Liquefied gas electrolyte container device and dispensing method

Abstract

A method and structure for dispensing liquefied gas electrolyte from a liquefied gas electrolyte (LGE) container is disclosed. The LGE includes a liquefied gas solvent having a vapor pressure above 100 kPa at a temperature of 293.15 K and a salt. The LGE container includes a temperature sensor that detects the temperature of the liquefied gas electrolyte within the LGE container. The temperature of the LGE container is controlled using a temperature control element and a processor connected to the temperature sensor and the temperature control element. The LGE is transferred from the container to a secondary container through a valve. The method includes the following steps: (a) opening the valve to allow the LGE to flow from the LGE container into the secondary container; (b) obtaining a reading from the temperature sensor; and (c) heating the LGE container to maintain the temperature of the LGE container at a predetermined temperature or temperature range based on the temperature reading.

Description

[Technical Field]

[0001] Cross-reference to related applications This application claims priority to U.S. Provisional Application No. 63 / 391,220, filed July 21, 2022, entitled "LIQUEFIED GAS ELECTROLYTE CONTAINER APPARATUS AND METHOD FOR DISPENSING," which is incorporated by reference in its entirety.

[0002] This application is incorporated herein by reference in its entirety for all applications and patents, each of which is incorporated herein by reference: U.S. Patent No. 10,608,284, issued March 31, 20; U.S. Patent No. 10,988,143, issued May 4, 21; U.S. Patent No. 10,784,532, issued September 22, 20; PCT / US19 / 032413, filed May 15, 19; PCT / US20 / 26086, filed April 1, 20; U.S. Patent No. 11,088,396, issued August 10, 21 ;U.S. Patent No. 11,049,668, issued June 29, 2021; U.S. Patent No. 10,873,070, issued December 22, 2020; U.S. Application No. 63 / 195592, filed June 1, 2021; U.S. Application No. 16 / 666155, filed October 28, 2019; U.S. Application No. 17 / 326093, filed May 20, 2021; U.S. Application No. 63 / 306396, filed February 3, 2022; and U.S. Application No. 63 / 328480, filed April 7, 2022.

[0003] STATEMENT REGARDING FEDERALLY SPONSORED RESEARCH OR DEVELOPMENT none.

[0004] Embodiments of the present invention relate to an apparatus and method for the bulk delivery of liquefied gas solvents for making electrochemical energy storage devices. [Background technology]

[0005] The preparation of liquefied gas electrolytes (LGE) requires an accurate and efficient flow control mechanism. Temperature monitoring of the LGE container can enable efficient and accurate flow control during the preparation process. Flow control is commonly achieved using electronic mass flow controllers (MFCs). However, MFCs are typically not configured within the flow system to utilize temperature feedback from the source or receiving container.

[0006] If the LGE container temperature increases during LGE preparation, backpressure exceeding the MFC's operating window can negatively affect the flow rate or accuracy of the MFC. These effects can affect the performance of electrochemical devices fabricated using liquefied gas solvents.

[0007] Prior art has demonstrated that the performance of electrochemical devices is significantly affected by the mass and composition of the electrolyte. Deviations in the mass of the electrolyte can negatively affect the performance of the electrochemical device. For example, too little electrolyte will not allow for full utilization of the entire electrode capacity within the device. Furthermore, too much electrolyte will reduce the energy density of the electrochemical device through increased mass. Similarly, deviations in the composition of the electrolyte can negatively affect the performance of the electrochemical device. For example, an inaccurate ratio of one electrolyte component to another will not allow for full utilization of all electrode capacity within the device.

[0008] Therefore, it is necessary to fabricate electrochemical devices with precise electrolyte mass and composition to match a specific energy density. A need exists for an apparatus and method that utilizes temperature feedback to improve accuracy and efficiency during the LGE preparation process. Summary of the Invention

[0009] A method and structure are disclosed for filling a container with a liquefied gas solvent having a vapor pressure above atmospheric pressure of 100 kPa at a room temperature of 293.15 K. The method includes providing a filling arrangement having a mass flow controller (MFC), a liquefied gas solvent source connected to the MFC, and a container connected to the MFC, the container containing salt and a temperature sensor for detecting the temperature of the liquefied gas electrolyte when present in the container. A processor connected to the MFC and the temperature sensor receives a temperature reading from the temperature sensor and is used to operate a flow rate on the MFC. The flow rate is adjusted to maintain the temperature reading from the temperature sensor below a predetermined maximum temperature. The liquefied gas solvent is mixed with the salt in the container to form the liquefied gas electrolyte.

[0010] The method may include pre-dosing the container with non-salt ingredients.

[0011] The method may include setting a predetermined maximum temperature for the temperature sensor and adjusting the flow rate to the MFC to maintain a temperature reading below the predetermined maximum temperature.

[0012] A method and structure are disclosed for dispensing liquefied gas electrolyte from an LGE container. The LGE includes a liquefied gas solvent having a vapor pressure above 100 kPa at a temperature of 293.15 K and a salt. The container includes a temperature sensor for detecting the temperature of the liquefied gas electrolyte in the liquefied gas electrolyte container. The container temperature is controlled using a temperature control element and a processor connected to the temperature sensor and the temperature control element. The LGE is transferred from the container to a secondary container through a valve. The method includes the following steps: (a) opening the valve to allow the liquefied gas electrolyte to flow from the liquefied gas electrolyte container into the secondary container; (b) obtaining a reading from the temperature sensor; and (c) heating the liquefied gas electrolyte container to maintain the temperature of the liquefied gas electrolyte container at a predetermined temperature or temperature range based on the temperature reading.

[0013] The method may include the secondary container being an electrochemical device. The arrangement may include an electrochemical device such as a battery or a capacitor.

[0014] The method may include a predetermined temperature range for the container of 303.15 K ± 2 K. Similarly, the method may include a predetermined temperature range for the secondary container of 293.15 K ± 5 K.

[0015] Additional aspects, alternatives, and modifications, as will be appreciated by those skilled in the art, are also disclosed herein and are specifically contemplated to be included as part of the present invention. The present invention is set forth solely in the claims, as permitted by the Patent Office in this or any related application, and the following summary description of certain specific embodiments does not in any way limit, define, or otherwise establish the scope of legal protection. [Brief explanation of the drawings]

[0016] [Figure 1] FIG. 1 is a block diagram illustrating an embodiment of an apparatus for liquefied gas solvent delivery to a container. [Figure 2] FIG. 1 is a block diagram illustrating an embodiment of an apparatus for liquefied gas solvent delivery to a container, including additional pressure and flow control components. [Figure 3] FIG. 1 is a block diagram illustrating an embodiment of an apparatus for liquefied gas solvent delivery to a container in which the liquefied gas source and / or gas delivery line are temperature controlled. [Figure 4] FIG. 1 is a block diagram illustrating an embodiment of an apparatus for liquefied gas solvent delivery to a container in which the gas line between the valve and the container is temperature controlled. [Figure 5] FIG. 1 is a block diagram illustrating an embodiment of an apparatus for liquefied gas solvent delivery to a container in which the gas line between the source cylinder and the mass flow controller is temperature controlled. [Figure 6] FIG. 1 is a block diagram illustrating an embodiment of an apparatus for liquefied gas solvent delivery to a container in which a heat exchanger is used to cool the gas entering the container. [Figure 7] FIG. 1 is a block diagram illustrating an embodiment of an apparatus for liquefied gas solvent delivery to a container in which two or more liquefied gas solvent sources are connected in parallel to the container. [Figure 8] FIG. 1 is a block diagram illustrating an embodiment of an apparatus for dispensing liquefied gas electrolyte into a secondary container. [Figure 9] FIG. 1 is a block diagram illustrating an embodiment of an apparatus for dispensing a liquefied gas electrolyte into a secondary container including an input volume. [Figure 10] FIG. 1 is a block diagram illustrating an embodiment of an apparatus for dispensing liquefied gas electrolyte into a secondary container, where the secondary container is cooled using a heat sink. [Figure 11] FIG. 1 is a block diagram illustrating an embodiment of an apparatus for dispensing liquefied gas electrolyte into a secondary container, where the liquefied gas flow is controlled using a liquid mass flow controller. [Figure 12] FIG. 1 is a block diagram illustrating an embodiment of an apparatus for dispensing liquefied gas electrolyte into a secondary container, in which the liquefied gas electrolyte is dispensed through a dip tube. [Figure 13] FIG. 1 is a block diagram illustrating an embodiment of an apparatus for dispensing liquefied gas electrolyte into a secondary container, where the temperature-controlled reservoir is filled before the secondary container. [Figure 14] FIG. 11 is a block diagram illustrating an embodiment of an apparatus for dispensing liquefied gas electrolyte into a secondary container similar to FIG. 10, in which the valves are mass flow controllers connected to a processor. DETAILED DESCRIPTION OF THE INVENTION

[0017] Reference will be made herein to certain specific embodiments of the present invention, including any best mode contemplated by the inventors for carrying out the invention. Examples of these specific embodiments are illustrated in the accompanying drawings. While the invention will be described in conjunction with these specific embodiments, it will be understood that they are not intended to limit the invention to the embodiments described or illustrated. On the contrary, they are intended to cover alternatives, modifications, and equivalents which may be included within the spirit and scope of the invention as defined by the appended claims.

[0018] In the following description, numerous specific details are set forth to provide a thorough understanding of the present invention. Certain exemplary embodiments of the present invention may be practiced without some or all of these specific details. In other instances, process operations well known to those skilled in the art have not been described in detail so as not to unnecessarily obscure the present invention. Various techniques and mechanisms of the present invention will sometimes be described in the singular for clarity. However, it should be noted that some embodiments include multiple iterations of a technique or multiple mechanisms, unless otherwise stated. Similarly, the various steps of the methods shown and described herein may not necessarily be performed in the order shown, or at all, in a particular embodiment. Thus, some implementations of the methods discussed herein may include more or fewer steps than those shown or described. Furthermore, the techniques and mechanisms of the present invention will sometimes describe connections, relationships, or communications between two or more entities. It should be noted that a connection or relationship between entities does not necessarily imply a direct, uninterrupted connection, as various other entities or processes may exist or occur between any two entities. As a result, a designated connection does not necessarily imply a direct, unobstructed connection unless otherwise stated.

[0019] The proposed novel method for preparing LGE uses a container equipped with a temperature sensor to detect the temperature of the liquefied gas electrolyte within the container. The proposed setup for preparing LGE includes a liquefied gas solvent supply, a flow controller, a container containing salt, a temperature sensor to detect the temperature of the LGE, and a processor connected to both the temperature sensor and the flow controller. During LGE preparation, the flow rate of the liquefied gas solvent is controlled using a mass flow controller, and the flow rate is set by a processor connected to the flow controller. The processor is also connected to a temperature sensor that monitors the temperature of the LGE during the liquefied gas solvent filling step.

[0020] In some embodiments, the container may be initially cooled to a temperature below that of the liquefied gas solvent source. As the liquefied gas solvent fills the container, significant heat may be released into the container and increase the temperature of the LGE. If the LGE temperature increases, the vapor pressure within the container may exceed the backpressure limit of the mass flow controller and impair the accuracy of the MFC.

[0021] The processor may reduce the MFC flow rate to mitigate the rate of heating due to the liquefied gas solvent charge. The processor may use temperature feedback from a temperature sensor and adjust the MFC flow rate to ensure that backpressure on the MFC is not exceeded. The processor may optimize the MFC flow rate during the liquefied gas solvent charge to minimize the time required to prepare the LGE. [Example]

[0022] Four non-limiting examples illustrating various embodiments of the present invention are set forth below. One such embodiment is shown in Figure 1. In arrangement 100-1, liquefied gas is supplied by liquefied gas solvent source 1 (shown as a cylinder throughout this disclosure). The liquefied gas solvent may be any of the following: fluoromethane, difluoromethane, trifluoromethane, fluoroethane, tetrafluoroethane, pentafluoroethane, 1,1-difluoroethane, 1,2-difluoroethane, 1,1,1-trifluoroethane, 1,1,2-trifluoroethane, 1,1,1,2-tetrafluoroethane, 1,1,2,2-tetrafluoroethane, pentafluoroethane, chloromethane, chloroethane, thionyl fluoride, thionyl chloride, phosphoryl fluoride, phosphoryl chloride, sulfuryl fluoride, sulfuryl chloride, 1-fluoropropane, 2-fluoropropane, 1,1-difluoroethane ... The gas delivery device may include one or more of the following: fluoropropane, 1,2-difluoropropane, 2,2-fluoropropane, 1,1,1-trifluoropropane, 1,1,2-trifluoropropane, 1,2,2-trifluoropropane, fluoroethylene, cis-1,2-fluoroethylene, 1,1-fluoroethylene, 1-fluoropropylene, 2-propylene, chlorine, chloromethane, bromine, iodine, ammonia, molecular oxygen, molecular nitrogen, carbon monoxide, carbon dioxide, sulfur dioxide, dimethyl ether, nitrous oxide, nitrogen dioxide, nitric oxide, carbon disulfide, hydrogen fluoride, hydrogen chloride, combinations thereof, and isomers thereof. The components of the gas delivery device are connected by metal, plastic, or ceramic tubing. In some embodiments, the components of the gas delivery device are connected by tubing or piping of various sizes. In some embodiments, the tubing may have an outer diameter of 1 / 16 inch, 1 / 8 inch, 1 / 4 inch, 1 / 2 inch, 1 inch, or 2 inches. In some embodiments, the tube size may be 1 / 8, 1 / 4, 1 / 2, 1, 2, or larger nominal tube size.

[0023] The liquefied gas solvent vapor passes through a mass flow controller (MFC) 3. The MFC 3 may include, but is not limited to, a thermal-type flow controller or a Coriolis-type flow controller. The MFC 3 has an upstream pressure P1 and a downstream pressure P2. A sufficient pressure differential between P1 and P2 is required for proper MFC 3 operation as discussed herein. The upstream pressure P1 is the operating pressure of the MFC 3. The downstream pressure P2 is approximately 15 pounds per square inch lower than P1. In a preferred embodiment, the pressure differential P1-P2 can be greater than 0.1 psi, preferably greater than 1 psi, and more preferably greater than 10 psi. The liquefied gas solvent vapor is transported through the MFC 3 into a container 4, where it mixes with a salt 5 to form a liquefied gas electrolyte 6. The container 4 may be any suitable metal, ceramic, or plastic device capable of holding a liquefied gas electrolyte having a vapor pressure above atmospheric pressure of 100 kPa at a temperature of 293.15 K. The container 4 may be any suitable size for containing the LGE. In some embodiments, container 4 may be larger than 1 cubic centimeter, larger than 10 cubic centimeters, larger than 100 cubic centimeters, larger than 1000 cubic centimeters, larger than 10,000 cubic centimeters, larger than 100,000 cubic centimeters, or larger than 1,000,000 cubic centimeters. Salt 5 is lithium bis(trifluoromethanesulfonyl)imide (LiTFSI), lithium hexafluorophosphate (LiPF6), lithium perchlorate (LiClO4), lithium hexafluoroarsenate (LiAsF6), lithium tetrachloroaluminate (LiAlCl4), lithium tetragalliumaluminate, lithium bis(oxalato)borate (LiBOB), lithium hexafluorostannate, lithium difluoro(oxalato)borate (LiDFOB), lithium bis(fluorosulfonyl)imide (LiFSI), lithium aluminum fluoride (LiAlF3), lithium nitrate (LiNO3), lithium chloroaluminate, lithium tetrafluoroborate (LiBF4), lithium tetrachloroaluminate, lithium difluorophosphate,The salts may include one or more of lithium tetrafluoro(oxalato)phosphate, lithium difluorobis(oxalato)phosphate, lithium borate, lithium oxalate, lithium thiocyanate, lithium tetrachlorogallate, lithium chloride, lithium bromide, lithium iodide, lithium carbonate, lithium fluoride, lithium oxide, lithium hydroxide, lithium nitride, lithium superoxide, lithium azide, lithium deltaate, dilithium squarate, lithium croconic acid dihydrate, dilithium rhodizonate, lithium oxalate, dilithium ketomalonate, lithium diketosuccinate, or any applicable salt in which the positively charged lithium cation is replaced with sodium or magnesium, or any combination thereof. Further useful salts include those with positively charged cations, such as tetramethylammonium, tetraethylammonium, tetrapropylammonium, tetrabutylammonium, triethylmethylammonium, spiro-(1,1')-bipyrrolidinium, 1,1-dimethylpyrrolidinium and 1,1-diethylpyrrolidinium, N,N-diethyl-N-methyl-N(2methoxyethyl)ammonium, N,N-diethyl-N-methyl-N-propylammonium, N,N-dimethyl-N-ethyl-N-(3-methoxypropyl)ammonium, N,N-dimethyl-N-ethyl-N-benzylammonium, N,N-dimethyl-N-ethyl-N-phenylethylammonium, N-ethyl-N,N-dimethyl-N-(2-methoxyethyl ...phenylethylammonium, N-ethyl-N,N-dimethyl-N-(2-methoxyethyl)ammonium, N,N-dimethyl-N-ethyl-N-propylammonium, N,N-dimethyl-N-ethyl-N-phenylethylammonium, N-ethyl-N,N-dimethyl-N-(2-methoxyethyl)ammonium, N,N-dimethyl-N-ethyl-N-benzylammonium, N,N-dimethyl-N-ethyl-N-phenylethylammonium, N-ethyl-N,N-dimethyl-N-(2-methoxyethyl)ammonium, N, Ammonium, N-tributyl-N-methylammonium, N-trimethyl-N-hexylammonium, N-trimethyl-N-butylammonium, N-trimethyl-N-propylammonium, 1,3-dimethylimidazolium, 1-(4-sulfobutyl)-3-methylimidazolium, 1-allyl-3H-imidazolium, 1-butyl-3-methylimidazolium, 1-ethyl-3-methylimidazolium, 1-hexyl-3-methylimidazolium, 1-octyl-3-methylimidazolium, 3-methyl-1-propylimidazolium, H-3-methylimidazolium, trihexyl(tetradecyl)phosphonium, N-butyl-N-methylpiperidinium, N-propyl-N-methylpiperidinium, 1-butyl-1-methylpyrrolidinium,Included are 1-methyl-1-(2-methoxyethyl)pyrrolidinium, 1-methyl-1-(3-methoxypropyl)pyrrolidinium, 1-methyl-1-octylpyrrolidinium, 1-methyl-1-pentylpyrrolidinium, or N-methylpyrrolidinium paired with negatively charged anions such as acetate, bis(fluorosulfonyl)imide, bis(oxalato)borate, bis(trifluoromethanesulfonyl)imide, bromide, chloride, dicyanamide, diethyl phosphate, hexafluorophosphate, hydrogen sulfide, iodide, methanesulfonate, methyl-phosphonate, tetrachloroaluminate, tetrafluoroborate, and trifluoromethanesulfonate, combinations thereof, and isomers thereof.

[0024] The temperature of the LGE is detected using a temperature sensor 7. The temperature sensor 7 may be enclosed in any suitable feedthrough housing, such as a dip tube. The temperature sensor 7 may be any sensor capable of a wide dynamic range, such as a thermocouple. In some embodiments, the temperature sensor 7 may be a resistive sensor, a semiconductor sensor, or a thermistor. The temperature sensor 7 is connected to a processor 8. The processor 8 provides an initial flow rate setting to the MFC 3 and continuously monitors the flow rate during the liquefied gas solvent filling process. The processor 8 also monitors the temperature of the LGE via the temperature sensor 7 and adjusts the flow rate of the MFC 3 if the temperature of the LGE 8 rises above a predetermined maximum temperature. Those skilled in the art will appreciate that the predetermined maximum temperature will correlate to a particular vapor pressure of the LGE 8. The vapor pressure of the LGE 8 may be the same as the downstream pressure P2. Thus, the predetermined maximum temperature of the LGE 8 may correlate to the predetermined pressure differential P1-P2 discussed above. The container 4 may be in contact with a heat sink 9 connected and regulated by the processor 8. Those skilled in the art will appreciate that maintaining the container 4 at a temperature lower than that of the source 1 will result in condensation of the liquefied gas solvent within the container 4. The heat sink 9 may be connected to a refrigeration unit to cool the container 4 below room temperature. The container 4 may be cooled to less than 50 degrees Celsius, preferably less than 25 degrees Celsius, more preferably less than 0 degrees Celsius, and even more preferably less than -20 degrees Celsius. The heat sink 9 may include a thermally conductive material in contact with the container 4. The heat sink 9 may be, but is not limited to, a solid container, a bed of metal shot, a liquid bath, an ice bath, a dry ice bath, or a gas stream. The refrigeration unit may be, but is not limited to, a circulating chiller, a Peltier cooler, or a refrigerated gas. The container 4 may be pre-cooled below the temperature of the liquefied gas solvent source 1 to allow condensation of the liquefied gas within the container 4. In a preferred embodiment of the present invention, the container 4 is maintained at a temperature lower than that of the liquefied gas solvent source 1.

[0025] Another embodiment of the present invention is shown in FIG. 2. In arrangement 100-2, liquefied gas solvent is supplied from liquefied gas solvent source 1. The liquefied gas solvent vapor passes through upstream isolation valve 10, mass flow controller 3, downstream isolation valve 11, and container isolation valve 12. The section of tubing between downstream isolation valve 11 and container isolation valve 12 is defined as waste volume 13, with pressure transducer 14 connected to processor 8 to monitor the pressure. Those skilled in the art will appreciate that the pressure monitor can be used to calculate the density of the vapor in waste volume 13. The mass of vapor in waste volume 13 can be calculated and utilized when delivering liquefied gas solvent to container 4. When container 4 is filled, container isolation valve 12 closes, and waste volume 13 is vented through vent valve 15 and pump 16. Utilizing waste volume 13 can improve the accuracy of liquefied gas solvent delivery to container 4.

[0026] Another embodiment of the present invention is shown in FIG. 3. In arrangement 100-3, the temperatures of liquefied gas solvent source 1, isolation valve 10, tubing 2, and MFC 3 are controlled by temperature control element 17, which may be connected to processor 8 and may further include a temperature sensor. In one embodiment, the temperature deviation between liquefied gas solvent source 1 and the gas delivery line is less than 10 degrees Celsius, preferably less than 5 degrees Celsius, more preferably less than 1 degree Celsius, and even more preferably less than 0.1 degrees Celsius. The temperature may be controlled to be higher than room temperature. The temperature may be controlled between -30 degrees Celsius and 100 degrees Celsius, preferably between 0 degrees Celsius and 50 degrees Celsius, and more preferably between 20 degrees Celsius and 30 degrees Celsius. The processor may control temperature control element 17 to maintain the temperature variance within ±2.0 degrees Celsius, more preferably within 0.5 degrees Celsius, during the filling process. As the liquefied gas solvent source 1 delivers gas during the filling process, it cools, and fluctuations in the temperature of the gas can affect the accuracy of the MFC 3. Using a temperature control element 17 to maintain a nearly constant temperature during the filling process can minimize inaccuracies in the MFC 3. Those skilled in the art will appreciate that the temperature of the liquefied gas solvent source 1 can be adjusted to provide sufficient vapor pressure and flow rate. The temperature control element 17 can be, but is not limited to, a heating blanket, heating tape, heating rope, or a thermally regulated enclosure.

[0027] Another embodiment of the present invention is shown in FIG. 4. In configuration 100-4, the downstream side of valve 11 (which is also the waste volume) is temperature controlled using temperature control element 18 (which may be connected to processor 8 and may further include a temperature sensor). The temperature may be controlled between -30 and 100 degrees Celsius, preferably between 0 and 50 degrees Celsius, and more preferably between 20 and 30 degrees Celsius. Temperature control element 18 may be, but is not limited to, a heating blanket, heating tape, heating rope, or a thermally regulated enclosure. Temperature control element 18 (through processor 8) may maintain the temperature variance within the waste volume to within ±2.0 degrees Celsius, more preferably within 0.5 degrees Celsius. Temperature control element 18 may be set to a specific preset temperature, which can be used in conjunction with the pressure reading from pressure sensor 14 to determine the gas mass within the waste volume. This method may further improve the accuracy of liquefied gas solvent delivery to container 4.

[0028] Another embodiment of the present invention is shown in Figure 5. In arrangement 100-5, the temperature of the isolation valve 10 and the tubing 2 between the liquefied gas solvent source 1 and the MFC 3 is controlled by a temperature control element 19 (which may be connected to the processor 8 and may further include a temperature sensor). One skilled in the art will appreciate that the temperature between the gas outlet of the liquefied gas solvent source 1 and the MFC 3 may be adjusted to be higher than the temperature of the liquefied gas solvent source 1 to prevent condensation of the liquefied gas. The temperature control element 19 may be, but is not limited to, a heating blanket, heating tape, heating rope, or a thermally regulated enclosure.

[0029] Another embodiment of the present invention is shown in FIG. 6. In configuration 100-6, heat exchanger 20 is upstream of container 4. Heat exchanger 20 cools the inlet gas to container 4. The heat exchanger may cool the gas to below 50 degrees Celsius, below 20 degrees Celsius, below 0 degrees Celsius, below -20 degrees Celsius, below -40 degrees Celsius, or below -60 degrees Celsius. The gas condenses above container 4 and flows into container 4, where it mixes with salt 5 to form LGE 6. One skilled in the art will appreciate that the use of heat exchanger 20 may improve the collection of condensed liquefied gas solvent within container 4.

[0030] Another embodiment of the present invention is shown in FIG. 7. Arrangement 100-7 includes two or more parallel gas delivery lines supplying liquefied gas solvent to container 4. Liquefied gas source 1 is connected to gas delivery line 21, and liquefied gas source 22.1 is connected to gas delivery line 23.1, with both gas delivery lines 21 and 23.1 delivering gas to container 4. This embodiment may be extended to any number of liquefied gas sources and gas delivery lines (shown as liquefied gas sources 22.x and gas delivery lines 23.x, all of which are connected to and deliver gas to container 4). The gas delivery lines may include components of any of the above embodiments to deliver precise masses of liquefied gas solvent at desired flow rates. The various gases may be delivered to container 4 simultaneously or sequentially.

[0031] Another embodiment of the present invention is shown in FIG. 8. In arrangement 100-8, container 4, container isolation valve 12, liquefied gas electrolyte 6, and temperature sensor 7 are used to dispense LGE 6 into secondary container 24. Secondary container 24 may be any suitable metal, ceramic, or plastic device capable of holding a liquefied gas electrolyte having a vapor pressure above atmospheric pressure of 100 kPa at a temperature of 293.15 K. Secondary container 24 may be an electrochemical device such as a battery or capacitor. When container isolation valve 12 opens, LGE 6 flows from container 4 to secondary container 24. Processor 8 monitors temperature sensor 7 and controls temperature control element 25. Those skilled in the art will appreciate that during the filling process, the liquid volume in container 4 decreases during the filling process, resulting in LGE 6 vaporizing into the headspace of container 4. This vaporization process may remove heat from the surroundings of LGE 6, lowering the temperature of LGE 6. If the temperature of LGE 6 decreases, the LGE density may change and reduce the accuracy of the mass of LGE transferred to secondary container 19. The vapor pressure of the LGE headspace may also decrease if the LGE temperature decreases. The system may use the pressure difference between container 4 and secondary container 24 to facilitate LGE transfer. If the vapor pressure in the headspace decreases, the efficiency of LGE transfer may decrease. Therefore, a temperature control element 25 is used to provide heat to container 4 to maintain a constant temperature. The temperature may be controlled between -30°C and 100°C, preferably between 20°C and 50°C, and more preferably between 30°C and 40°C. The temperature control element 25 may be, but is not limited to, a heating blanket, heating tape, heating rope, or a thermally regulated enclosure. The temperature control element 25 may maintain the temperature variance within the container to within ±2.0°C, more preferably within 0.5°C.

[0032] Another embodiment of the present invention is shown in FIG. 9. In configuration 100-9, container 4 dispenses LGE 6 into an intermediate container called input volume 26. LGE 6 is transferred from container 4 to input volume 26 when container isolation valve 12 opens. During this step, isolation valve 27 closes, and LGE 6 completely fills input volume 26. Isolation valve 12 is then closed. In a subsequent step, input volume isolation valve 27 opens, and input volume 26 dispenses LGE 6 into secondary container 24. Input volume 26 may be any suitable metal, ceramic, or plastic device capable of holding a liquefied gas electrolyte having a vapor pressure above atmospheric pressure of 100 kPa at a temperature of 293.15 K. Input volume 26 may be constructed to a predetermined volume to dispense a precise mass of LGE 6 into secondary container 24. Temperature sensor 28 is connected to input volume 26 and processor 8 to monitor the temperature. Those skilled in the art will appreciate that both the container 4 and the input volume 26 should be maintained at the same temperature to have a uniform density within the LGE 6. A known uniform density of the LGE 6 may be required for accurate mass delivery of the LGE 6 into the secondary container 24. Therefore, a temperature control element 25 is used to maintain a constant, uniform temperature in the container 4 and the input volume 26. The temperature may be controlled between -30°C and 100°C, preferably between 20°C and 50°C, and more preferably between 30°C and 40°C. The temperature control element 25 may be, but is not limited to, a heating blanket, heating tape, heating rope, or a thermally regulated enclosure. The temperature control element 25 may maintain the temperature variance within the container to within ±2.0°C, and more preferably within 0.5°C.

[0033] The flow of LGE 6 from input volume 26 into secondary container 24 may be facilitated by a pressure differential. Secondary container 24 may initially be evacuated to a pressure below 14.7 psi at a room temperature of 293.15 K. When input volume isolation valve 27 opens, LGE 6 is dispensed into secondary container 24 and will partially vaporize in the headspace of the secondary container. To achieve efficient flow of LGE 6 into secondary container 24, input volume 26 may be heated to a higher temperature than secondary container 24 so that the vapor pressure in input volume 26 is always higher than the vapor pressure in secondary container 24. In one embodiment, the temperature difference between input volume 26 and secondary container 24 is greater than 1 degree Celsius, preferably greater than 5 degrees Celsius, and more preferably greater than 10 degrees Celsius.

[0034] Another embodiment of the present invention is shown in Figure 10. In arrangement 100-10, secondary container 24 has a heat sink 29 and a temperature sensor 30, both of which are connected to processor 8. Heat sink 29 may be used to remove heat from secondary container 24 as it is filled with LGE 6 so that secondary container 24 maintains a constant temperature during the LGE 6 filling process. Heat sink 29 may be used to maintain a temperature differential between input volume 26 and secondary container 24, as discussed above. Temperature sensor 30 may be connected to processor 8 so that processor 8 can monitor the temperature differential between input volume 26 and secondary container 24 and adjust the heat sink as needed.

[0035] Another embodiment of the present invention is shown in Figure 11. In arrangement 100-11, a liquid mass flow controller 31 is used to transfer LGE 6 from container 4 into secondary container 24. Liquid mass flow controller 31 may be thermal, Coriolis, magnetic induction, or vortex type. Liquid mass flow controller 31 may be connected to processor 8 such that a predetermined mass of LGE 6 can be input to processor 8 and automatically dispensed using liquid mass flow controller 31.

[0036] Another embodiment of the present invention is shown in FIG. 12. In configuration 100-12, the device is oriented so that container isolation valve 32 is above container 4 and dip tube 33 extends from container isolation valve 32 into LGE 6. LGE 6 is transferred through dip tube 33, through container isolation valve 32, through valve 34, and into secondary container 24. LGE 6 may be transferred from container 4 to secondary container 24 by utilizing the pressure differential between the two containers. Thus, temperature control element 35 is used to maintain a constant, uniform temperature within container 4, and heat sink 36 is used to remove heat from secondary container 24. Secondary container 24 may be initially evacuated to a pressure below 15 psia at room temperature of 293.15 K. Processor 8 may receive temperature measurements from temperature sensor 7 and adjust temperature control element 20 so that the temperatures of container 4 and LGE 6 are maintained at predetermined set points. The processor may adjust heat sink 29 based on readings from temperature sensor 30. Those skilled in the art will appreciate that having container 4 at a higher temperature than secondary container 24 will result in greater pressure within container 4 than in secondary container 24 and facilitate the flow of LGE 6 from container 4 into secondary container 24. The temperature of container 4 may be controlled between -30°C and 100°C, preferably between 20°C and 50°C, and more preferably between 30°C and 40°C. Temperature control element 20 may be, but is not limited to, a heating blanket, heating tape, heating rope, or a thermally regulated enclosure. Temperature control element 20 may maintain a temperature variance within the container within ±2.0°C, more preferably within 0.5°C. Heat sink 29 in secondary container 24 may be connected to a refrigeration unit so that secondary container 24 can be cooled to room temperature or below. Secondary container 24 may be cooled to less than 50°C, preferably less than 25°C, and more preferably less than 20°C. The heat sink 29 may include a thermally conductive material in contact with the secondary container 24. The heat sink 29 may be, but is not limited to, a solid container, a bed of metal shot, a liquid bath, an ice bath, a dry ice bath, or a gas stream.The refrigeration unit may be, but is not limited to, a circulating chiller, a Peltier cooler, or refrigerated gas. In one embodiment, the temperature difference between container 4 and secondary container 24 is greater than 1 degree Celsius, preferably greater than 5 degrees Celsius, and more preferably greater than 10 degrees Celsius. In a preferred embodiment of the present invention, secondary container 24 is maintained at a temperature near room temperature, 20 degrees Celsius. The temperature of secondary container 24 may be monitored by a temperature sensor 30 connected to processor 8.

[0037] Another embodiment of the present invention is shown in FIG. 13. In configuration 100-13, the apparatus includes a reservoir 35 with a temperature sensor 36, a valve 37 isolating the reservoir from tubing connected to valve 12 and container 4, an input volume 26 with a temperature sensor 28, a valve 38 isolating reservoir 38 and input volume 26, and a temperature control element 39. Reservoir 35 is filled with LGE 6 from container 4 using a similar method as discussed above. The temperatures of reservoir 35 and input volume 26 are maintained below the temperature of container 4 to facilitate the flow of LGE 6 via a pressure differential. Temperature control element 39, temperature sensor 28, and temperature sensor 36 are connected to processor 8 to maintain a temperature below that of temperature sensor 7. In preferred embodiments, the temperature differential is greater than 1 degree Celsius, greater than 5 degrees Celsius, or greater than 10 degrees Celsius. In a preferred embodiment, the temperature of reservoir 35 and input volume 26 is controlled between -30°C and 100°C, preferably between 20°C and 50°C, and more preferably between 30°C and 40°C. Temperature control element 39 may be, but is not limited to, a heating blanket, heating tape, heating rope, or a thermally regulated enclosure. Temperature control element 39 may maintain the temperature variance within the container to within ±2.0°C, more preferably within 0.5°C. Reservoir 35 may improve the accuracy of LGE6 delivery to secondary container 24 by bringing LGE6 to thermal equilibrium prior to delivery to secondary container 24.

[0038] Another embodiment of the present invention is shown in Figure 14. Configuration 100-14 is similar to configuration 100-13 shown in Figure 13, except that valves 37, 38, 27, and 32 are mass flow controllers connected to processor 8. In this configuration 100-14, processor 8 can operate the mass flow controllers of valves 32, 37, and 38 to regulate flow between container 4 and reservoir 35. Similarly, processor 8 can operate the mass flow controllers of valves 37, 38, and 27 to regulate flow between reservoir 35 and secondary container 24. Flow regulation can be used in conjunction with temperature control elements 20 and 39 along with heat sink 29 to maintain optimal temperatures for filling reservoir 35 and / or filling secondary container 24.

[0039] Although exemplary embodiments and applications of the invention have been described herein, including those described above and shown in the included exemplary figures, the invention is not limited to these exemplary embodiments and applications or to the manner in which they operate or are described herein. In fact, many variations and modifications to the exemplary embodiments are possible, as will be apparent to those skilled in the art. The invention may include any device, structure, method, or functionality so long as the resulting device, system, or method falls within the scope of one of the claims granted by the Patent Office on this or any related patent application.

[0040] The following list of exemplary features, which pertain to the accompanying drawings, is provided for ease of reference, with like reference numerals referring to corresponding features throughout the specification and drawings. [Explanation of symbols]

[0041] 1. Supply Cylinder 2 Tube material 3 Mass Flow Controller 4. Container 5. Salt 6. Liquefied Gas Electrolytes 7 Temperature Sensor 8 processors 9 Heatsink 10 Isolation valve 11 Downstream isolation valve 12 Container isolation valve 13 Waste volume 14 Pressure Transducer 15 Exhaust valve 16 Vacuum pump 17 Temperature Control Elements 18 Temperature Control Elements 19 Temperature Control Elements 20 Heat exchanger 21 Gas delivery line 22.1 Liquefied Gas Sources22.1 22.x Parallel liquefied gas supply source 23.1 Gas Delivery Lines 23.x Parallel gas delivery lines 24 Secondary Container 25 Temperature Control Elements 26 Input volume 27 Input volume isolation valve 28 Temperature Sensor 29 Heatsink 30 Temperature Sensor 31 Liquid mass flow controller 32 Isolation valve 33 Dip tube 34 Isolation valve 35 reservoir 36 Temperature Sensor 37 Isolation valve 38 Isolation valve 39 Temperature Control Elements

Claims

1. 1. An apparatus for dispensing a liquefied gas electrolyte, comprising: a liquefied gas electrolyte container containing said liquefied gas electrolyte composed of a liquefied gas solvent and a salt having a vapor pressure above 100 kPa at a temperature of 293.15 K; a temperature sensor for detecting the temperature of the liquefied gas electrolyte in the liquefied gas electrolyte container; a temperature control element configured to heat the liquefied gas electrolyte container; a valve connected to the liquefied gas electrolyte container and to a secondary container; A processor connected to the temperature sensor and the temperature control element wherein the processor comprises the steps of: a. receiving a temperature reading from the temperature sensor; b. activating the temperature control element based on the temperature reading to maintain the temperature of the liquefied gas electrolyte container at a predetermined temperature or temperature range. An apparatus adapted to perform the steps of:

2. 2. The apparatus of claim 1, wherein the valve is a mass flow controller connected to the processor, the processor being adapted to operate the mass flow controller to regulate the flow of liquefied gas electrolyte from the liquefied gas electrolyte container into the secondary container.

3. The apparatus of claim 1 , wherein the secondary container is an electrochemical device.

4. The apparatus of claim 3 , wherein the electrochemical device is a battery or a capacitor.

5. 2. The apparatus of claim 1, wherein the predetermined temperature range is 303.15 K±2 K.

6. 1. An apparatus for dispensing a liquefied gas electrolyte, comprising: a liquefied gas electrolyte container containing said liquefied gas electrolyte composed of a liquefied gas solvent and a salt having a vapor pressure above 100 kPa at a temperature of 293.15 K; a first temperature sensor for detecting a temperature of the liquefied gas electrolyte in the liquefied gas electrolyte container; a first temperature control element configured to heat the liquefied gas electrolyte container; a first valve connected to the liquefied gas electrolyte container and to a reservoir; a second temperature sensor for detecting the temperature of the liquefied gas electrolyte in the reservoir; a second temperature control element configured to heat the reservoir; a second valve connected to the reservoir and a secondary container; a processor connected to the first and second temperature sensors and the first and second temperature control elements; wherein the processor comprises the steps of: a. receiving temperature readings from the first temperature sensor and the second temperature sensor; b. activating the first temperature control element based on a temperature reading from the first temperature sensor to maintain the temperature of the liquefied gas electrolyte container at a predetermined temperature or temperature range; c) activating the second temperature control element based on a temperature reading from the second temperature sensor to maintain the temperature of the reservoir at a second predetermined temperature or temperature range. An apparatus adapted to perform the steps of:

7. 7. The apparatus of claim 6, wherein the first valve is a mass flow controller connected to the processor, the processor being adapted to operate the mass flow controller to regulate the flow of liquefied gas electrolyte from the liquefied gas electrolyte container into the reservoir.

8. 7. The apparatus of claim 6, wherein the second valve is a mass flow controller connected to the processor, the processor being adapted to operate the mass flow controller to regulate the flow of liquefied gas electrolyte from the reservoir to the secondary container.

9. The apparatus of claim 6 , wherein the secondary container is an electrochemical device.

10. The apparatus of claim 9 , wherein the electrochemical device is a battery or a capacitor.

11. 7. The apparatus of claim 6, wherein the first predetermined temperature range is 313.15K±2K.

12. 7. The apparatus of claim 6, wherein the second predetermined temperature range is 303.15K±2K.

13. a third temperature sensor for detecting the temperature of the liquefied gas electrolyte in the secondary container; a heat sink for cooling the secondary container; further comprising the processor is connected to the third temperature sensor and the heat sink; activating the heat sink based on a temperature reading from the third temperature sensor to maintain the temperature of the secondary container at a third predetermined temperature or temperature range. The apparatus of claim 6 , adapted to:

14. 8. The apparatus of claim 7, wherein the third predetermined temperature range is 293.15K±5K.

15. 1. A method of dispensing a liquefied gas electrolyte comprising a liquefied gas solvent and a salt having a vapor pressure above 100 kPa at a temperature of 293.15 K from a liquefied gas electrolyte container through a valve to a secondary container, wherein the liquefied gas electrolyte container includes a temperature sensor for detecting a temperature of the liquefied gas electrolyte within the liquefied gas electrolyte container; a. opening the valve to allow liquefied gas electrolyte to flow from the liquefied gas electrolyte container into the secondary container; b. obtaining a reading from said temperature sensor; c. heating the liquefied gas electrolyte container based on the temperature reading to maintain the temperature of the liquefied gas electrolyte container at a predetermined temperature or temperature range. A method comprising:

16. The method of claim 15 , wherein the secondary container is an electrochemical device.

17. 17. The method of claim 16, wherein the electrochemical device is a battery or a capacitor.

18. 16. The method of claim 15, wherein the predetermined temperature range is 303.15 K±2 K.

19. the secondary container including a second temperature sensor configured to detect a temperature of the liquefied gas electrolyte within the secondary container and a heat sink configured to cool the secondary container; d. obtaining a reading from the second temperature sensor; e. cooling the secondary container to maintain the temperature of the secondary container at a second predetermined temperature or temperature range based on the temperature reading from the second sensor.

16. The method of claim 15, further comprising:

20. 20. The method of claim 19, wherein the predetermined temperature range is 293.15 K ± 5 K.

21. the secondary container includes a reservoir including a second temperature sensor for detecting a temperature of the liquefied gas electrolyte in the reservoir and a second temperature control element; d. obtaining a reading from the second temperature sensor; e. activating the second temperature control element based on the temperature reading from the second temperature sensor to maintain the temperature of the reservoir at a second predetermined temperature or temperature range.

16. The method of claim 15, further comprising:

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