J. Semicond. > 2021, Volume 42 > Issue 10 > 101603, doi: 10.1088/1674-4926/42/10/101603
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REVIEWS

Recently advances in flexible zinc ion batteries

Chuan Li1, Pei Li1, Shuo Yang1 and Chunyi Zhi1, 2,

+ Author Affiliations

 Corresponding author: Chunyi Zhi, cy.zhi@cityu.edu.hk

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Abstract: Flexible batteries are key component of wearable electronic devices. Based on the requirements of medical and primary safety of wearable energy storage devices, rechargeable aqueous zinc ion batteries (ZIBs) are promising portable candidates in virtue of its intrinsic safety, abundant storage and low cost. However, many inherent challenges have greatly hindered the development in flexible Zn-based energy storage devices, such as rigid current collector and/or metal anode, easily detached cathode materials and a relatively narrow voltage window of flexible electrolyte. Thus, overcoming these challenges and further developing flexible ZIBs are inevitable and imperative. This review summarizes the most advanced progress in designs and discusses of flexible electrode, electrolyte and the practical application of flexible ZIBs in different environments. We also exhibit the heart of the matter that current flexible ZIBs faces. Finally, some prospective approaches are proposed to address these key issues and point out the direction for the future development of flexible ZIBs.

Key words: flexible electrodes, flexible electrolytes, wearable zinc batteries



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Fig. 1.  (a) SEM image of the zinc anode by electrically depositing onto a carbon cloth. Adopted with permission from Ref. [18], Copyright 2019, Royal Society of Chemistry. (b) SEM image and the photographs (the inset) of the MnO2/rGO sample on carbon cloth. Adopted with permission from Ref. [19], Copyright 2018, Nature Publishing Group.

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Fig. 2.  (Color online) (a) The process diagram of SA-based hydrogel electrolyte. Adopted with permission from Ref. [22], Copyright 2020, Elsevier. (b) The schematic diagram of PAM-based hydrogel. Adopted with permission from Ref. [23], Copyright 2018, American Chemical Society. (c) The structure diagram of fabricating PVA-based self-healing electrolyte. Adopted with permission from Ref. [24], Copyright 2019, Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

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Fig. 3.  (Color online) (a) The schematic process of design and (b) the cycle performance of ultrathin all-in-one ZIBs. Adopted with permission from Ref. [25], Copyright 2021, John Wiley & Sons. (c) Schematic illustration of fabrication procedures and (d) cycle performance of in-plane batteries. Adopted with permission from Ref. [26], Copyright 2020, Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

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Fig. 4.  (Color online) (a) Illustrations of the Zn-MnO2 battery i) being placed under foot and ii) going through car run-over. (b) Discharge curve of the battery after 2 days' everyday treading. (c) Discharge curve of the battery after 20 times of random run-over by cars on road. All the discharge curves were recorded at 0.924 A/g (3C rate). Adopted with permission from Ref. [28], Copyright 2019, Elsevier. (d) Schematics of the evolution of the Zn-reinforced SA-PAM SE hydrogel structure. (e) Tensile strength of the Zn-reinforced SA-PAM SE. (f) Capacity loss per cycle of all kinds of flexible ZIBs. Adopted with permission from Ref. [29], Copyright 2020, American Chemical Society. Optical images of a “ZIBs” LED powered by four all-in-one ZIBs in series (g) without bending and (h) under bending. (i) Cycling performance of the all-in-one and stacked ZIBs at 0.5 A/g under flat and different bending states. Adopted with permission from Ref. [30], Copyright 2019, Royal Society of Chemistry. (j) The flexible ZIB is subjected to fold deformation. (k) Galvanostatic charge/discharge curves of the ZIB cell under different mechanical deformations. Adopted with permission from Ref. [31], Copyright 2021, Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

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Fig. 5.  (Color online) (a) Cycling performance of the obtained flexible Zn-MnO2 battery before healing and after fourth healing. (b) Demonstration of a self-healing flexible Zn-MnO2 battery powering an electric watch before and after cutting and after healing. Adopted with permission from Ref. [32], Copyright 2019, American Chemical Society. (c) Charging and discharging profiles of alkaline flexible NiCo-Zn batteries before and after multiple cutting/healing cycles. (d) Healing efficiency calculated from (c). (e) Demonstration of a self-healing flexible NiCo-Zn battery powering an electric watch before and after cutting and after healing. Adopted with permission from Ref. [33], Copyright 2018, Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim. (f) Demonstration of hydrogel electrolytes and the battery using all-in-one electrodes after each time of the self-healing process. Adopted with permission from Ref. [34], Copyright 2021, Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

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Fig. 6.  (Color online) (a) The demonstration of AF-battery powered a series of electronic devices. Adopted with permission from Ref. [18], Copyright 2019, Royal Society of Chemistry. (b) The schematic diagram of anti-freezing gel electrolyte based on PAM/EG gel electrolyte. Adopted with permission from Ref. [35], Copyright 2020, Frontiers Media S.A. (c) The voltage curves of Zn plating-stripping in ZL-PAAm under different temperatures. Adopted with permission from Ref. [36], Copyright 2020, Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

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Fig. 7.  (Color online) (a) The process of the smart reaction of flexible ZIBs when temperature changes. Adopted with permission from Ref. [37], Copyright 2018, Science China Press. (b) The schematic diagram of smart rection. Adopted with permission from Ref. [38], Copyright 2020, John Wiley & Sons. (c) The demonstration of practical submarine-use of flexible ZIBs assembled by XG-PAM/CNF hydrogel electrolyte. Adopted with permission from Ref. [39], Copyright 2020, American Chemical Society. (d) Ion conductivity of zwitterionic sulfobetaine/cellulose semi-interpenetrating networks gel (ZSC-gel). Adopted with permission from Ref. [40], Copyright 2020, Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

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Table 1.   The performance comparison of flexible ZIBs using in different situations.

FunctionCathode materialFlexible electrolytePlateau (V)Capacity (mA·h/g)CycleRef.
Mechanical propertiesα-MnO2PAAm1.35/1.1594 (4 C)1000[27]
α-MnO2Zn-alginate/PAAm1.35/1.15144.5 (0.88 A/g)500[28]
Na0.5FeFe(CN)6Zn-alginate/PAAm1.1/1.050 (20 C)10 000[29]
rGO/PANICellulose nanofiber1.0~ 100 (1 A/g)500[30]
MnO2/graphene–1.35/1.15~ 125 (2 A/g)2000[31]
Self-repairabilityδ-MnO2CPU1.35/1.15106 (20 C)10 000[32]
NiCoPANa-Fe3+1.55225 (24 C)–[33]
VS2PVA0.7/0.6~ 135 (0.2 A/g)40[34]
Low temperature resistanceα-MnO2EG-waPUA/PAM1.35/1.15~ 75 (2.4 A/g, –20 °C)600[18]
α-MnO2PAM/GO/EG1.35/1.15~ 90 (1 A/g, –20 °C)1000[35]
LiFePO4ZL-PAAm1.13~ 40 (0.5 A/g, –20 °C)500[36]
OthersSmart reactionα-MnO2PNA1.35/1.15104 (0.5 A/g)550[37]
PANIPNIPAM/AM1.0 (25°)~ 125 (1 A/g)1000[38]
Submarine-useα-MnO2XG−PAM/CNF1.35/1.15~ 147 (4 C)1000[39]
Ion-conductivityα-MnO2ZSC-gel1.35/1.1574 (30 C)10 000[40]
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[1]
Cai Y C, Shen J, Yang C W, et al. Mixed-dimensional MXene-hydrogel heterostructures for electronic skin sensors with ultrabroad working range. Sci Adv, 2020, 6, eabb5367 doi: 10.1126/sciadv.abb5367
[2]
Wang Z, Fu D M, Xie D Z, et al. Magnetic helical hydrogel motor for directing T cell chemotaxis. Adv Funct Mater, 2021, 31, 2101648 doi: 10.1002/adfm.202101648
[3]
Rodriguez R D, Shchadenko S, Murastov G, et al. Ultra-robust flexible electronics by laser-driven polymer-nanomaterials integration. Adv Funct Mater, 2021, 31, 2008818 doi: 10.1002/adfm.202008818
[4]
Wu K, Huang J H, Yi J, et al. Recent advances in polymer electrolytes for zinc ion batteries: Mechanisms, properties, and perspectives. Adv Energy Mater, 2020, 10, 1903977 doi: 10.1002/aenm.201903977
[5]
Yu P, Zeng Y X, Zhang H Z, et al. Flexible Zn-ion batteries: Recent progresses and challenges. Small, 2019, 15, 1804760 doi: 10.1002/smll.201804760
[6]
Yang Q, Wang Y K, Li X L, et al. Recent progress of MXene-based nanomaterials in flexible energy storage and electronic devices. Energy Environ Mater, 2018, 1, 183 doi: 10.1002/eem2.12023
[7]
Song Z S, Ding J, Liu B, et al. A rechargeable Zn-air battery with high energy efficiency and long life enabled by a highly water-retentive gel electrolyte with reaction modifier. Adv Mater, 2020, 32, 1908127 doi: 10.1002/adma.201908127
[8]
Mo F N, Li Q, Liang G J, et al. A self-healing crease-free supramolecular all-polymer supercapacitor. Adv Sci, 2021, 8, 2100072 doi: 10.1002/advs.202100072
[9]
Wang D H, Sun J F, Xue Q, et al. A universal method towards conductive textile for flexible batteries with superior softness. Energy Storage Mater, 2021, 36, 272 doi: 10.1016/j.ensm.2021.01.001
[10]
Xu Y T, Zhu J J, Feng J Z, et al. A rechargeable aqueous zinc/sodium manganese oxides battery with robust performance enabled by Na2SO4 electrolyte additive. Energy Storage Mater, 2021, 38, 299 doi: 10.1016/j.ensm.2021.03.019
[11]
Yang Q, Guo Y, Yan B X, et al. Hydrogen-substituted graphdiyne ion tunnels directing concentration redistribution for commercial-grade dendrite-free zinc anodes. Adv Mater, 2020, 32, 2001755 doi: 10.1002/adma.202001755
[12]
Yi Z H, Chen G Y, Hou F, et al. Strategies for the stabilization of Zn metal anodes for Zn-ion batteries. Adv Energy Mater, 2021, 11, 2003065 doi: 10.1002/aenm.202003065
[13]
Chen P H, Zhou W Y, Xiao Z J, et al. An integrated configuration with robust interfacial contact for durable and flexible zinc ion batteries. Nano Energy, 2020, 74, 104905 doi: 10.1016/j.nanoen.2020.104905
[14]
Wang F, Borodin O, Gao T, et al. Highly reversible zinc metal anode for aqueous batteries. Nat Mater, 2018, 17, 543 doi: 10.1038/s41563-018-0063-z
[15]
Guo Z W, Ma Y Y, Dong X L, et al. An environmentally friendly and flexible aqueous zinc battery using an organic cathode. Angew Chem Int Ed, 2018, 57, 11737 doi: 10.1002/anie.201807121
[16]
Wan F, Zhang L L, Dai X, et al. Aqueous rechargeable zinc/sodium vanadate batteries with enhanced performance from simultaneous insertion of dual carriers. Nat Commun, 2018, 9, 1656 doi: 10.1038/s41467-018-04060-8
[17]
Tan P, Chen B, Xu H R, et al. Flexible Zn– and Li–air batteries: Recent advances, challenges, and future perspectives. Energy Environ Sci, 2017, 10, 2056 doi: 10.1039/C7EE01913K
[18]
Mo F N, Liang G J, Meng Q Q, et al. A flexible rechargeable aqueous zinc manganese-dioxide battery working at –20 °C. Energy Environ Sci, 2019, 12, 706 doi: 10.1039/C8EE02892C
[19]
Huang Y, Liu J W, Huang Q Y, et al. Flexible high energy density zinc-ion batteries enabled by binder-free MnO2/reduced graphene oxide electrode. npj Flex Electron, 2018, 2, 21 doi: 10.1038/s41528-018-0034-0
[20]
Li H F, Han C P, Huang Y, et al. An extremely safe and wearable solid-state zinc ion battery based on a hierarchical structured polymer electrolyte. Energy Environ Sci, 2018, 11, 941 doi: 10.1039/C7EE03232C
[21]
Wang D H, Li H F, Liu Z X, et al. A nanofibrillated cellulose/polyacrylamide electrolyte-based flexible and sewable high-performance Zn-MnO2 battery with superior shear resistance. Small, 2018, 14, 1803978 doi: 10.1002/smll.201803978
[22]
Tang Y, Liu C X, Zhu H R, et al. Ion-confinement effect enabled by gel electrolyte for highly reversible dendrite-free zinc metal anode. Energy Storage Mater, 2020, 27, 109 doi: 10.1016/j.ensm.2020.01.023
[23]
Li H F, Liu Z X, Liang G J, et al. Waterproof and tailorable elastic rechargeable yarn zinc ion batteries by a cross-linked polyacrylamide electrolyte. ACS Nano, 2018, 12, 3140 doi: 10.1021/acsnano.7b09003
[24]
Huang S, Wan F, Bi S S, et al. A self-healing integrated all-in-one zinc-ion battery. Angew Chem Int Ed, 2019, 58, 4313 doi: 10.1002/anie.201814653
[25]
Yao M J, Yuan Z S, Li S S, et al. Scalable assembly of flexible ultrathin all-in-one zinc-ion batteries with highly stretchable, editable, and customizable functions. Adv Mater, 2021, 33, 2008140 doi: 10.1002/adma.202008140
[26]
Ma L T, Chen S M, Li X L, et al. Liquid-free all-solid-state zinc batteries and encapsulation-free flexible batteries enabled by in situ constructed polymer electrolyte. Angew Chem, 2020, 132, 24044 doi: 10.1002/ange.202011788
[27]
Wang Z F, Mo F N, Ma L T, et al. Highly compressible cross-linked polyacrylamide hydrogel-enabled compressible Zn-MnO2 battery and a flexible battery–sensor system. ACS Appl Mater Interfaces, 2018, 10, 44527 doi: 10.1021/acsami.8b17607
[28]
Liu Z X, Wang D H, Tang Z J, et al. A mechanically durable and device-level tough Zn-MnO2 battery with high flexibility. Energy Storage Mater, 2019, 23, 636 doi: 10.1016/j.ensm.2019.03.007
[29]
Huang J, Chi X, Yang J, et al. An ultrastable Na-Zn solid-state hybrid battery enabled by a robust dual-cross-linked polymer electrolyte. ACS Appl Mater Interfaces, 2020, 12, 17583 doi: 10.1021/acsami.0c01990
[30]
Zhang Y, Wang Q R, Bi S S, et al. Flexible all-in-one zinc-ion batteries. Nanoscale, 2019, 11, 17630 doi: 10.1039/C9NR06476A
[31]
Wang J J, Wang J G, Liu H Y, et al. A highly flexible and lightweight MnO2/graphene membrane for superior zinc-ion batteries. Adv Funct Mater, 2021, 31, 2007397 doi: 10.1002/adfm.202007397
[32]
Wang D, Wang L, Liang G, et al. A superior δ-MnO2 cathode and a self-healing Zn-δ-MnO2 battery. ACS Nano, 2019, 13, 10643 doi: 10.1021/acsnano.9b04916
[33]
Huang Y, Liu J, Wang J Q, et al. An intrinsically self-healing NiCo||Zn rechargeable battery with a self-healable ferric-ion-crosslinking sodium polyacrylate hydrogel electrolyte. Angew Chem Int Ed, 2018, 57, 9810 doi: 10.1002/anie.201805618
[34]
Liu J Y, Long J W, Shen Z H, et al. A self-healing flexible quasi-solid zinc-ion battery using all-in-one electrodes. Adv Sci, 2021, 8, 2004689 doi: 10.1002/advs.202004689
[35]
Quan Y, Chen M, Zhou W, et al. High-performance anti-freezing flexible Zn-MnO2 battery based on polyacrylamide/graphene oxide/ethylene glycol gel electrolyte. Front Chem, 2020, 8, 603 doi: 10.3389/fchem.2020.00603
[36]
Zhu M S, Wang X J, Tang H M, et al. Antifreezing hydrogel with high zinc reversibility for flexible and durable aqueous batteries by cooperative hydrated cations. Adv Funct Mater, 2020, 30, 1907218 doi: 10.1002/adfm.201907218
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    Received: 30 June 2021 Revised: 30 July 2021 Online: Accepted Manuscript: 25 August 2021Uncorrected proof: 27 August 2021Published: 15 October 2021

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      Article Navigation >  Journal of Semiconductors  > 2021  >  42(10): 101603
      Chuan Li, Pei Li, Shuo Yang, Chunyi Zhi. Recently advances in flexible zinc ion batteries[J]. Journal of Semiconductors, 2021, 42(10): 101603. doi: 10.1088/1674-4926/42/10/101603 C Li, P Li, S Yang, C Y Zhi, Recently advances in flexible zinc ion batteries[J]. J. Semicond., 2021, 42(10): 101603. doi: 10.1088/1674-4926/42/10/101603.Export: BibTex EndNote
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      Chuan Li, Pei Li, Shuo Yang, Chunyi Zhi. Recently advances in flexible zinc ion batteries[J]. Journal of Semiconductors, 2021, 42(10): 101603. doi: 10.1088/1674-4926/42/10/101603

      C Li, P Li, S Yang, C Y Zhi, Recently advances in flexible zinc ion batteries[J]. J. Semicond., 2021, 42(10): 101603. doi: 10.1088/1674-4926/42/10/101603.
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      Recently advances in flexible zinc ion batteries

      doi: 10.1088/1674-4926/42/10/101603
      • 1.

        Department of Materials Science and Engineering, City University of Hong Kong, Hong Kong 999077, China

      • 2.

        Center for Advanced Nuclear Safety and Sustainable Development, City University of Hong Kong, Hong Kong 999077, China

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      • Author Bio:

        Chuan Li got his B.S. degree from Tiangong University in 2015 and master degree from Tianjin University in 2018. Now, he is a PhD student at City University of Hong Kong under the supervision of Prof. Chunyi Zhi. His research focuses on flexible hydrogel electrolytes for all kinds of aqueous metal ion batteries

        Chunyi Zhi obtained Ph.D. degree in condensed matter physics from Institute of Physics, Chinese Academy of Sciences. After two years’ postdoc in National Institute for Materials Science (NIMS) in Japan, he was promoted to be a ICYS researcher, researcher (faculty) and senior researcher (permanent position) in NIMS. Dr. Zhi is now a professor in MSE, CityU. Dr. Zhi has extensive experiences in flexible energy storage, aqueous electrolyte batteries and zinc ion batteries. Dr. Zhi is Clarivate Analytics Global highly cited researcher (2019, 2020, Materials Science), RSC fellow and member of The Hong Kong Young Academy of Sciences

      • Corresponding author: cy.zhi@cityu.edu.hk
      • Received Date: 2021-06-30
      • Revised Date: 2021-07-30
      • Published Date: 2021-10-10

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