Rechargeable solid-state lithium-based batteries enabled by hybrid solid electrolyte and multi-functional cathode

다국어 초록 (Multilingual Abstract)

Hybrid solid electrolyte (HSE) is a potential candidate in lithium secondary batteries to replace the traditional liquid electrolyte with the superiority of solid state. Poly(vinyl alcohol) (PVA) emerges as a suitable host polymer for solid-state electrolyte membranes, owing to its exceptional attributes, including a high dielectric constant, favorable mechanical properties, and cost-effectiveness. In this study, PVA is utilized for ion-conduction material in cooperation with ionic liquid (IL) and inorganic filler to be applied as a solid-state electrolyte in lithium batteries.
This work proposes innovative designs for high-performance solid-state lithium secondary batteries, specifically focusing on lithium-ion and lithium-sulfur battery systems. First, a high-voltage stable lithium-ion battery system is introduced, incorporating a HSE composed of poly(vinyl alcohol)-g-pyrrole-2-carboxylic acid (PVA-g-PCA), pyrrolidinium-bases IL and pyrrole-2-carboxylic acid modified hydrotalcite (HTpca) nano-conductor, along with an Al2O3 coated LiCoO2 active material. The HSE exhibits outstanding Li+ conductivity, transference number, and stability, resulting in solid-state lithium batteries with high specific capacity and long-term cycling stability.
Secondly, a solid-state lithium-sulfur battery system is presented, combining a multi-functional cathode with sulfur-loaded Al2O3-modified carbon nanotubes (S@ACNTs) and a flexible HSE. Combined with polycation poly(diallyldimethylammonium bis(trifluoromethylsulfonyl)imide) (PDATFSI) binder possessed excellent Li+ conductivity, thermal stability, adhesion strength, non-flammability, and flexibility, the battery system exhibits effective polysulfide trapping behavior, resulting in high discharge capacity and long-term stability.
Thirdly, an advanced model for a high-performance solid-state lithium-sulfur battery is proposed, incorporating a force-bearing cathode with sulfur-loaded carboxylated-carbon nanotube (S@CNT-COOH) and an ionic liquid encapsulated 5-sulfoisophthalic acid monolithium-anchored poly(vinyl alcohol) (IL@PVA-SPALi) conductive binder. The system includes a multifunctional double-layer hybrid solid electrolyte (DLHSE) for effective polysulfide-blocking and lithium dendrite suppression. The LiSB assembled with this design exhibits high specific discharge capacity and long-term cyclic stability.
The research concludes by applying the proposed model to a solid-state Zn-S battery, reflecting superior electrochemical properties compared to systems using aqueous electrolytes. The positive results suggest the potential application of the developed model to other metal-sulfur battery systems in the future.

목차 (Table of Contents)

• Chapter 1. Introduction 1
• 1. Lithium batteries 1
• 1.1. Overview of lithium batteries 1
• 1.2. Operation of lithium batteries 3
• 2. Materials for lithium batteries 5
• 3. Solid-state electrolyte membrane 9
• 3.1. Poly (vinyl alcohol) - based electrolyte membrane 10
• 3.2. Ionic liquid 12
• 4. Motivation and outline of this research 14
• Chapter 2. Application of nano-conductor imbedded flexible poly(vinyl alcohol)-based hybrid solid electrolyte for high voltage stable solid-state lithium batteries 16
• 1. Introduction 16
• 2. Experimental section 21
• 2.1. Materials 21
• 2.2. Synthesized process and preparation of HSEs and cathode materials 21
• 2.3. Materials characterization 22
• 2.4. Electrochemical property measurements 25
• 3. Results and Discussion 26
• 3.1. Morphology of HSE and Li-ion transporting evaluation 26
• 3.2. Mechanical, adhesive, and thermal properties of HSE 34
• 3.3. Interfacial resistances and electrochemical window of HSE 39
• 3.4. Electrochemical investigation of LCO(ALCO)/HSE
• HSE
• Li cells 43
• Chapter 3. Application of multi-functional cathode and flexible poly(vinyl alcohol)-based hybrid solid electrolyte for high performance solid-state lithium-sulfur batteries 46
• 1. Introduction 46
• 2. Experimental section 50
• 2.1. Materials 50
• 2.2. Synthesis of S@ACNT active material and PDATFSI conductive binder 50
• 2.3. Synthesis of PVA–g–PCA−80IL−5HTpca HSE 51
• 2.4. Materials Characterization 51
• 2.5. Electrochemical measurements 52
• 3. Results and Discussion 53
• 3.1. Morphologies and characterizations of S@ACNTs active material and PDATFSI conductive binder 53
• 3.2. Electrochemical performance of the solid-state lithium–sulfur battery 63
• Chapter 4. Application of the force-bearing cathode and multifunctional double-layer hybrid solid electrolyte for high energy and sustainable solid-state lithium-sulfur battery 67
• 1. Introduction 67
• 2. Experimental section 70
• 2.1. Materials 70
• 2.2. Fabrication of DLHSE 70
• 2.3. Fabrication of sulfur cathode 71
• 2.4. Materials Characterization 72
• 2.5. Electrochemical measurements 73
• 3. Results and Discussion 74
• 3.1. Characterization of S@CNT-COOH and PVA-SPALi 74
• 3.2. Structural characterizations and multifunctional properties of DLHSE 80
• 3.3. Compatibility of DLHSE with electrode 95
• 3.4. Electrochemical performance of solid-state LiSB 99
• Chapter 5. Future work – applied potential of multifunctional hybrid solid electrolyte in various solid-state metal-sulfur systems 103
• 1. Introduction 103
• 2. Experimental section 104
• 2.1. Materials 104
• 2.2. Fabrication of DLHSE and sulfur cathode 105
• 2.3. Electrochemical measurements 105
• 3. Results and Discussion 106
• Chapter 6. Conclusions 111
• References 114
• 논문요약 135

참고문헌 (Reference)

1. progress and prospects, S. H. Chung, Lithium–sulfur, C. Zu, A. Manthiram, 27(12) 19802006, , 2015

2. Building better batteries,, M. Armand, J.-M. Tarascon, 451 652657, , 2008

3. History of lithium batteries, Scrosati, B., 15(7):162330, , 2011

4. Ionic liquid polymer electrolytes, Hwang BJ, Ye YS, Rick J, 1(8):271943, , 2013

5. An advanced lithium‐sulfur battery, B. Scrosati, H. G. Jung, D. J. Lee, J. Hassoun, J. Kim, Y. K. Sun, 23(8) 10761080, , 2013

6. Rechargeable lithium–sulfur batteries, A. Manthiram, S.H. Chung, Y.S. Su, Y. Fu, C. Zu, 114 1175111787, , 2014

7. Xray diffraction and the Bragg equation, C. G. Pope, 74 129, , 1997

8. challenges for rechargeable Li batteries, Y. Kim, J. B. Goodenough, 22 587603, , 2010

9. Carbon nanotubes for lithium ion batteries, DiLeo RA, Landi BJ, Raffaelle RP, Ganter MJ, Cress CD, 2(6):63854, , 2009

10. Interfaces in solidstate lithium batteries, C. Liu, L. Mai, Y.C. Cao, Y. Cheng, S. Tang, L. Xu, K. Wang, J. Liang, F. Wei, 2 19912015, , 2018

11. Li-ion battery materialspresent and future, J. T. Lee, N. Nitta, G. Yushin, F. Wu, 18 252264, , 2015

12. Lithium batteries: To the limits of lithium, E. C. Evarts, 5267575 S93S95, , 2015

13. A solid sulfur cathode for aqueous batteries, Peramunage, D., Licht, S., 261 (5124), 1029−1032, , 1993

14. An outlook on lithium ion battery technology, Manthiram A, 3(10):10639, , 2017

15. Li-ion battery materials: present and future, Wu, F., Yushin, G., Nitta, N., Lee, J. T., 18(5):25264, , 2015

16. Electrolytes for highenergy lithium batteries, S. S. Moganty, N. Jayaprakash, Y. Lu, L. A. Archer, J. L. Schaefer, P. Agarwal, 2 91109, , 2012

17. Allsolidstate thinfilm lithiumsulfur batteries, B. Ke, B. Lu, S. Cheng, R. Deng, C. Zhang, Y. Xie, X. Wang, H. Zhang, 15(1) (2023) 73, , 2023

18. Lithium sulfur batteries, a mechanistic review, G. Minton, T. Zhang, M. Marinescu, M. Wild, L. O'neill, G. Offer, R. Purkayastha, 8 34773494, , 2015

19. Lithium batteries: Status, prospects and future, B. Scrosati, J. Garche, 195 24192430, , 2010

20. The renaissance of hydrides as energy materials, R. Mohtadi, S.i. Orimo, 2 1 15, , 2016

21. Recent advances in lithium ion battery materials, B. Scrosati, 45 24612466, , 2000

22. Recent advances in lithium ion battery materials, Scrosati B, 45(15 16):24616, , 2000

23. Ultrathin 2D metal–organic framework nanosheets, H. Xu, Q. Lu, X. Zhang, Y. Wang, Z. Zhang, Q. Ma, Y. Huang, J. Ping, M. Zhao, Y. Yu, 27(45) 73727378, , 2015

24. Li–O2 and Li–S batteries with high energy storage, S. A. Freunberger, J.M. Tarascon, P. G. Bruce, L. J. Hardwick, 11 1929, , 2012

25. Microporous bamboo biochar for lithiumsulfur batteries, C. Lai, N. Mahmood, W. Martens, Y. Hou, Y. Wang, J. Qiu, X. Gu, S. Zhang, S. Li, 129139, , 2015

26. A review of electrolytes for lithium–sulphur batteries, S. Fantini, J. Scheers, P. Johansson, 255 204218, , 2014

27. Electrolyte solutions design for lithiumsulfur batteries, Y. Liu, R. Zou, D. Aurbach, D. Xia, Y. Elias, J. Meng, Q. Pang, 5(9) 23232364, , 2021

28. Progress towards commercially viable Li–S battery cells, P. Novák, T. Poux, S. Urbonaite, 5 1500118, , 2015

29. Strategies toward high‐loading lithium–sulfur battery, J. Huang, Y. Jiao, X. Wang, J. Xiong, C. Yan, Y. Hu, T. Lei, C. Gong, A. Hu, W. Chen, 10(17) 2000082, , 2020

30. Adsorptioncatalysis design in the lithium‐sulfur battery, C. Gong, L. Xue, C. Yan, T. Lei, Y. Yan, Y. Jiao, W. Chen, M. Zhang, J. Huang, J. Chu, 10(2) 1903008, , 2020

31. Electrical energy storage for the gridA battery of choices, H. Kamath, JM Tarascon, B. Dunn, Science, 334 928935, , 2011

32. NCA NCM811, and the Route to NiRicher LithiumIon Batteries, Mauger A., Julien CM, 13(23):6363, , 2020

33. Issues and challenges facing rechargeable lithium batteries, M. Armand, J. M. Tarascon, 414 359367, , 2001

34. Issues and challenges facing rechargeable lithium batteries, Armand M., Tarascon JM, Materials for sustainable energy: a collection of peerreviewed research and review articles from Nature Publishing Group, , 2011

35. Progress in flexible lithium batteries and future prospects, F. Li, G. Zhou, H.M. Cheng, 4) 13071338, , 2014

36. A review of functional binders in lithium–sulfur batteries, M. M. Titirici, R. Xiang, Q. Zhang, Q. Liu, R. Chen, H. Yuan, H. J. Peng, J. Q. Huang, 8(31) 1802107, , 2018

37. Electrical energy storage for the grid: A battery of choices, Dunn, B., Tarascon, J.-M., Kamath, H., 334 (6058), 928−935, , 2011

38. Ultrahighpower iron oxysulfide thin films for microbatteries, R. Deng, S. Cheng, W. Li, D.L. Peng, B. Ke, X. Wang, Q. Xie, J. Lin, C. Zhang, 66(1) (2023) 118126, , 2023

39. Recent advances in electrolytes for lithium–sulfur batteries, S. Zhang, K. Ueno, M. Watanabe, K. Dokko, 5(16) 1500117, , 2015

40. A review of multifunctional polymermatrix structural composites, Chung D., 160:64460, , 2019

41. Review on highloading and highenergy lithium−sulfur batteries, Huang, J. Q., Cheng, X. B., Zhang, Q, Peng, H. J., 7 (24), 1700260, , 2017

42. A review of solid electrolyte interphases on lithium metal anode, Q. Zhang, R. Zhang, X. B. Cheng, C. Z. Zhao, J. G. Zhang, F. Wei, 3 1500213, , 2016

43. Optimizing redox reactions in aprotic lithium–sulfur batteries, M. Zhou, J. Long, C. Shu, Y. Hu, T. Lei, J. Zhu, A. Hu, W. Chen, C. Gong, X. Du, 10(42) 2002180, , 2020

44. Rechargeable iron−sulfur battery without polysulfide shuttling, Kim, K. i., Zhang, C., Wu, X., Leonard, D. P., Ji, X., Xu, Y., Dai, K. T., Markir, A., Hu, E. C., Shin, W., 9 (40), 1902422, , 2019

45. The lithiumion battery: State of the art and future perspectives, Carvalho M, Pasaoglu G., DufoLópez R, Zubi G, 89:292308, , 2018

46. Thermal runaway caused fire and explosion of lithium ion battery, Chen, C., Ping, P., Chu, G., Wang, Q., Zhao, X., Sun, J., J Power Sources208:21024, , 2012

47. Revisiting the role of polysulfides in lithium–sulfur batteries, S. Wang, M. Li, Y. Zhang, Z. Chen, J. Lu, G. Li, 30 1705590, , 2018

48. Toward safe lithium metal anode in rechargeable batteries: a review, Q. Zhang, R. Zhang, X.B. Cheng, C.Z. Zhao, 117 1040310473, , 2017

49. A Low Cost Aqueous Zn–S Battery Realizing Ultrahigh Energy Density, Wang, K., Li, W., Jiang, K., 7 (23), 2000761, , 2020

50. A comprehensive understanding of lithium–sulfur battery technology, U. Gulzar, R. Proietti Zaccaria, X. Bai, W. Deng, Z. Feng, C. Capiglia, Z. Liu, Y. J. Bai, X. Zhou, T. Li, 29(32) 1901730, , 2019

51. Challenges in the development of advanced Li-ion batteries: a review, G. Salitra, R. Marom, V. Etacheri, D. Aurbach, R. Elazari, 4(9) 32433262, , 2011

52. Ionic liquids and derived materials for lithium and sodium batteries, Y.S. Hu, S. Dai, Q. Yang, H. Xing, X.G. Sun, Z. Zhang, 47 20202064, , 2018

53. A highly efficient polysulfide mediator for lithium–sulfur batteries, A. Garsuch, L. F. Nazar, X. Liang, T. Weiss, Q. Pang, C. Hart, 6 18, , 2015

54. A toolbox for lithium–sulfur battery research: methods and protocols, H. J. Peng, G. Zhang, Q. Zhang, Z. W. Zhang, J. Q. Huang, Small Methods, 1 1700134, , 2017

55. Ionicliquid materials for the electrochemical challenges of the future, Armand M, Ohno H, MacFarlane DR, Scrosati B., Endres F, Materials for sustainable energy: a collection of peerreviewed research and review articles from Nature Publishing Group, , 2011

56. Lithium–sulfur batteries: electrochemistry, materials, and prospects, S. Xin, L. J. Wan, Y. X. Yin, Y. G. Guo, 52 1318613200, , 2013

57. A novel carboncoated LiCoO2 as cathode material for lithium ion battery, Q. Cao, G. Wang, H. Wu, H. Zhang, Q. Xia, Y. Wu, 9 12281232, , 2007

58. An aqueous dissolved polysulfide cathode for lithium−sulfur batteries, Zhou, H., Li, F., Wang, Y., Li, N., Weng, Z., Cheng, H.M., 7 (10), 3307−3312, , 2014

59. Initiating a reversible aqueous Zn/sulfur battery through a liquid film, Li, Q., Yang, Q., Wang, D., Li, H., Zhi, C., Guo, Y., Zhao, Y., Peng, C., Mo, F., Li, X., 32 (32), 2003070, , 2020

60. Metal–organic frameworkbased separator for lithium–sulfur batteries, H. Zhou, S. Bai, X. Liu, K. Zhu, S. Wu, 1(7) 16, , 2016

61. Nanostructured metal oxides and sulfides for lithium–sulfur batteries, Q. Zhang, L. Mai, J. Q. Huang, X. Liu, 29 1601759, , 2017

62. Applications of lithiumion batteries in gridscale energy storage systems, Liu M, Chen T, Chen B, et al, Lv H, Jin Y, Yang A, Transactions of Tianjin University26(3):20817, , 2020

63. Hydrotalcitetype anionic clays: Preparation, properties and applications, F. Cavani, F. Trifiro, A. Vaccari, 11 173301, , 1991

64. More reliable lithium‐sulfur batteries: status, solutions and prospects, R. Fang, D. W. Wang, Z. Sun, F. Li, H. M. Cheng, S. Zhao, 29(48) 1606823, , 2017

65. Recent advances in shuttle effect inhibition for lithium sulfur batteries, B. Tang, S. Zhang, W. Ma, W. Ren, 707732, , 2019

66. Insitu activated polycation as a multifunctional additive for LiS batteries, H. Chen, L. Chen, J. Yang, J. Ge, W. Lu, C. Wang, Y. Dai, 26 4349, , 2016

67. Progress in solid electrolytes toward realizing solidstate lithium batteries, Takada K., 394:7485, , 2018

68. Ionic shield for polysulfides towards highlystable lithium–sulfur batteries, Q. Zhang, X.Y. Liu, W.Z. Qian, J.Q. Huang, H.J. Peng, F. Wei, 1) 347353, , 2014

69. Thin and flexible lithiumion batteries: investigation of polymer electrolytes, Alloin F, Saunier J, Sanchez JY, Caillon G., 119:4549, , 2003

70. Energy storage system: Current studies on batteries and power condition system, C. Zhang, Y.L. Wei, P.F. Cao, M.C. Lin, 82 30913106, , 2018

71. A strategic approach to recharging lithiumsulphur batteries for long cycle life, A. Manthiram, T. Cochell, Y. Fu, Y.S. Su, 4 18, , 2013

72. An anionimmobilized composite electrolyte for dendritefree lithium metal anodes, P.Y. Chen, C.Z. Zhao, J.Q. Huang, H.J. Peng, X.Q. Zhang, R. Zhang, R. Xu, Q. Zhang, X.B. Cheng, 114, , 2017

73. A review on the key issues for lithiumion battery management in electric vehicles, Han X, Li J, Ouyang M., Lu L, Hua J, J Power Sources226:27288, , 2013

74. Designing safe electrolyte systems for a high‐stability lithium–sulfur battery, K. Hu, W. Chen, C. Gong, W. Lv, M. Deng, C. Wu, Y. Ma, T. Lei, W. He, L. Dai, 8(10) 1702348, , 2018

75. In situformed Li2S in lithiated graphite electrodes for lithium–sulfur batteries, C. Zu, Y. Fu, A. Manthiram, 135 1804418047, , 2013

76. Recent progress on solidstate hybrid electrolytes for solidstate lithium batteries, Yang X, Sun Q, Luo J, Li R, Sun X, Liang J, 21:30834, , 2019

77. In situ formed lithium sulfide/microporous carbon cathodes for lithiumion batteries, F. Yi, Y. Chen, Y. Liu, S. Zheng, C. Wang, Y. Zhu, J. Yang, Y. Xu, 7 1099511003, , 2013

78. Material design and structure optimization for rechargeable lithiumsulfur batteries, Y. Li, S. Guo, Matter 4(4) 11421188, , 2021

79. Beyond PEO—Alternative host materials for Li+ conducting solid polymer electrolytes, Mindemark J, Lacey MJ, Brandell D., Bowden T, 81:11443, , 2018

80. Flexible graphenebased lithium ion batteries with ultrafast charge and discharge rates, Ren W, Cheng HM, Chen Z, Li F, Li N, 109(43):173605, , 2012

81. Improvement of electrochemical stability of LiCoO2 cathode by a nanocrystalline coating, X. Zhang, H. Zhao, W. Qiu, L. Gao, 195200, , 2004

82. Understanding electrochemical potentials of cathode materials in rechargeable batteries, Liu C, Cao G., Neale ZG, 19(2):10923, , 2016

83. Crystalline lithium imidazolate covalent organic frameworks with high Liion conductivity, S. Huang, Y. Hu, S.h. Lee, S. Wan, W. Zhang, S. Lu, M. Ortiz, I. Sellinger, N. Dunlap, Y. Jin, 141(18) 75187525, , 2019

84. Advances in lithium–sulfur batteries based on multifunctional cathodes and electrolytes, L. F. Nazar, X. Liang, C. Y. Kwok, Q. Pang, 1(9) 111, , 2016

85. LiTFSIBEPyTFSI as an improved ionic liquid electrolyte for rechargeable lithium batteries, B. Scrosati, F. Croce, H. Ohno, T. Watanabe, A. Fernicola, 174 342348, , 2007

86. Al2O3doped ZnO coating of carbon nanotubes as cathode material for lithiumsulfur batteries, T. Huang, A. Yu, T. Ma, M. Liu, 398 7582, , 2018

87. Ionic liquids as electrolytes for Liion batteries—An overview of electrochemical studies, Lewandowski A, ŚwiderskaMocek A., 194(2):6019, , 2009

88. Lithium–sulfur batteries under lean electrolyte conditions: challenges and opportunities, J. Q. Huang, B. Q. Li, M. Zhao, H. Yuan, H. J. Peng, J. Y. Wei, 59(31) 1263612652, , 2020

89. A roomtemperature sodium−sulfur battery with high capacity and stable cycling performance, Li, B., Rojo, T., Qin, X., Kang, F., Xu, X., Zhou, D., Wang, G., Shanmukaraj, D., Lin, K., Armand, M., 9 (1), 1−12, , 2018

90. Decoupling segmental relaxation and ionic conductivity for lithium-ion polymer electrolytes, Bresser, D., Lyonnard, S., Iojoiu, C., Passerini, S., Picard, L., 4(4):77992, , 2019

91. LiCl/PVA gel electrolyte stabilizes vanadium oxide nanowire electrodes for pseudocapacitors, G. Wang, T. Zhai, H. Wang, Y. Tong, Y. Ling, X. Lu, Y. Li, 6 1029610302, , 2012

92. Progress on the critical parameters for lithium–sulfur batteries to be practically viable, A. Manthiram, C. H. Chang, S. H. Chung, 28 1801188, , 2018

93. A review on lithiumion battery ageing mechanisms and estimations for automotive applications, Deguilhem B, Riu D., Barré A, Suard F, Gérard M, Grolleau S, 241:6809, , 2013

94. Cathode porosity is a missing key parameter to optimize lithiumsulfur battery energy density, J. Xiao, Y. Lin, M. Cai, L. Yang, N. Kang, D. Lu, Y. Qi, 10(1) 4597, , 2019

95. Designing host materials for sulfur cathodes: from physical confinement to surface chemistry, H. J. Peng, Q. Zhang, 54 1101811020, , 2015

96. Monodisperse molybdenum nanoparticles as highly efficient electrocatalysts for LiS batteries, Y. Liu, P. Nan, F. Bettels, A. Chatterjee, P. Rusch, C. Zhang, T. Li, C. Wu, M. Peng, C. Ma, 15(9) 1504715056, , 2021

97. Polymer electrolytes for high energy density ternary cathode materialbased lithium batteries, G. Cui, J. Zhang, J. Ma, G. Xu, H. Zhang, T. Dong, 2 128148, , 2019

98. Solidstate rigidrod polymer composite electrolytes with nanocrystalline lithium ion pathways, C. J. Zanelotti, X. Wang, M. Forsyth, L. A. Madsen, Y. Wang, R. Kerr, T. J. Dingemans, W. H. Kan, L. Jin, 20(9) 12551263, , 2021

99. A graphene foam electrode with high sulfur loading for flexible and high energy LiS batteries, L. Li, N. Koratkar, H.M. Cheng, Y. Shi, S. Wang, F. Li, G. Zhou, W. Ren, C. Ma, 11 356 365, , 2015

100. Electrochemical (de) lithiation of 1D sulfur chains in Li–S batteries: a model system study, C.P. Yang, L.J. Wan, Y.X. Yin, Y.G. Guo, 137 22152218, , 2015

101. Challenges and Development of Composite Solid Electrolytes for Allsolidstate Lithium Batteries, Liu L, Liu J, Liu Z, Xu X, Zhang D, Chem Res Chin Univ, , 2021

102. Enhanced electrochemical kinetics on conductive polar mediators for lithium–sulfur batteries, H. J. Peng, W. T. Xu, Q. Zhang, J. Q. Huang, X. Chen, G. Zhang, Z. W. Zhang, 55 1299012995, , 2016

103. Progress and perspective of ceramic/polymer composite solid electrolytes for lithium batteries, Q. Liu, W. Lv, Y. B. He, S. Q. Zhang, J. B. Ma, Q. H. Yang, S. Li, L. Shen, 7 1903088, , 2020

104. Insights into changes in voltage and structure of Li2FeSiO4 polymorphs for lithiumion batteries, Armstrong A, Bruce P, Islam M., Eames C, 24(11):215561, , 2012

105. The synergistic effect of cation and anion of an ionic liquid additive for lithium metal anodes, J. W. Choi, K. J. Kim, D. J. Yoo, 8(11) 1702744, , 2018

106. Creating lithium‐ion electrolytes with biomimetic ionic channels in metal–organic frameworks, H. B. Wu, J. I. Zink, G. Wang, F. Liu, J. L. Brosmer, X. Wang, G. Shen, L. Shen, Q. Xiao, M. Cai, 3023) 1707476, , 2018

107. Tailoring of interfacial properties by ionic liquids in a fluorinated matrix based nanocomposites, J. DuchetRumeau, S. Livi, J.F. Gérard, 47 13611369, , 2011

108. Intermolecular chemistry in solid polymer electrolytes for highenergy‐ density lithium batteries, J. Ma, Q. Zhou, X. Li, S. Dong, G. Cui, 31 1902029, , 2019

109. Single-Ion Lithium Conducting Polymers with High Ionic Conductivity Based on Borate Pendant Groups, S. Cotte, A. Guéguen, S. Vauthier, M. Alvarez-Tirado, D. Mecerreyes, L. Castro, N. Casado, G. Guzmán-González, 134(7) (2022) e202114024, , 2022

110. Biomaterials of PVA and PVP in medical and pharmaceutical applications: Perspectives and challenges, Bercea M, Morariu S., Teodorescu M, 37(1):10931, , 2019

111. Developing a polysulfide‐phobic strategy to restrain shuttle effect in lithium–sulfur batteries, P. He, X. Cao, H. Zhou, M. Jia, Z. Chang, Y. Qiao, Y. He, 58(34) 1177411778, , 2019

112. Review of ionic liquids containing, polymer/inorganic hybrid electrolytes for lithium metal batteries, L. Deng, Y. Song, G. Yang, Q. Wang, L. Zhang, 190 108563, , 2020

113. Catalytic effects in lithium–sulfur batteries: promoted sulfur transformation and reduced shuttle effect, C. Zhang, W. Lv, Q. H. Yang, G. Zhou, L. Zhi, G. Ling, D. Liu, 5(1) 1700270, , 2018

114. Multifunctional separator/interlayer system for highstable lithiumsulfur batteries: Progress and prospects, J.Q. Huang, Q. Zhang, F. Wei, 127145, , 2015

115. interfaces Lithium sulfonate/carboxylateanchored polyvinyl alcohol separators for lithium sulfur batteries, S. Gao, J. Han, S. Cheng, M. Liu, T. Gu, R. Wang, M. Jiang, K. Jiang, K. Wang, 10(21) 1831018315, , 2018

116. Ordered SnO nanoparticles in MWCNT as a functional host material for highrate lithiumsulfur battery cathode, M. K. Kim, J. Y. Kim, H.S. Choi, Y. Wen, V.D. Dao, D. Byun, L. Gu, A. Kim, J. K. Lee, 10 20832095., , 2017

117. 36 Preparation and electrochemical performance of sulfuralumina cathode material for lithiumsulfur batteries, J. Wu, H. Zhang, S. Wang, K. Dong, 48 20792083, , 2013

118. Current research trends and prospects among the various materials and designs used in lithiumbased batteries, Preschitschek N, Winter M., Passerini S, Wagner R, Leker J, 43(5):48196, , 2013

119. Hydroxylated Ndoped carbon nanotubesulfur composites as cathodes for highperformance lithiumsulfur batteries, J. S. Lee, A. Manthiram, 343 5459, , 2017

120. Low Tortuosity and Reinforced Concrete Type Ultra‐Thick Electrode for Practical Lithium–Sulfur Batteries, H. Zhou, C. Yu, Z. Han, Z. Jiang, W. Hu, S. Li, R. He, M. Sun, R. Xiong, L. Peng, 32(12) 2108669, , 2022

121. Poly (ionic liquid) sinsalt electrolytes with cocoordinationassisted lithiumion transport for safe batteries, H. Zhu, M. Forsyth, G. M. Girard, D. R. MacFarlane, P. C. Howlett, X. Wang, M. Armand, F. Chen, D. Mecerreyes, 3 26872702, , 2019

122. Pyrrolidiniumbased polymeric ionic liquids as mechanically and electrochemically stable polymer electrolytes, De Meatza I, Mecerreyes D., Grande H, Marcilla R, Pont AL, 188(2):55863, , 2009

123. Solid polymer electrolytes with poly (vinyl alcohol) and piperidinium based ionic liquid for Liion batteries, Thayumanasundaram S, Rangasamy VS, Locquet JP, 333:7682, , 2019

124. Challenges and key parameters in exploring the cyclability limitation of practical lithium–sulfur batteries, S. Li, C. Yu, Z. Han, Y. Wu, S. Cheng, J. Xie, A 943) 2421524240, , 2021

125. Lithium dendrite in allsolidstate batteries: growth mechanisms, suppression strategies, and characterizations, D. Cao, X. Sun, P. Xiang, A. Natan, Q. Li, H. Zhu, Matter, 3 5794, , 2020

126. Redox Catalysis Promoted Activation of Sulfur Redox Chemistry for EnergyDense Flexible SolidState ZnS Battery, Cao, R., Luo, G., Zhang, H., Shang, Z., Lu, K., Jiao, S., Chen, Q., 16 (5), 7344– 7351, , 2022

127. The pursuit of solidstate electrolytes for lithium batteries: from comprehensive insight to emerging horizons, Guo X, Wu F., Li L, Qu W, Chen R, Mater Horiz3(6):487516, , 2016

128. Water soluble binder, an electrochemical performance booster for electrode materials with high energy density, Z. Y. Wu, J. T. Li, Q. S. Huang, L. Huang, Y. Zhou, Y. Q. Lu, S. G. Sun, 7 1701185, , 2017

129. interfaces Sulfonic groups originated dualfunctional interlayer for high performance lithium–sulfur battery, J. Jin, Z. Wen, Y. Lu, J. Yang, K. Rui, C. Chen, S. Gu, J. Guo, S. Zhang, 9(17) 1487814888, , 2017

130. Ionic liquid modified poly (vinylidene fluoride): crystalline structures, miscibility, and physical properties, J. You, M. Zhao, C. Xing, Y. Li, L. Zhao, X. Cao, 4 57265734, , 2013

131. [BMIM] BF 4modified PVDFHFP composite polymer electrolyte for highperformance solidstate lithium metal battery, Ma D, Wang Y, Yong B, Mi H, Huang K, Zhang P., 8(39):20593603, , 2020

132. High Voltage Stable Polyoxalate Catholyte with Cathode Coating for All‐Solid‐State Li‐Metal/NMC622 Batteries, S. Wang, Z. Wang, J. Li, J. Gao, Q. Chang, H. Sun, H. Huang, H. Xu, X. Pan, Y. Li, 10 2002416, , 2020

133. Ultrathin MOF nanosheet assembled highly oriented microporous membrane as an interlayer for lithiumsulfur batteries, G. Xu, Z. Fu, M. Tian, H. Kitagawa, F. Pei, M. Yao, L. Lin, G. Wu, X. Fang, 1421, , 2019

134. Charge/discharge performances of glyme– lithium salt equimolar complex electrolyte for lithium secondary batteries, N. Serizawa, K. Takei, S. Seki, K. Dokko, M. Watanabe, 243 323327, , 2013

135. Interconnected cathodeelectrolyte doublelayer enabling continuous Liion conduction throughout solidstate LiS battery, N. Wu, P. Bradford, M. Dirican, Y. Zhou, P. Zhu, H. Cheng, O. Yildiz, J. Jur, C. Yan, R. Orenstein, 136144, , 2022

136. Mechanical surface modification of lithium metal: towards improved Li metal anode performance by directed Li plating, M. H. Ryou, P. Bieker, Y. M. Lee, M. Winter, Y. Lee, 25 834 841, , 2015

137. Ionic liquid modified poly (vinyl alcohol) with improved thermal processability and excellent electrical conductivity, Chen G, Chen N, Duan W., Wang Q, Li L, 57(15):547281, , 2018

138. 3D graphene‐foam–reduced‐grapheneoxide hybrid nested hierarchical networks for high‐performance Li–S batteries, S. Wang, F. Li, H. M. Cheng, G. Hu, C. Xu, Z. Sun, W. Ren, 28 16031609, , 2016

139. A review on inorganic nanoparticles modified composite membranes for lithiumion batteries: recent progress and prospects, Anwar MT, Asghar MR, Naveed A, Membranes9(7):78, , 2019

140. Strong sulfur binding with conducting magnéliphase Ti n O2 n–1 nanomaterials for improving lithium–sulfur batteries, H. Huang, Z. Ying, J. Wang, Y. Gan, Q. Cai, C. Liang, G. Zheng, Y. Xia, X. Tao, W. Zhang, 14 52885294, , 2014

141. Covalently bonded sulfur anchored with thiolmodified carbon nanotube as a cathode material for lithium–sulfur batteries, X.P. Gao, Y.W. Xu, S. Liu, G.R. Li, B.H. Zhang, 3(1) 487494, , 2019

142. Twodimensional layered transition metal disulphides for effective encapsulation of highcapacity lithium sulphide cathodes, Hsu, P.C., Sun, Y., Li, W., Seh, Z. W., Yu, J. H., Wang, H., Yao, H., Zhang, Q., Cui, Y., 5 (1), 1−8., , 2014

143. Comparing triflate and hexafluorophosphate anions of ionic liquids in polymer electrolytes for supercapacitor applications, Ramesh S., Liew CW, 7(5):401933, , 2014

144. Toward high performance lithium–sulfur batteries based on Li2S cathodes and beyond: status, challenges, and perspectives, C. Wang, G. Wang, D. Su, D. Zhou, 28 1800154, , 2018

145. Threedimensional flowershaped activated porous carbon/sulfur composites as cathode materials for lithium–sulfur batteries, L. Zhou, T. Huang, A. Yu, 2 2442 2447, , 2014

146. Ethercompatible sulfurized polyacrylonitrile cathode with excellent performance enabled by fast kinetics via selenium doping, J. Xiang, J. Yang, Z. Hao, X. Chen, L. Wang, L. Yuan, L. Peng, B. Shan, Y. Huang, K. Yuan, 10(1) 1021, , 2019

147. PEO/Garnet Composite Electrolytes for Solid-State Lithium Batteries: From ‘Ceramic-in-Polymer’ to ‘Polymer-in-Ceramic,, Li, S. P., Goodenough, J. B., Li, Y., Fan, L. Z., Nan, C. W., Chen, L., 46:17684, , 2018

148. Recent advances and historical developments of high voltage lithium cobalt oxide materials for rechargeable Li-ion batteries, M. Wang, Y. Yang, J. Zhu, J. Wan, Q. Leng, K. Wang, Y. Xiang, L. Xu, 460 228062, , 2020

149. Balancing surface adsorption and diffusion of lithiumpolysulfides on nonconductive oxides for lithium–sulfur battery design, G. Zhou, W. Li, X. Tao, H. Wang, G. Zheng, C. Liu, Z. W. Seh, Q. Cai, J. Wang, H. Yao, 7 19, , 2016

150. Bifunctional Electrolyte Additive with Redox Mediation and Capacity Contribution for Sulfur Cathode in Aqueous Zn S Batteries, Chen, X., Huang, C., Hu, A., Tang, Q., Yang, Y., Hao, Y., Chang, G., Qian, Y., Liu, J., 2023, 457, 141083, , 2023

151. Nitrogen, sulfurcodoped graphene sponge as electroactive carbon interlayer for highenergy andpower lithium–sulfur batteries, L.B. Xing, R. V. Kumar, Q. Li, K. Xi, Z. Su, X. Zhao, C. Lai, 303 2228, , 2016

152. Single‐ion conducting polymer electrolytes for solid‐state lithium–metal batteries: design, performance, and challenges, I. Belharouak, S. Zhao, A. S. Westover, J. Zhu, Z. Zhang, P. F. Cao, 11(14) (2021) 2003836, , 2021

153. Effect of hydrotalcite on the thermal stability, mechanical properties, rheology and flame retardance of poly (vinyl chloride), Q. Zhang, X. Wang, Polym. Int., 53 698707, , 2004

154. Flexible PVA/BMIMOTf/LLZTO composite electrolyte with liquidcomparable ionic conductivity for solidstate lithium metal battery, D. Kim, H. Jeon, H. A. Hoang, 128139, , 2022

155. Ceramic nanoparticledecorated meltelectrospun PVDF nanofiber membrane with enhanced performance as a LithiumIon Battery Separator, Ning J, Wu S, Jiang F, Shi J, Huang F., 4(15):1630917, , 2019

156. Effect of alkylchain length of imidazolium based ionic liquid on ion conducting and interfacial properties of organic electrolytes, Kim K, Kim S., 26:13642, , 2015

157. Electrolyte membrane for lithium secondary battery and membraneelectrode structure for lithium secondary battery having the same in, L. Anh, D. J. Kim, T. Zhenchuan, H. A. Hoang, S. G. Kim, Google Patents, , 2021

158. Fast Liion transport and uniform Liion flux enabled by a double–layered polymer electrolyte for high performance Li metal battery, S. Chen, X. Tan, S. Zhang, T. Chen, K. Wen, 32 5564, , 2020

159. Liquid electrolyte based on lithium bisfluorosulfonyl imide salt: Aluminum corrosion studies and lithium ion battery investigations, Abouimrane A, Davidson I, Ding J, 189(1):6936, , 2009

160. High Performance Solid‐State Lithium‐Sulfur Battery Enabled by Multi‐ Functional Cathode and Flexible Hybrid Solid Electrolyte, D. Kim, H. A. Hoang, 18(34) 2202963, , 2022

161. A Metal–organic‐framework‐based electrolyte with nanowetted interfaces for high‐energy‐density solid‐state lithium battery, H. Wang, R. Tan, J. Hu, F. Pan, L. Yang, H. Chen, Z. Wang, 30(2) 1704436, , 2018

162. Achieving uniform Li plating/stripping at ultrahigh currents and capacities by optimizing 3D nucleation sites and Li2Se‐enriched SEI, S. Cheng, X. Wang, Q. Zhang, W. Li, S. Ma, J. Cao, B. Lu, Y. Xie, Y. Yang, 9(9) 2104689, , 2022

163. ZnO hard templating for synthesis of hierarchical porous carbons with tailored porosity and high performance in lithium‐sulfur battery, M. Oschatz, P. Strubel, T. Biemelt, H. Althues, A. Helmer, S. Thieme, S. Kaskel, J. Brückner, 25 287297., , 2015

164. Flexible solid electrolyte based on UV cured polyurethane acrylate/succinonitrilelithium salt composite compatibilized by tetrahydrofuran, Lv P, Liu G, Yang J, Liu H, Li S, Tang C et al, 120:3541, , 2017

165. Influence of hydrophilic/hydrophobic protic ionic liquids (PILs) on the poly(vinylidene fluoride) (PVDF-ionic liquid) membrane properties, M. Anouti, J. Bigarré, A. Bouzina, M. Raghibi, L. Timperman, I. Vázquez-Fernández, 55 1669716717., , 2020

166. Rational design of statically and dynamically stable lithium–sulfur batteries with high sulfur loading and low electrolyte/sulfur ratio, S. H. Chung, A. Manthiram, 30(6) 1705951, , 2018

167. 3D graphene framework supported Li 2 S coated with ultrathin Al 2 O 3 films: binderfree cathodes for highperformance lithium sulfur batteries, Y. Chen, O. Ogoke, J. Zhou, X. Wu, W. Qin, G. Wu, S. Lu, 5 102112, , 2017

168. Effects of octadecylamine functionalization of carbon nanotubes on dispersion, polarity, and mechanical properties of CNT/HDPE nanocomposites, B. Silva, B. De Menezes, F. Ferreira, T. Bastos, E. Simonetti, L. Cividanes, G. Thim, 53(20) 1431114327, , 2018

169. A brief review on solid electrolyte interphase composition characterization technology for lithium metal batteries: challenges and perspectives, J. Tu, X. Shan, X. Xia, X. Wang, L. Zhang, Y. Zhong, Y. Zhang, 125 1906019080, , 2021

170. Coupling a Sponge Metal Fibers Skeleton with In Situ Surface Engineering to Achieve Advanced Electrodes for Flexible Lithium–Sulfur Batteries, Q. Liu, S. Liu, Y. Zhang, S. Deng, Z. Wang, S. Lin, P. Liu, C. Ai, B. Liu, Y. Zhong, 32 2003657., , 2020

171. Brain‐Coral‐Like Mesoporous Hollow CoS2@ N‐Doped Graphitic Carbon Nanoshells as Efficient Sulfur Reservoirs for Lithium–Sulfur Batteries, D. W. Kim, S. Park, S. D. Seo, D. Park, 29(38) 1903712, , 2019

172. Janus separator of polypropylene‐supported cellular graphene framework for sulfur cathodes with high utilization in lithium– sulfur batteries, D. W. Wang, Z. Yuan, X. B. Cheng, J. Q. Huang, H. J. Peng, F. Wei, Q. Zhang, 3 1500268, , 2016

173. Hydrophilic polyvinyl alcohol coating on hydrophobic electrospun nanofiber membrane for high performance thin film composite forward osmosis membrane, H. K. Shon, A. AbdelWahab, S. Phuntsho, R. R. Gonzales, M. J. Park, Desalination, 426 5059, , 2018

174. Crosslinked Nanofiber‐Reinforced Solid‐State Electrolytes with Polysulfide Fixation Effect Towards High Safety Flexible Lithium–Sulfur Batteries, G. Zhou, X. Zhong, J. Sheng, Q. Zhang, R. Gao, C. Li, B. Chen, Z. Han, C. Sun, J. Wang, 32(40) (2022) 2203272., , 2022

175. Multifunctional bilayer carbon structures with micrometerlevel physical encapsulation as a flexible cathode host for highperformance lithiumsulfur batteries, S. Cheng, L. Zhang, X. Wang, J. Ao, H. Zhang, Y. Xie, Y. Shao, 4512023) 139017, , 2023

176. A straightforward fabrication of solidstate lithium secondary batteries based on multifunctional poly (arylene ether sulfone)gpoly (ethylene glycol) material, D. Kim, A. Le Mong, H. A. Hoang, 507 230288, , 2021

177. Simultaneously Suppressing Shuttle Effect and Dendrite Growth in Lithium–Sulfur Batteries via Building Dual‐Functional Asymmetric‐Cellulose Gel Electrolyte, Y. Fu, C. Cai, F. Cheng, Y. Huang, Small (2023) 2300076, , 2023

178. LithiumSaltContaining Ionic LiquidIncorporated Li–AlLayered Double HydroxideBased Solid Electrolyte with HighPerformance and Safety in SolidState Lithium Batteries, T. Yu, J. Wang, A. Abudula, Z. Wang, X. Hao, G. Guan, Z. Xie, Z. Wu, 8, , 2020

179. Trifluoromethanesulfonate (triflate) as a moderately coordinating anion: Studies from chemistry of the cationic coordinatively unsaturated monoand diruthenium amidinates, Kirchner K, Hayashida T, Kondo H, Terasawa Ji, Nagashima H., Sunada Y, 692(1 3):38294., , 2007

180. A synergistic engineering layer with a versatile H 2 Ti 3 O 7 electrocatalyst for a suppressed shuttle effect and enhanced catalytic conversion in lithium–sulfur batteries, D.W. Kim, C. Choi, J. B. Park, A 8(47) 2541125424, , 2020

181. High voltage stable solidstate lithium battery based on the nanoconductor imbedded flexible hybrid solid electrolyte with hyperion conductivity and thermal, mechanical, and adhesive stability, H. A. Hoang, D. Kim, 435 135092, , 2022