WO2017178412A1 - Milieu accumulateur de chaleur à base de nitrate et centrale solaire thermique - Google Patents

Milieu accumulateur de chaleur à base de nitrate et centrale solaire thermique Download PDF

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Publication number
WO2017178412A1
WO2017178412A1 PCT/EP2017/058509 EP2017058509W WO2017178412A1 WO 2017178412 A1 WO2017178412 A1 WO 2017178412A1 EP 2017058509 W EP2017058509 W EP 2017058509W WO 2017178412 A1 WO2017178412 A1 WO 2017178412A1
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Prior art keywords
nitrate
storage medium
heat storage
mol
potassium
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PCT/EP2017/058509
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German (de)
English (en)
Inventor
Matthias ÜBLER
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Siemens Aktiengesellschaft
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Publication of WO2017178412A1 publication Critical patent/WO2017178412A1/fr

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    • C—CHEMISTRY; METALLURGY
    • C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09K—MATERIALS FOR MISCELLANEOUS APPLICATIONS, NOT PROVIDED FOR ELSEWHERE
    • C09K5/00—Heat-transfer, heat-exchange or heat-storage materials, e.g. refrigerants; Materials for the production of heat or cold by chemical reactions other than by combustion
    • C09K5/08—Materials not undergoing a change of physical state when used
    • C09K5/10—Liquid materials
    • C09K5/12—Molten materials, i.e. materials solid at room temperature, e.g. metals or salts
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F24—HEATING; RANGES; VENTILATING
    • F24S—SOLAR HEAT COLLECTORS; SOLAR HEAT SYSTEMS
    • F24S60/00—Arrangements for storing heat collected by solar heat collectors
    • F24S60/10—Arrangements for storing heat collected by solar heat collectors using latent heat
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F24—HEATING; RANGES; VENTILATING
    • F24S—SOLAR HEAT COLLECTORS; SOLAR HEAT SYSTEMS
    • F24S80/00—Details, accessories or component parts of solar heat collectors not provided for in groups F24S10/00-F24S70/00
    • F24S80/20—Working fluids specially adapted for solar heat collectors
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E10/00—Energy generation through renewable energy sources
    • Y02E10/40—Solar thermal energy, e.g. solar towers

Definitions

  • the invention relates to a heat storage medium based on nitrate, in particular a binary Nitratsalzgemisch and / or a heat storage medium based on a binary Nitratsalzgemisches and a solar thermal power plant in which such a salt mixture is provided as a heat storage medium.
  • Receiver tubes in the form of heat via a heat exchanger to transfer a water-steam cycle with generator.
  • Schlechtwetterperi ⁇ oden is ⁇ det during the daytime phase continu ously ⁇ a portion of the collected heat for heating a liquid salt mixture of about 290 ° C to about 390 ° C USAGE.
  • This salt mixture used as thermal energy storage is known by the name SolarSalt and is usually a mixture of 60 wt .-% sodium nitrate and 40 wt .-% potassium nitrate, with a non-eutectic melting point of 238 ° C, where the "cold" salt mixture at 290 ° C in the cold tank is heated up to 393 ° C via a special oil-salt heat exchanger against the hot heat transfer medium leaving the solar field Hot tank pumped and stored for night use. After sunset, this now hot salt mixture is again used to heat the heat transfer medium, thereby thermally discharged via oil-salt heat exchanger from about 390 ° C to about 290 ° C and pumped from the hot tank in the cold tank.
  • TES thermal energy storage
  • the heat oil heated by these heat provided by the TES system is thus able to supply the turbine of the generator with steam during the night phase, thus maintaining the continuous generation of electricity through the generator.
  • This TES system is thus essential for the solar thermal power plant technology, as it allows to provide energy in a simple manner according to the principle of "heat-to-power" for a later date and thereby save relatively inexpensively.
  • the costs for the known solar duty fluctuate since the nitrates are used not only for TES storage salt production, but mainly for fertilizer production. Apart from that, the low-cost nitrate salt mixtures also always entail the risk that chloride-contaminated salt mixtures are used which, when used in storage facilities, cause corrosive damage there.
  • Power generation such as solar thermal power plant technology, to bring more and more economic in (socio-) compete with fossil Ener ⁇ gieermaschineung.
  • EP 0 049 761 A1 discloses a ternary mixture with crystalline calcium nitrate as heat transfer medium.
  • WO 2015043810 A1 discloses a heat storage medium based on a double salt of potassium calcium nitrate and a sodium nitrate, which can optionally be used in solar thermal power plants in the presence of water of crystallization.
  • a disadvantage of the previously known nitrate-based heat transfer and / or heat storage media is the high potassium content, which, as explained above, with cost-effective availability, entails the risk of corrosive damage to the installation.
  • CSP experts so far will focus on the lowest-melting formulation of a salt mixture into ⁇ particular with regard to the possible use as a heat transfer medium, so instead of conventionally ver Liste- th thermal oils laid.
  • Nitrate-based salt mixtures are available which, owing to the risk of corrosion in the power plants, are as low-chloride and inexpensive as possible and nevertheless can be used as storage medium in solar thermal power plants, as described above, with regard to their liquidus temperature and / or their thermal stability.
  • nitrite mixtures in combination or as a replacement of nitrate-based salt mixtures for varnish arrivedme- is serving disadvantageous because nitrite mixtures are toxic and easily react un ⁇ ter air and / or oxygen to the respective Nitra ⁇ th, which with a change in the thermophysical properties and therefore can not be tolerated in solar power plant operation.
  • the subject of the present invention is therefore a heat storage medium for solar power plants based on nitrate, characterized in that nitrates of the alkali and alkaline earth group are combined so that the smallest possible proportion of potassium nitrate results and still a liquidus temperature of 270 ° C, in particular 250 ° C, particularly preferably of 230 ° C is not exceeded.
  • Potassium nitrate arms or even potassium nitrate-free salt mixtures nitrate based as heat storage media are to unanswered shouted ⁇ ben, as is understood in the art from a continuous operating temperature of 565 ° C and above, as for used there heat transfer media, prevails in parabolic trough solar power plants.
  • this requirement does not apply; rather, it is possible to start from a continuous service temperature of 450 ° C., so that no stability of the salt mixture above this temperature is required.
  • the maximum Ge ⁇ use temperature of thermal oils, which are used in the considered here solar thermal power plants as a heat transfer medium is approximately at 400 ° C to 450 ° C, so that a pure heat storage medium in these solar power plants, which are just operated with thermal oils, no stability above must have this temperature.
  • potassium nitrate-free is in the present case a salt mixture is characterized loading which does not hold appreciable amounts of potassium nitrate ent ⁇ , wherein in case of technical salts and salt mixtures usual impurities with potassium, so as salt mixtures with potassium amounts up to 0.5 mol% here also as “ Potassium free ".
  • This technical see salt mixtures are used and no high-purity Sal ⁇ ze, as are common for example in medical technology.
  • corrosion-demanding substances such as hydroxides, carbonates, halides, halogens and / or sulfates in the salt mixture of the heat storage medium ⁇ killed, directly or indirectly, be avoided.
  • directly in Salzge ⁇ mixing it is meant the addition of salts of these anions, whereas an "indirect presence” of these anions in the salt mixture is referred to when the possible reaction of the salt mixture carbonate for example, a hydroxide and / or carbonyl in air is likely and / or the contamination of the salt mixture by a manufacturing process of a Heat storage medium salt used, for example, a halide, such as a chloride comprises.
  • the heat storage medium to more than 60 mol%, in particular more than 70 mol%, and particularly preferably more than 90 mol ⁇ 6 a binary salt mixture of calcium nitrate and sodium nitrate, calculated free of water of crystallization, but can be containing water of crystallization.
  • the heat storage medium is a binary salt mixture of calcium and sodium nitrate, containing water of crystallization or free of water of crystallization. It can be provided that the salt mixture contained potassium amounts less than 40 mol%, in particular less than 30 mol%, particularly be less than 5 mol% ⁇ vorzugt.
  • the ratio of potassium to calcium ions in the salt mixture is 1 to 6 or greater, ie for example 1 to 7 to 1 to 999 or more, that is to say 999 in the analysis of the salt mixture used as the heat storage medium
  • Calcium ions only a single potassium ion or even less potassium ions.
  • Figure 1 shows the liquidus of the binary salt mixture Ca (N03) 2 _ NaNÜ3.
  • Ca (NO 3) 2 has a melting point of about 233 ° C and thus a very low solidification temperature. It is potassium nitrate-free and shows a relatively high specific heat capacity due to the high sodium nitrate content. This is particularly the case since the specific heat capacity in the liquid state at 400 ° C. of potassium nitrate, over sodium nitrate towards lithium nitrate in the alkali group increases sharply and sodium is known to be above potassium in the Periodic Table of the Elements (PSE) (LiNO 3 : 2.04 J / (gK), NaN0 3 : 1.63 J / (gK), KN0 3 : 1.38 J / (gK)).
  • PSE Periodic Table of the Elements
  • the binary salt mixture of calcium and sodium nitrate and / or it comprises a high proportion of sodium nitrate and a lower proportion of calcium nitrate, a leveling of volumetric energy storage density takes place, since the reduction of the specific total heat capacity by the calcium Part is partially compensated due to the higher density of calcium nitrate.
  • the dynamic viscosity is due to the calcium nitrate ge ⁇ slightly higher than that of the solar Salts such as Ge in Figure 2 shows ⁇ is.
  • Figure 2 shows the dynamic viscosity of solar ⁇ salt and the Na-Ca / nitrate eutectic in the relevant temperature range of 290 ° C (about 9 mPa-s) to 390 ° C (about 4 mPa-s).
  • the viscosity values differ accordingly le ⁇ diglich to five (290 ° C) or two mPa.s requires that for common salt pumps, for example of the type submersible pump, no change of a design, and / or a pump power.
  • the binary sodium nitrate-calcium nitrate salt mixture differs from SolarSalt mainly in the use of calcium nitrate instead of potassium nitrate.
  • This component is mostly commercially available as a tetrahydrate of the chemical formula Ca (NO 3 ) 2 H 2 O (so-called "Norway Salpeter ”) and represents a relatively inexpensive material compared to potassium nitrate (about 50-60% of the price of KNO 3 ).
  • Na-Ca / nitrate melts in the preparation of binary Na-Ca / nitrate melts, in
  • Premelter mixes in which the two salt components are usually first and once melted together at about 300 ° C and pumped into the cold storage tank, expelled this crystalline water content of calcium nitrate. This represents an easily manageable process beginning at 110 ° C. and concluded at 250 ° -300 ° C.
  • FIG. 3 the expulsion behavior investigated by means of differential scanning calorimetry is correspondingly shown.
  • Figure 3 shows the heating behavior of the crystal water-containing mixture of calcium nitrate tetrahydrate and sodium nitrate, which yields the anhydrous eutectic when heated to 300 ° C, un ⁇ ter indicate the enthalpies (above), second melting of the unique dehydrated mixture with evidence of formation of the eutectic with melting point 230 ° C (center) and the Clearar ⁇ approximately behavior during cooling (below).
  • the ammonium nitrate content of the NaNO 3 Ca (NO 3) 2 melt is less than 0.5% by weight, preferably less than 0.3% by weight. It is also provided according to a further embodiment of the invention that the chloride content should be as low as possible in order to minimize the tendency to corrode to keep, according to an advantageous embodiment below 0.05 wt .-%.
  • Parabolic trough power plants are in the range of about 280 ° C to 400 ° C and should not be used as heat transfer media.
  • the base mixture of sodium nitrate and anhydrous calcium nitrate, in particular close to the binary eutectic, that is in the range 60-75 mol% a 03 and 25-40 mol% Ca (03) 2 have, however, it can be used to optimize the egg ⁇ properties purposeful as a heat storage medium be said binary base mixture with alkali and Erdalkalinitraten, in particular lithium nitrate, potassium nitrate, rubidium nitrate, Stron ⁇ tiumnitrat and barium nitrate, to ternarise, quaternarize or quinitize.
  • tempera ⁇ ren below 400 ° C such as maximum supply Injection ⁇ temperatures in the range below 350 ° C, in particular below ⁇ semi-300 ° C,
  • Trustzugtesten at below 200 ° C are used, for example, Magnesium, aluminum and / or zinc nitrate, which form decomposition-free dehydratable nitrates in these temperature ranges, added as additives of the binary Nitratsalzgemisches of calcium and Natriumnit ⁇ rat.
  • Figures 4 to 7 show calculated liquidus temperature projections of ternary mixtures of the base mixture
  • the nitrates of lithium nitrate, potassium nitrate, cesium nitrate and strontium nitrate are according to a preferred execution of the invention form to the Ca (N03) 2 _ NaN03 salt mixture for the preparation of the heat storage medium in an amount Be ⁇ ranging from 0.001 to 40 mol%, in particular in a Amount of 0.01 to 20 mol%, and particularly preferably in an amount of 0.1 to 10 mol% added.
  • Advantageous embodiments of the invention with respect to the respective concrete Salzmi ⁇ research on the basis of the binary salt mixture of calcium, sodium nitrate, will become apparent to the skilled person in an obvious manner from the results shown here diagrams.
  • Ca (N03) 2 _ NaNÜ3 has a Salzmi ⁇ research from 30 to 95 mol% NaN03, in particular 60Mol% to 95Mol% and 5 to 70 mol% Ca (N0 3) 2, in particular from 5 to 45 mol %, proven.
  • the eutectic mixture is Ca (N03) 2 _ Na NO 3 with 69 mol% sodium nitrate and 31 mol% 3 NaNÜ kristallwas ⁇ serbuildm calcium nitrate Ca (N03) 2 with up to 10 mol% of
  • Nitrate additive and this mixture for the responsible here expert solar thermal power plants obvious salt mixtures.
  • nitrates provided according to an exemplary embodiment of the invention, as stated above, arise at least ternary, so three-component mixtures Salzmi ⁇ which preferably 60-75 mol% (43.5-61 wt .-%) a 03 so as ⁇ 25-40 mol% (39-56.5 wt .-%) Ca (N0 3) 2 and 0.001-10 mol%, so for example 6-22 wt .-%, of at least one additive from the group lithium nitrate, potassium nitrate, rubidium nitrate, cesium nitrate, magnesium nitrate, strontium nitrate and / or
  • Barium nitrate include. Characterized 280-400 ° C are thermiekraftwerksanlagen liquid, sensible unloading, loadable ther ⁇ mix energy storage salts for thermo oil-based solar preferably in the temperature range, in particular of the type parabolic trough available.
  • the solidification behavior of the salt mixtures for the first time described here as heat accumulators for solar thermal power ⁇ works on thermal oil-based, firstly because of the freezing point is low and calcium nitrate itself known to act as a cooler and retarded solidification falls below the actual solidification temperature of the mixture for a time.
  • the thermal stability of the anhydrous, here for the first time as a heat storage medium for solar thermal power plants was measured by thermo gravimetric analysis at very low heating rates (1 K / min) of 290 ° C to 400 detected without loss of mass, and thus permits the use of the salt mixture over years or decades almost without refill and / or purification.
  • the invention is first a heat storage medium for use in solar thermal power plants, operated with thermal oil as a heat transfer medium proposed which is ⁇ adjustable nitrate-based, in particular on the basis of egg ⁇ nes binary salt mixture of sodium and calcium nitrate forth and either without potassium nitrate or manages with ge ⁇ ringer amount of potassium nitrate. This is particularly important because in those countries where solar thermal power plants can become an important source of energy, potassium nitrate is needed primarily for agriculture as fertilizer for the production of food.

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  • Chemical Kinetics & Catalysis (AREA)
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Abstract

La présente invention concerne un milieu accumulateur de chaleur à base de nitrate, en particulier un mélange binaire de sels de nitrate. L'invention concerne d'abord un milieu accumulateur de chaleur qui est utilisé dans des centrales solaires thermiques fonctionnant avec des huiles thermiques en tant que milieu de transfert de chaleur qui peut être préparé à base de nitrate, en particulier à base d'un mélange binaire de sels de sodium et de nitrate de calcium et qui est soit totalement dépourvu de nitrate de potassium, soit contient une quantité réduite de nitrate de potassium. C'est notamment important puisque dans les régions où les centrales solaires thermiques peuvent représenter une source d'énergie importante, le nitrate de potassium est utilisé surtout en agriculture sous forme d'engrais pour la production de denrées alimentaires.
PCT/EP2017/058509 2016-04-12 2017-04-10 Milieu accumulateur de chaleur à base de nitrate et centrale solaire thermique WO2017178412A1 (fr)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
DE102016206082.1A DE102016206082A1 (de) 2016-04-12 2016-04-12 Wärmespeichermedium auf Nitratbasis und solarthermische Kraftwerksanlage
DE102016206082.1 2016-04-12

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Families Citing this family (3)

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Publication number Priority date Publication date Assignee Title
ES2579763B1 (es) * 2015-01-15 2017-05-29 Quimica Del Estroncio, S.A.U. Nuevas formulaciones de sales de nitratos para su empleo como fluido de almacenamiento y transferencia de calor
GB201816380D0 (en) * 2018-10-08 2018-11-28 Sunamp Ltd Group II metal nitrate based compositions for use as phase change materials
DE102019205161A1 (de) * 2019-04-10 2020-10-15 Siemens Aktiengesellschaft Phasenwechselspeichermaterial für einen Phasenwechselspeicher eines Kraftwerks, Phasenwechselspeicher, Kraftwerk sowie Verfahren

Citations (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP0049761A1 (fr) 1980-10-15 1982-04-21 Goerig & Co. GmbH & Co. KG Usage d'une mélange de sels ternaires comme composition de transfert de chaleur et/ou comme accumulateur de chaleur
US7588694B1 (en) 2008-02-14 2009-09-15 Sandia Corporation Low-melting point inorganic nitrate salt heat transfer fluid
US20120056125A1 (en) 2010-04-19 2012-03-08 Halotechnics, Inc Inorganic salt heat transfer fluid
WO2014044652A1 (fr) 2012-09-18 2014-03-27 Yara International Asa Utilisation d'un sel nitrate de calcium et de potassium dans la fabrication d'un fluide caloporteur
DE202013005845U1 (de) * 2013-07-01 2014-08-04 Deutsches Zentrum für Luft- und Raumfahrt e.V. Latentwärmespeichermaterial
WO2015043810A1 (fr) 2013-09-27 2015-04-02 Siemens Aktiengesellschaft Mélange de sels en tant que substance d'accumulation pour une centrale héliothermique fonctionnant à l'huile

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* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP0049761A1 (fr) 1980-10-15 1982-04-21 Goerig & Co. GmbH & Co. KG Usage d'une mélange de sels ternaires comme composition de transfert de chaleur et/ou comme accumulateur de chaleur
US7588694B1 (en) 2008-02-14 2009-09-15 Sandia Corporation Low-melting point inorganic nitrate salt heat transfer fluid
US20120056125A1 (en) 2010-04-19 2012-03-08 Halotechnics, Inc Inorganic salt heat transfer fluid
WO2014044652A1 (fr) 2012-09-18 2014-03-27 Yara International Asa Utilisation d'un sel nitrate de calcium et de potassium dans la fabrication d'un fluide caloporteur
DE202013005845U1 (de) * 2013-07-01 2014-08-04 Deutsches Zentrum für Luft- und Raumfahrt e.V. Latentwärmespeichermaterial
WO2015043810A1 (fr) 2013-09-27 2015-04-02 Siemens Aktiengesellschaft Mélange de sels en tant que substance d'accumulation pour une centrale héliothermique fonctionnant à l'huile
DE102013219498A1 (de) * 2013-09-27 2015-04-02 Siemens Aktiengesellschaft Salzgemisch als Speichermedium für ein ölbasiertes solarthermisches Kraftwerk

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ERNST JANECKE: "DAS QUATERNARE SYSTEM DER NITRATE VON Na-K-Ca-Mg UND SEINE TEILSYSTEME", ZEITSCHRIFT FÜR ELEKTROCHEMIE UND ANGEWANDTE PHYSIKALISCHE CHEMIE, vol. 48, no. 9, 1 September 1942 (1942-09-01), pages 453 - 512, XP055380992 *
JUDITH C GOMEZ ET AL: "Ca(NO3)2-NaNO3-KNO3 Molten Salt Mixtures for Direct Thermal Energy Storage Systems in Parabolic Trough Plants", JOURNAL OF SOLAR ENERGY ENGINEER, ASME INTERNATIONAL, US, vol. 135, no. 2, 25 January 2013 (2013-01-25), pages 21016 - 1, XP008165879, ISSN: 0199-6231, [retrieved on 20130125], DOI: 10.1115/1.4023182 *
ZHAO C Y ET AL: "Investigation of the Ca(NO3)2-NaNO3mixture for latent heat sto", SOLAR ENERGY MATERIALS AND SOLAR CELLS, vol. 140, 14 May 2015 (2015-05-14), pages 281 - 288, XP029210794, ISSN: 0927-0248, DOI: 10.1016/J.SOLMAT.2015.04.005 *

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