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Rechargeable aqueous zinc‐ion batteries (ZIBs) have been considered as a promising candidate for the large‐scale energy storage device owing to their low cost and high safety. However, the practical application of aqueous ZIBs at low temperature environment is hindered by the freezing aqueous electrolytes, which leads to a sharp drop in ionic conductivity, and thereby a rapid deterioration of battery performance. Herein, a chaotropic salt electrolyte based on low concentration aqueous Zn(ClO4)2 with superior ionic conductivity under low temperature (4.23 mS/cm at −50°C) is reported. The anti‐freezing methodology introduced here is completely different from conventional freeze‐resistant design of using “water‐in‐salt” electrolyte, cosolvents, or anti‐freezing agent additives strategy. Experimental analysis and molecular dynamics simulations reveal that the as‐prepared Zn(ClO4)2 electrolyte possesses faster ionic migration compared with other commonly used Zn‐based salts (i.e., Zn(CF3SO3)2 and ZnSO4) electrolyte. It is found that Zn(ClO4)2 electrolyte can suppress the ice crystal construction by forming more hydrogen bonds between solute ClO4− and solvent H2O molecules, thus leading to a superior anti‐freezing property. The fabricated ZIBs using this aqueous electrolyte exhibits a dramatically enhanced specific capacity, remarkable rate capability, and great cycling stability over a wide temperature range, from −50 to 25°C. The aqueous ZIBs also exhibit an outstanding energy density of 238.4 Wh/kg without compromising the power density (7.9 kW/kg) under −20°C. Moreover, the assembled aqueous ZIBs can also cycle stably over 1000 cycles at an ultra‐low −50°C. The high‐safety and cost‐effective chaotropic salt electrolyte presented here is a promising strategy for low temperature energy storage application. A cost‐effective, anti‐freezing, and high ionic conductivity Zn(ClO4)2 chaotropic salt electrolyte is discovered and applied in low‐temperature aqueous zinc‐ion battery.

HighlightsDetailed discussion and summary of aqueous electrolyte chemistry, parasitic reactions chemistry, and storage energy chemistry and their relationship in aqueous zinc ions batteries are conducted.The recent development of strategies for enhancing the inherent stability of electrolyte and zinc anode to restrain parasitic reactions is reviewed from a thermodynamic perspective.The regulation strategies of electrolyte/electrode interfaces to block parasitic reactions by adsorbents and solid electrolyte interphase are reviewed from a kinetic perspective. Based on the attributes of nonflammability, environmental benignity, and cost-effectiveness of aqueous electrolytes, as well as the favorable compatibility of zinc metal with them, aqueous zinc ions batteries (AZIBs) become the leading energy storage candidate to meet the requirements of safety and low cost. Yet, aqueous electrolytes, acting as a double-edged sword, also play a negative role by directly or indirectly causing various parasitic reactions at the zinc anode side. These reactions include hydrogen evolution reaction, passivation, and dendrites, resulting in poor Coulombic efficiency and short lifespan of AZIBs. A comprehensive review of aqueous electrolytes chemistry, zinc chemistry, mechanism and chemistry of parasitic reactions, and their relationship is lacking. Moreover, the understanding of strategies for suppressing parasitic reactions from an electrochemical perspective is not profound enough. In this review, firstly, the chemistry of electrolytes, zinc anodes, and parasitic reactions and their relationship in AZIBs are deeply disclosed. Subsequently, the strategies for suppressing parasitic reactions from the perspective of enhancing the inherent thermodynamic stability of electrolytes and anodes, and lowering the dynamics of parasitic reactions at Zn/electrolyte interfaces are reviewed. Lastly, the perspectives on the future development direction of aqueous electrolytes, zinc anodes, and Zn/electrolyte interfaces are presented.

Zinc electrodeposition serves as a crucial electrochemical process widely employed in various industries, particularly in automotive manufacturing, owing to its cost effectiveness compared to traditional methods. However, traditional zinc electrodeposition using aqueous solutions faces challenges related to toxicity and hydrogen gas generation. Non-aqueous electrolytes such as ionic liquids (ILs) and deep eutectic solvents (DESs) have gained attention, with choline-chloride-based DESs showing promise despite raising environmental concerns. In this study, zinc electrodeposition on mild steel was investigated using three distinct electrolytes: (i) halide-free aqueous solutions, (ii) chloride-based DES, and (iii) halide-free acetate-based organic solutions. The study examined the influence of deposition time on the growth of Zn on mild steel substrates from these electrolytes using physical characterization techniques, including scanning electron microscopy (SEM) and X-ray diffraction (XRD). The results indicate that glycol + acetate-based non-aqueous organic solutions provide an eco-friendly alternative, exhibiting comparable efficiency, enhanced crystalline growth, and promising corrosion resistance. This research contributes valuable insights into the impact of electrolyte choice on zinc electrodeposition, offering a pathway towards more sustainable and efficient processes. Through a comprehensive comparison and analysis of these methods, it advances our understanding of the practical applications of zinc electrodeposition technology.

Recently, the electrochemical N 2 reduction reaction (NRR) in aqueous electrolytes at ambient temperature and pressure has demonstrated its unique advantages and potentials. The reactants are directly derived from gaseous N 2 and water, which are naturally abundant, and NH 3 production is important for fertilizers and other industrial applications. To improve the conversion yield and selectivity (mainly competing with water reduction), electrocatalysts must be rationally designed to optimize the mass transport, chemisorption, and transduction pathways of protons and electrons. In this review, we summarize recent progress in the electrochemical NRR. Studies of electrocatalyst designs are summarized for different categories, including metal-based catalysts, metal oxide-derived catalysts, and hybrid catalysts. Strategies for enhancing the NRR performance based on the facet orientation, metal oxide interface, crystallinity, and nitrogen vacancies are presented. Additional system designs, such as lithium-nitrogen batteries, and the solvent effect are introduced. Finally, existing challenges and prospects are discussed.

Supercapacitors are promising energy storage devices that combine high power density, fast charge/discharge rates, and excellent cycling stability. However, their relatively low energy density compared to batteries remains a major challenge. To address this limitation, redox additive electrolytes have emerged as a key strategy to introduce reversible Faradaic reactions, significantly enhancing the energy storage capacity of supercapacitors. This mini-review systematically summarizes recent advancements in the use of redox-active species across aqueous, non-aqueous, and solid-state/gel electrolytes. We highlight the role of both inorganic and organic redox additives, detailing their mechanisms, advantages, and limitations in improving energy density and stability. Furthermore, we discuss the challenges associated with redox species, such as solubility, long-term stability, and parasitic side reactions, which hinder their practical applications. Future research directions are proposed to optimize redox-active materials and electrolyte systems, aiming to develop next-generation supercapacitors with superior energy density, extended cycling life, and enhanced applicability.

HighlightsThis Review encompasses the role, requirement, and development direction of water-based electrolytes for sustainable, safe, high-performance Li-ion batteries.Water-based electrolytes (aqueous liquid and gel electrolytes) and their mechanisms are comprehensively summarized to widen the electrolyte electrochemical stability window and battery operating voltage and to achieve long-term operation stability.Current lithium-ion batteries (LIBs) rely on organic liquid electrolytes that pose significant risks due to their flammability and toxicity. The potential for environmental pollution and explosions resulting from battery damage or fracture is a critical concern. Water-based (aqueous) electrolytes have been receiving attention as an alternative to organic electrolytes. However, a narrow electrochemical-stability window, water decomposition, and the consequent low battery operating voltage and energy density hinder the practical use of aqueous electrolytes. Therefore, developing novel aqueous electrolytes for sustainable, safe, high-performance LIBs remains challenging. This Review first commences by summarizing the roles and requirements of electrolytes–separators and then delineates the progression of aqueous electrolytes for LIBs, encompassing aqueous liquid and gel electrolyte development trends along with detailed principles of the electrolytes. These aqueous electrolytes are progressed based on strategies using superconcentrated salts, concentrated diluents, polymer additives, polymer networks, and artificial passivation layers, which are used for suppressing water decomposition and widening the electrochemical stability window of water of the electrolytes. In addition, this Review discusses potential strategies for the implementation of aqueous Li-metal batteries with improved electrolyte–electrode interfaces. A comprehensive understanding of each strategy in the aqueous system will assist in the design of an aqueous electrolyte and the development of sustainable and safe high-performance batteries.

The growing demands for ammonia in agriculture and transportation fuel stimulate researchers to develop sustainable electrochemical methods to synthesize ammonia ambiently, to get past the energy-intensive Haber-Bosch process. However, the conventionally used aqueous electrolytes limit N₂ solubility, leading to insufficient reactant molecules in the vicinity of the catalyst during electrochemical nitrogen reduction reaction (NRR). This hampers the yield and production rate of ammonia, irrespective of how efficient the catalyst is. Herein, we introduce an aqueous electrolyte (NaBF₄), which not only acts as an N₂-carrier in the medium but also works as a full-fledged “co-catalyst” along with our active material MnN₄ to deliver a high yield of NH₃ (328.59 μg h−1 mgcat −1) at 0.0 V versus reversible hydrogen electrode. BF₃-induced charge polarization shifts the metal d-band center of the MnN₄ unit close to the Fermi level, inviting N₂ adsorption facilely. The Lewis acidity of the free BF₃ molecules further propagates their importance in polarizing the N≡N bond of the adsorbed N₂ and its first protonation. This push-pull kind of electronic interaction has been confirmed from the change in d-band center values of the MnN₄ site as well as charge density distribution over our active model units, which turned out to be effective enough to lower the energy barrier of the potential determining steps of NRR. Consequently, a high production rate of NH₃ (2.45 × 10−9 mol s−1 cm−2) was achieved, approaching the industrial scale where the source of NH₃ was thoroughly studied and confirmed to be chiefly from the electrochemical reduction of the purged N₂ gas.

With the increasing demand and striking upsurge in the price of lithium carbonate, sodium-ion batteries (SIBs) have gained significant attentions due to their abundance over lithium-ion batteries (LIBs). Some prototype SIBs have achieved great progress in terms of energy densities. Although SIBs show a relatively higher tolerance at the low temperature than LIBs due to the weaker cation–solvent interaction, the low-temperature performance of SIBs remains a critical challenge restricted by the electrolyte solidification and sluggish interphasial kinetics. In this review, we briefly cover the latest research progress in usable low-temperature electrolytes for SIBs. In the meantime, the mitigating mechanism and low-temperature performance of the electrolytes in different SIB configurations are also discussed. The merits and demerits of ether-based and carbonate-based electrolytes are compared to demonstrate their potential and limitations, thus providing application principles for ether-based and carbonate-based electrolytes at low temperatures to maximize their advantages. Furthermore, mitigation strategies for low-temperature electrolytes are emphasized to guide the future electrolyte design. Finally, we provide some perspectives on the development of the low-temperature electrolytes for SIBs.

Aqueous Zn‐ion batteries (AZIBs) are regarded as a promising alternative to the widely used lithium‐ion batteries in large‐scale energy storage systems. The researches on the development of novel aqueous electrolyte to improve battery performance have also attracted great interest since the electrolyte is a key component for Zn2+ migration between cathode and anode. Herein, we briefly summarized and illuminated the recent development tendency of aqueous electrolyte for AZIBs, then deeply analyzed its existing issues (water decomposition, cathode dissolution, corrosion and passivation, and dendrite growth) and discussed the corresponding optimization strategies (pH regulation, concentrated salt solution, electrolyte composition design, and functional additives). The internal mechanisms of these strategies were further revealed and the relationships between issues and solutions were clarified, which could guide the future development of aqueous electrolytes for AZIBs. This review reveals the internal mechanisms of these strategies and clarifies the relationships between different issues and solutions for aqueous Zn‐ion batteries.

The present work reports the synthesis of biomass derived activated carbon and its electrochemical behaviour in different electrolytes. Ricinus communis shell (RCS) was used as a raw material in this study for the synthesis of activated carbon (AC) following a high-temperature activation procedure using potassium hydroxide as the activating agent. The physical and structural characterization of the prepared Ricinus communis shell-derived activated carbon (RCS-AC) was carried by Brunauer-Emmett-Teller analysis, X-ray diffraction analysis, Fourier Transform Infrared Spectroscopy, Raman Spectroscopy and Scanning Electron Microscopy. The synthesized AC was electrochemically characterized using various techniques such as Cyclic voltammetry (CV), galvanostatic charge–discharge (GCD) tests, and Electrochemical impedance spectroscopy (EIS) measurements in different aqueous electrolytes (KOH, H2SO4, and Na2SO4). The results show that the double layer properties of the RCS-AC material in different electrolytes are distinct. In specific, the working electrode tested in 3 M KOH showed excellent electrochemical performance. It demonstrated a specific capacitance of 137 F g−1 (at 1 A g−1 in 3 M KOH) and exhibited high energy and power densities of 18.2 W hkg−1 and 663.4 W kg−1, respectively. The observed capacitance in 3 M KOH remains stable with 97.2% even after 5000 continuous charge and discharge cycles, indicating long-term stability. The study confirmed that the synthesized RCS-derived activated carbon (RCS-AC) exhibits good stability and physicochemical characteristics, making them commercially promising and appropriate for energy storage applications.