Review
Chemistry, Multidisciplinary
Nan Meng, Yuning Ye, Zhaoxia Yang, Hao Li, Fang Lian
Summary: Single-ion conductive polymer electrolytes (SICPEs) with a high cationic transference number have advantages in solid-state batteries (SSBs), but face challenges in terms of inferior ionic conductivity at room temperature. This review discusses recent advancements in improving ambient ionic conductivity in order to develop solid polymer electrolytes for SSBs. Strategies such as delocalizing charges in polyanions, designing highly conductive polymer matrices, and utilizing synergistic effects in SICPEs are highlighted.
ADVANCED FUNCTIONAL MATERIALS
(2023)
Article
Multidisciplinary Sciences
Michael J. Lee, Junghun Han, Kyungbin Lee, Young Jun Lee, Byoung Gak Kim, Kyu-Nam Jung, Bumjoon J. Kim, Seung Woo Lee
Summary: Elastomeric solid-state electrolytes with mechanical robustness, high ionic conductivity, low interfacial resistance and high lithium-ion transference number enable stable operation of high-energy, solid-state lithium batteries.
Article
Chemistry, Multidisciplinary
Dai Wang, Hui Xiea, Qiang Liu, Kexin Mu, Zhennuo Song, Weijian Xu, Lei Tian, Caizhen Zhu, Jian Xu
Summary: A low-cost cellulose acetate-based quasi-solid composite polymer electrolyte with high Li+ transference number and excellent interface stability was developed. The partially esterified side groups in the cellulose acetate matrix were found to enhance the migration of Li+ and improve electrochemical stability. This work provides a promising strategy for fabricating cost-effective, stable polymer electrolytes for solid-state lithium batteries.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Review
Chemistry, Multidisciplinary
Nan Meng, Yuning Ye, Zhaoxia Yang, Hao Li, Fang Lian
Summary: Single-ion conductive polymer electrolytes (SICPEs) with a cationic transference number close to unity have various advantages in solid-state batteries (SSBs), but their ionic conductivity at room temperature remains a major challenge. This review discusses recent achievements in improving the ambient ionic conductivity to make it compatible with SICPEs with a high transference number, focusing on strategies such as charge delocalization in polyanions, designing a highly conductive polymer matrix, and utilizing synergistic effects in SICPEs to further develop solid polymer electrolytes for SSBs.
ADVANCED FUNCTIONAL MATERIALS
(2023)
Article
Polymer Science
Jennifer Imbrogno, Kazuya Maruyama, Frederick Rivers, Jacob R. Baltzegar, Zidan Zhang, Paul W. Meyer, Venkat Ganesan, Sadahito Aoshima, Nathaniel A. Lynd
Summary: The study reveals a correlation between the dielectric constant of polymers and the ionic conductivity of polymer-salt mixtures. For polymer electrolyte mixtures with dielectric constants ranging from 1.3 to 9.0, the ionic conductivity increases with the dielectric constant and plateaus around 9.0, similar to poly(ethylene oxide) commonly used in this field.
Article
Chemistry, Physical
Eun Ju Jeon, Annelise Jean-Fulcrand, Arno Kwade, Georg Garnweitner
Summary: Polymer-based hybrid electrolytes (HEs) have high ionic conductivity and good mechanical strength, making them suitable for safe lithium metal anode batteries. A cross-linked polymer-based HE with high ionic conductivity was developed, integrating LLZO particles and capable of operating at room temperature, which can promote the development of safe all-solid-state batteries.
Article
Chemistry, Multidisciplinary
Michael A. Stolberg, Benjamin A. Paren, Pablo A. Leon, Christopher M. Brown, Gavin Winter, Kiarash Gordiz, Alberto Concellon, Rafael Gomez-Bombarelli, Yang Shao-Horn, Jeremiah A. Johnson
Summary: Solid polymer electrolytes have the potential to enable safer and more energy-dense batteries. This study investigates the impact of anion dissociation energy on ion conduction in solid polymer electrolytes. The researchers developed ionenes with various cations and found that the addition of a cation-coordinating solvent greatly enhanced ionic conductivity without disrupting the lamellar structure. This work demonstrates that molecular design can facilitate significant improvements in ion conduction in solid polymer electrolytes.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Electrochemistry
Fei Chen, Jamans Luo, Mao-xiang Jing, Jie Li, Zhen-hao Huang, Hua Yang, Xiang-qian Shen
Summary: Introducing a flexible polymer buffer layer to the surface of solid electrolyte enhances the interface contact and stability between electrodes. The layered structure composite solid electrolyte membrane shows good electrochemical stability window and ion conductivity, demonstrating great potential for use in high-performance solid-state lithium batteries.
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
(2021)
Article
Chemistry, Multidisciplinary
Yanfang Zhai, Wangshu Hou, Mingming Tao, Zhongting Wang, Zongyuan Chen, Zhong Zeng, Xiao Liang, Peerasak Paoprasert, Yong Yang, Ning Hu, Shufeng Song
Summary: This study reports a unique superconcentrated ionogel-in-ceramic (SIC) electrolyte with high ionic conductivity, large Li+-ion transference numbers, and good compatibility with both Li-metal anodes and high-voltage cathodes. The SIC electrolyte exhibits ultrahigh ionic conductivity, high Li+-ion transference number, low electronic conductivity, and wide electrochemical stability window, making it promising for safe and high-energy lithium-metal batteries.
ADVANCED MATERIALS
(2022)
Review
Chemistry, Multidisciplinary
Feifan Zheng, Chunwei Li, Zongcheng Li, Xin Cao, Hebin Luo, Jin Liang, Xiaodong Zhao, Jie Kong
Summary: Composite solid electrolytes are crucial for all-solid-state lithium batteries, which are considered the next-generation energy storage devices. Numerous studies have shown that fillers in composite solid electrolytes can improve ion transport behavior by optimizing the ion transport path. The performance is closely related to filler structure and its interaction with other electrolyte components. This review focuses on dimensional design of fillers, as well as ion transport mechanism and filler-electrolyte interaction in advanced composite solid electrolytes. Strategies for designing composite solid electrolytes with high room temperature ionic conductivity are summarized to assist research for high-performance composite solid electrolytes.
Article
Polymer Science
Nacer Badi, Azemtsop Manfo Theodore, Saleh A. Alghamdi, Hatem A. Al-Aoh, Abderrahim Lakhouit, Aashis S. Roy, Ayshah S. Alatawi, Alex Ignatiev
Summary: In this study, solid flexible polymer blend electrolyte films composed of polyvinyl alcohol and polyvinyl pyrrolidone with different amounts of sodium thiocyanate were prepared. The addition of sodium thiocyanate improved the ionic conductivity, and the optimized ion-conducting polymer blend film showed good electrochemical stability and capacitance characteristics when used in a supercapacitor device with graphene oxide coated electrodes.
Review
Polymer Science
Jelena Popovic
Summary: Dry polymer electrolytes are a promising material for safer high-energy-density battery technologies in the future. This review examines their physico-chemical properties, ionic transport mechanism, molecular structure, and interfacial issues in a widely studied model system. The latest macromolecular approaches for high-performance lithium battery applications are also discussed.
MACROMOLECULAR CHEMISTRY AND PHYSICS
(2022)
Article
Chemistry, Physical
Shantao Han, Peng Wen, Huaijiao Wang, Yang Zhou, Yu Gu, Lu Zhang, Yang Shao-Horn, Xinrong Lin, Mao Chen
Summary: This study demonstrates a method to achieve highly ion-conductive solid-state materials by precisely positioning designed repeating units to enable homogenized Li+ distribution, non-aggregated solvation, and site-to-site ion migration. Assembled all-solid-state batteries allow reversible cycling against Li metal at ambient and elevated temperatures, mitigating dendrite formation.
Article
Energy & Fuels
Long Chen, Shaobo Huang, Dongjuan Ma, Yongchuang Xiong, Jingyi Qiu, Gaoping Cao, Hao Zhang
Summary: This study fabricated a flexible hybrid ceramic-based electrolyte with superior ionic conductivity and stable electrode/electrolyte interface contact, while also demonstrating the ability to impede lithium dendrite growth. The self-viscous modification strategy of the solid electrolyte shows promising options for implementing intimate electrode/electrolyte interfacial contact in high-energy-density solid-state batteries.
Article
Chemistry, Inorganic & Nuclear
Jiaying Bi, Ling Zhang, Borong Wu, Meixia Xiao, Lei Wang, Zhao Li
Summary: The interaction between Li0.33La0.56TiO3 (LLTO) and metallic lithium leads to interfacial instability in LLTO-containing solid-state electrolytes. To improve stability, a heterogeneous composite electrolyte PVDF-HFP@LLTO/PEO (PLTP) is designed. The PLTP electrolyte demonstrates high ionic conductivity and stable electrochemical properties. The enhanced interfacial stability makes the heterogeneous electrolyte a promising alternative for solid-state lithium metal batteries.
DALTON TRANSACTIONS
(2023)
Article
Physics, Applied
Anurag Tiwari, Shishir K. Singh, Nitin Srivastava, Dipika Meghnani, Raghvendra Mishra, Rupesh K. Tiwari, Anupam Patel, Himani Gupta, Vimal K. Tiwari, Rajendra K. Singh
Summary: A novel sulfide-based inorganic solid electrolyte (Na11Sn2AsS12) was synthesized and characterized for its various properties. The results showed that the solid electrolyte exhibited good ionic conductivity, thermal stability, and electrolyte properties suitable for solid-state sodium ion battery applications.
JOURNAL OF PHYSICS D-APPLIED PHYSICS
(2022)
Article
Chemistry, Physical
Dipika Meghnani, Shishir Kumar Singh, Nitin Srivastava, Rupesh Kumar Tiwari, Raghvendra Mishra, Anupam Patel, Anurag Tiwari, Rajendra Kumar Singh
Summary: In this study, a chemical strategy was adopted to improve the rate performance of the sodium superionic conductor (NASICON)-Na3V2(PO4)(3) (NVP) cathode for sodium-ion batteries. Partial replacement of V3+ by low-valence Mn2+ and high-valence Mo6+ substitution resulted in enhanced electronic conductivity and improved electrochemical performance. The Mn-Mo-doped NVP cathode exhibited smoother charge-discharge profiles, better rate performance, higher energy density and superior Na-ion kinetics compared to the unsubstituted NVP@C cathode.
Article
Chemistry, Physical
Nitin Srivastava, Shishir Kumar Singh, Dipika Meghnani, Raghvendra Mishra, Rupesh Kumar Tiwari, Anupam Patel, Anurag Tiwari, Rajendra Kumar Singh
Summary: A series of cathode materials, Li1.2Mn0.6-xNi0.1Co0.1MoxO2 (x = 0, 0.005, and 0.01), were synthesized via the sol-gel method. The Mo-doped cathode, Li1.2Mn0.59Ni0.1Co0.1Mo0.01O2, showed excellent electrochemical performance with high specific discharge capacity, initial Coulombic efficiency, and cyclic stability. The substitution of Mn4+ by Mo6+ resulted in low charge transfer resistance and enhanced stability of the layered structure, leading to outstanding electrochemical performance.
ACS APPLIED ENERGY MATERIALS
(2022)
Article
Electrochemistry
Shishir K. Singh, Dimple P. Dutta, Himani Gupta, Nitin Srivastava, Raghvendra Mishra, Dipika Meghnani, Rupesh K. Tiwari, Anupam Patel, Anurag Tiwari, Rajendra K. Singh
Summary: In this study, a double-layer coated Li-NMC111 cathode with improved electrochemical performance was synthesized, and a freestanding/flexible nanocomposite gel polymer electrolyte suitable for high-temperature Li-battery applications was prepared. The optimized cathode material with the flexible nanocomposite gel polymer electrolyte exhibited high discharge capacity and energy density.
ELECTROCHIMICA ACTA
(2022)
Article
Energy & Fuels
Raghvendra Mishra, Shishir K. Singh, Nitin Srivastava, Rupesh K. Tiwari, Dipika Meghnani, Anupam Patel, Anurag Tiwari, Vimal K. Tiwari, Rajendra K. Singh
Summary: A high-capacity and long-life layered NMC cathode material coated with Na2SiO3 and RGO has been synthesized and tested for half-cell and full-cell applications. The coating layers provide diffusion channels for Na-ion migration and electron-conducting pathways for enhanced charge transfer. The dually surface-modified cathode exhibits superior electrochemical performance with improved Na-ion kinetics, resulting in high capacity retention and coulombic efficiency in both half-cell and full-cell testing.
Article
Nanoscience & Nanotechnology
Rupesh K. K. Tiwari, Raghvendra Mishra, Anupam Patel, Anurag Tiwari, Dipika Meghnani, Rajendra K. K. Singh
Summary: This research focuses on preventing polysulfide migration in Lithium-sulfur batteries (LiSBs) by using an electrostatic rejection and trapping strategy. An SIL-based IC-GPM70 interlayer membrane with high lithium-ion conductivity and thermal stability is introduced to suppress the migration of polysulfide and prevent its dissolution in the electrolyte. The prepared IC-GPM70 interlayer greatly improves the cycling stability, rate performance, and structural integrity of LiSBs, making them a viable alternative to conventional LiBs.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Review
Engineering, Environmental
Vimal K. Tiwari, Rajendra Kumar Singh
Summary: Due to the scarcity and high cost of lithium-based energy storage systems, sodium-ion batteries have emerged as a potential alternative, utilizing low-cost components such as abundant sodium as an anode. However, their practical application has been significantly limited by structural instability, low conductivity, severe polarization, and low operating potential. To address these challenges, surface engineering of cathode materials through nanostructured organic and inorganic coatings has been explored to improve their performance by providing uniform charge distribution, enhancing strength, facilitating fast electron and ion transport, and preventing undesirable reactions at the cathode-electrolyte interface.
CHEMICAL ENGINEERING JOURNAL
(2023)
Article
Chemistry, Physical
Anurag Tiwari, Dipika Meghnani, Raghvendra Mishra, Rupesh Kumar Tiwari, Anupam Patel, Rajendra Kumar Singh
Summary: Recently, sodium super-ionic conducting (NASICON) type solid electrolytes, known for their high ionic conductivity, low cost, and excellent stability, have attracted attention for next generation batteries. In this study, a NASICON-type solid electrolyte, Na3Zr2Si2PO12, is synthesized using a solution assisted-solid state reaction (SA-SSR) method and sintered at different temperatures. The optimized electrolyte exhibits wide electrochemical stability and is used to assemble a sodium half-cell, which delivers high discharge capacity and good capacity retention.
JOURNAL OF POWER SOURCES
(2023)
Article
Electrochemistry
Rupesh K. Tiwari, Shishir K. Singh, Nitin Srivastava, Raghvendra Mishra, Dipika Meghnani, Anupam Patel, Anurag Tiwari, Vimal K. Tiwari, Rajendra K. Singh
Summary: A mesoporous and conducting carbon-rich graphitic carbon nitride (GCN) nanosheets host covered by nano sulfur copolymer is reported as a cathode material for rechargeable lithium-sulfur batteries (LiSBs) with high capacity and long cyclability.
BATTERIES & SUPERCAPS
(2022)
Article
Energy & Fuels
Nitin Srivastava, Shishir Kumar Singh, Dipika Meghnani, Rajendra Kumar Singh
Summary: In this study, a high capacity layered Li/Mn-rich NMC cathode and nanocomposite blend gel polymer electrolytes (NBGPEs) were synthesized. The NBGPE with 2 wt.% SiO2 nanofiller exhibited the highest ionic and Li-ion conductivity, as well as wide electrochemical stability. The electrochemical performance of the cell using this cathode and NBGPEs was investigated and showed promising results.
