Aqueous zinc-ion battery based on pyrene-4, 5, 9, 10-tetrone anode and zinc cathode
`SEISSSSRSRRRnana
`
`DOCUMENTID
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`CN-107565134-A
`
`DATE PUBLISHED
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`2018-01-09
`
`INVENTOR INFORMATION
`
`NAME
`
`WANG, YONG-GANG
`MA, Yuan-yuan
`XIA, Yong-yao
`
`CITY
`
`N/A
`N/A
`N/A
`
`STATE
`
`ZIP CODE
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`COUNTRY
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`N/A
`N/A
`N/A
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`N/A
`N/A
`N/A
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`N/A
`N/A
`N/A
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`DATE FILED
`
`2017-07-22
`
`CPC CURRENT
`
`TYPE
`
`CGPCA
`
`Abstract
`
`CPC
`
`Y02E60/10
`
`DATE
`
`2013-01-01
`
`The invention belongs to the technicalfield of electrochemistry, specifically an aqueous zinc-ion battery
`based on pyrene-4, 5, 9, 10-tetrone anode and zinc cathode; the battery system specifically includes an
`aqueous electrolyte solution containing zinc ion using pyrene -4, 5, 9, 10-tetrone as anode, metal zinc as
`cathode; when the battery discharges, cathode zinc loses electrons to the zinc ion, zinc ion diffuses to the
`anode, anode of pyrene-4, 5, 9, 10-tetrone obtains electrons to perform enolization reaction, storing zinc ion,
`electron flows to the anode through an external circuit from the cathode, when charging, zinc ion diffuses
`from the anode organic to the cathode, the cathode surface is deposited, electrons flows from the anode
`through an external circuit to the cathode. The invention avoids using metal ion embeddedin the electrode
`material/off and lead to damage of the electrode material structure, so as to improvethe cycle life of the
`battery. the battery having a long cycle life, high energy density, high safety and environmental protection
`and so on, the large energy field with wide application prospect.
`
`Description
`
`INVENTION-TITLE
`technical field
`This invention belongs to battery technology field, specifically relates to a water system with high safety and
`high stability can be chargeable battery.
`BACKGROUND
`With the increasing deterioration of coal, petroleum and other fossil fuel exhaustion and application
`environment, the development of solar energy, wind energy and renewable energy has become a worldwide
`trend. However, since solar energy, wind energy and renewable energy ofitself not stability, effective
`utilization thereof must depend on the large energy storage device. rechargeable battery has been widely
`applied to electric automobile, mobile phone mobile communication field such as a kind of high-efficient
`
`

`

`electrochemical energy storage device. In recent years, large battery system also has attracted attention in
`application of large scale energy storage aspect. However, often relates to the electrode material and the
`electrolyte material is not friendly to the environment, and exhibit limited cycle life and a certain safety
`problem of existing rechargeable battery system. These factors greatly limits its application in large energy
`storage aspect. Therefore, the development of green environmental protection, high specific energy, safety
`of the new battery systems bythe wide attention.
`secondary battery (such asa lithium ion battery or lithium metal battery) to anhydrous organic solution as the
`electrolyte has a wide potential window, can typically be achieved with high energy density. However, the
`organic electrolyte typically toxic and flammable, so it has great safety problem in the process of using, and
`the anhydrous preparation condition so that the production cost is increased. battery system uses aqueous
`electrolyte solution to replace traditional organic electrolyte and is expected to further reduce the
`manufacture cost and improve the safety of the battery. the traditional aqueous battery with a lead-acid
`battery, nickel-chromium battery, nickel-hydrogen battery, aqueous lithium ion battery, aqueous sodium-ion
`battery and so on. lead-acid battery has high power density, low price, but low energy density, limited cycle
`life, and leadis toxic, in the process of preparation and use will cause pollution to the environment. nickel-
`cadmium battery has higher energy density compared with the lead-acid battery, but it has serious memory
`effect, after charging and discharging several times of low capacity cannotdirectly perform the discharge of
`large quantity, therefore it is used by certain limit, besides cadmium will pollute the environment. nickel-
`hydrogen battery using hydrogen storage alloy to replace the cadmium electrode in nickel cadmium
`electrode has larger weight energy density and cycle stability, but finite reserve of hydrogen storage alloy,
`whichis not suitable for large scale energy storage. aqueous lithium ion, sodium ion battery, primarily
`dependent upon the metal cation (i.e., lithium ion, sodium ion) in the electrode material of
`intercalation/deintercalation reaction to realize the reversible charge and discharge, its working principle and
`based on anhydrous (i.e., organic) electrolyte oflithium ion battery of the same, the differenceis thatit
`adopts the more safety of the nonaqueous electrolytic solution. However, after many times of these battery
`system after intercalation/deintercalation, electrode structure is damagedso that the cycle performanceis
`bad, the servicelife of the battery is limited. more seriously, in aqueous electrolyte of proton (H +) can be
`accompaniedbylithium ion or sodium ion embeddedin the crystal structure of the electrode material,
`causing severe capacity fade, the aqueous lithium ion battery or sodium ion battery is difficult to meet the
`long service life requirement of large energy storage device. zinc metal has rich resource, low cost, high
`safety, no pollution and so on, so the new chargeable zinc ion battery is considered as an ideal green
`aqueous battery system. However, metal zinc battery of the existing report, the reaction mechanism and the
`aqueous lithium ion battery and sodium ion battery are similar, based on embeddedreaction, namely
`embedded reaction of zinc ion in the crystal structure of the electrode material. Because the far greater than
`lithium ion or sodium ion radius of the zinc ion, which is embedded/structure more easily removing process
`caused by electrode material of collapse, so aqueous zinc-ion battery often exhibits a poor cycle life.
`nearly two years, enolization reaction of organic material is applied to the lithium ion battery or sodium ion
`battery. battery system in these organic-based electrodein the organic substancein a single C=O can by
`enolization reaction (i.e. C-Li-O or C-O-Na) charge storage can be reversible. reaction of the organic matter
`and avoid the ion in the crystal structure of the electrode material of the embedding and taking, the cycle life
`tends to make the corresponding cell exhibits long. However, such enolization reaction is can be applied to
`reversible storage bivalent zinc ion, has not been reported. In this invention, wefirstly verifies C=O the zinc
`ion in the organic reversible storage, the reaction mechanism is based on two C=O groups the Zn2 + of the
`reversible storage (i.e., C-O-Zn-O-C). and based on this reaction, the invention design based on aqueous
`zinc ion battery system of organic positive electrode and the metal zinc cathode, which exhibits large energy
`storage device with high energy density, long cycle life and environment-friendly, so it is expected to be used
`in the future.
`summaryof the invention
`The purpose of the invention is to provide a long-life, aqueous zinc ion battery with high stability, high energy
`density, capable of charging and discharging is green and environment-friendly.
`the inventors found that using pyrene as the anode -4, 5, 9, 10-10-tetrone, after charge and discharge cycle
`for a long time, the structure of the electrode material does not have obvious change, so as to improve the
`cycle life of the corresponding battery.
`
`

`

`aqueous zinc ion battery capable of charging and discharging claimed by the invention adopts the pyrene -4,
`5, 9, 10, - 10-tetrone as a positive electrode active material, metal zinc as the negative electrode material,
`the battery system specifically comprises: -4, 5, 9, 10-10-tetrone zinc positive electrode, a metal negative
`electrode, and the aqueous electrolyte solution (i.e., zinc ion electrolyte) containing zinc ion. the working
`mechanism of the battery as shownin FIG. 1. when discharging, the negative electrode zinc loses electrons
`into zinc ion, zinc ion diffusion to the positive electrode, positive electrode of pyrene -4, 5, 9, 10, - 10-tetrone
`to obtain an electron generating enolization reaction storage with zinc ions, electrons flow to the positive
`electrode from the negative electrode through an externalcircuit (see FIG. 1), when charging, zinc ion
`organic diffusion from the positive electrode to the negative electrode, the negative electrode surface
`deposition, electron from the anode through an externalcircuit to negative electrode (see FIG. 1). The
`invention avoids using metal ion embeddedin the electrode material/off and lead to damage of the electrode
`material structure, so as to improve the cycle life of the battery. the battery having a long cycle life, high
`energy density, high safety and environmental protection and so on, the large energy field with wide
`application prospect.
`the electrode reaction of the battery is summarized as follows:
`positive electrode:
`
`negative electrode:
`As described above, relates to enolization reaction of reversible positive electrode reaction of the battery,
`and the negative electrode is based on the dissolved precipitation reaction of metal zinc. positive and
`negative electrode reaction are notreferring to a traditional embedded reaction so as to not generate the ion
`embedding capacity attenuation caused by reaction, exhibits long cycle life. In addition, the battery also
`exhibits characteristics of high capacity (see FIG. 2).
`In the invention, the preparation methodof the positive electrode as follows: the active material -4, 5, 9, 10-
`10-tetrone mixed with the conductive agent and the binder, by means of roller pressing into electrode film,
`finally the electrode film press-formed positive electrode on the current collector.
`In the present invention, the positive electrode film material, according to mass percentage asfollows:
`positive electrode film of active material, 60-80 % of conductive agent, 10-30 %, the rest is adhesive (e.g., 2-
`8 %), and the total amount is 100 %.
`the conductive agent can be active carbon, mesoporous carbon, graphene, carbon nanotube, carbon fiber,
`acetylene black and carbon blackin the one kind of or several kinds. binder can be polytetrafluoroethylene,
`polyvinylidene fluoride, polyolefin, polyvinyl alcohol, styrene-butadiene rubber. net-shapedcollector can be
`titanium, nickel net, copper net, stainless steel net.
`In the invention, the negative electrode can be metal zinc plate, a zinc foil, powder porous zinc electrode or
`coated/deposited on other conductive substrate of metal zinc. the metal zinc plate and a metal zinc foil can
`be directly used as negative electrode sheet, using porous powder zinc powder, the preparation method of
`the negative electrode is as follows: the powder porous zinc powder and caking agent uniformly mixing roller
`pressed into electrode film, finally pressing on the collector, the massratio of active substance in the mixture
`is 90-98 %.
`In the invention, the electrolyte is an aqueous solution containing zinc ion. the cation in the solution may also
`contain Li +, Na +, K + in the one kind of or several kinds of anion addition to Zn2 + can be sulfate (SO4-),
`nitrate (NO3 -), chloride ion (Cl -), hydroxide (OH -) in the one kind of or several kinds. zinc ion in electrolyte
`concentration may range from 0.01 mol/L -10 mol/liter. pH value of the electrolyte is 3.0-14.0.
`In the invention, the zinc ion in the electrolyte, further can be added with a volume ratio of 1 %-20 % ethanol,
`for inhibiting the growth of zinc dendrite.
`battery capacity of aqueous zinc-ion battery of this invention, based on the amount of positive electrode
`active material calculated up to more than 350 mAhg-1, the current density is 0.1A g-1 cycle after 2000
`circles, the capacity retention rate is more than 80%.
`Description
`FIG.
`1 based on pyrene -4, 5, 9, 10, - 10-tetrone positive electrode and the metal zinc cathode of aqueous
`zinc ion battery charging and discharging the working schematic diagram.
`FIG. 2 based on the charge and discharge curve graph of pyrene -4, 5, 9, 10, - 10-tetrone positive electrode
`and the metal zinc cathode aqueous zinc ion battery.
`
`

`

`Specific implementation methods
`the following can be further explained by the embodiment of the present invention.
`Example 1: positive electrode using carbon nanotubeis used aselectric conductive agent. preparation of
`positive electrode film is as follows: The active material (-4, 5, 9, 10, - 10-tetrone): conductive agent (carbon
`nanotube) binder (polytetrafluoroethylene) =60: ratio of 30:10, the mixedslurry on the roller pressrolling into
`film of uniform thickness, after drying, cutting into 1cm * 1 cm of size, the loading amount of pyrene-10-
`tetrone -4, 5, 9, 10 is 5 mg cm-2, then the positive electrode film uniformly pressed on the titanium net, out to
`form positive electrode electrode to nickel wire. cathode with zinc foil, cut into the size of 1 cm * 1 cm, nickel
`wire led out form the cathodeelectrode. the electrolyte is 1 M Zn2SO4solution as to form into aqueous zinc
`ion battery. the assembled aqueous zinc ion battery carry out charge-discharge test on the electrochemical
`workstation (PARSTAT). charging and discharging curve shownin FIG. 1, the working section of the cell is
`1-1.7 V, current density of the cell to 0.05A g-1 (amount calculated based on the anode active substance) of
`the charging and discharging capacity of the battery calculated based on the anode active substance in an
`amount of up to 398 mAh g-1, the current density is 0.1A g-1 cycle after 2000 circles, the capacity retention
`rate is 87% (see FIG. 2 and Table 1).
`Example 2: positive electrode made of active carbon is used as electric conductive agent. preparation of
`positive electrode film is as follows: The active material (-4, 5, 9, 10, - 10-tetrone): conductive agent (active
`carbon), binder (polytetrafluoroethylene) =60: 30:10 proportion, the mixed slurry on the roller pressrolling
`into film of uniform thickness, after drying, cutting into 1cm * 1 cm of size, the loading amount of pyrene-10-
`tetrone -4, 5, 9, 10 is 5 mg cm-2, then the positive electrode film uniformly pressed on the titanium net, out to
`form positive electrode electrode to nickel wire. cathode with zinc foil, cut into the size of 1 cm * 1 cm, nickel
`wire led out form the cathodeelectrode. the electrolyte is 1 M Zn2SO4solution as to form into aqueous zinc
`ion battery. the assembled aqueous zinc ion battery carry out charge-discharge test on the electrochemical
`workstation (PARSTAT). the working area of the battery is 1-1.7 V, current density of the cell to 0.05A g-1
`(based on the amountof positive electrode active material basis) of charging and discharging of the battery
`capacity calculated based on the anode active substance in an amount of up to 352 mAh g-1, the current
`density is 0.1A g-1 cycle, the capacity retention rate after 2000 rings up to 80%(see Table 1).
`Example 3: positive electrode adopting ordered mesoporous carbon (CMK-3) as conductive agent.
`preparation of positive electrode film is as follows: The active material (-4, 5, 9, 10, - 10-tetrone): conductive
`agent (CMK-3): a binder (polytetrafluoroethylene) =60: 30:10 proportion, the mixed slurry on the roller press
`rolling into film of uniform thickness, after drying, cutting into 1cm * 1 cm of size, the loading amount of
`pyrene-10-tetrone -4, 5, 9, 10 is 5 mg cm-2, then the positive electrode film uniformly pressed on the titanium
`net, out to form positive electrode electrode to nickel wire. cathode with zinc foil, cut into the size of 1 cm * 1
`cm, nickel wire led out form the cathode electrode. the electrolyte is 1 M Zn2S04solution as to form into
`aqueous zinc ion battery. the assembled aqueous zinc ion battery carry out charge-discharge test on the
`electrochemical workstation (PARSTAT). the working area of the battery is 1-1.7 V, current density of the cell
`to 0.05A g-1 (based on the amount of positive electrode active material basis) of charging and discharging of
`the battery capacity calculated based on the anode active substance in an amountof up to 367 mAhg-1, the
`current density is 0.1A g-1 cycle, the capacity retention rate after 2000 rings up to 82%(see Table 1).
`Example 4: positive electrode using carbon nanotube as a conductive agent, a negative electrode using
`powder porous zinc powder as the active material. preparation of positive electrode film is as follows: The
`active material (-4, 5, 9, 10, - 10-tetrone): conductive agent (carbon nanotube) binder
`(polytetrafluoroethylene) =60: ratio of 30:10, the mixed slurry on the roller pressrolling into film of uniform
`thickness, after drying, cutting into 1cm * 1cm of size, the loading amount of pyrene-10-tetrone -4, 5, 9, 10 is
`5 mg cm-2, then the positive electrode film uniformly pressed on the titanium net, out to form positive
`electrode electrode to nickel wire. preparation of negative electrode film is as follows: The powder porous
`zinc powder, the proportion of binder (polytetrafluoroethylene) = 95:5 mixed, the mixedslurryis rolling into
`film of uniform thicknesson the roller press, dried, cut into 1 cm * 1 cm size, the loading amount of the zinc
`powder is 25 mg cm-2, then the negative electrode film uniformly pressed on the titanium net, nickel wire led
`out to form the cathode electrode. the electrolyte is 1 M Zn2S04solution as to form into aqueouszinc ion
`battery. the assembled aqueous zinc ion battery carry out charge-discharge test on the electrochemical
`workstation (PARSTAT). the working area of the battery is 1-1.7 V, current density of the cell to 0.05A g-1
`(amount calculated based on the anode active substance) of the charging and discharging of the battery
`
`

`

`capacity calculated based on the anode active substance in an amount of up to 384mAhg-1, the current
`density is 0.1A g-1 cycle, the capacity retention rate after 2000 rings up to 81%(see Table 1).
`Example 5: positive electrode using carbon nanotubeis used aselectric conductive agent. preparation of
`positive electrode film is as follows: The active material (-4, 5, 9, 10, - 10-tetrone): conductive agent (carbon
`nanotube) binder (polytetrafluoroethylene) =60: ratio of 30:10, the mixedslurry on the roller pressrolling into
`film of uniform thickness, after drying, cutting into 1cm * 1 cm of size, the loading amount of pyrene-10-
`tetrone -4, 5, 9, 10 is 5 mg cm-2, then the positive electrode film uniformly pressed on the titanium net, out to
`form positive electrode electrode to nickel wire. cathode with zinc foil, cut into the size of 1 cm * 1 cm, nickel
`wire led out form the cathodeelectrode. the electrolyte is 1 M Zn2SO04 + 1 M Na2S0O4solution as to form
`into aqueous zinc ion battery. the assembled aqueous zinc ion battery carry out charge-discharge test on the
`electrochemical workstation (PARSTAT). the working area of the battery is 1-1.7 V, current density of the cell
`to 0.05A g-1 (based on the amount of positive electrode active material basis) of charging and discharging of
`the battery capacity calculated based on the anode active substance in an amount of up to 390 mAhg-1, the
`current density is 0.1A g-1 cycle, the capacity retention rate after 2000 rings up to 84%(see Table 1).
`Example 6: positive electrode using carbon nanotubeis used aselectric conductive agent. preparation of
`positive electrode film is as follows: The active material (-4, 5, 9, 10, - 10-tetrone): conductive agent (carbon
`nanotube) binder (polytetrafluoroethylene) =60: ratio of 30:10, the mixedslurry on the roller pressrolling into
`film of uniform thickness, after drying, cutting into 1cm * 1 cm of size, the loading amount of pyrene-10-
`tetrone -4, 5, 9, 10 is 5 mg cm-2, then the positive electrode film uniformly pressed on the titanium net, out to
`form positive electrode electrode to nickel wire. cathode with zinc foil, cut into the size of 1 cm * 1 cm, nickel
`wire led out form the cathodeelectrode. the electrolyte is 1 M Zn2SO04 + 1 M Li2SO4 solution as to form into
`aqueous zinc ion battery. the assembled aqueous zinc ion battery carry out charge-discharge test on the
`electrochemical workstation (PARSTAT). the working area of the battery is 1-1.7 V, current density of the cell
`to 0.05A g-1 (based on the amount of positive electrode active material basis) of charging and discharging of
`the battery capacity calculated based on the anode active substance in an amount of up to 386 mAhg-1, the
`current density is 0.1A g-1 cycle, the capacity retention rate after 2000 rings up to 85%(see Table 1).
`Example 7: positive electrode using carbon nanotubeis used aselectric conductive agent. preparation of
`positive electrode film is as follows: The active material (-4, 5, 9, 10, - 10-tetrone): conductive agent (carbon
`nanotube) binder (polytetrafluoroethylene) =60: ratio of 30:10, the mixedslurry on the roller pressrolling into
`film of uniform thickness, after drying, cutting into 1cm * 1 cm of size, the loading amount of pyrene-10-
`tetrone -4, 5, 9, 10 is 5 mg cm-2, then the positive electrode film uniformly pressed on the titanium net, out to
`form positive electrode electrode to nickel wire. cathode with zinc foil, cut into the size of 1 cm * 1 cm, nickel
`wire led out form the cathodeelectrode. the electrolyte is 1 M Zn2SO04 + 0.1 M C2H5OH solution as to form
`into aqueous zinc ion battery. the assembled aqueous zinc ion battery carry out charge-discharge test on the
`electrochemical workstation (PARSTAT). the working area of the battery is 1-1.7 V, current density of the cell
`to 0.05A g-1 (based on the amount of positive electrode active material basis) of charging and discharging of
`the battery capacity calculated based on the anode active substance in an amount of up to 400 mAhg-1, the
`current density is 0.1A g-1 cycle, the capacity retention rate after 2000 rings up to 90%(see Table 1).
`
`Claims
`
`1. An aqueous zinc-ion battery, wherein, -4, 5, 9, 10, - 10-tetrone as positive electrode active material, the
`metal zinc as the negative electrode material, the electrolyte is zinc ion electrolyte.
`2. The aqueous zinc ion battery according to claim 1, wherein, the anode comprises active material -4, 5, 9,
`10-tetrone, conductive additive and binder, pyrene -4, 5, 9, 10-tetrone and the conductive agent and binder
`are mixed, by means of a roller press to prepare an electrode film, the electrode film pressure on the current
`collector to obtain a positive electrode.
`3. The aqueous zinc ion battery according to claim 2, wherein the positive electrode film materials, based on
`weight percent, are as follows: anodefilm of active material, 60-80 %of conductive agent, 10-30 %, the rest
`is caking agent, the total weight is 100 %.
`4. The aqueous zinc ion battery according to claim 2, wherein said conductive additive is activated carbon,
`
`

`

`mesoporous carbon, graphite, carbon nanometer tube, carbon fiber, acetylene black and carbon black in one
`or more of the binder is one of polyfluortetraethylene, polyvinylidene fluoride, polyolefin, polyvinyl alcohol,
`styrene-butadiene rubber.
`5. The aqueous zinc ion battery according to claim 1, wherein, the said negative electrode is metal zinc
`plate, a zinc foil, powder porous zinc electrode or coated/deposited metal zinc on the other conductive
`substrate.
`6. The aqueous zinc-ion battery according to claim 5, wherein the metal zinc plate and a metal zinc foil as
`cathode sheetdirectly, using porous powder zinc powder, zinc powder and the powder porous binder
`uniformly mixed roller pressure preparation to obtain negative electrode on the current collector, wherein the
`mass ratio of active material is 90-98 %.
`7. The aqueous zinc-ion battery according to claim 6, wherein the zinc ion in the electrolyte, cation except
`Zn2 +, it also can include Li +, Na +, K + in the one kind of or several kinds of anion is sulphate (SO42-),
`nitrate (NO3 -), chloride ion (Cl -), hydroxide (OH -) in the one kind of or several kinds.
`8. The aqueous zinc ion battery according to claim 7, wherein the concentration of the zinc ion in the
`electrolyte, containing zinc ion is 0.01/L to -10/L.
`9. The aqueous zinc-ion battery according to claim 1, wherein the zinc ion in the electrolyte is further added
`with a volume ratio of 1 %-20 %ethanol.
`
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`

`

`
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