CN102050957B - The Azeotrope-like compositions of 1,1,1,3,3-pentafluoropropane, 1,1,1,3,3-3-pentafluorobutane and pentamethylene - Google Patents
The Azeotrope-like compositions of 1,1,1,3,3-pentafluoropropane, 1,1,1,3,3-3-pentafluorobutane and pentamethylene Download PDFInfo
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- CN102050957B CN102050957B CN200910253087.2A CN200910253087A CN102050957B CN 102050957 B CN102050957 B CN 102050957B CN 200910253087 A CN200910253087 A CN 200910253087A CN 102050957 B CN102050957 B CN 102050957B
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Abstract
Provide the composition and use thereof that one comprises the azeotrope-like mixture of 1,1,1,3,3-pentafluoropropane, 1,1,1,3,3-3-pentafluorobutane and pentamethylene.
Description
Technical field
The present invention relates to the composition and use thereof that one comprises the azeotrope-like mixture of 1,1,1,3,3-pentafluoropropane, 1,1,1,3,3-3-pentafluorobutane and pentamethylene.
Background technology
Find that fluorocarbon based fluid is widely used in multiple industrial use, comprised as refrigeration agent, aerosol propellant, whipping agent, heat-transfer medium and gaseous dielectric medium.Use these fluids of part to cause environmental problem owing to suspecting, ites is desirable to use consumption ozone possibility low or be even zero fluid, as hydrogen fluorohydrocarbon (HFCs).Therefore wish to use the fluid not comprising Chlorofluorocarbons (CFCs) (CFCs) or hydrogen chlorine fluorine hydrogen (HCFCs).In addition, the one-component fluid of not fractionation when iting is desirable to be used in explosive evaporatoin or azeotropic mixture.But, due to the fact that azeotrope formula is not easily predicted, determine that mixture new, environmental safety, not fractionation is complicated.
Summary of the invention
In preferred embodiments, the invention provides composition that environment is wished, that do not consume ozone, it shows the characteristic of Azeotrope-like, as lower constant boiling point.This characteristic makes these compositions become than any azeotrope-like mixture (namely 1,1,1,3,3-pentafluoropropane (HFC-245fa), 1,1,1,3,3-3-pentafluorobutane (HFC-365mfc) and pentamethylene) the surrogate of better CFC and HCFC of single component.
Therefore, in one aspect of the invention, provide-kind to comprise the composition of the azeotrope-like mixture of 1,1,1,3,3-pentafluoropropane, 1,1,1,3,3-3-pentafluorobutane and pentamethylene.In some preferred embodiments, azeotrope-like mixture is substantially by the pentamethylene of about 0.1 ~ 40 weight percent, 1,1,1 of about 0.1 ~ 99.9 weight percent, 1,1 of 3,3-pentafluoropropane and about 0.1 ~ 99.9 weight percent, 1,3,3-3-pentafluorobutane forms, prerequisite is pentamethylene, 1,1,1,3,3-pentafluoropropane and 1,1, the weight percent sum of 1,3,3-3-pentafluorobutane is percent 100.
On the other hand, a kind of whipping agent comprising azeotrope-like mixture described herein is provided.
On the other hand, a kind of foamable composite comprising azeotrope-like mixture described herein is provided.
On the other hand, a kind of polyvalent alcohol Preblend comprising azeotrope-like mixture described herein is provided.
On the other hand, provide-kind form the method for foam, comprise to foaming and/or add the whipping agent comprising azeotrope-like mixture as described herein in foaming composition.
On the other hand, provide a kind of foam with cell gasses, this gas comprises azeotrope-like mixture described herein.
Also have on the other hand, provide refrigerator, refrigerator and the insulating panel or plate that comprise the foam with cell gasses, this gas comprises azeotrope-like mixture described herein.
Accompanying drawing explanation
Fig. 1 is the diagram of the data of the embodiment 1 using Lemmon and Jacobsen mixing principle;
Fig. 2 is the diagram of the data of the embodiment 2 using Lemmon and Jacobsen mixing principle; With
Fig. 3 is the diagram of the temperature glide of HFC-245fa, HFC-365mfc and pentamethylene tertiary mixture under 14.7psia.
Embodiment
The present inventor has developed and has contributed to meeting several compositions to the lasting demand of the substitute of CFCs and HCFCs.According to some embodiments, the invention provides the Azeotrope-like compositions of 1,1,1,3,3-pentafluoropropane (HFC-245fa), 1,1,1,3,3-3-pentafluorobutane (HFC-365mfc) or the pentamethylene including effective amount.
In addition, applicant unexpectedly recognizes the Azeotrope-like compositions that can form HFC-245fa, HFC-365mfc and pentamethylene.Therefore, in other embodiments, the invention provides the method for producing Azeotrope-like compositions, the method comprises significant quantity mixing HFC-245fa, the HFC-365mfc and the pentamethylene that generate Azeotrope-like compositions.
In addition, applicant recognizes and sends as an envoy to Azeotrope-like compositions of the present invention display they are advantageously used for or for the performance of refrigeration agent, aerosol and foaming agent composotion.Therefore, also having in other embodiment, the invention provides the foaming agent composotion of the Azeotrope-like compositions comprising HFC-245fa, HFC-365mfc and pentamethylene.
As used herein, term " Azeotrope-like " purport comprises the composition of strict azeotropic in its broad sense and shows class with the composition of azeotropic mixture.According to ultimate principle, the thermodynamic state of fluid is made up of pressure, temperature, liquid and steam forms and determines.Azeotropic mixture is the system of two or more components, and wherein liquid composition and steam composition are identical under the temperature and pressure of regulation.In fact, this means that the component of azeotropic mixture is azeotropic and can not be separated during phase transformation.
As used herein, " significant quantity " refers to that each component causes being formed the amount of Azeotrope-like compositions of the present invention when mixing with other component as the term is employed herein.
As used herein, the term " substantially by ... composition " about the component of Azeotrope-like compositions means that said composition contains the shown component of Azeotrope-like ratio, and can contain annexing ingredient, as long as this annexing ingredient does not form new Azeotrope-like system.Such as, substantially the azeotrope-like mixture be made up of two kinds of compounds is those mixtures forming binary azeotrope, wherein optionally can comprise one or more annexing ingredients, as long as annexing ingredient does not make mixture non-azeotrope and do not form azeotrope with one or both in this compound.
Except azeotrope-like mixture, composition of the present invention can comprise the annexing ingredient not forming new Azeotrope-like system, or the annexing ingredient not in the first cut.First cut is the starting fraction obtained after distillation tower demonstrates steady-state operation under total reflux conditions.A kind of determine whether the interpolation of component forms new Azeotrope-like system to such an extent as to be method outside the scope of the invention be expect zeotrope is separated into independent component condition under distillation there is the composition sample of this component.If the mixture containing annexing ingredient is non-azeotrope-like, then annexing ingredient will fractionation be out from the component of Azeotrope-like.If mixture is Azeotrope-like, then can obtain quite limited containing entire mixture component and be azeotropic or the first cut showing as one matter.
As can be seen here, another characteristic of Azeotrope-like compositions be the Azeotrope-like having a series of same composition containing different ratios or the composition of azeotropic.All such compositions are all attempted to be contained by term " Azeotrope-like " and " azeotropic ".Such as, as everyone knows, the composition of given azeotrope changes slightly to I haven't seen you for ages at various pressures, and the boiling point of said composition is like this equally.Therefore, the azeotrope of A and B represents the relation of unique type, but has the variable composition depending on temperature and/or pressure.Visible, for Azeotrope-like compositions, there is the Azeotrope-like compositions of a series of same composition containing different ratios.All such compositions are all attempted to be contained by " Azeotrope-like " as used herein, the term.
Except azeotrope-like mixture, composition of the present invention can comprise the annexing ingredient not forming new Azeotrope-like system.Such as, composition can comprise lubricant, stablizer, fire retardant, solubilizing agent, co-foaming agent, cosolvent, altogether propellant, biological activity, personal care and/or cosmetic composition, washing composition, the component that can form foam, catalyzer, tensio-active agent, tinting material etc.
The formation can not predicting azeotrope recognized in the art.(see, such as, U.S. Patent No. 5,648,017 (the 3rd hurdle, 64-65 is capable) and U.S. Patent No. 5,182,040 (the 3rd hurdle, 62-63 is capable), the two is all incorporated herein by reference).Applicant is surprised to find that, HFC-245fa, HFC-365mfc and pentamethylene form Azeotrope-like compositions.
According to some preferred embodiments, Azeotrope-like compositions of the present invention comprises and is preferably substantially made up of HFC-245fa, HFC-365mfc of significant quantity and pentamethylene.
Azeotrope compositions of the present invention can be prepared by HFC-245fa, the HFC-365mfc and pentamethylene being mixed with effective amount.Can adopt known in the art for mixing two or more components to form any one in many methods of composition for present method to prepare Azeotrope-like compositions.Such as, as interval or the part of successive reaction and/or technique, can to mix with hand and/or by machinery, blended or contact HFC-245fa, HFC-365mfc and pentamethylene, or via the combination of two or more such steps.According to disclosure herein, the test that those skilled in the art need not be excessive just can easily prepare Azeotrope-like compositions of the present invention.It has been generally acknowledged that, in whipping agent application, to there is annexing ingredient in mixture, as polyvalent alcohol, tensio-active agent etc. can not affect Azeotrope-like characteristic of the present invention in essence.
Composition of the present invention has effectiveness in application widely.Such as, one embodiment of the invention relate to the whipping agent, aerosol, clean-out system and the refrigerant composition that comprise this Azeotrope-like compositions.
One embodiment of the invention relate to formation thermosetting foams and the method for optimization polyurethane and polyisocyanurate foam.As known in the art, these methods generally include provides a kind of foaming agent composotion of the present invention, foaming agent composotion (directly or indirectly) is added in foamable composite, then makes foamable composite react under the condition effectively forming foam or pore structure.These foams can be perforate or closed pore.Any one method as known in the art as at " PolyurethanesChemistryandTechnology; " VolumesIandII, SaundersandFrisch, 1962, JohnWileyandSons, those description in NewYork, NY (being incorporated to by reference herein) may be used to or be applicable to foam embodiment of the present invention.In general, such preferred method comprises prepares urethane or polyisocyanurate foam by mixing isocyanic ester, polyvalent alcohol or polyol blends, the whipping agent comprising the one or more of present composition or blowing agent blends and other material (as catalyzer, tensio-active agent and optional fire retardant, tinting material or other additive).
The component of urethane or polyisocyanurate foam can be provided in numerous applications easily with pre-blend formula.The most typically, by foam formulation pre-blend be two kinds of components.Isocyanic ester and some optional tensio-active agents and whipping agent form the first component, are usually referred to as " A " component.Polyvalent alcohol or polyol blends, tensio-active agent, catalyzer, whipping agent, fire retardant and other isocyanate-reactive components form second component, are usually referred to as " B " component.Therefore, preferably use machine-mixing techniques mixing A and B component to form bulk, tabular, stratiform, in-site pouring plate and other article, spray application foam (foam) by the manual mixing prepared for short run, steep (froth) etc. and easily prepare urethane or polyisocyanurate foam.Optionally, can using other composition as fire retardant, tinting material, auxiliary blowing agent and even other polyvalent alcohol be added to mixing head or reactive site as third―party logistics.But, they to be all attached in a B component most preferably as mentioned above.In some embodiments, prepare Azeotrope-like compositions, be then added in B component.In other embodiments, be added to separately in B component by the one-component of Azeotrope-like compositions, original position forms azeotrope-like mixture.
Composition of the present invention can also be used to prepare thermoplastic foam.Such as, in a conventional manner the polystyrene of routine and polyethylene formulation can be mixed with said composition and prepare rigid foams.The example of thermoplastic foam component comprises polyolefine, such as polystyrene.Other example of thermoplastic resin comprises polyethylene, ethylene copolymer, polypropylene and polyethylene terephthalate.In some embodiments, thermoplastic foamable composition is a kind of squeezable composition.Usually also think, thermoplastic foamable composition can comprise auxiliary, as nucleator, flame retardant materials, pore regulator, hole pressure conditioning agent etc.
For thermoplastic foam, preferred method generally includes to be introduced according to whipping agent of the present invention in thermoplastic material, then makes thermoplastic material stand the condition that can effectively cause foaming.Such as, the step introduced by whipping agent in thermoplastic material can comprise to be introduced in the extrusion machine containing thermoplastic material by whipping agent, and cause the step foamed can comprise the pressure on reduction thermoplastic material thus cause whipping agent to expand, contribute to the foaming of material.
Particularly in view of disclosure herein, those skilled in the art can be appreciated that usually, forms the operability that whipping agent of the present invention and/or the order added in described foamable composite and mode do not affect thermoset of the present invention or thermoplastic foam usually.
In another embodiment, Azeotrope-like compositions of the present invention can individually or with known propellant in combination as the propellant in jettable compositions.This propellant composition comprises, more preferably substantially by and be even more preferably made up of Azeotrope-like compositions of the present invention.Activeconstituents to be sprayed and inert fraction, solvent and other material also can appear at described can in spray mixture.Preferably, described jettable compositions is aerosol.The active material to be sprayed be applicable to includes but not limited to that cosmetics material is as reodorant, perfume, hair jelly, sanitising agent, deflux and polishing agent, and medicinal materials is as anti-asthma and anti-halitosis medications.
Of the present invention also have another embodiment to relate to the whipping agent comprising one or more of Azeotrope-like compositions of the present invention.In other embodiments, the invention provides foamable composite, and the foam composition of optimization polyurethane and poly-isocyanurate, and prepare the method for foam.As known in the art, in such foam embodiment, one or more of Azeotrope-like compositions are comprised in foamable composite as whipping agent, and said composition preferably comprises the component of one or more of can react under suitable conditions and foam formation foam or pore structure.Any one method as known in the art as at " PolyurethanesChemistryandTechnology; " VolumesIandII, SaundersandFrisch, 1962, JohnWileyandSons, those description in NewYork, NY (being incorporated to by reference herein) may be used to or be applicable to foam embodiment of the present invention.
Other purposes of Azeotrope-like compositions of the present invention comprises as solvent, sanitising agent etc.Those skilled in the art need not be excessive test just can easily make Azeotrope-like compositions of the present invention be applicable to such application.
Embodiment 1
The temperature range of bubble point more than 10 ~ 50 DEG C of the mixture of HFC-245fa, HFC-365mfc and pentamethylene.At first thorough mixture that is degassed, 19.78gmHFC-245fa and 18.50gmHFC-365mfc is loaded a 182.6cm
3stainless steel vessel in.This container pressure transmitter is installed and be heated to 100 DEG C any potential concentrated with what avoid higher than at the temperature of envrionment conditions.Then this container is immersed in water bath with thermostatic control.Before each measurement, under each condition, allowable temperature and pressure reach balance.By adding pentamethylene, so change total concn.6 pentamethylene are added until the total concn of pentamethylene is 47.6wt% in system.Experimental data display in table 1 below.
The ternary PTz data of table 1HFC-245fa, HFC-365mfc and pentamethylene
Embodiment 2
The bubble point of the mixture of HFC-245fa, HFC-365mfc and pentamethylene crosses the temperature range of 10 ~ 30 DEG C.At first thorough mixture that is degassed, 97.24gmHFC-245fa and 5.51gmHFC-365mfc is loaded a 182.6cm
3stainless steel vessel in.This container pressure transmitter is installed and be heated to 100 DEG C any potential concentrated with what avoid higher than at the temperature of envrionment conditions.Then this container is immersed in water bath with thermostatic control.Before each measurement, under each condition, allowable temperature and pressure reach balance.By adding pentamethylene, so change total concn.6 pentamethylene are added until the total concn of pentamethylene is 10.5wt% in system.Experimental data is presented in following table 2.
The ternary PTz data of table 2HFC-245fa, HFC-365mfc and pentamethylene
Embodiment 3
With the data regression interaction coefficient of table 1 and table 2 so that can by using the mixing principle (Lemmmon proposed by Lemmon and Jacobsen, E.W.andJacobsen, R.T, " AGeneralizedModelfortheThermodynamicPropertiesofMixtures ", Int.J.Thermophys., 20 (3): 825-835,1999.) by these data modelings.Fig. 1 and Fig. 2 gives and fits data (line) and experimental data point (◆).These figure show this model can accurate reproduction data.
Embodiment 4
Use the interaction parameter returned in embodiment 3 can calculate whole phase vaults (phasedome) of HFC-245fa, HFC-365mfc and pentamethylene tertiary mixture.Determine that mixture be whether the method for Azeotrope-like is consider a difference for dew point and bubble point temperature, it is considered to the slippage under setting pressure usually.Under azeotropic point, the difference between slippage is zero.Azeotrope-like mixture has low slippage.Fig. 3 has marked and drawed the slippage of HFC-245fa, HFC-365mfc and pentamethylene tertiary mixture.Can see from this figure, comprising the pentamethylene of 40wt% at the most and surplus is that the tertiary mixture of the HFC-245fa of 1 ~ 99wt% and the HFC-365mfc of 1 ~ 99wt% forms azeotrope-like mixture.
Claims (26)
1. a composition, comprises 1, and 1,1,3,3-pentafluoropropane, 1,1,1,3, the azeotrope-like mixture of 3-3-pentafluorobutane and pentamethylene, wherein said azeotrope-like mixture by the pentamethylene of 0.1 to 40 weight percents, 1,1 of 0.1 to 99.9 weight percents, 1,3,1,1,1,3,3-3-pentafluorobutane composition of 3-pentafluoropropane and 0.1 to 99.9 weight percents, prerequisite is pentamethylene, 1,1,1,3,3-pentafluoropropane and 1, the weight percent sum of 1,1,3,3-3-pentafluorobutane is percent 100.
2. composition according to claim 1, wherein based on the gross weight of azeotrope-like mixture, 1,1,1,3,3-described pentafluoropropane exists with the amount of 27 to 52 weight percents.
3. composition according to claim 1, wherein based on the gross weight of azeotrope-like mixture, 1,1,1,3,3-described 3-pentafluorobutane exists with the amount of 25 to 49 weight percents.
4. composition according to claim 1, wherein based on the gross weight of azeotrope-like mixture, described 1,1,1,3,3-pentafluoropropane exists with the amount of 27 to 52 weight percents, and described 1,1,1,3,3-3-pentafluorobutane exists with the amount of 25 to 49 weight percents.
5. composition according to claim 1, wherein based on the gross weight of azeotrope-like mixture, described pentamethylene exists with the amount of 1 to 38 weight percents.
6. composition according to claim 1, wherein based on the gross weight of azeotrope-like mixture, described pentamethylene exists with the amount of 1 to 33 weight percents.
7. composition according to claim 1, wherein based on the gross weight of azeotrope-like mixture, described pentamethylene exists with the amount of 1 to 24 weight percents.
8. composition according to claim 1, wherein based on the gross weight of azeotrope-like mixture, described pentamethylene exists with the amount of 1 to 13 weight percents.
9. composition according to claim 1, wherein said azeotrope-like mixture by the pentamethylene of 0.1 to 10.5 weight percents, 1,1 of 84.7 to 94.6 weight percents, 1,1,1 of 3,3-pentafluoropropane and 4.8 to 5.4 weight percents, 1,3,3-3-pentafluorobutane forms, prerequisite is pentamethylene, 1,1,1,3,3-pentafluoropropane and 1,1, the weight percent sum of 1,3,3-3-pentafluorobutane is percent 100.
10. one kind comprises the whipping agent of the Azeotrope-like compositions any one of claim 1 ~ 9.
11. 1 kinds of foamable composites comprising the Azeotrope-like compositions any one of claim 1 ~ 9.
12. foamable composites according to claim 11, wherein said composition can produce the foam being selected from polyurethane foam, polyisocyanurate foam, phenol formaldehyde foam, polystyrene foam, polyethylene, polypropylene foam and polyethylene terephthalate foam.
13. 1 kinds of polyvalent alcohol Preblendes comprising the whipping agent of claim 10.
14. 1 kinds of methods forming foam, comprise to foaming and/or add the whipping agent of claim 10 in foaming composition.
15. 1 kinds comprise multiple abscess and are included in the foam of the cell gasses in abscess described at least one, and described cell gasses comprises the composition any one of claim 1 ~ 9.
16. foams according to claim 15, wherein said foam has the shape being selected from bulk, tabular and stratiform.
17. foams according to claim 15, wherein said foam is open celled foam.
18. foams according to claim 15, wherein said foam is closed-cell foam.
19. foams according to claim 15, wherein said foam is rigid foams.
20. foams according to claim 15, it is the form of flexible foam.
21. foams according to claim 15, it is the form of integral skin foam.
22. foams according to claim 15, wherein by being selected from spray application, in-site pouring, injected hole and forming described foam as steeping the method used.
23. foams according to claim 15, wherein produce described foam in a continuous process.
24. foams according to claim 15, wherein produce described foam in batch technology.
25. 1 kinds of refrigerator or refrigerators comprising the foam according to any one of claim 15-24.
26. 1 kinds of insulating panel or plates comprising the foam according to any one of claim 15-24.
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