Review
Chemistry, Multidisciplinary
Xue Tian, Qizhen Zhu, Bin Xu
Summary: Water-in-salt (WIS) electrolytes show great potential for application in supercapacitors due to their wide electrochemical stability window and other advantages, but also face challenges. This Review discusses the working mechanisms, reasons for the wide stability window, improvement strategies, and applications of WIS electrolytes in various types of supercapacitors.
Article
Chemistry, Multidisciplinary
Xuan Qiu, Nan Wang, Zhuo Wang, Fei Wang, Yonggang Wang
Summary: In this study, a Zn-based hybrid supercapacitor has been developed with high energy density and high Zn-utilization. By utilizing a metal organic framework derived porous carbon cathode and a specific electrolyte, high rate performance at high mass loading was achieved.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Multidisciplinary
Lewis W. Le Fevre, Andinet Ejigu, Rebecca Todd, Andrew J. Forsyth, Robert A. W. Dryfe
Summary: Water-in-salt electrolytes were tested for high-temperature performance with a carbon-based electrode and commercial cell components. Supercapacitors using these electrolytes demonstrated satisfactory operation at 100°C and 120°C, with gravimetric capacitances exceeding 100 F g(-1) at a voltage of 2 V.
CHEMICAL COMMUNICATIONS
(2021)
Article
Chemistry, Multidisciplinary
Xiaoqing Zhu, Chenchen Ji, Qiangqiang Meng, Hongyu Mi, Qi Yang, Zixiao Li, Nianjun Yang, Jieshan Qiu
Summary: In this study, a freeze-tolerant hydrogel electrolyte with high ionic conductivity and superior mechanical properties was developed for portable zinc-ion hybrid supercapacitors. The hydrogel exhibited excellent durability and stable electrochemical performance at low temperatures.
Article
Chemistry, Multidisciplinary
Yanan Zhang, Dingsheng Wu, Fenglin Huang, Yibing Cai, Yonggui Li, Huizhen Ke, Pengfei Lv, Qufu Wei
Summary: A water-in-salt gel polymer electrolyte with a double network structure has been developed for solid-state zinc-air batteries. The electrolyte captures water from ambient air and achieves a dynamic balance of adsorption and desorption, leading to an ultra-long cycle time for the batteries. The gel polymer electrolyte also exhibits excellent adhesion property and can adapt to complex deformations, showing enormous potential for practical wearable applications.
ADVANCED FUNCTIONAL MATERIALS
(2022)
Article
Energy & Fuels
Xinren Zhang, Chen Chen, Shan Gao, Xianyou Luo, Yan Mo, Bokai Cao, Yong Chen
Summary: The use of graphene as surface layer on zinc foil in Zinc ion hybrid supercapacitors (ZIHS) successfully inhibits dendrite formation and significantly improves cyclic stability, leading to an ultra-long cycle life compared to traditional zinc foil anodes. The abundance of active sites on graphene facilitates uniform zinc deposition, contributing to the enhanced performance of the electrode.
JOURNAL OF ENERGY STORAGE
(2021)
Article
Chemistry, Physical
Jin Han, Alessandro Mariani, Alberto Varzi, Stefano Passerini
Summary: A highly concentrated solution of potassium, lithium, and zinc acetate is proposed as a green Water-in-Salt electrolyte, showing excellent performance, particularly in terms of zinc plating/stripping efficiency and long-term cycling stability. Dual-ion cells using this electrolyte with zinc metal anode and different cathodes demonstrate good discharge capacity and cycling stability at low C-rate.
JOURNAL OF POWER SOURCES
(2021)
Article
Chemistry, Multidisciplinary
Minhyung Kwon, Jina Lee, Sunghyun Ko, Gukhyun Lim, Seung-Ho Yu, Jihyun Hong, Minah Lee
Summary: This study successfully constructs a stable zinc metal anode by identifying the growth mechanism of densely packed micrometer-sized Zn particles on Cu foil, which contributes to improving the performance of aqueous Zn-ion batteries.
ENERGY & ENVIRONMENTAL SCIENCE
(2022)
Review
Chemistry, Multidisciplinary
Ziyauddin Khan, Divyaratan Kumar, Xavier Crispin
Summary: Zn-metal batteries (ZnBs) are safe and sustainable due to their operability in aqueous electrolytes, abundance of Zn, and recyclability. However, the thermodynamic instability of Zn in aqueous electrolytes hinders its commercialization. To address this issue, the concept of water-in-salt-electrolyte (WISE) has been utilized to propel the hydrogen evolution reaction (HER) and improve the performance of ZnBs. This article provides an overview and discussion on the application of WISE in ZnBs.
ADVANCED MATERIALS
(2023)
Article
Chemistry, Physical
Yaheng Geng, Licheng Miao, Zichao Yan, Wenli Xin, Lei Zhang, Huiling Peng, Junwei Li, Zhiqiang Zhu
Summary: A super-zincophilic di-2-picolylamine (DPA) has been developed as an effective additive for enhancing the reversibility of Zn plating/stripping, leading to long-life Zn anodes under severe cycling conditions. The DPA molecule preferentially adsorbs on the Zn surface, retarding water adsorption and regulating Zn2+ diffusion, stabilizing the anode/electrolyte interphase and enabling highly reversible Zn plating/stripping even under high-current conditions. Additionally, the Zn||Zn cell with trace amounts of the DPA additive showed significantly improved lifespan, surpassing previously reported values, while the Zn||polyaniline full cell also demonstrated enhanced performance.
JOURNAL OF MATERIALS CHEMISTRY A
(2022)
Article
Chemistry, Multidisciplinary
Jun Zheng, Chenyang Zhan, Kai Zhang, Wenwu Fu, Qiaojun Nie, Ming Zhang, Zhongrong Shen
Summary: A new type of aqueous Zn-ion battery was constructed in this study to address the issues of poor cycling stability, Zn dendrite formation, and electrolyte decomposition. The improved interaction between the electrode and electrolyte resulted in excellent electrochemical performances.
Article
Chemistry, Physical
Xuejun Lu, Jose Manuel Vicent-Luna, Sofia Calero, Rafael M. Madero-Castro, Maria C. Gutierrez, M. Luisa Ferrer, Francisco del Monte
Summary: This study designed a tri-solvent-in-salt (TSIS) electrolyte where every solvent (with IL such as EMIMBF4) contributed to the formation of an electrochemically active hydrogen bond (HB) complex structure. The TSIS electrolyte composed of 1.5EMIMBF(4):2H(2)O:DMSO:3.5CH(3)CN (5.8 m, TSIS-5.8) was cost efficient and exhibited self-extinction rates as low as 40 s g(-1).
ENERGY STORAGE MATERIALS
(2021)
Review
Chemistry, Physical
Tobias F. Burton, Rossukon Jommongkol, Yachao Zhu, Siraprapha Deebansok, Khwanrudee Chitbankluai, Jie Deng, Olivier Fontaine
Summary: Water-in-salt electrolytes (WISEs) have gained incredible attention since 2015 due to their enlarged electrochemical stability window and ability to overcome limitations of Zn-ion technologies. The heavy reliance on expensive and complex LiTFSI in WISEs production raises concerns about practicality and sustainability, leading to a belief that Zn-ion batteries with WISEs are the most promising candidates. Alternative substitutes for highly concentrated electrolytes in aqueous zinc-ion batteries are being explored to address these concerns and advance the use of WISEs in practical applications.
CURRENT OPINION IN ELECTROCHEMISTRY
(2022)
Article
Green & Sustainable Science & Technology
Dawid Kasprzak, Jian Liu
Summary: Zinc-ion hybrid supercapacitors (ZIHS) are cost-effective, environmentally friendly energy storage devices with high-power performance and satisfactory energy density. By introducing biopolymer components, ZIHS technology becomes more sustainable, showing high ionic conductivity, expanded electrochemical stability, and suppression of zinc dendrites growth. The use of biopolymer binders in combination with zinc foil electrodes results in efficient operation and excellent cycle stability in various ZIHS cell configurations.
SUSTAINABLE MATERIALS AND TECHNOLOGIES
(2023)
Article
Chemistry, Multidisciplinary
Shengying Cai, Xingyuan Chu, Chang Liu, Haiwen Lai, Hao Chen, Yanqiu Jiang, Fan Guo, Zhikang Xu, Chunsheng Wang, Chao Gao
Summary: This study reports a highly soluble ZnCl2/ZnBr2/Zn(OAc)(2) aqueous electrolyte, which breaks through the physical solubility limit by forming acetate-capped water-salt oligomers, enabling high-performance aqueous dual-ion batteries.
ADVANCED MATERIALS
(2021)
Review
Chemistry, Multidisciplinary
Wenhua Zuo, Alessandro Innocenti, Maider Zarrabeitia, Dominic Bresser, Yong Yang, Stefano Passerini
Summary: Sodium-ion batteries (NIBs) have emerged as ideal alternatives for large-scale energy storage systems due to their abundant resources, low-cost materials, and improved energy density and cycling stability. However, challenges such as irreversible phase transformations, poor air stability, and relatively high cost need to be addressed for the commercialization of NIBs. This Account discusses recent progress in the development of air-stable, electrochemically stable, and cost-effective NaxTMO2 cathode materials for NIBs.
ACCOUNTS OF CHEMICAL RESEARCH
(2023)
Article
Chemistry, Multidisciplinary
Yuriy Yusim, Enrico Trevisanello, Raffael Ruess, Felix H. Richter, Alexander Mayer, Dominic Bresser, Stefano Passerini, Juergen Janek, Anja Henss
Summary: Solid-state batteries (SSBs) with high-voltage cathode active materials (CAMs) often face voltage related cell failure caused by lithium dendrite penetration. In this study, it is shown that using higher molecular weight poly(ethylene oxide) (PEO) as a modification to the solid polymer electrolyte (SPE) can improve cycling stability.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Biographical-Item
Chemistry, Physical
Diana Golodnistky, Steve Greenbaum, Kristina Edstro, Stefano Passerini
JOURNAL OF POWER SOURCES
(2023)
Article
Chemistry, Physical
Bingsheng Qin, Maider Zarrabeitia, Alexander Hoefling, Zenonas Jusys, Xu Liu, Jens Tuebke, R. Jurgen Behm, Guanglei Cui, Alberto Varzi, Stefano Passerini
Summary: The utilization of ether electrolytes in sodium batteries has been restricted due to oxidation stability concerns. In this study, the use of a 1M NaPF6-diglyme solution on Na3V2(PO4)(2)F-3 polyanionic cathodes is found to form a unique polymer-inorganic cathode-electrolyte-interphase (CEI), resulting in excellent cyclability (96.2% capacity retention after 300 cycles at 0.5C) and outstanding rate capability (124, 120, and 112 mAh g(-1) at 5C, 10C, and 20C, respectively). This peculiar interfacial chemistry may open up new opportunities for high-performance sodium batteries.
JOURNAL OF POWER SOURCES
(2023)
Article
Electrochemistry
Zenonas Jusys, R. Juergen Behm
Summary: Reversible Mg deposition/stripping and O-2 reduction/evolution reactions on a Pt film electrode immersed in neat and O-2-saturated 1-butyl-1-methylpyrrolidinium bis(trifluoromethylsulfonyl)imide (BMP-TFSI) electrolytes were studied using online differential electrochemical mass spectrometry (DEMS) and scanning electron microscopy/energy dispersed X-ray spectroscopy. The presence of Mg(TFSI)(2), Mg(BH4)(2), and the crown ether 18-c-6 as additives was also investigated. The results reveal a complex network of parallel reactions, including borohydride electro-oxidation, Mg deposition/stripping, and oxygen reduction/evolution, as well as electrolyte decomposition. These findings provide insights into the reactions occurring under these conditions and have implications for Mg-air battery applications.
Article
Electrochemistry
Daniel Roscher, Yongil Kim, Dominik Stepien, Maider Zarrabeitia, Stefano Passerini
Summary: Transitioning to solid-state batteries with polymer electrolytes can enhance safety and enable higher energy densities. This study develops solvent-free ternary polymer electrolytes based on cross-linked polyethylene oxide (PEO), sodium bis(fluorosulfonyl) imide (NaFSI) or sodium bis(trifluoromethanesulfonyl) imide (NaTFSI), and N-butyl-N-methyl-pyrrolidinium-based ionic liquids (ILs, Pyr(14)FSI or Pyr(14)TFSI). These polymer electrolytes demonstrate good thermal and electrochemical stability, as well as high ionic conductivities, making them suitable for use in sodium-metal batteries operating at room temperature.
BATTERIES & SUPERCAPS
(2023)
Article
Chemistry, Physical
Alessandro Innocenti, Isaac Alvarez Moises, Jean-Francois Gohy, Stefano Passerini
Summary: Dual-ion batteries are a viable option for electrochemical energy storage, but the participation of both cations and anions in redox reactions requires the addition of sufficient salt in the electrolyte. To address this, a modified pseudo-2D Doyle-Fuller-Newman model is proposed to simulate the variation of average salt concentration in dual-ion batteries. The model has been validated with experimental data and can help optimize the design of practical dual-ion batteries.
JOURNAL OF POWER SOURCES
(2023)
Article
Chemistry, Physical
Mariam Maisuradze, Min Li, Angelo Mullaliu, Andrea Sorrentino, Dino Tonti, Stefano Passerini, Marco Giorgetti
Summary: Manganese hexacyanoferrate shows promise as a cathode material for lithium and sodium ion batteries, but it experiences capacity fading during cycling. Soft X-ray microscopy is used to investigate the structural and functional characteristics of fresh and cycled electrodes at the nanometer scale. The study reveals inhomogeneities within the samples, particularly in the aged electrodes, and a correlation between different oxidation states and electron delocalization over the host framework.
Review
Chemistry, Physical
Huihua Li, Zhen Chen, Leilei Zheng, Jian Wang, Henry Adenusi, Stefano Passerini, Huang Zhang
Summary: This review examines the functionalities of the solid-electrolyte interphase (SEI) in rechargeable aqueous zinc-metal batteries (AZBs) and how its composition affects the reversibility of the zinc-metal anode. It also discusses recent developments in improving the long-term stability of the zinc anode through controlling key interfacial behaviors. Finally, remaining challenges and future perspectives are presented for the rational design of high-performance AZBs.
Article
Materials Science, Multidisciplinary
Fanglin Wu, Angelo Mullaliu, Thomas Diemant, Dominik Stepien, Tatjana N. Parac-Vogt, Jae-Kwang Kim, Dominic Bresser, Guk-Tae Kim, Stefano Passerini
Summary: High-voltage nickel-rich layered cathodes have excellent discharge capacity and high energy density but are structurally and interfacially unstable at high voltages (>4.3 V). By using lithium borate salts as electrolyte additives, an enhanced cathode-electrolyte interphase is generated to improve the stability. Specifically, the use of lithium bis(oxalato)borate (LiBOB) leads to enhanced cycling stability and almost no voltage hysteresis after 200 cycles at 1C.
Article
Chemistry, Multidisciplinary
Jin Han, Alessandro Mariani, Stefano Passerini, Alberto Varzi
Summary: Highly concentrated aqueous electrolytes with increased salt concentration have the potential to improve the stability and energy of batteries by changing various properties of the electrolyte, such as ionic interactions, solvation structure, ion transport, hydrolysis tendency, and solid electrolyte interphase formation, which significantly depend on the salt anion. This review aims to analyze and explain the role of the salt anion in these properties to offer guidelines for future developments.
ENERGY & ENVIRONMENTAL SCIENCE
(2023)
Review
Chemistry, Multidisciplinary
Wenhua Zuo, Alessandro Innocenti, Maider Zarrabeitia, Dominic Bresser, Yong Yang, Stefano Passerini
Summary: Lithium-ion batteries (LIBs) are widely used in portable electronic devices and electric vehicles, but the high cost of lithium has led to the exploration of sodium-ion batteries (NIBs) as a cheaper alternative. NIBs have the advantages of abundant sodium resources and the use of inexpensive materials. However, the development of NIBs faces challenges such as irreversible phase transformations, poor air stability, and complex charge-compensation mechanisms.
ACCOUNTS OF CHEMICAL RESEARCH
(2023)
Article
Electrochemistry
Fanglin Wu, Huihua Li, Thomas Diemant, Angelo Mullaliu, Huang Zhang, Stefano Passerini
Summary: Investigating materials for sodium-ion batteries is challenging due to the lack of suitable reference electrode. This study explores a new Na0.6Ni0.22Al0.11Mn0.66O2 material as a negative electrode, which exhibits outstanding cycling performance and high stability, serving as a reference for the investigation of other electrode materials.
Article
Chemistry, Physical
Fanglin Wu, Zhen Chen, Shan Fang, Wenhua Zuo, Guk-Tae Kim, Stefano Passerini
Summary: Interfacial issues hinder the progress of current solid-state battery technology, and interface engineering approaches are needed to achieve solid-state configuration. Ionic liquids, which are viscous and nonflammable, can optimize the interface between solid electrodes and solid electrolytes, accelerate ion transport at the interface, and create engineered interphases using robust chemical building blocks. This review summarizes the roles of ionic liquids in solid-state batteries, with a focus on the interface, and highlights their functionality and applicability in next-generation battery systems.
ENERGY STORAGE MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Xu Liu, Alessandro Mariani, Thomas Diemant, Maria Enrica Di Pietro, Xu Dong, Andrea Mele, Stefano Passerini
Summary: Trifluoromethoxybenzene as a cosolvent in locally concentrated ionic liquid electrolytes (LCILEs) can enhance the protective electrode/electrolyte interphases (EEIs) in lithium metal batteries, leading to stable cycling of the batteries.
ADVANCED MATERIALS
(2023)
