CN102559146B - Non-combustible mixing refrigerant suitable for deep refrigeration temperature of minus 80 DEG C to minus 100 DEG C - Google Patents
Non-combustible mixing refrigerant suitable for deep refrigeration temperature of minus 80 DEG C to minus 100 DEG C Download PDFInfo
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Abstract
The invention relates to a non-combustible mixing refrigerant suitable for deep refrigeration temperature of minus 80 DEG C to minus 100 DEG C. The non-combustible mixing refrigerant comprises five groups of materials, where the first group of material is tetrafluoromethane; the second group of material is trifluoromethane, hexafluoroethane or a mixture of the trifluoromethane and the hexafluoroethane; the third group of material is pentafluoroethane, trifluoroethane, perfluoropropane, difluoromethane or a mixture of two, three or multiple of the pentafluoroethane, the trifluoroethane, the perfluoropropane and the difluoromethane; the fourth group of material is iodotrifluoromethane, 1, 1, 2, 2-tetrafluoroethane, 1,1-difluoroethane, 2, 3, 3, 3-tetrafluoropropene, 1, 3, 3, 3-tetrafluoropropene or a mixture of two, three or multiple of the iodotrifluoromethane, the 1, 1, 2, 2-tetrafluoroethane, the 1,1-difluoroethane, the 2, 3, 3, 3-tetrafluoropropene and the 1, 3, 3, 3-tetrafluoropropene; the fifth group of material is perfluoro-n-butane, 1, 1, 1, 3, 3-perfluoropropane or a mixture of the perfluoro-n-butane and the 1, 1, 1, 3, 3-perfluoropropane; the molar concentrations of the five groups of materials are respectively 25-50%, 15-40%, 10-30%, 5-20% and 10-25%; and the non-combustible mixing refrigerant is safe in a back-heating type throttling refrigeration system, can realize the refrigeration in the temperature range of minus 80 DEG C to minus 100 DEG C and has low whole green house effect without ozone depletion effect.
Description
Technical field
The present invention relates to the refrigeration agent in refrigeration and low temperature technique field, the particularly non-combustible mix refrigerant of a kind of being applicable to-80～-100 ℃ cryogenic temperature.
Background technology
Utilize the Cryogenic mixed-refrigerants j-t refrigerator of backheat measure to have efficiently, the advantage such as reliable and low cost of manufacture, be widely used in the energy, chemical industry and cryogenic engineering field, such as, for realizing the aspect such as liquefaction of the cooling and industrial gasses of device depth, the field such as cryogenic refrigerator, natural gas liquefaction.Except the hardware facilities such as refrigeration system flow process and compressor and interchanger, what this Refrigeration Technique was the most key is Diversity refrigeration agent.Be applied to the Diversity refrigeration agent of mixed work medium for throttling refrigeration system according to requirement and the system structure design of refrigeration warm area, conventionally require 3～7 kinds of constituent elements to form, show as typical non-azeotropic feature, and utilize the temperature variant nonlinear characteristic of enthalpy between its phase change zone, realize the thermal equivalent coupling between high-low pressure refrigeration agent, thereby improve refrigerating efficiency.From another one angle, set forth, the temperature range that each constituent element undergoes phase transition at it has higher isothermal throttling effect, and each constituent element with different boiling temperature is according to the relay of boiling point High-low Match, can forms mix refrigerant and across scope, there is higher refrigeration effect in whole refrigeration temperature.Relevant refrigeration agent screening and thermodynamic optimization principle can, referring to relevant academic documents, repeat no more here.
Owing to being subject to the Basic Physical Properties parameter limit such as boiling point, freezing point temperature of constituent element, also have in addition other physicochemical property such as combustibility, toxicity of constituent element working medium, the optional constituent element under the effective constituent element of mixing medium, especially low temperature is very limited.At present by some mandates or apply for a patent and relate to deep cooling mixing medium and form and concentration proportioning, wherein granted patent ZL 97115295.0, ZL 03121423.1,03121466.5 point of warm area of ZL 03121467.3 and ZL has proposed the serial multicomponent mixture work medium for copious cooling throttle Refrigeration Technique, wherein constituent element has the fluorochemical of nitrogen, alkane and part alkane to form, mixture ozone free damage effect.The each constituent element of mixture is divided into cold zone constituent element, the normal warm area constituent element that freezes according to boiling point difference, middle high-temperature zone constituent element and high-temperature zone constituent element, and each warm area constituent element, according to the multicomponent mixture work medium of a concentration ratio acquiring demand, has higher thermodynamic(al) efficiency.The alkanes substances such as the methane, ethane and the propane that wherein contain have the mutual solubility good with lubricating oil, and Greenhouse effect are little, and environmental protection characteristic is good, but it is certain flammable to cause system to exist.And due to the existence of combustiblecomponents, make system all need to consider the measures such as explosion-proof in links such as production, debugging, maintenances, increase the difficulty that production cost and user accept, especially in North America market.
There is patent application ZL 01802606.0 (publication number: CN 1388887A, similar content appears in the middle of US6502410 patent with it) hydrofluoride (HFCs) and perfluoro-compound (FC) with nitrogen (N2), argon gas (Ar) and alkane proposed, the non-combustible Diversity refrigeration agent of the composition such as such as R23, R125, R134a, R236fa and R245fa, wherein minimum temperature can realize 105K, also contains the compositions such as neon (Ne), helium (He).This patent according to refrigeration warm area difference, is divided into different zones for the constituent element in mixture according to its boiling point equally, by each warm area different boiling constituent element, according to finite concentration proportional range, forms whole mixt.Its whole mixture is not containing flammable alkanes composition, and also not hydrogeneous fluorochlorohydrocarbon (HCFC) class has the component of ozone layer destroying.It is poor that but its efficiency contains the mixture of alkane.Wherein in order to adopt, avoid flammable, its non-combustible HFC class material of choosing all has the higher Greenhouse effect value (GWP) of diving as high boiling point constituent elements such as HFC125, HFC236fa.
Separately there is U.S. Pat 5408848 to propose the mixing medium Refrigeration Technique that a kind of employing does not contain CFC constituent element,-150 minimum to meet ℃ above refrigeration demand, has wherein provided in an embodiment take R142b, R134a, R23, R14 and Ar as main mixing medium composition.In this compositions of mixtures, not containing combustibleconstituents, still wherein containing R142b is HCFC material, has depletion of the ozone layer effect, belongs to the row of restriction and forbidding.
When adopting mixed work medium for throttling Refrigeration Technique to realize the situation of deep refrigerating, according to deep cooling mixing medium Refrigeration Technique principle, the boiling point of the required constituent element of multicomponent mixture work medium that it adopts should be according to refrigeration warm area, (concrete elaboration seen Cryogenics Volume 44 by minimum temperature (should lower than or at least equal lowest refrigerating temperature), to start to be increased to gradually envrionment temperature, Issue 12, December 2004, Pages 847-857).Therefore realize cryogenic refrigeration, for example, in the time of-100 ℃, in mixture, must have the constituent element lower than-100 ℃, for example CF4 (R14), even Ar or N2 exist.Due to the lower boiling constituent element limited amount that nature exists, in natural medium, non-flammable material, generally by materials such as He, Ne, N2, Ar, only has R14 etc. in the middle of synthetic material.To realize in addition cryogenic refrigeration, except the boiling point of material is applicable to, also need freezing point temperature enough low, to avoid separating out at low temperatures solid, stop up fluid channel, especially throttle capillary tube.Therefore when realizing cryogenic refrigeration, in the constituent element of minimum warm area, the materials such as He, Ne, N2, Ar and R14 are essential according to the refrigeration warm area that will realize substantially, especially the material such as N2, Ar, R14 and R23.This also can find out from patent ZL 01802606.0 and US5408848, these two patents have all comprised the materials such as N2, Ar, R14 and R23, but in the mixture of its composition, also contain different compositions, for example US5408848 has R142b, and ZL 01802606.0 contains the materials such as R125, R245fa and R236fa.
As everyone knows, for a kind of mixture being formed by many kinds of substance, its hot physical property is determined by mixture constituent element and constituent element concentration, but the wherein identical concentration difference of the difference of constituent element or constituent element, all can form diverse mixture, this shows that the hot physical property such as the equivalent weight, critical parameter, enthalpy entropy of mixture are all variant.Constituent element is identical and concentration difference shows more in general cold mixt refrigeration agent, the zeotrope for example being formed by R32, R125 and tri-kinds of materials of R134a, because the difference of composition concentration can be divided into different refrigeration agents, its application scenario is also not quite similar, the mixture and the business-like numbering that above-mentioned three kinds of materials, consist of at present can specifically be divided into the refrigeration agents such as R407A～R407E, and it has diverse physical property and alternative object.These are set forth and analyze is just a problem of explanation, and by comprising the even identical constituent element of part same components, different concns can form diverse mixture, and it specifically can be determined by corresponding target.
According to above-mentioned analysis, can know in the middle of prior art and realize and comprised the polynary non-combustible mix refrigerant of deep cooling being formed by N2, Ar, R14, R23 and other high boiling substances etc., but in the middle of this type of mix refrigerant in high boiling point constituent element or adopted R142b etc. to contain the dive material of value (ODP) of ozone layer destroying, adopted R236fa etc. to have the hydrogen fluorohydrocarbon material of high-temperature chamber effect (GWP), these all make its environmental protection characteristic be affected.The mutual solubility of most HFC and FC class material and lubricating oil is poor in addition, there is in addition the HFC of higher and the freezing point temperature of FC class material is all higher, and the molten oiliness of the low temperature of its mix refrigerant is poor, therefore above-mentioned non-combustible mix refrigerant is generally applied in the middle of multistage automatic cascade refrigeration system.And multistage vapor-liquid separating device is set in the middle of system conventionally, and lubricating oil and the constituent element with high-solidification point temperature are separated in higher temperatures district, with assurance system, normally work.
Summary of the invention
The object of the invention is to: for solving the combustibility of deep cooling mixing medium, and reduction Greenhouse effect, improve its environmental protection characteristic, and provide a kind of and be applicable to the non-combustible mix refrigerant of-80～-100 ℃ of cryogenic temperatures, can be applicable in back-heating type mixed work medium for throttling refrigeration system to realize the refrigeration of-80～-100 ℃ of warm areas, for a kind ofly thering is safety, environmental protection, being applied to the non-combustible mix refrigerant that is applicable to-80～-100 ℃ of cryogenic temperatures.
Technical scheme of the present invention is as follows:
The non-combustible mix refrigerant of provided by the invention being applicable to-80～-100 ℃ cryogenic temperature, it is comprised of following five groups of materials, and these five groups of materials are respectively:
First group of material is tetrafluoromethane (CF
4, R14);
Second group of material is trifluoromethane (CHF
3, R23), hexafluoroethane (CF
3cF
3, R116) or the mixture of the two composition;
The 3rd group of material is pentafluoride ethane (CHF
2cF
3, R125), Halothane (CH
3cF
3, R143a), perfluoropropane (C
3f
8, R218), methylene fluoride (CH
2f
2, R32) or these materials in the mixture of two kinds of materials, three kinds of materials or many kinds of substance composition;
The 4th group of material is CF3I (CF
3i, R13I1), 1,1,2,2-Tetrafluoroethane (CHF
2cHF
2, R134), 1,1-C2H4F2 C2H4F2 (CH
3cHF
2, R152a), 2,3,3,3-tetrafluoeopropene (CF
3cF=CH
2, R1234yf), 1,3,3,3-tetrafluoeopropene (CF
3cH=CHF, R1234ze) or these materials in the mixture of two kinds of materials, three kinds of materials or many kinds of substance composition;
The 5th group of material is perfluorinated butane (C
4f
10, R3110), 1,1,1,3,3-pentafluoropropane (CHF
2cH
2cF
3, R245fa) or the mixture of the two composition;
In the mixture of described five groups of materials composition, the volumetric molar concentration sum of each group material is 100%;
Wherein, the volumetric molar concentration of described first group of material is 25%～50%;
The volumetric molar concentration of described second group of material is 15%～40%;
The volumetric molar concentration of described the 3rd group of material is 10%～30%;
The volumetric molar concentration of described the 4th group of material is 5%～20%;
The volumetric molar concentration of described the 5th group of material is 10%～25%.
What the present invention proposed is applicable to-80～-100 ℃ of efficient non-combustible mix refrigerants of warm area, and when the 3rd group of material taked methylene fluoride (R32), Halothane (R143a) or the mixture of the two, its volumetric molar concentration is 10%～15%.
What the present invention proposed is applicable to-80～-100 ℃ of efficient non-combustible mix refrigerants of warm area, and when the 4th group of material taked 1,1-C2H4F2 C2H4F2 (R152a), its volumetric molar concentration is 10%～15%.
What the present invention proposed is applicable to-80～-100 ℃ of efficient non-combustible mix refrigerants of warm area, when the 3rd group of material taked methylene fluoride (R32), Halothane (R143a) or the mixture of the two, and the 4th group of material takes 1 simultaneously, during 1-C2H4F2 C2H4F2 (R152a), the volumetric molar concentration sum of the 3rd group of material and the 4th group of material is 15%～25%.
Above-mentioned mixing medium concentration range exists corresponding to working pressure range: high pressure is in 1.6～2.3MPa scope, and low pressure (is absolute pressure) within the scope of 0.2～0.6MPa, and normal pressure ratio scope is between 3～10.Wherein the change in concentration general trend of each constituent element is to increase with low pressure, and lower boiling constituent element concentration increases, and corresponding middle high boiling point constituent element concentration reduces, and vice versa.Adopt the back-heating type mixed work medium for throttling refrigeration system of above-mentioned mix refrigerant can take in higher temperatures district one-level vapour liquid separator, lubricating oil and part high boiling point constituent element are separated to reflux, guarantee security of system reliability service, concrete refrigeration cycle structure can be referring to public technologies such as patent ZL00136709.9, or other similar cycle structures, repeat no more here.
In the non-combustible mix refrigerant of above-mentioned being applicable to-80～-100 ℃ cryogenic temperature, in the 3rd group of material, chosen R32 and the R143a with moderate flammable nature, and chosen the R152a with moderate flammable nature in the middle of the 4th group; Although above-mentioned three kinds of materials have the flammable characteristic of moderate, are divided into A2 classification according to refrigeration agent security classes, its combustibility is not strong, and itself and other non-combustible class material composition can form the complete non-flammable mixture of entirety.This has embodiment in business-like refrigeration agent in general cold field more, for example business-like R410A refrigeration agent, its composition is R32/R125, mass concentration ratio is 50%/50%, and volumetric molar concentration is 69.8%/30.2%, and the mixture of its composition is completely non-flammable, security classification is A1, for substituting R22, even if in this mixture, the volumetric molar concentration of R32 is up to approximately 70%, it is non-flammable that whole mixt remains at present.For example R401 series mixture refrigeration agent, wherein contains R152a component again, and the maximum volumetric molar concentration of R152a exceedes 22%, but mixture entirety remains non-flammable.Compared with boiling point constituent element close to other, R32 and R152a material all have higher thermomechanical property, and its GWP value is far below similar HFC class material, and the GWP value of for example R32 is 550, and the GWP value of R152a is 120, at present conventional HFC class refrigeration agent, there is the material of minimum GWP.
The non-combustible mix refrigerant tool of of the present invention being applicable to-80～-100 ℃ cryogenic temperature has the following advantages: adopt the regenerative refrigerating system of non-combustible mix refrigerant of the present invention can be safely, realize efficiently-80～-100 ℃ of warm areas refrigeration, compared with existing deep cooling mix refrigerant, it does not have combustibility completely, and overall Greenhouse effect are low, non ozone depleting effect, has significant advantage completely.
Embodiment
Embodiment 1-3
Preparation the present invention runs on the non-combustible Diversity refrigeration agent of-80 ℃ of warm areas, and the inner minimum heat transfer temperature difference of interchanger is 1K, and envrionment temperature is 27 ℃, and its non-combustible Diversity refrigeration agent working medium concentration and performance see the following form:
Embodiment 2: preparation runs on the non-combustible Diversity refrigeration agent of-86 ℃ of warm areas, the inner minimum heat transfer temperature difference of interchanger is 1K, and envrionment temperature is 27 ℃, and its non-combustible Diversity refrigeration agent working medium concentration and performance see the following form:
Embodiment 3: preparation runs on the non-combustible Diversity refrigeration agent of-100 ℃ of warm areas, the inner minimum heat transfer temperature difference of interchanger is 1K, and envrionment temperature is 27 ℃, and its non-combustible Diversity refrigeration agent working medium concentration and performance see the following form:
In above-described embodiment, the regenerative refrigerating system of the non-combustible mix refrigerant adopting can be safely, realize efficiently-80～-100 ℃ of warm areas refrigeration, compared with existing deep cooling mix refrigerant, it does not have combustibility completely, and overall Greenhouse effect are low, non ozone depleting effect, has significant advantage completely.
Claims (2)
1. be applicable to a non-combustible mix refrigerant for-80～-100 ℃ of deep cooling warm areas, it is comprised of following five groups of materials, and these five groups of materials are respectively:
First group of material is tetrafluoromethane;
Second group of material is trifluoromethane, hexafluoroethane or the mixture of the two;
The 3rd group of material is the mixture of two kinds of materials in pentafluoride ethane, Halothane, perfluoropropane, methylene fluoride or these materials, three kinds of materials or many kinds of substance composition;
The 4th group of material is CF3I, 1,1,2,2-Tetrafluoroethane, 2,3,3,3-tetrafluoeopropene, 1,3,3, the mixture of two kinds of materials in 3-tetrafluoeopropene or these materials, three kinds of materials or many kinds of substance composition;
The 5th group of material is 1,1,1,3,3-pentafluoropropane;
In the mixture of described five groups of materials composition, each group material volumetric molar concentration sum is 100%;
Wherein: the volumetric molar concentration of described first group of material is 25%～50%;
The volumetric molar concentration of described second group of material is 15%～40%;
The volumetric molar concentration of described the 3rd group of material is 10%～30%;
The volumetric molar concentration of described the 4th group of material is 5%～20%;
The volumetric molar concentration of described the 5th group of material is 10%～25%.
2. by the non-combustible mix refrigerant of claimed in claim 1 being applicable to-80～-100 ℃ deep cooling warm area, it is characterized in that: described the 3rd group of material is methylene fluoride, Halothane or the mixture of the two, and the volumetric molar concentration of described the 3rd group of material is 10%～15%.
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|---|---|---|---|
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| CN105885797A (en) * | 2014-09-07 | 2016-08-24 | 张永康 | Incombustible mixed refrigerant suitable for -50 to -70 DEG C temperature range of refrigeration |
| JP6555315B2 (en) * | 2017-10-16 | 2019-08-07 | ダイキン工業株式会社 | Refrigerant composition containing HFO-1234ze (E) and HFC-134 and use thereof |
| CN108531135B (en) | 2018-04-10 | 2021-05-07 | 龙志刚 | Mixed refrigerant suitable for cryogenic temperature zone and preparation method and application method thereof |
| JP6693589B2 (en) | 2018-04-19 | 2020-05-13 | ダイキン工業株式会社 | Composition containing refrigerant and application thereof |
| KR20210034033A (en) * | 2018-07-20 | 2021-03-29 | 더 케무어스 컴퍼니 에프씨, 엘엘씨 | Refrigerant composition |
| CN114111113B (en) * | 2018-11-30 | 2023-11-14 | 特灵国际有限公司 | Lubricant Management for HVACR Systems |
| CN110257011A (en) * | 2019-06-13 | 2019-09-20 | 深圳市泰祺科技有限公司 | The non-combustible ice making agent of -20~-80 degrees Celsius of low-temperature energy-savings |
| CN110305631A (en) * | 2019-07-03 | 2019-10-08 | 上海沛芾航天科技发展有限公司 | A kind of mixed working fluid refrigerant for environmental test chamber |
| CN110645743A (en) * | 2019-09-12 | 2020-01-03 | 珠海格力电器股份有限公司 | Centrifugal water chilling unit adopting environment-friendly refrigerant |
| CN110878197B (en) * | 2019-10-16 | 2020-12-22 | 珠海格力电器股份有限公司 | Mixed working medium and heat exchange system |
| CN111592858B (en) * | 2020-05-21 | 2022-01-11 | 冰山松洋生物科技(大连)有限公司 | Mixed refrigerant, refrigeration system and refrigeration device |
| CN113480979A (en) * | 2021-07-16 | 2021-10-08 | 湖北绿冷高科节能技术有限公司 | Special refrigerant for quick-freezing refrigeration house, refrigeration equipment and quick-freezing refrigeration house |
| CN116606632B (en) * | 2023-07-19 | 2023-10-20 | 中科美菱低温科技股份有限公司 | Refrigerant and method for producing the same |
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|---|---|---|---|---|
| CN1460703A (en) * | 2002-05-17 | 2003-12-10 | 中国科学院理化技术研究所 | Multicomponent mixed work medium throttling refrigerant applicable to 200-204K refrigerating temperature zone |
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| CN1460703A (en) * | 2002-05-17 | 2003-12-10 | 中国科学院理化技术研究所 | Multicomponent mixed work medium throttling refrigerant applicable to 200-204K refrigerating temperature zone |
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