JP5359485B2 - Control method of all-solid-state lithium ion secondary battery - Google Patents
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Description
本発明は、全固体リチウムイオン二次電池の制御方法に関する。 The present invention relates to a method for controlling an all solid lithium ion secondary battery.
近年、環境に配慮した自動車としてハイブリッド車両が大きく注目を集めている。ハイブリッド車両には、従来のエンジンに加えて二次電池からなる蓄電装置と蓄電装置からの電力を用いて車両の駆動力を発生するモータとを備える。このようなハイブリッド車両に搭載される蓄電装置は、車両の発進時や加速時にモータへ電力を供給する一方、車両の回生制動時にモータ（発電機として機能）が発生する電力を蓄電することが要求される。そのため、蓄電装置の充電状態を示すＳＯＣ（Ｓｔａｔｅ Ｏｆ Ｃｈａｒｇｅ）が所定の管理範囲内となるように、充放電制御が実行される。 In recent years, hybrid vehicles have attracted a great deal of attention as environmentally friendly vehicles. In addition to a conventional engine, a hybrid vehicle includes a power storage device including a secondary battery and a motor that generates driving force of the vehicle using electric power from the power storage device. A power storage device mounted on such a hybrid vehicle is required to store electric power generated by a motor (functioning as a generator) during regenerative braking of the vehicle while supplying electric power to the motor when the vehicle starts or accelerates. Is done. Therefore, charge / discharge control is performed so that SOC (State Of Charge) indicating the state of charge of the power storage device is within a predetermined management range.
上記のような蓄電装置の充放電制御に関する技術がこれまでにいくつか提案されており、例えば、下記特許文献１〜４に開示されている。
Several techniques relating to charge / discharge control of the power storage device as described above have been proposed so far, and are disclosed in, for example, the following
自動車に搭載するための二次電池としては、高性能（高効率）、高耐久性の電池の設計が要求される。その要求を満たし得る電池の一つとして、電解質を固体とした全固体リチウムイオン二次電池が検討されている。しかし、全固体リチウムイオン二次電池を自動車搭載用へと応用するにはまだ課題が残されており、その一つとして、耐久性劣化が挙げられる。全固体リチウムイオン二次電池の耐久性劣化の要因の一つとしては、該全固体リチウムイオン二次電池の使用時の使用電位幅が挙げられる。全固体リチウムイオン二次電池の運転領域において、高効率な電池電圧の領域と高耐久な電池電圧の領域とが存在するが、全固体リチウムイオン二次電池を搭載した自動車の運転時において、該全固体リチウムイオン二次電池の高効率と高耐久を両立させる制御技術がないことが問題であり、かかる問題は上記特許文献１〜４に記載された技術を用いても解決できなかった。
As a secondary battery to be mounted on an automobile, a battery design with high performance (high efficiency) and high durability is required. As one of the batteries that can satisfy the requirement, an all-solid lithium ion secondary battery using an electrolyte as a solid has been studied. However, there are still problems in applying all-solid lithium ion secondary batteries to automobiles, and one of them is durability deterioration. One of the causes of durability deterioration of the all-solid-state lithium ion secondary battery is a usable potential width when the all-solid-state lithium ion secondary battery is used. In the operation region of the all-solid-state lithium ion secondary battery, there are a high-efficiency battery voltage region and a highly-durable battery voltage region. There is a problem that there is no control technique that achieves both high efficiency and high durability of the all-solid-state lithium ion secondary battery, and such a problem cannot be solved even by using the techniques described in
そこで本発明は、使用電位幅が増大した全固体リチウムイオン二次電池の劣化を抑えられる、全固体リチウムイオン二次電池の制御方法を提供することを課題とする。 Therefore, an object of the present invention is to provide a control method for an all-solid-state lithium ion secondary battery that can suppress deterioration of the all-solid-state lithium ion secondary battery having an increased usable potential width.
上記課題を解決するために、本発明は以下の構成をとる。すなわち、
本発明は、充電状態を示す状態値の上限値及び下限値が予め設定されており、該上限値及び下限値によって決まる使用電位幅で使用される全固体リチウムイオン二次電池の制御方法であって、全固体リチウムイオン二次電池の使用条件によって下限値が新たな下限値まで低下して使用電位幅が増大した場合、下限値と新たな下限値との差分を検知するとともに、該差分だけ上限値を低下させて新たな上限値を設定する第１の制御方法と、その後、新たな下限値を該差分だけ低下させて、さらに新たな下限値を設定する第２の制御方法と、を有する、全固体リチウムイオン二次電池の制御方法である。
In order to solve the above problems, the present invention has the following configuration. That is,
The present invention is a control method for an all-solid-state lithium ion secondary battery that is used with a potential range determined by the upper limit value and the lower limit value. When the lower limit value decreases to a new lower limit value due to the use conditions of the all-solid-state lithium ion secondary battery and the use potential width increases, the difference between the lower limit value and the new lower limit value is detected, and only the difference is detected. A first control method for setting a new upper limit value by lowering the upper limit value, and a second control method for setting a new lower limit value by lowering the new lower limit value by the difference thereafter. It is the control method of the all-solid-state lithium ion secondary battery which has.
全固体リチウムイオン二次電池が自動車に搭載される場合、該全固体リチウムイオン二次電池は、充電状態を示す状態値の上限値（以下、「上限ＳＯＣ」ということがある。）と下限値（以下、「下限ＳＯＣ」ということがある。）とが予め設定されており、その上限ＳＯＣと下限ＳＯＣと間の電位幅（以下、「ＳＯＣ幅」ということがある。）で使用される。「全固体リチウムイオン二次電池の使用条件によって下限値が新たな下限値まで低下して使用電位幅が増大した場合」とは、例えば、全固体リチウムイオン二次電池が自動車に搭載された場合に、アクセルを長く踏むなどして全固体リチウムイオン二次電池に高出力が要求され、電池容量を多く使用することで放電時間が増加する場合などが考えられる。 When an all-solid-state lithium ion secondary battery is mounted on an automobile, the all-solid-state lithium ion secondary battery has an upper limit value (hereinafter sometimes referred to as “upper limit SOC”) and a lower limit value indicating a state of charge. (Hereinafter, also referred to as “lower limit SOC”) is set in advance, and is used with a potential width between the upper limit SOC and the lower limit SOC (hereinafter also referred to as “SOC width”). “When the lower limit value decreases to a new lower limit value due to the use conditions of the all-solid-state lithium ion secondary battery and the use potential width increases”, for example, when the all-solid-state lithium ion secondary battery is mounted on an automobile In addition, there is a case where a high output is required for the all-solid-state lithium ion secondary battery by stepping on the accelerator for a long time, and the discharge time is increased by using a large battery capacity.
本発明によれば、使用電位幅が増大した全固体リチウムイオン二次電池の劣化を抑えられる、全固体リチウムイオン二次電池の制御方法を提供することができる。 ADVANTAGE OF THE INVENTION According to this invention, the control method of the all-solid-state lithium ion secondary battery which can suppress deterioration of the all-solid-state lithium ion secondary battery whose use electric potential width increased can be provided.
本発明の全固体リチウムイオン二次電池の制御方法（以下、単に「本発明の制御方法」ということがある。）は、所定のＳＯＣ幅で使用される全固体リチウムイオン二次電池の制御方法であって、全固体リチウムイオン二次電池の使用条件によって下限ＳＯＣが新たな下限ＳＯＣまで低下してＳＯＣ幅が増大した場合、元の下限ＳＯＣと新たな下限ＳＯＣとの差分を検知するとともに、その差分だけ上限ＳＯＣを低下させて新たな上限ＳＯＣを設定する第１の制御方法と、その後、新たな下限ＳＯＣを上記差分だけ低下させて、さらに新たな下限ＳＯＣを設定する第２の制御方法と、を有する制御方法である。 The control method for an all-solid-state lithium ion secondary battery of the present invention (hereinafter sometimes simply referred to as “control method of the present invention”) is a control method for an all-solid-state lithium ion secondary battery used with a predetermined SOC width. In the case where the lower limit SOC is lowered to the new lower limit SOC and the SOC width is increased due to the use conditions of the all solid lithium ion secondary battery, the difference between the original lower limit SOC and the new lower limit SOC is detected, and A first control method for setting a new upper limit SOC by lowering the upper limit SOC by the difference, and then a second control method for setting a new lower limit SOC by lowering the new lower limit SOC by the difference. And a control method.
以下、図１を参照しつつ、本発明の全固体リチウムイオン二次電池の制御方法について説明する。図１は、本発明の全固体リチウムイオン二次電池の制御方法による制御例を概略的に示す図である。 Hereinafter, the control method of the all-solid-state lithium ion secondary battery of this invention is demonstrated, referring FIG. FIG. 1 is a diagram schematically showing a control example according to the control method of an all solid lithium ion secondary battery of the present invention.
図１（ａ）は、本発明による制御を行う前の全固体リチウムイオン二次電池のＳＯＣ幅を示している。すなわち、本発明による制御を行う前は、全固体リチウムイオン二次電池の上限ＳＯＣはＥｍａｘ１であり、下限ＳＯＣはＥｍｉｎ１であったとする。ここで、全固体リチウムイオン二次電池を搭載した機器の使用状況によって、全固体リチウムイオン二次電池に高出力が要求された場合、全固体リチウムイオン二次電池は電池容量を多く使用することとなり、放電時間が増加し、その電池容量を回復するための回生時間も増加する。このようにして下限ＳＯＣが低下してＳＯＣ幅が増大した状態を図１（ｂ）に示す。 FIG. 1 (a) shows the SOC width of the all-solid-state lithium ion secondary battery before the control according to the present invention is performed. That is, before performing the control according to the present invention, it is assumed that the upper limit SOC of the all solid lithium ion secondary battery is Emax1 and the lower limit SOC is Emin1. Here, if a high output is required for the all-solid-state lithium ion secondary battery depending on the usage status of the device equipped with the all-solid-state lithium ion secondary battery, the all-solid-state lithium ion secondary battery should use a large amount of battery capacity. Thus, the discharge time increases, and the regeneration time for recovering the battery capacity also increases. FIG. 1B shows a state where the lower limit SOC is lowered and the SOC width is increased as described above.
本発明の第１の制御方法では、上述したようにして全固体リチウムイオン二次電池の下限ＳＯＣＥｍｉｎ１がＥｍｉｎ２まで低下した場合（図１（ｂ）参照）、元の下限ＳＯＣＥｍｉｎ１と新たな下限ＳＯＣＥｍｉｎ２との差分ΔＥを検知するとともに、その差分ΔＥだけ、図１（ｃ）に示すように上限ＳＯＣＥｍａｘ１を低下させ、新たな上限ＳＯＣＥｍａｘ２を設定する。すなわち、Ｅｍｉｎ１≦Ｅｍｉｎ２であるときは第１の制御方法は行われずＥｍｉｎ１＞Ｅｍｉｎ２となった場合に第１の制御方法が行われ、Ｅｍａｘ２＝Ｅｍａｘ１−ΔＥ（ただし、ΔＥ＝Ｅｍｉｍ１−Ｅｍｉｎ２）となる。 In the first control method of the present invention, when the lower limit SOCEmin1 of the all-solid-state lithium ion secondary battery has decreased to Emin2 as described above (see FIG. 1B), the original lower limit SOCEmin1 and the new lower limit SOCEmin2 The difference ΔE is detected, and the upper limit SOCEmax1 is lowered by the difference ΔE as shown in FIG. 1C, and a new upper limit SOCEmax2 is set. That is, when Emin1 ≦ Emin2, the first control method is not performed, and when Emin1> Emin2, the first control method is performed, and Emax2 = Emax1-ΔE (where ΔE = Emim1-Emin2). .
上記第１の制御方法が行われただけの状態（図１（ｃ）参照）では、ＳＯＣ幅が元の幅（図１（ａ）参照）と同じ幅になっている。全固体リチウムイオン二次電池に要求されている高出力に応じるためには、本発明の第２の制御方法によって、図１（ｄ）に示すように、下限ＳＯＣＥｍｉｎ２からさらにΔＥだけ低下させた新たな下限ＳＯＣＥｍｉｎ３を設定し、ＳＯＣ幅を増大させる。すなわち、Ｅｍａｘ１＝Ｅｍａｘ２であるときは第２の制御方法は行われず、第１の制御方法によってＥｍａｘ１＞Ｅｍａｘ２となった場合に第２の制御方法が行われ、Ｅｍｉｎ３＝Ｅｍｉｎ２−ΔＥ（ただし、ΔＥ＝Ｅｍｉｍ１−Ｅｍｉｎ２）となる。 In a state where the first control method is just performed (see FIG. 1C), the SOC width is the same as the original width (see FIG. 1A). In order to respond to the high output required for the all-solid-state lithium ion secondary battery, the second control method of the present invention, as shown in FIG. 1 (d), is newly reduced by ΔE from the lower limit SOCEmin2. A lower limit SOCEmin3 is set to increase the SOC width. That is, when Emax1 = Emax2, the second control method is not performed, and when Emax1> Emax2 is satisfied by the first control method, the second control method is performed, and Emin3 = Emin2−ΔE (where ΔE = Emim1-Emin2).
上述したように、本発明の制御方法によれば、上限ＳＯＣを下げつつ下限ＳＯＣも下げることによって、ＳＯＣ幅を増大させる。このようにしてＳＯＣ幅を増大させることによって、ＳＯＣ幅を増大させても全固体リチウムイオン二次電池の劣化を抑えることができる。 As described above, according to the control method of the present invention, the SOC width is increased by lowering the lower limit SOC while lowering the upper limit SOC. By increasing the SOC width in this way, deterioration of the all-solid-state lithium ion secondary battery can be suppressed even when the SOC width is increased.
なお、本発明に用いることができる全固体リチウムイオン二次電池の形態は特に限定されず、公知のものを用いることができる。 In addition, the form of the all-solid-state lithium ion secondary battery which can be used for this invention is not specifically limited, A well-known thing can be used.
以下、実施例に基づいて本発明を説明する。 Hereinafter, the present invention will be described based on examples.
１．評価用セルの作製
まず、電解質層、正極層、及び負極層を作製した。電解質層は、固体電解質としてＬｉ７Ｐ３Ｓ１１を用意し、これを混合した後、１．０ｔｏｎ／ｃｍ２の圧力でプレス成形して作製した。正極層は、リチウム遷移金属酸化物であるＬｉＣｏＯ２を含む正極材と固体電解質であるＬｉ７Ｐ３Ｓ１１とを混合した後、１．０ｔｏｎ／ｃｍ２の圧力でプレス成形して作製した。負極層は、カーボンを含む負極材と固体電解質であるＬｉ７Ｐ３Ｓ１１とを混合した後、４．０ｔｏｎ／ｃｍ２の圧力でプレス成形して作製した。
このようにして得られた正極層、電解質層、及び負極層と集電体とを、その順に重ね合わせて積層体を作製した。さらに、該積層体をプレス機で圧縮し、電池ケース内に収容して、充電、及び放電可能な全固体リチウムイオン二次電池とした。
1. Production of Evaluation Cell First, an electrolyte layer, a positive electrode layer, and a negative electrode layer were produced. The electrolyte layer was prepared by preparing Li 7 P 3 S 11 as a solid electrolyte, mixing it, and press-molding it at a pressure of 1.0 ton / cm 2 . The positive electrode layer was prepared by mixing a positive electrode material containing LiCoO 2 that is a lithium transition metal oxide and Li 7 P 3 S 11 that is a solid electrolyte, and then press-molding it at a pressure of 1.0 ton / cm 2 . The negative electrode layer was prepared by mixing a negative electrode material containing carbon and Li 7 P 3 S 11 which is a solid electrolyte, and then press-molding it at a pressure of 4.0 ton / cm 2 .
The positive electrode layer, the electrolyte layer, and the negative electrode layer thus obtained and the current collector were superposed in that order to produce a laminate. Further, the laminate was compressed with a press machine and housed in a battery case to obtain an all-solid lithium ion secondary battery that can be charged and discharged.
２．抵抗上昇率の測定
上記のように作製した評価用セルを６つ（Ａ〜Ｆ）用意して、それぞれの評価用セルについて異なるＳＯＣ幅で充電、及び放電を３０サイクル繰り返した。そして、その後の抵抗上昇率（３０サイクル後の抵抗値／最初の抵抗値）を測定した。その結果を図２に示す。図２（ａ）及び図２（ｂ）において、横軸はＳＯＣ幅［％］を示し、縦軸は抵抗上昇率［％］を示している。また、図２（ａ）及び図２（ｂ）中の直線は線形近似直線である。
2. Measurement of Resistance Increase Rate Six evaluation cells (A to F) prepared as described above were prepared, and charging and discharging were repeated 30 cycles for each evaluation cell with different SOC widths. Then, the subsequent rate of increase in resistance (resistance value after 30 cycles / initial resistance value) was measured. The result is shown in FIG. 2A and 2B, the horizontal axis indicates the SOC width [%], and the vertical axis indicates the resistance increase rate [%]. Moreover, the straight line in Fig.2 (a) and FIG.2 (b) is a linear approximation straight line.
図２（ａ）において、Ａは上限ＳＯＣを１００、下限ＳＯＣを７５として、ＳＯＣ幅を２５とした場合、Ｂは上限ＳＯＣを１００、下限ＳＯＣを５０として、ＳＯＣ幅を５０とした場合、Ｃは上限ＳＯＣを１００、下限ＳＯＣを４０として、ＳＯＣ幅を６０とした場合、Ｄは上限ＳＯＣを１００、下限ＳＯＣを１０として、ＳＯＣ幅を９０とした場合の結果を示している。また、図２（ｂ）において、Ａは上記と同じものであり、Ｅは上限ＳＯＣを９０、下限ＳＯＣを６０として、ＳＯＣ幅を３０とした場合、Ｆは上限ＳＯＣを５０、下限ＳＯＣを１０として、ＳＯＣ幅を４０とした場合の結果を示している。 In FIG. 2A, A is 100 when the upper limit SOC is 100 and the lower limit SOC is 75 and the SOC width is 25, B is C when the upper limit SOC is 100, the lower limit SOC is 50, and the SOC width is 50. Shows the result when the upper limit SOC is 100, the lower limit SOC is 40, and the SOC width is 60, and D is the result when the upper limit SOC is 100, the lower limit SOC is 10, and the SOC width is 90. In FIG. 2 (b), A is the same as above, E is the upper limit SOC is 90, the lower limit SOC is 60, and the SOC width is 30, and F is the upper limit SOC is 50 and the lower limit SOC is 10 The results when the SOC width is 40 are shown.
図２（ａ）に示すように、上限ＳＯＣが同一（１００％）で、下限ＳＯＣが異なることによってＳＯＣ幅が異なる評価用セル（Ａ〜Ｄ）による結果を比較すると、ＳＯＣ幅が大きな評価用セルの方が、抵抗上昇率が大きかった。一方、図２（ｂ）に示すように、上限ＳＯＣ及び下限ＳＯＣが異なり、ＳＯＣ幅が異なる評価用セル（Ａ，Ｅ，Ｆ）による結果を比較すると、ＳＯＣ幅が大きくても、上限ＳＯＣ及び下限ＳＯＣが低い評価用セルの方が、抵抗上昇率を抑制できていた。したがって、本発明の制御方法によって、上限ＳＯＣ及び下限ＳＯＣを下げながらＳＯＣ幅を調整する制御を行うことによって、ＳＯＣ幅が増大した全固体リチウムイオン二次電池の劣化を抑えられることがわかる。 As shown in FIG. 2A, when the results of evaluation cells (A to D) having the same upper limit SOC (100%) and different SOC widths due to different lower limit SOCs are compared, the evaluation results have a large SOC width. The cell had a higher resistance increase rate. On the other hand, as shown in FIG. 2B, when the results of the evaluation cells (A, E, F) having different upper limit SOC and lower limit SOC and different SOC widths are compared, even if the SOC width is large, the upper limit SOC and The evaluation cell having a lower lower limit SOC could suppress the rate of increase in resistance. Therefore, it can be seen that the control method of the present invention can suppress the deterioration of the all-solid-state lithium ion secondary battery having an increased SOC width by controlling the SOC width while lowering the upper limit SOC and the lower limit SOC.
以上、現時点において、もっとも、実践的であり、かつ、好ましいと思われる実施形態に関連して本発明を説明したが、本発明は、本願明細書中に開示された実施形態に限定されるものではなく、請求の範囲および明細書全体から読み取れる発明の要旨或いは思想に反しない範囲で適宜変更可能であり、そのような変更を伴う全固体リチウムイオン二次電池の制御方法もまた本発明の技術的範囲に包含されるものとして理解されなければならない。 While the present invention has been described in connection with embodiments that are presently the most practical and preferred, the present invention is not limited to the embodiments disclosed herein. However, the present invention can be changed as appropriate without departing from the spirit or concept of the invention that can be read from the claims and the entire specification, and the control method of the all-solid-state lithium ion secondary battery accompanying such a change is also a technique of the present invention. Should be understood as being included in the scope.
Claims (1)
前記全固体リチウムイオン二次電池の使用条件によって前記下限値が新たな下限値まで低下して前記使用電位幅が増大した場合、
前記下限値と前記新たな下限値との差分を検知するとともに、前記差分だけ前記上限値を低下させて新たな上限値を設定する第１の制御方法と、
その後、前記新たな下限値を前記差分だけ低下させて、さらに新たな下限値を設定する第２の制御方法と、
を有する、全固体リチウムイオン二次電池の制御方法。 An upper limit value and a lower limit value of a state value indicating a state of charge are preset, and is a control method of an all-solid-state lithium ion secondary battery that is used in a use potential range determined by the upper limit value and the lower limit value,
When the lower limit value is lowered to a new lower limit value due to use conditions of the all solid lithium ion secondary battery and the use potential width is increased,
A first control method for detecting a difference between the lower limit value and the new lower limit value, and lowering the upper limit value by the difference and setting a new upper limit value;
Then, a second control method of setting the new lower limit value by lowering the new lower limit value by the difference,
A method for controlling an all-solid-state lithium ion secondary battery.
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