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`Notice
`This translation is machine-generated. It cannot be guaranteedthatit is intelligible, accurate,
`complete, reliable or fit for specific purposes. Critical decisions, such as commercially relevant or
`financial decisions, should not be based on machine-translation output.
`
`DESCRIPTION J P2006244734A
`10 All-solid-state lithium secondary battery
`
`[0001]
`14 The present invention relates to an all-solid-state lithium secondary battery having good
`charge-discharge characteristics.
`
`[0002]
`19 2, Description of the Related Art With the rapid spread of information-related devices and
`communication devices, such as personal computers, video cameras, and mobile phones,in
`recent years, importance has been placed on the development of excellent lithium secondary
`batteries as power sourcesfor these devices. In addition to the fields of information-related
`and communication-related devices, for example, in the automobile industry, developmentis
`underway of high-output, high-capacity lithium secondary batteries for electric and hybrid
`automobiles as low-pollution vehicles.
`
`[0003]
`29 However,lithium secondary batteries currently available on the market use an organic
`electrolyte that uses an organic solvent as a solvent, and therefore have the risk of ignition or
`explosion in the event of a short circuit.
`32 This is essentially the same as whatis called a Li-polymer battery, in which case the separator
`separating the positive electrodes is simply a polymer impregnated with an organic
`electrolyte, and the risk of fire or explosion in the event of a short circuit remains almost the
`same.In particular, in the case of large batteries for vehicle use, the risk of fire or explosion is
`high and the problem is serious.
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`[0004]
`40 In order to solve the above-mentioned problemsoffire and explosion, the developmentof an
`all-solid-state lithium secondary battery using a solid having Li ion conductivity as an
`electrolyte has been considered (Non-Patent Document1).
`43 Since all-solid-state lithium secondary batteries do not use flammable organic solvents in the
`batteries, the risk of fire or explosion in the event of a short circuit is extremely low, and they
`are considered to be excellent in safety. However,in all-solid-state lithium secondary batteries,
`the positive electrode, negative electrode, and electrolyte areall solid, and therefore the
`electrochemical resistance at the positive electrode-electrolyte interface or the negative
`electrode-electrolyte interface is large compared to batteries that use an electrolytic solution,
`makingit difficult to obtain a battery with desired charge-discharge characteristics.
`
`[0005]
`53 PAWS AS 8 1 SSSR S 675
`54 49H 2003- 346901 aR
`
`[0006]
`58 The present invention has been made in view of the above circumstances, and hasas its main
`object to provide an all-solid-state lithium secondary battery having good charge-discharge
`characteristics.
`
`[0007]
`64 In order to achieve the above object, the present invention provides a positive electrode
`including a positive electrode layer containing a positive electrode active material containing
`Li element and a positive electrode current collector, a negative electrode including a negative
`electrode layer containing a negative electrode active material and a negative electrode
`current collector, and a negative electrode having a negative electrode layer and a negative
`electrode current collector sandwiched betweenthe positive electrode layer and the negative
`electrode layer and represented by the following general formula
`Li_{3- 2 X}M_XIn_{1 —- Y}M'_YL_{6- Z
`
`}L'_Z (wherein M and M' are metal elements, and L and L' are halogen
`elements.
`74 Furthermore, X, Y and Z independently satisfy the following: 0 $X<1.5,0SY<1,08ZS6.
`75 and a solid electrolyte comprising a compound represented by the formula (I) and (ID), wherein
`the negative electrode active material has an average potential vs. Li of 0.7 V orless.
`
`[0008]
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`so According to the present invention, by setting the Li potential of the negative electrode active
`material to 0.7 V or less on average,a film made of decomposition products due to reductive
`decomposition is well formed between the solid electrolyte and the negative electrode layer,
`and an all-solid-state lithium secondary battery with good charge-discharge characteristics can
`be obtained.
`
`[0009]
`ss In the above invention, the positive electrode active material preferably has an average Li
`potential of 3.9 V or less.
`90 A film made of decomposition products produced by oxidative decomposition has the function
`of inhibiting the transmission of Li ions, and therefore, by setting the Li potential of the
`positive electrode active material to the above value, the formation of the film can be
`suppressed, and an all-solid-state lithium secondary battery having good charge/discharge
`characteristics can be obtained.
`
`[0010]
`93 The present invention has an effect of providing an all-solid-state lithium secondary battery
`having good charge/discharge characteristics.
`
`[0011]
`103 The all-solid-state lithium secondary battery of the present invention will be described in
`detail below.
`
`[0012]
`108 The all solid-state lithium secondary battery of the present invention comprises a positive
`electrode including a positive electrode layer containing a positive electrode active material
`containing Li element and a positive electrode current collector, a negative electrode
`including a negative electrode layer containing a negative electrode active material and a
`negative electrode current collector, and a solid-state lithium secondary battery sandwiched
`between the positive electrode layer and the negative electrode layer and represented by the
`following general formula
`Li_{3- 2 X}M_XIn_{1 —- Y}M'_YL_{6 —
`
`Z}L'_Z (wherein M and M' are metal elements, and L and L' are halogen
`elements).
`778 Furthermore, X, Y and Z independently satisfy the following: 0 £X<1.5,0SY<1,0£ZS6.
`779 and a Solid electrolyte comprising a compound represented by the formula (I) and wherein
`the negative electrode active material has an average potential vs. Li of 0.7 V or less.
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`[0013]
`124 In the present invention, the potentials of the negative electrode active material and the
`positive electrode active material against Li were determined from the open circuit
`electromotive force during charging and discharging by preparing a half cell using Li metal
`as the counter electrode.
`
`128 The average value of the potential relative to Li was determined by integrating the potential
`with respect to the capacity and dividing the result by the total capacity.
`
`[0014]
`133 According to the present invention, by setting the Li potential of the negative electrode active
`material to 0.7 V or less on average,a film made of decomposition products due to reductive
`decomposition is well formed between the solid electrolyte and the negative electrode layer,
`and it is considered that this film makes it possible to obtain an all-solid-state lithium
`secondary battery having good charge-discharge characteristics.
`138 Although the reason for this is unclear, it is presumed to be due to the following reasons.
`139 Thatis, it has been confirmed that the above-mentioned film is formed at the interface
`between the solid electrolyte and the negative electrode layer by repeatedly charging and
`discharging the all-solid-state lithium secondary battery several times.
`142 Since a similar film was formed regardless of the type of negative electrode active material,
`the film is considered to be a decomposition product generated by the reductive
`decomposition of a part of the solid electrolyte.
`745 Furthermore, experimental results and the like suggest that the formation of the above-
`mentioned film reduces the electrochemical resistance between the solid electrolyte and the
`negative electrode layer, and it can be said that promoting the formation of the above-
`mentioned film is preferable in terms of improving charge-discharge characteristics.
`749 In the present invention, it can be considered that by setting the Li potential of the negative
`electrode active material to be 0.7 V or less on average, an environmentis created in which
`the reductive decomposition of the solid electrolyteis likely to occur, the formation of the
`film is promoted, and the charge/discharge characteristics of the all-solid-state lithium
`secondary battery are improved.
`
`[0015]
`157 Next, the all-solid-state lithium secondary battery of the present invention will be described
`with reference to the drawings.
`159 FIG. 1
`is a schematic cross-sectional view showing an example of the all-solid-state lithium
`secondary battery of the present invention.
`161 The all-solid-state lithium secondary battery 10 shown in FIG. 1 comprises a positive
`electrode 4 including a positive electrode layer 2 containing a positive electrode active
`material 1
`including Li element and a positive electrode current collector 3, a negative
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`electrode 8 including a negative electrode layer 6 containing a negative electrode active
`material 5 and a negative electrode current collector 7, and a solid electrolyte 9 sandwiched
`between the positive electrode layer 2 and the negative electrode layer 6 and made of a
`compound represented by the general formula above, and the negative electrode active
`material 6 has an average potential vs. Li of 0.7 V or less.
`169 Hereinafter, each of the componentsofthe all-solid-state lithium secondary battery of the
`present invention will be described.
`
`[0016]
`174 (1) Negative Electrode First, the negative electrode used in the present invention will be
`described.
`
`176 The negative electrode used in the present invention comprises at least a negative electrode
`layer and a negative electrode current collector.
`
`[0017]
`181 (a) Negative Electrode Layer The negative electrode layer used in the present invention
`contains at least a negative electrode active material, and is formed on a negative electrode
`current collector described below.
`
`184 The negative electrode active material used in the present invention has the property of
`taking in Li ions during charging and releasing Li ions during discharging.
`786 In the present invention, the Li potential of the negative electrode active material is 0.7 V or
`less on average, and preferably in the range of 0.5 to 0.0 V on average.
`188 Within the above range, an environment can be created in which the above-mentionedfilm is
`easily formed by reductive decomposition.
`
`[0018]
`793 The negative electrode active material used in the present invention is not particularly limited
`as long as it has an average potential vs. Li of 0.7 V or less. Specific examples of the negative
`electrode active material include metal-based active materials such as Li, In, Si, Sn, Al, Zn, Bi,
`Cd, Sb, Pb, and wood metal (Bi-Pb-Cd-Sn eutectic alloy), and carbon-based active materials
`such as mesocarbon microbeads (MCMB), highly oriented graphite (HOPG), hard carbon, and
`soft carbon.
`
`799 In the present invention, it is particularly preferable to use Li metal as the negative electrode
`active material.
`
`201 This is because the potential of Li metal relative to Li is 0 V, and an all-solid-state lithium
`secondary battery having good charge/discharge characteristics can be obtained.
`
`[0019]
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`206 Next, the negative electrode layer used in the present invention will be described.
`207 The negative electrode layer used in the present invention contains the above-mentioned
`negative electrode active material, and its structure, composition, etc. are not particularly
`limited.
`
`210 Specifically, examples of the active material include a metal film of the above-mentioned
`metal-based active material, or a compressed powder of the above-mentioned metal-based
`active material or the above-mentioned carbon-based active material. Among these, in the
`present invention, a metal film of the metal-based active material is preferred.
`
`[0020]
`217 The metal film of the above-mentioned metal-based active material is not particularly limited,
`but specific examples include metal foil, plated foil, vapor-deposited foil, etc. of the above-
`mentioned metal-based active material, and amongthese, the metal foil of the above-
`mentioned metal-based active material is preferred.
`
`[0021]
`224 In the present invention, it is particularly preferable to use a metal foil of Li metal as the
`negative electrode layer.
`226 Whena Liln alloy foil is used as the negative electrode layer, the In content in the LiIn alloy is
`preferably within the range of 0 to 20 wt %.
`
`[0022]
`231 In the case wherethe negative electrode layer used in the present invention is made of a
`material other than the above-mentioned metal film, the conductivity can be improved by
`adding a conductive agent.
`234 Specifically, there can be mentioned a method in which, when the negative electrode layeris
`formed by compressing powderof the negative electrode active material, a conductive agent
`is added to improve the conductivity of the negative electrode layer.
`237 Such a conductive agentis not particularly limited, but specific examples include acetylene
`black, Ketjen Black (trade name, manufactured by Lion Corporation), carbon fiber, and the
`like.
`
`240 The conductive agent can be added in any amountas long as it does not impair the function
`of the negative electrode layer.
`
`[0023]
`245 (b) Negative Electrode Current Collector Next, the negative electrode current collector used in
`the present invention will be described.
`247 The negative electrode current collector used in the present invention has a function of
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`

`transferring electrons generated by the reaction.
`249 The negative electrode current collector is not particularly limited as long as it is conductive,
`and examples thereof include metal foils such as Al, Ni, and Ti, and carbon paper.
`251 The negative electrode current collector used in the present invention may also function as a
`battery cell.
`253 Specifically, a battery cell made of stainless steel is prepared, and a part of the battery cell is
`used as the negative electrode current collector.
`
`[0024]
`258 (2) Positive Electrode Next, the positive electrode used in the present invention will be
`described.
`
`260 The positive electrode used in the present invention comprises at least a positive electrode
`layer and a positive electrode current collector.
`
`[0025]
`265 (a) Positive Electrode Layer The positive electrode layer used in the present invention
`contains at least a positive electrode active material, and is formed on a positive electrode
`current collector described below.
`
`268 The positive electrode active material used in the present invention has the property of
`releasing Li ions during charging and taking in Li ions during discharging, and contains Li
`element.
`
`[0026]
`274 The potential versus Li of the positive electrode active material used in the present invention
`is not particularly limited as long as an all-solid-state lithium secondary battery having good
`charge/discharge characteristics can be obtained, but specifically, it is preferably 3.9 V or
`less on average.
`278 Within the above range, an environmentcan be created in which the formation ofa film due
`to oxidative decomposition is unlikely.
`280 Although the reason for this is not yet clear, it is presumed to be due to the following reasons.
`281 That is, it has been confirmed that the above-mentionedfilm is formed at the interface
`between the solid electrolyte and the positive electrode layer by repeatedly charging and
`discharging the all-solid-state lithium secondary battery several times.
`284 Since a similar film was formed regardless of the type of positive electrode active material, the
`film is considered to be a decomposition product generated by oxidative decomposition of a
`part of the solid electrolyte.
`287 The above-mentioned film differs from the film formed by the reductive decomposition of the
`solid electrolyte described above, and experiments have suggested that the electrochemical
`resistance between the solid electrolyte and the negative electrode layer increases. Therefore,
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`suppressing the formation of the above-mentioned film is considered to be preferable in
`terms of improving charge/discharge characteristics.
`292 Therefore, in the present invention, it is considered preferable to set the Li potential of the
`positive electrode active material to 3.9 V or less on average, thereby creating an
`environment in which oxidative decomposition of the solid electrolyte is unlikely to occur,
`and thus suppressing the formation ofthe film.
`
`[0027]
`299 The positive electrode active material used in the present invention is not particularly limited
`as long as it contains Li element and can provide a desiredall-solid-state lithium secondary
`battery, but specific examples thereof include oxide-based positive electrode active materials
`and phosphoric acid-based positive electrode active materials.
`
`[0028]
`306 Examples of the oxide-based positive electrode active material include the following
`compoundis(i) to(iii).
`308 (i) LININER13MNER14M'NER150NER16 (wherein M and M' independently represent a metal
`element.
`
`370 Furthermore, x and y satisfy 0 $ x+y<1.
`371 In the above (i), examples of the metal element used for M and M' include Co,Al, Mn, etc.
`312 Specific examples of the compound represented by (i) above include LiNiO₂,
`LiAl<sub>0 . 0 5</sub>Ni<sub>0O . 8</sub>Co<sub>0 .
`1 5</sub>O₂, and
`
`the like.
`
`[0029]
`378 (ii) LIMMNNER22AINER23ONER24 (wherein x satisfies 0 S$ x<1).
`379) Specific examples of the compound represented by(ii) above include
`LiMn<sub> 2 </sub>O<sub> 4 </sub> and
`
`LiMn<sub>1 . 9</sub>Al<sub>0 .
`
`1 </sub>O<sub> 4 </sub>.
`
`[0030]
`325 (iii) Compoundsother than those mentioned above Specific examples of compounds other
`than those mentionedin (i) and (ii) above include LiCoO<sub> 2 </sub>,
`LiMnO₂, Li₂NiMn₃O₈,
`LiVO<sub> 2 </sub>, LiCrO<sub> 2 </sub>, and the like.
`
`[0031]
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`

`332 Specific examples of the phosphoric acid-based positive electrode active material include
`LiFePO₄ and LiCoPO₄.
`
`[0032]
`337 Among the above-mentioned oxide-based positive electrode active materials and phosphate-
`based positive electrode active materials, in the present invention, from the viewpoint of an
`average Li potential of 3.9 V or less, LiCoO<sub> 2 </sub>,
`LiAl_{0 . 0 5}Ni_{0 . 8}Co_{0 .
`
`1 5}O₂,
`
`LiMn_{1 . 9}Al_{0 .
`are preferred, and
`LiAl_{0 . 0 5}Ni_{0 . 8}Co_{0 .
`
`1}O₄, and LiFePO₄
`
`1 5}O₂ is
`
`particularly preferred.
`
`[0033]
`348 Next, the positive electrode layer used in the present invention will be described.
`349 The positive electrode layer used in the present invention contains the above-mentioned
`positive electrode active material, and its structure, composition, etc. are not particularly
`limited.
`
`352 Specifically, the positive electrode active material may be compressed into a powder form.
`
`[0034]
`356 The positive electrode layer used in the present invention may contain a conductive agentin
`order to improve the conductivity.
`358 Specifically, when the positive electrode layer is formed by compressing powder of the
`positive electrode active material, the conductivity of the positive electrode layer can be
`improved by adding a conductive agent.
`361 Such a conductive agentis not particularly limited, but specific examples include acetylene
`black, Ni powder, and the like.
`363 The conductive agent can be added in any amountas long as it does not impair the function
`of the positive electrode layer.
`
`[0035]
`368 (b) Positive Electrode Current Collector Next, the positive electrode current collector used in
`the present invention will be described.
`370 The positive electrode current collector used in the present invention has a function of
`transferring electrons generated by the reaction.
`372 The positive electrode current collector used in the present invention is not particularly
`limited as long as it has the above-mentioned properties, but since it can be the same as the
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`

`negative electrode current collector described above, a description thereof will be omitted
`here.
`
`[0036]
`379 (3) Solid Electrolyte Next, the solid electrolyte used in the present invention will be described.
`380 The solid electrolyte used in the present invention has the following general formula:
`Li<sub>3- 2 X</sub>M<sub> X </sub>In<sub> 1 — Y </sub>M'<sub> Y </sub>L<sub> 6 -
`
`Z </sub>L'<sub> Z </sub> (wherein M and M' are metal elements, and L and L' are halogen
`elements).
`384 Furthermore, X, Y and Z independently satisfy the following: 0 £X<1.5,0SY<1,0SZS6.
`385 ) is expressed as:
`
`[0037]
`389 In the above general formula, M represents a metal element.
`390 The metal element used for M is not particularly limited, but specific examples include Ca, Sr,
`Ba, Mg, etc., and among these, Ba and Mg are preferable.
`392 In the above general formula, M' represents a metal element.
`393 The metal element used for M' is not particularly limited, but specific examples include Fe,
`Nd, Co, Zn, Sb, Y, etc., and amongthese, Nd is preferable.
`395 Furthermore, in the above general formula, L and L' independently represent a halogen
`element.
`
`397 The halogen element used for L and L' is not particularly limited, but specific examples
`include Br, Cl, I, etc., and among these, Br and Cl are preferred.
`
`[0038]
`402 In the present invention, among the compoundsrepresented by the above general formula,
`Li<sub> 3 </sub>InBr<sub> 6 </sub> and
`
`Li<sub> 3 </sub>InBr<sub> 3 </sub>Cl<sub> 3 </sub> are preferred.
`405 This is because it has high Li ion conductivity, and when used asa solid electrolyte,it is
`possible to obtain an all-solid-state lithium secondary battery having good charge/discharge
`characteristics.
`
`[0039]
`411 The stable region of the potential of the solid electrolyte used in the present invention with
`respect to Li is usually within the range of 0 to 4.2 V, although this varies depending on the
`composition of the solid electrolyte.
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`[0040]
`417 The thickness of the solid electrolyte used in the present invention is not particularly limited,
`but is preferably 0.1 to 1 mm, and more preferably 0.1 to0.2 mm.
`479 In order to reduce the internal resistance of the battery,it is preferable that the film thickness
`is thin, and within the above range,an all-solid-state lithium secondary battery having good
`charge/discharge characteristics can be obtained.
`
`[0041]
`425 It should be noted that the present invention is not limited to the above-described
`embodiment.
`
`427 The above-described embodiments are merely examples, and anything that has substantially
`the same configuration as the technical idea described in the claims of the present invention
`and exhibits similar effects is included within the technical scope of the present invention.
`
`[0042]
`433 The presentinvention will be described in more detail below with reference to examples.
`434 Example 1 An all-solid-state lithium secondary battery was fabricated using a SUS cell.
`435 First, a Li metal foil (average potential relative to Li: 0 V) was placed on the bottom ofthe cell,
`and an acrylic guide with a hole (@ 7 cm) in the center was placed on top ofit. 150 mg of
`Li<sub> 3 </sub>InBr<sub> 3 </sub>Cl<sub> 3 </sub> was filled through the hole as a solid
`electrolyte.
`439 Then, the surface of the solid electrolyte was smoothedwith a stainless steel rod, and 20 mg
`of LiAl_{0 . 0 5}Ni_{0 . 8}Co<sub>0 .
`1 5 </sub>O<sub> 2 </sub>
`
`(average potential vs. Li: 3.6 V) and Ketjen Black (product name, manufactured by Lion
`Corporation) in a weight ratio of 95:5 was prepared and sprinkled onto the solid electrolyte.
`443 A Stainless steel current collector was inserted into the hole, and the cell container was closed
`to obtain an all-solid-state lithium secondary battery.
`
`[0043]
`448 A constant current charge/discharge test was carried out on the obtainedall solid-state
`lithium secondary battery at a charge/discharge current of 10 p A.
`450 The results are shown in Figure 2.
`
`[0044]
`454 Example 2 An all-solid-state lithium secondary battery was obtained in the same manner as in
`Example 1, except that a LiIn alloy foil (average potential relative to Li: 0.7 V) was used
`instead of the Li metal foil.
`
`457 A constant current charge/discharge test was carried out on the obtainedall solid-state
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`

`lithium secondary battery at a charge/discharge current of 10 p A.
`459 The results are shown in Figure 3.
`
`[0045]
`463 Example 3 An all-solid-state lithium secondary battery was obtained in the same manner as in
`Example 1, except that LiCoO₂ (average potential relative to Li: 3.7 V) was used
`instead of the
`
`LiAl<sub>0 . 0 5</sub>Ni<sub>0 . 8</sub>Co<sub>0 .
`
`1 5 </sub>O<sub> 2 </sub>.
`
`467 A constant current charge/discharge test was carried out on the obtainedall solid-state
`lithium secondary battery at a charge/discharge current of 10 p A.
`469 The results are shown in Figure 4.
`
`[0046]
`473 [Example 4] An all-solid-state lithium secondary battery was obtained in the same manneras
`in Example 1, except that a LiIn alloy foil (average potential relative to Li: 0.7 V) was used
`instead of the Li metal foil, and
`
`LiAl_{0 . 0 5}Ni_{0 . 8}Co_{0 .
`
`1 5}O₂ was
`
`used instead of LiCoO₂ (average potential relative to Li: 3.7 V).
`478 A constant current charge/discharge test was carried out on the obtainedall solid-state
`lithium secondary battery at a charge/discharge current of 10 p A.
`4so The results are shown in Figure 5.
`
`[0047]
`484 [Comparative Example 1] An all-solid-state lithium secondary battery was obtained in the
`same manner as in Example 1, except that
`Li₄Ti₅O_{1 2} (average potential relative to Li: 1.5 V)
`was usedinstead of the above Li metal foil, and LiCoO<sub> 2 </sub> (average potential
`relative to Li: 3.7 V) was used instead of the above
`LiAl<sub>0 . 0 5</sub>Ni<sub>0 . 8</sub>Co<sub>0 .
`
`1 5 </sub>O<sub> 2 </sub>.
`
`490 A constant current charge/discharge test was carried out on the obtainedall solid-state
`lithium secondary battery at a charge/discharge current of 100 p A.
`492 The results are shown in Figure 6.
`
`[0048]
`496 [Results] The following results became clear from FIGS.
`497 That is, in Example 1, although the charge/discharge capacity in the first cycle was small, the
`charge/discharge capacity improved with each cycle.
`499 In addition, in Examples 2 to 4, the charge/discharge capacity decreased with each cycle, but
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`

`charging and discharging were possible.
`501 In contrast, in Comparative Example 1, no discharge was possible atall.
`502 From theseresults, it was confirmed that charging and discharging were possible in Examples
`1 to 4, which used the positive electrode active material and the negative electrode active
`material that satisfied the condition of the Li potential in the present invention.
`
`510 1
`
`512 1
`
`[0049]
`508 1
`is a schematic cross-sectional view showing an example ofan all-solid-state lithium
`secondary battery of the present invention.
`is a graph showingthe relationship between potential and charge/discharge capacity ina
`constant current charge/discharge test in Example 1.
`is a graph showingthe relationship between potential and charge/discharge capacity ina
`constant current charge/discharge test of Example 2.
`5141 is a graph showingthe relationship between potential and charge/discharge capacity ina
`constant current charge/discharge test of Example 3.
`is a graph showingthe relationship between potential and charge/discharge capacity ina
`constant current charge/discharge test in Example 4.
`is a graph showing the relationship between potential and charge/discharge capacity ina
`constant current charge/discharge test of Comparative Example 1.
`520 Explanation of symbols
`
`516 1
`
`518 1
`
`[0050]
`524 REFERENCE SIGNS LIST 1 positive electrode active material 2 positive electrode layer 3
`positive electrode current collector 4 positive electrode 5 negative electrode active material 6
`negative electrode layer 7 negative electrode current collector 8 negative electrode 9 solid
`electrolyte 10 all-solid-state lithium secondary battery
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`