the DE-AS 21 31 145, issued January 14, 1982. It mixes the reaction Illi~.lulc coming from the reaction zone with the fresh ethylene feed and the recycled ethylene coming from the low-pres~.lre sep~tor.

JJ: ~l . 3 A~

``_ 20 1 0850 Both processes lead only to a slight reduction in the concentration of low-molecular weight ad~ Lures in the polymer. Moreover, additional appa,~tus is required for their pt;lÇol",al~ce.

It is also known that unreacted gas origin~ting from the low-pres~ure S sep~lor can be recycled to the high-plt;s~u~ cycle with the aid of an injector (cf. DD-PS 202 882, issued October 5, 1983). However, this process does not reduce the concentration of the low-molecular components re~ inillg in the product.

With liquid products, the low-molecular weight compounds can be sepal~led by gas scrubbing with nitrogen or other inert gaseous substances. However, 10 additional appa-~lus is also required for this process and the sep~r~ted co",~onents cannot be returned without çl~ning.

BRIEF DESCRIPIION OF THE INVENTION

Therefore, the problem was to develop a process which avoids the disadvantages described above, guarantees nearly complete removal of the volatile 15 co,.,~nents from the polymer melt, and insures that little or no condensed conll?ollents are contained in the cycle gas of the low-pressure stage.

JJ: 4 The invention consists in a process for separating volatile components from polymer melts formed during the homopolymerization of ethylene or the copolymerization of ethylene with other copolymerizable compounds at elevated pressures and elevated temperatures. It is characterized in that ethylene is passed in countercurrent flow through the melt at pressures of 5 to 70 MPa and a temperature in the melt of at least approximately 120C.

Surprisingly, with the new process it is possible to almost completely remove the volatile components contained in the polymer melt formed during high-pressure polymerization. Further cleaning, e.g. in the extruder or during storage of the product, is not necessary. The concentration of the low~molecular components in the recycled ethylene is reduced until condensation products do not form during the compression of the ethylene and product losses are avoided.

The claimed procedure can be performed with different polymerizations and copolymerizations o~
ethylene using the high-pressure process, in both tubular reactors and autoclaves. It can be used both with solvent and solvent~free processes, and also with processes for the preparation of linear low~density polyethylenes (LLDPE).

Volatile components contained in the polymer melt are understood to be low~molecular weight compounds which are contained in the polymerization products, e.g. as comonomers, decomposition products of comonomers, and oligomers. Thus, for example, in the preparation of copolymers of ethylene and vinyl acetate, acetic acid formed by the decomposition of vinyl acetate is to be found in the products. Furthermore, volatile compounds include solvents which, for example, enter the reaction mixture with initiators and molecular mass regulators.
Lubricants and other auxiliaries, which are required to operate the polymerization plant, also are present in the polymer melt.

According to the claimed process, the polymer melt is treated at elevated pressure, preferably at 5 to 70 ~Pa and in particular at 10 to 40 MPa. It is not necessary to provide a separate reactor for treatment; it can be successfully performed in the polymer separator of a high~pressure polymerization plant. It is expedient to remove most of the unreacted gas mixture by reducing the pressure to the above~mentioned range and then bringing the melt into contact with the ethylene. The high~pressure separator used in the polymerization process is particularly suitable for this purpose.

~ 2010850 To insure that the volatile components are separated either completely or nearly completely from the melt, it is necessary to maintain a temperature of at least 120C therein. It has proved particularly valuable to treat the ethylene at temperatures above approximately 150C. The higher the temperature, the more completely the volatile substances are separated.
The only upper limit for the treatment temperature is the temperature at which the melt from the polymerization enters the chamber where the volatile substances are separated.

In order to guarantee as high a temperature as possible in the melt, it is expedient to pass heated ethylene in countercurrent flow to the melt. It is important to the claimed procedure that the ethylene and melt flow in opposing directions when they meet each other. This insures an extremely intimate mixture of melt and olefin.

The effectiveness of the ethylene stream can be further increased by forcefully diverting it from a straight path in the chamber where the melt is treated.

In this manner, fresh ethylene is passed several times through the precipitated product. The ethylene is diverted by means of suitable installations in the reactor, in the simplest case by plates which are located on opposite sides thereof and in staggered formation.

- 8- 201~850 The amount of ethylene required for treating the polymer melt depends on the temperature, the viscosity, and the comonomer content of the melt. The required amount of ethylene increases with the viscosity and the comonomer content and decreases with increasing temperature. In general, 0.1 to 2 parts by weight of ethylene are used per one part by weight of melt.

Pure ethylene can be used to separate the volatile components from the melt. It is compressed in the low~pressure compressor and fed into the polymer melt in the high~pressure separator. The ethylene charged with the volatile components of the melt is passed through the high~pressure gas system and then, after separation of the volatile components, is fed via a partial stream to the inlet side of the high pressure compressor and on into the polymerization reactor.

BRIEF DESCRIPTION OF THE DRAWINGS

In the accompanying drawings, constituting a part hereof and in which like reference characters indicate like parts, Figure l is a flow diagram of a prior art process;

~ 9 _ 20~C~8S0 Figure 2 is a flow diagram of the process of the present invention; and Figure 3 is a schematic view of the high pressure separator of the present invention.

DETAILED DESCRIPTION OF THE INVENTION

A diagram of the claimed process is shown in Figure 2. Fresh ethylene from pipe 19 is compressed in low~pressure compressor 18 to 10 to 35 MPa, heated in heating device 22 to at least 120C and passed through line 21 into high~pressure separator 13. There it meets the polymer flowing in the countercurrent direction.

Charged with volatile, low~molecular weight components of the polymer melt, the ethylene enters a high~pressure gas recycling system. The low molecular components such as solvent, lubrication oil, and oligomers are separated by means of pressure-relieving device 23 and line 24. The ethylene, optionally containing comonomers which can be replenished via line 20, is fed to high~pressure compressor 15 and then to reactor 11. The polymer is separated at a pressure of 5 to 70 MPa in high~pressure separator 13, after it has been cooled in cooler 12, if necessary. The gaseous parts enter high~pressure gas recycling system 14 together with the fresh ethylene passed in the countercurrent direction.

201(~850 The polymer is pressure~relieved via low-pressure separator 16 and low-pressure cooler 17; the liberated low-molecular weight compounds are compressed in the low~pressure compressor together with fresh ethylene from line 19.

Figure 3 shows separator 13 with baffles 25 where the polymer is treated with ethylene. The melt enters into the separator through line 27 and the ethylene through line 21. The melt leaves the separator through line 29 and the ethylene charged with volatile components from the melt through line 30.

The new process is explained in the following examples which are intended to be illustrative, not limitative.

Example 1 A reaction mixture obtained from the polymerization of 720 parts by weight of ethylene and 280 parts by weight of vinyl acetate, and which has a percentage of 32.9 % by weight of polymer, is fed into a high~pressure separator without baffles. The polymer is precipitated and can be drawn off via a bottom valve.
Countercurrent to the polymer, 250 parts of ethylene are introduced and withdrawn from the head together with the low-molecular weight components of the melt. The treated polymer contains 0.62 % by weight of monomeric vinyl acetate, and the vinyl acetate concentration of the low-pressure gas cycle is 12.5 % by volume.

20~0850 Example 2 (Comparison) The same procedure as in Example 1 is carried out, except that the ethylene is not fed into the high~pressure separator but is passed directly to the high-pressure compressor in known manner. The polymer contains 2 % by weight of monomeric vinyl acetate, and the vinyl acetate concentration in the low~pressure gas cycle is more than 40 ~ by volume.

Example 3 A reaction mixture obtained from the polymerization of 720 parts by weight of ethylene and 2~0 parts by weight of vinyl acetate, and which has a percentage of 33 % by weight of polymer, is fed into a high~pressure separator with baffles according to Figure 3. The polymer is precipitated and can be drawn off via the bottom valve.

Countercurrent to the polymer, 260 parts of ethylene are introduced and withdrawn from the head together with low~molecular weight components of the melt. The treated polymer contains 0.33 % by weight of monomeric vinyl acetate, and the vinyl acetate concentration in the low~pressure gas cycle is 4.4 ~ by volume.

~ _ 20iO850 Example 4 (Comparison) The procedure of Example 3 is followed except that the ethylene is not fed into the high-pressure separator, but is passed directly to the high~pressure compressor in known manner. The polymer contains 1.1 % by weight of vinyl acetate, and the vinyl acetate concentration in the low~pressure gas cycle is 33 % by volume.

The viscosity of the polymers prepared according to Examples 1 to 4 is the same and is 250 mPa x sec at 140C.

Claims (15)

1. The process for the separation of volatile components from polymer melts formed during the homopolymerization of ethylene or the copolymerization of ethylene with other copolymerizable compounds at elevated pressures and elevated temperatures, wherein a ratio of ethylene is passed countercurrently to said melts at a separation pressure of about 5 to about 70 MPa and a melt temperature of at least about 120°C.
2. The process of Claim 1 wherein said pressure is about 10 to about 40 MPa.
3. The process of Claim 1 wherein said separation takes place in a polymer separator of a high-pressure polymerization plant.
4. The process of Claim 1 wherein said homopolymerization or said copolymerization is carried out at a polymerization pressure of about 50 to 400 MPa and said polymerization pressure is thereafter reduced to said separation pressure of about 5 to 70 MPa before said ethylene contacts said melt, whereby a portion of unreacted gas mixture present is removed from said melt.
5. The process of Claim 4 wherein said portion is a majority of said mixture.
6. The process of Claim 4 wherein said separation pressure is about 10 to 40 MPa.
7. The process of Claim 1 wherein said melt temperatures are above about 150°C.
8. The process of Claim 4 wherein said polymerization pressure is 140 to 250 MPa.
9. The process of Claim 1 wherein said melts are cooled after said homopolymerization or said copolymerization and before said polymerization pressure is reduced.
10. The process of Claim 1 wherein said ratio is 0.1 to 2.0 parts by weight of said ethylene to 1 part by weight of said melt.
11. The process of Claim 3 wherein flows of said ethylene and said melt are diverted from a direct path.
12. The process of Claim 11 wherein said flows are diverted by means of at least one impediment to direct flow located in said separator.
13. The process of Claim 12 wherein said impediment is at least one baffle.
14. The process of Claim 13 wherein there are a plurality of said baffles located on opposite sides of said separator.
15. The process of Claim 14 wherein said baffles are staggered.
CA002010850A 1988-12-29 1990-02-23 Process for separating volatile components from reaction mixtures obtained through high-pressure polymerization Expired - Fee Related CA2010850C (en)

Priority Applications (7)

Application Number Priority Date Filing Date Title
DE3844180A DE3844180A1 (en) 1988-12-29 1988-12-29 METHOD FOR SEPARATING VOLATILE COMPONENTS FROM REACTION MIXTURES OBTAINED BY HIGH PRESSURE POLYMERIZATION
EP90102255A EP0440838B1 (en) 1988-12-29 1990-02-06 Process for separating volatile materials from reaction mixtures obtained by high-pressure polymerization
ES90102255T ES2057200T3 (en) 1988-12-29 1990-02-06 PROCEDURE FOR THE SEPARATION OF VOLATILE COMPONENTS FROM REACTION MIXTURES OBTAINED BY A HIGH PRESSURE POLYMERIZATION.
AU49395/90A AU622278B2 (en) 1988-12-29 1990-02-14 Process for separating volatile components from reaction mixtures obtained through high-pressure polymerisation
JP3642190A JP2904846B2 (en) 1988-12-29 1990-02-19 Method for separating volatile components from reaction mixture obtained by high pressure polymerization
CA002010850A CA2010850C (en) 1988-12-29 1990-02-23 Process for separating volatile components from reaction mixtures obtained through high-pressure polymerization
US07/790,126 US5200486A (en) 1988-12-29 1991-11-06 Process for separating volatile components from reaction mixtures obtained through high-pressure polymerization

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
DE3844180A DE3844180A1 (en) 1988-12-29 1988-12-29 METHOD FOR SEPARATING VOLATILE COMPONENTS FROM REACTION MIXTURES OBTAINED BY HIGH PRESSURE POLYMERIZATION
CA002010850A CA2010850C (en) 1988-12-29 1990-02-23 Process for separating volatile components from reaction mixtures obtained through high-pressure polymerization

Publications (2)

Publication Number Publication Date
CA2010850A1 CA2010850A1 (en) 1991-08-23
CA2010850C true CA2010850C (en) 1995-10-24

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CA002010850A Expired - Fee Related CA2010850C (en) 1988-12-29 1990-02-23 Process for separating volatile components from reaction mixtures obtained through high-pressure polymerization

Country Status (6)

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EP (1) EP0440838B1 (en)
JP (1) JP2904846B2 (en)
AU (1) AU622278B2 (en)
CA (1) CA2010850C (en)
DE (1) DE3844180A1 (en)
ES (1) ES2057200T3 (en)

Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US9012577B2 (en) 2005-07-29 2015-04-21 Saudi Basic Industries Corporation Method for preparing linear alpha-olefins with improved heat removal

Families Citing this family (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
NZ264288A (en) * 1993-09-30 1996-08-27 Boc Group Inc Preparation of ethylene and propylene polymers from mixtures of ethylene/ethane and propylene/propane, respectively, with either pre-polymerisation or post-polmerisation adsorption of the unsaturated component and recycling of at least part of the unreacted monomer
DE19922677C1 (en) 1999-05-18 2001-04-19 Elenac Gmbh Process for drying and degassing polyolefins and polyethylene produced by this process
EP1749808B1 (en) * 2005-07-29 2010-02-03 Linde AG Method for the preparation of linear alpha-olefins and reactor system therefore with improved disposal of high molecular weight oligomers

Family Cites Families (7)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
BG25100A3 (en) * 1970-06-23 1978-07-12 Snamprogetti S.P.A. A method of obtaining of polyethilene at yigh pressure
DD131824A3 (en) * 1975-11-13 1978-07-26 Manfred Raetzsch METHOD FOR SEPARATING THE REACTION MIXTURE IN HIGH-PRESSURE POLYMERIZATION PLANTS
JPS5813563B2 (en) * 1976-04-03 1983-03-14 信越化学工業株式会社 Method and apparatus for removing unreacted monomers from an aqueous dispersion of vinyl chloride
DE2746909C3 (en) * 1977-10-19 1982-03-11 Hoechst Ag, 6000 Frankfurt Process for the continuous removal of residual hydrocarbons from polyolefins
DD202882A1 (en) * 1981-10-27 1983-10-05 Leuna Werke Veb METHOD FOR RECYCLING COMONOMER-CONTAINING LOW-PRESSURE RECYCLING GAS IN THE HIGH-PRESSURE POLYMERIZATION PROCESS
DE3815487A1 (en) * 1988-05-06 1989-11-16 Basf Ag METHOD FOR LOW-PRESSURE COPOLYMERISATION OF ETHYLENE WITH (ALPHA) -OLEFINES AND ETHYLENE COPOLYMERISATE WITH LOW RESIDUAL MONOMER CONTENT
IT1226303B (en) * 1988-07-26 1990-12-27 Montedipe Spa PROCESS AND APPARATUS FOR DEVOLATILIZATION OF POLYMER SOLUTIONS.

Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US9012577B2 (en) 2005-07-29 2015-04-21 Saudi Basic Industries Corporation Method for preparing linear alpha-olefins with improved heat removal

Also Published As

Publication number Publication date
ES2057200T3 (en) 1994-10-16
AU4939590A (en) 1991-08-15
AU622278B2 (en) 1992-04-02
DE3844180A1 (en) 1990-07-05
JPH03239705A (en) 1991-10-25
CA2010850A1 (en) 1991-08-23
EP0440838A1 (en) 1991-08-14
EP0440838B1 (en) 1993-04-14
JP2904846B2 (en) 1999-06-14

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