Die PVT-Daten eines Polyethylen-und cines (Ethen-Vinylacetat)-Copolymerwachses sowie die Loslichkeit von Ethen, Propan, Propen und But-1-en in der Schmelze werden mitgeteilt. Im untersuchten Druck-und Temperaturbereich nimmt die Loslichkeit mit steigendem Druck, fallender Temperatur, steigender C-Atom-Zahl der gasformigen Komponente und sinkendem z,, des Wachses zu. Aufbau und Funktionsweise der entwickclten Apparaturen werden erlautert.
Mccaeaoeanm pacmeopwocmu ammena, nponaHa, nponena u 6ymena e pacnaaeax oauzoaepoe noauamuaena, a m a z w e (amusen-sunmayemam) eonoauaepax n p u memtepamypeao 473.15 Ec u aaeaenuax ao 30 M U a , Zlacmb I . Ycmanoeza u peayabmambs BopmocTb a~nJieaa, nponaaa, nponeaa II 6 y~e n a B pacnnase. B HccnenyeMoM mwepsane TeMnepaTyp R AasnemB Coo61qa1o~c~ PVT-naaHbIe HR3KOMOJTeKynHpHOrO IIOJIR3TMJIeHa R (3THJleH-BHHRnaqeTaT) COnOJIRMepa, a TaKme PaCTPaCTBOPIIMOCTb IIOBbILLIaeTCH C nOBbIUIeHHeM RaBJIeHIIH, nOHUXEeHHeM TeMIIepaTypbI, IIOBbIIIIeHHeM aTOMHOrO 9RCJIa c ra3006pa3~oro KOMnOHeHTa I4 yMeHblueHHeM MOneKynHpHOfi MaCCbI HH3KOMOneKynHpHOI' O nOJlII3TRneHEl. 06%-HCHHeTCH YCTpOfiCTBO II lIpBHqlln pa6OTbI pa3pa60TaHHOfi YCTaHOBKR.Investigations on solubility of ethene, propane, propene, and but-1-ene in molten oligomers of polyethylene and poly(etheneco-oinylacetate) at temperatures u p to 473.15 K and pressures u p to 30 MPa. Part I . Apparatuses and results Results of P-V-2'-measurements of a polyethylene and a poly(ethene-co-vinyl acetate) wax and solubility data of ethene, propane, propene, and but-1-ene in the molten waxes are reported. The solubility increases with increasing pressure, decreasing temperature, increasing number of C-atoms of the gaseous component, and decreasing 2" of the wax. The construction and the working principles of the developed equipment are explained.
Some measurements of the vapour-liquid and/or the demixing equilibrium at moderate pressures were carried out in systems containing the monomers ethene, 1-butene, 4-methyl-1-pentene and a polyethylene wax. A group-contribution-modified chain-of-rotators (COR) equation of state was used to calculate the phase diagrams in all binary and ternary subsystems and in the whole quarternary mixture. The calculations lead to a satisfying description of the vapour-liquid equilibrium and its intersection by a liquid-liquid region at higher pressures and temperatures. The miscibility gaps in both mixtures of the polyethylene wax with 1-butene and 4-methyl-1 -pentene, respectively, were observed again after adding ethene to these binary mixtures. The calculations indicate a small three phase triangle in all corresponding ternary mixtures. A liquid-liquid demixing region intersecting the vapour-liquid surface could also be found in the whole quaternary system by calculation with the modified COR model. This surprisingly complicated phase behaviour has properly to be taken into account during the separation of the monomers after the co-or terpolymerization process.
ZUSAMMENFASSUNG:Es wurden Untersuchungen zum Flussig-Dampf-und Flussig-Fliissig-Gleichgewicht in Mischungen aus den Monomeren Ethen, 1-Buten, 4-Methyl-1 -penten und einem Polyethylenwachs bei mittleren Drucken durchgefuhrt. Auf der Basis der Chainof-Rotators (COR) Zustandsgleichung, die mit einem Gruppenbeitragsmodell modifiziert wurde, wurden die Phasendiagramme der binaren und ternaren Subsysteme sowie fur das quaternare Gesamtsystem berechnet. Die Berechnungen ergeben eine zufriedenstellende Beschreibung des Flussig-Dampf-Gleichgewichtes und dessen Uberlappung mit einem Flussig-Flussig-Gleichgewicht bei hoheren Drucken und Temperaturen. Die
Some new measurements of the high pressure demixing behaviour have been done in the system ethylene, vinyl acetate and an (ethylene‐vinylacetate) copolymer. Calculations of phase equilibria using the chain‐of‐rotators equation of state are compared with these new experimental data The miscibility gap of the ternary mixture can be predicted on the basis of a group contribution approach using interaction parameters from low molecular weight binary mixtures only. The model describe the phase separation (besides of polydispersity effects) sufficiently accurate up to high pressures. The derivation of the spinodal equation for ternary mixtures facilitates the calculation procedures applied. The model calculations detect a closed miscibility gap at higher pressures than in the binary subsystem composed of ethylene and the (ethylenevinylacetate) copolymer. Experimental evidence for this behaviour is open, however.
Das freie Volumen‐Modell von Schotte wird zur Modellierung und Vorausberechnung der Löslichkeit von Ethen, Propan, Propen und But‐1‐en in geschmolzenem Polyethylen‐ bzw. (Ethen‐Vinylacetat)‐Copolymerwachs eingesetzt. Die Übereinstimmung zwischen Berechnung und experimentellen Daten ist zufriedenstellend. Für das ternäre System Ethen + But‐1‐en + Polyethylenwachs kann der experimentell gefundene Effekt, daß bei höheren But‐1‐en‐Konzentrationen im Gasgemisch Ethen stärker als But‐1‐en in der Schmelze gelöst wird, vom Modell korrekt vorausgesagt werden.
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