Cycling Performance Research Articles

Tailoring Practical Solid Electrolyte Composites Containing Ferroelectric Ceramic Nanofibers and All-Trans Block Copolymers for All-Solid-State Lithium Metal Batteries.

Ion transport efficiency, the key to determining the cycling stability and rate capability of all-solid-state lithium metal batteries (ASSLMBs), is constrained by ionic conductivity and Li+-migration ability across the multicomponent phases and interfaces in ASSLMBs. Here, we report a robust strategy for the large-scale fabrication of a practical solid electrolyte composite with high-throughput linear Li+-transport channels by compositing an all-trans block copolymer PVDF-b-PTFE matrix with ferroelectric BaTiO3-TiO2 nanofiber films. The electrolyte shows a sustainable electromechanical-coupled deformability that enables the rapid dissociation of anions with Li+ to create more movable Li+ ions and spontaneously transform the battery internal strain into Li+-ion migration kinetic energy. The ceramic framework homogenizes the interfacial potential with electrodes, endowing the electrolyte with a high conductivity of 0.782 mS·cm-1 and stable ion transport ability in ASSLMBs at room temperature. The batteries of LiFePO4/Li can stably cycle 1000 times at 0.5 C with a high capacity retention of 96.1%, and Ah-grade pouch or high-voltage Li(Ni0.8Mn0.1Co0.1)O2/Li batteries also exhibit excellent rate capability and cycling performance.

Protector-free, non-plasmonic silver quantum clusters by femtosecond pulse laser irradiation: in situ binding on nanocellulose filaments for improved catalytic activity and cycling performance.

This study introduces a new, facile method to synthesize silver clusters from aqueous silver ion solution by using high intensity femtosecond pulse laser irradiation. The particles obtained in the absence of reducing or capping agents are 1-17 nm in size and presented quantum properties, as characterized by fluorescence, but did not exhibit plasmon signals, which is not a common characteristic of conventional silver nanoparticles. In a further development, small silver quantum clusters (∼1 nm) were bound in situ to wet-spun filaments of cellulose nanofibrils by pulsed laser irradiation. The obtained hybrid filaments as well as free silver quantum clusters revealed a catalytic activity remarkably higher than that of free gold quantum clusters; moreover, the hybrid filaments were found to show improved stability and cycling performance for silver-based catalysis. The present results indicate the potential of femtosecond laser irradiation to generate clusters as well as hybrid systems with excellent performance and reactivity.

Thickness Variation of Conductive Polymer Coatings on Si Anodes for the Improved Cycling Stability in Full Pouch Cells.

Si-dominant anodes for Li-ion batteries provide very high gravimetric and volumetric capacity but suffer from low cycling stability due to an unstable solid electrolyte interphase (SEI). In this work, we improved the cycling performance of Si/NCM pouch cells by coating the Si anodes with the conductive polymer poly(3,4-ethylenedioxythiophene) (PEDOT) prior to cell assembly via an electropolymerization process. The thicknesses of the PEDOT coatings could be adjusted by a facile process parameter variation. Glow-discharge optical emission spectroscopy was used to determine the coating thicknesses on the electrodes prior to the cell assembly. During electrochemical testing, improvements were observed closely linked to the PEDOT coating thickness. Specifically, thinner PEDOT coatings exhibited a higher capacity retention and lower internal resistance in the corresponding pouch cells. For the thinnest coatings, the cell lifetime was 18% higher compared to that of uncoated Si anodes. Postmortem analyses via X-ray photoelectron spectroscopy and cross-sectional scanning electron microscopy revealed a better-maintained microstructure and a chemically different SEI for the PEDOT-coated anodes.

2D-on-2D Al-Doped NiCo LDH Nanosheet Arrays for Fabricating High-Energy-Density, Wide Voltage Window, and Ultralong-Lifespan Supercapacitors.

Battery-type electrode materials with high capacity, wide potential windows, and good cyclic stability are crucial to breaking through energy storage limitations and achieving high energy density. Herein, a novel 2D-on-2D Al-doped NiCo layered double hydroxide (NiCoAlx LDH) nanosheet arrays with high-mass-loading are grown on a carbon cloth (CC) substrate via a two-step hydro/solvothermal deposition strategy, and the effect of Al doping is employed to modify the deposition behavior, hierarchical morphology, phase stability, and multi-metallic synergistic effect. The optimized NiCoAl0.1 LDH electrode exhibits capacities of 5.43, 6.52, and 7.25 C cm-2 (9.87, 10.88, and 11.15 F cm-2) under 0-0.55, 0-0.60, and 0-0.65V potential windows, respectively, illustrating clearly the importance of the wide potential window. The differentiated deposition strategy reduces the leaching level of Al3+ cations in alkaline solutions, ensuring excellent cyclic performance (108% capacity retention after 40000 cycles). The as-assembled NiCoAl0.1 LDH//activated carbon cloth (ACC) hybrid supercapacitor delivers 3.11 C cm-2 at 0-2.0V, a large energy density of 0.84 mWh cm-2 at a power density of 10.00mW cm-2, and excellent cyclic stability with ≈135% capacity retention after 150000 cycles.

N-Doping-Induced Amorphization for Achieving Ultrastable Aqueous Zinc-Ion Batteries.

Vanadium-based oxides, known for their high capacity and low cost, have garnered significant attention as promising cathode candidates in aqueous zinc-ion batteries. Nonetheless, their poor rate performance and limited durability in aqueous electrolytes present a challenge to the realistic implementation of vanadium-based aqueous zinc-ion batteries. Here, we synthesized nitrogen-doped V2O3@C (N-V2O3@N-C) via ammonia treatment of V2O3@C derived from vanadium-based metal-organic framework (V-MOF), aiming to achieve outstanding rate and cycling performance. The N-V2O3@N-C electrode exhibits notable in situ self-transformation into an amorphous state. Density functional theory calculations reveal that the distorted N-V2O3 structure and uneven charge distribution result in the creation of an amorphous state. As expected, Zn/N-V2O3@N-C aqueous zinc-ion batteries can achieve remarkable specific capacity (349.0 mAh g-1 at 0.1 A g-1), along with impressive rate performance, showcasing a capacity of 253.5 mAh g-1 at 5 A g-1 and exceptional durability at 5 A g-1 (96.4% after 1350 cycles). The employed induced amorphization approach offers novel perspectives for designing high-performance cathodes that exhibit both sturdy structures and extended cycling lifespans.

Upgrading Electrolyte Antioxidant Chemistry by Constructing Potential Scaling Relationship.

Rational design of advanced electrolytes to improve the high-voltage capability has been attracting wide attention as one critical solution to enable next-generation high-energy-density batteries. However, the limited understanding of electrolyte antioxidant chemistry as well as the lack of valid quantization approaches have resulted in knowledge gap, which hinders the formulation of new electrolytes. Herein, we construct a standard curve based on representative solvation structures to quantify the oxidation stability of ether-based electrolytes, which reveals the linear correlation between the oxidation potential and the atomic charge of the least oxidation-resistant solvent. Dictating by the regularity between solvation composition and oxidation potential, a (Trifluoromethyl)cyclohexane-based localized high-concentration electrolyte dominated by anion-less solvation structures was designed to optimize the cycling performance of 4.5 V 30-μm-Li||3.8-mAh cm-2-LiCoO2 batteries, which maintained 80% capacity retention even after 440 cycles. The consistency of experimental and computational results validates the proposed principles, offering a fundamental guideline to evaluate and design aggressive electrochemical systems.

Inhibiting Residual Solvent induced side reactions in Vinylidene Fluoride-based Polymer Electrolytes enables ultra-stable Solid-State Lithium Metal Batteries.

Residual solvents in vinylidene fluoride (VDF)-based solid polymer electrolytes (SPEs) have been recognized as responsible for their high ionic conductivity. However, side reactions by the residual solvents with the lithium (Li) metal induce poor stability, which has been long neglected. This study proposes a strategy to achieve a delicate equilibrium between ion conduction and electrode stability for VDF-based SPEs. Specifically, 2,2,2-Trifluoro-N, N-dimethylacetamide (FDMA) is developed as the non-side reaction solvent for poly(vinylidene fluoride-co-hexafluoropropylene) (PVHF)-based SPEs, achieving both high ionic conductivity and significantly improved electrochemical stability. The developed FDMA solvent fosters the formation of a stable solid electrolyte interphase (SEI) through interface reactions with Li metal, effectively mitigating side reactions and dendrite growth on the Li metal electrode. Consequently, the Li||Li symmetric cells and Li||LiFePO4 cells demonstrate excellent cycling performance, even under limited Li (20μm thick) supply and high-loading cathodes (>10mg cm-2, capacity >1 mAh cm-2) conditions. The stable Li||LiCoO2 cells operation with a cutoff voltage of 4.48V indicates the high-voltage stability of the developed SPE. This study offers valuable insights into developing advanced VDF-based SPEs for enhanced lithium metal battery performance and longevity. This article is protected by copyright. All rights reserved.

Precycling Strategy in Suitable Voltage to Improve the Stability of Interfacial Film and Suppress the Decline of LiNi0.6Mn0.2Co0.2O2 Cathode at Elevated Temperatures.

Layered ternary oxide LiNixMnyCo1-x-yO2 is a promising cathode candidate for high-energy lithium-ion batteries (LIBs). However, the capacity of LIBs is significantly restricted by several factors, including the repeated dissolution-regeneration of the interfacial film at high temperatures, the dissolution of transition metals, and the increase of impedance. Herein, a new precycling strategy in suitable voltage scope at room temperature is proposed to construct a uniform, thermally stable, and insoluble cathode-electrolyte interface (CEI), which helps to maintain stable cycling performances at high temperatures. Specifically, after 5 precycles in the range of 3.85-4.3 V at room temperature, a CEI layer containing numerous inorganic components and oligomers is formed on the surface of LiNi0.6Mn0.2Co0.2O2. Subsequently, the harmful side reactions are effectively suppressed, endowing the cell with an excellent capacity retention of 84.67% after 50 cycles at 0.5C and 55 °C, much higher than that of 65.61% under the conventional film-forming process conditions. This work emphasizes the crucial role of the precycling strategy in regulating the characteristics of CEI layer on the surface of cathode electrode, opening up a new avenue for the high-temperature application of positive electrodes of LIBs.

Rational design of hollow C@SnS2/SnS@C cubes with N-doping to realize stepwise sodium storage induced structural stability for highly stable cycling performance

Current application of SnS2-based anodes in sodium-ion batteries fails to meet the demand for higher Na+ storage capacity due to the structural pulverization induced by significant volume changes during cycling. Herein, a novel composite of hollow C@SnS2/SnS@C cubes with excellent diffusion kinetics and structural stability from stepwise Na+ storage is designed. The SnS with gentle pseudocapacitive reaction acts as the self-supporter to prevent the collapse of SnS2/SnS heterostructure during the Na+ insertion/extraction. Together with the clamping of double carbon layers and hollow construction, the volume change caused structural instability in heterostructure is effectively alleviated. The rapid transport of electrons and ions within the built-in electric field of heterostructure endows the composite an excellent diffusion kinetics, which is generated from the narrow bandgap and outstanding Na+ absorption of heterostructure according to the first-principle calculation. Thus, the as-prepared composite maintains a remarkable capacity of 547.9 mAh g−1 after 200 cycles at current density of 0.5 A g−1. Even a capacity of 502.5 mAh g−1 with a low attenuation rate of 0.035 % per cycle is achieved at 2 A g−1 after 1000 cycles. The work proposes an effective approach to achieve effective Na + storage of SnS2-based anodes with long-lasting structural stability.

Behavior of group of geosynthetic encased granular piles with tire chips- aggregates mixture under static and cyclic loading – A model study

The current study addresses the dual challenges of improving the performance of soft soil beds subjected to static and cyclic stresses and managing the environmental impact of waste tire disposal. This research contributes valuable insights into the sustainable use of recycled tire chips in granular pile construction, coupled with the efficacy of combi-grid encasement for improved soft ground under static and cyclic loading conditions. A series of laboratory model tests were carried out on a group of granular piles to examine the principal parameters, such as the selection of geosynthetic materials and cyclic loading characteristics, including cyclic loading amplitude (qca) and cyclic loading frequency (f). The granular pile composition consists of (25% tire chips + 75% aggregates). The performance of granular piles on improved ground is assessed based on the settlement reduction ratio (Sc,r), accumulation of excess pore water pressure (Pexc), and stress concentration ratio (n). The key findings from static model tests are that the load-bearing capacity is significantly increased with installing a group of ordinary granular piles (= 58%) and substantially increased with combi-grid encasement (= 335%). The effectiveness of ordinary granular piles (OGP) in enhancing the performance of a soft soil bed becomes greater when subjected to lower cyclic loading frequencies (f) and smaller cyclic loading amplitudes (qca). The incorporation of combi-grid encasement greatly enhanced the cyclic performance of a group of granular piles by substantially minimizing cyclic-induced settlement (Sc) across both principle parameters f and qca. This study also examines the increased cyclic stresses on the improved soft bed, resulting in the accumulation of excess pore water pressure (Pexc) development, which is reduced to a greater extent with the help of combi-grid encasement across both principle parameters.

High-Temperature Cyclic Oxidation Behavior and Microstructure Evolution of W- and Ce-Containing 18Cr-Mo Type Ferritic Stainless Steel

Due to the recurrent starting and stopping operations of automobiles during service, their engines’ hot ends are continually subjected to high-temperature cyclic oxidation. Therefore, it is crucial to develop ferritic stainless steels with better high-temperature oxidation resistance. This study focuses on improving the high-temperature cyclic oxidation performance of 18Cr-Mo (444-type) ferritic stainless steel by alloying with high-melting-point metal W and the rare earth element Ce. For this purpose, a high-temperature cyclic oxidation experiment was designed to simulate the actual service environment and investigate the high-temperature cyclic oxidation behavior and microstructure evolution of 444-type ferritic stainless steel alloyed with W and Ce. The oxide structure and composition formed during this process were analyzed and characterized using scanning electron microscopy/energy dispersive spectroscopy (SEM-EDS) and electron probe X-ray micro-analyzer (EPMA), in order to reveal the mechanism of action of W and Ce in the cyclic oxidation process. The results show that 18Cr-Mo ferritic stainless steel alloyed with W and Ce exhibits an excellent resistance to high-temperature cyclic oxidation. The element W can promote the precipitation of the Laves phase between the matrix and the oxide film, and the small-sized Laves phase can inhibit the interfacial diffusion of oxidation reaction elements and prevent the inward growth of the oxide film. The element Ce can refine oxide particles and reduce the thickness of the oxide film. CeO2 particles within the oxide film can serve as nucleation sites for the formation of oxide particles from reactive elements, and they also contribute to pinning the oxide film, thereby enhancing its adhesion.

Stabilizing the Bulk-Phase and Solid Electrolyte Interphase of Silicon Microparticle Anode by Constructing Gradient-Hierarchically Ordered Conductive Networks.

The poor bulk-phase and interphase stability, attributable to adverse internal stress, impede the cycling performance of silicon microparticles (µSi) anodes and the commercial application for high-energy-density lithium-ion batteries. In this work, a groundbreaking gradient-hierarchically ordered conductive (GHOC) network structure, ingeniously engineered to enhance the stability of both bulk-phase and the solid electrolyte interphase (SEI) configurations of µSi, is proposed. Within the GHOC network architecture, two-dimensional (2D) transition metal carbides (Ti3C2Tx) act as a conductive "brick", establishing a highly conductive inner layer on µSi, while the porous outer layer, composed of one-dimensional (1D) Tempo-oxidized cellulose nanofibers (TCNF) and polyacrylic acid (PAA) macromolecule, functions akin to structural "rebar" and "concrete", effectively preserves the tightly interconnected conductive framework through multiple bonding mechanisms, including covalent and hydrogen bonds. Additionally, Ti3C2Tx enhances the development of a LiF-enriched SEI. Consequently, the µSi-MTCNF-PAA anode presents a high discharge capacity of 1413.7 mAh g-1 even after 500 cycles at 1.0 C. Moreover, a full cell, integrating LiNi0.8Mn0.1Co0.1O2 with µSi-MTCNF-PAA, exhibits a capacity retention rate of 92.0% following 50 cycles. This GHOC network structure can offer an efficacious pathway for stabilizing both the bulk-phase and interphase structure of anode materials with high volumetric strain.

LiF‐Rich Solid Electrolyte Interfaces Guarantee the Cycle Stability of Metal‐Organic Frameworks for Lithium Storage

Metal‐organic framework materials (MOFs) with hierarchical porosity, structural tunability, and rich redox‐active centers have attracted intensive attention as potential substitutes for carbonaceous anode materials. However, the practical commercialization of MOFs still remains a challenge, due to uncontrollable performance degradation. Inspired by the prolonged lifespans of traditional anode materials with LiF‐rich solid electrolyte interface (SEI), the roles of LiF are examined in enhancing the cycle stability of MOFs, with copper benzenedicarboxylate (Cu‐BDC) as an example. By adjusting the electrolyte composition, the cycle performance of Cu‐BDC material is optimized, due to the generation of LiF‐rich SEI. In the optimal 3 M LiPF6 electrolyte, the formed SEI membrane is the thinnest, and the LiF content is the highest, so the Cu‐BDC shows a specific charge/discharge capacity of 378/387.2 mAh g−1 after 100 cycles at 100 mA g−1, comparing to less than 200 mAh g−1 in the electrolyte with 1% vinyl carbonate.

Hybrid Ceramic Polymer Electrolytes Enabling Long Cycling in Practical 1 Ah‐Class High‐Voltage Solid‐State Batteries with Li Metal Anode

AbstractSolid polymer electrolytes offer a safer alternative to organic liquid electrolytes in high‐voltage lithium metal batteries, yet challenges remain in achieving adequate cyclability, energy density, scalability, and safety. This study presents the cycling performance of 1 Ah high‐voltage lithium polymer batteries featuring a hybrid ceramic polymer electrolyte (HCPE), a lithium metal anode, and a LiNi0.8Mn0.1Co0.1O2 (NMC‐811)‐based positive electrode. The HCPE stands out for its remarkable mechanical properties, with a Young's modulus exceeding 200 MPa at room temperature, providing robust resistance against dendrite formation. The Li||Li symmetric cells exhibited outstanding performance, cycling for over 1000 hours at a capacity of 2 mAh cm−2, highlighting the exceptional attributes of HCPE. Full cell testing is conducted under practical conditions, utilizing various cell configurations, from coin cells to large pouch cells with a 1 Ah capacity, achieving an energy density of nearly 250 Wh kg−1 and promising cyclability with 80% capacity retention after 110 cycles. The study also investigated thermal runaway characteristics, showing comparability with commercial lithium‐ion batteries. This research underscores the scalability and performance of high‐voltage lithium metal polymer batteries, advancing their potential for commercial viability.

Constructing sulfur-rich interphase to promote the cycle stability of graphite/LiNi0.8Co0.1Mn0.1O2 pouch battery at elevated temperature

Lithium-ion batteries (LIBs) with LiNi0.8Co0.1Mn0.1O2 (NCM811) cathodes have a high energy density, but their long-cycle performance, especially at high temperature, should still be improved due to the instability of the NCM811 cathode-electrolyte interphase. In this work, 2, 2, 2-Trifluoroethyl p-Toluenesulfonate (TPTS) is introduced as a functional film-forming electrolyte additive design to improve the long-term stability of graphite/NCM811 batteries. The preferential redox reactions of TPTS molecules play a pivotal role in fostering the creation of a sulfur-riched interphase, characterized by low impedance. This interphase works to fortify the interfacial structure, effectively inhibiting the dissolution of transition metal ions. Therefore, in comparison to the graphite/NCM811 pouch batteries lacking additive, TPTS enhance the long-cycle capacity retention from 47 % to 80 % after 450 cycles at 45 °C. What's more, TPTS suppresses outgassing and demonstrates enhanced capacity maintenance for the battery even after storage at 60 °C. This work not only demonstrates the stabilizing impacts of TPTS on the electrode-electrolyte interphase and its enhancement of cycling performance at elevated temperatures but also introduces a novel approach for the practical utilization of functional electrolytes matching high-nickel LIBs.

One-step fabrication of millimeter-scale hollow vesicles with chitosan /DADMAC/ sodium alginate graft copolymer for enhanced anionic dye adsorption

Hollow vesicles are promising in water treatment due to their unique structure of the membrane and inner cavity. However, the adsorption capacity needs to be improved for targeted pollutants. Herein, millimeter-scale hollow vesicles were prepared with a one-step process of sequential stirring and grafting using chitosan, diallyldimethylammonium chloride, and sodium alginate as raw materials with the purpose of efficient removal of anionic dyes from wastewater. The composite vesicles were characterized using scanning electron microscopy, Fourier transform infrared spectroscopy, X-ray photoelectron spectroscopy, and X-ray diffraction. The hollow vesicles showed the structure of the cationic membrane and the inner cavity, facilitating the dye adsorption. The adsorption capacity for the anionic dye Reactive Black 5 reached 698.1 mg/g, more than twice that of the binary composite vesicles without graft. The adsorption kinetics and isotherm data coincided with the pseudo-second-order and Langmuir models, respectively, and the adsorption mechanism was monolayer chemisorption. Moreover, the vesicles worked well in wide ranges of environment pH, temperature, and co-existing pollutants. They also possessed excellent cyclic regeneration performance, in which 93 % of the initial adsorption capacity was maintained after four cycles. These results indicate that the millimeter-scale hollow vesicles exhibit broad application prospects for wastewater purification.

Interfacial Spinel Local Interlocking Strategy Toward Structural Integrity in P3 Oxide Cathodes.

P3-layered transition oxide cathodes have garnered considerable attention owing to their high initial capacity, rapid Na+ kinetics, and less energy consumption during the synthesis process. Despite these merits, their practical application is hindered by the substantial capacity degradation resulting from unfavorable structural transformations, Mn dissolution and migration. In this study, we systematically investigated the failure mechanisms of P3 cathodes, encompassing Mn dissolution, migration, and the irreversible P3-O3' phase transition, culminating in severe structural collapse. To address these challenges, we proposed an interfacial spinel local interlocking strategy utilizing P3/spinel intergrowth oxide as a proof-of-concept material. As a result, P3/spinel intergrowth oxide cathodes demonstrated enhanced cycling performance. The effectiveness of suppressing Mn migration and maintaining local structure of interfacial spinel local interlocking strategy was validated through depth-etching X-ray photoelectron spectroscopy, X-ray absorption spectroscopy, and in situ synchrotron-based X-ray diffraction. This interfacial spinel local interlocking engineering strategy presents a promising avenue for the development of advanced cathode materials for sodium-ion batteries.

Largely enhanced Piezoelectric-Fenton capability in rationally designed PVDF/Fe2O3 flexible porous film

The burgeoning piezocatalysts have attracted huge attentions due to their ability to convert natural mechanical energy to degrade water pollutants. However, traditional powder-based piezocatalysts still face an inevitable bottleneck of the secondary pollution because of the diffusion of nanoparticles during the piezocatalysis process. In this work, novel porous polymer-based composite films combining Fenton fillers (α-Fe2O3) and ferroelectric polymer (polyvinylidene fluoride, PVDF) are prepared by rationally designed solution-casted method with a sacrificial “hard template” of table salt. The as-prepared porous PVDF/Fe2O3 film exhibits superior decomposition efficiency of organic pollutants under ultrasonication. Particularly, the easily recyclable porous film with optimized composition and spatial structure offers an ultrahigh rate constant of 0.0498 min−1, which means it can degrade 94.8% rhodamine B (RhB) in 60 min, exceeding that of most reported polymer-based piezocatalysts. Additionally, it has a comprehensive decomposition effect on dyes, antibiotics and natural water with a good cycle performance. The outstanding degradation performance is attributed to the massive hydroxyl radical generated from the enhanced Piezoelectric-Fenton effect, which is ascribed to the synergistic effect of improved piezoelectricity in PVDF, enhanced hydrophilicity and optimized spatial structures in the porous composite films.

Characteristics and properties of anode materials for lithium-ion batteries

Lithium-ion secondary batteries (LIBs) are battery systems with high energy densities. They are essential components of todays information-rich, mobile societys portable, entertainment, computing, and telecommunications technology. After 1981, most of the research on anode materials mainly focused on the anode containing Li, such as LiAl alloy, LiC alloy, etc. These materials have high prices, unstable cycling performance, and are difficult to be commercialized. The successful commercialization of LIBs began in 1991 with SONYs manufacturing of petroleum coke-based anode materials. Among them, anode plays a crucial role in LIBs. Anode materials that have been commercialized include carbon, alloys, and lithium titanate. Lithium-ion batteries using carbon anode materials and lithium titanate anode materials can meet the needs of electric vehicles (EVs) and large-scale energy storage applications to a certain extent, and alloy anode materials can promote the energy density of LIBs. The properties of the commercialized anode materials are covered in this paper. Next generation anode materials such as silicon anode materials are also introduced.

Ethylene Glycol Co‐Solvent Enables Stable Aqueous Ammonium‐Ion Batteries with Diluted Electrolyte

AbstractAqueous ammonium‐ion batteries (AAIBs) are considered as one of the most promising technologies for large scale energy storage applications, due to their intrinsic safety, environmental friendliness and low cost. Nevertheless, the practical application of AAIBs is impeded by hydrogen evolution reaction (HER) occurring in diluted aqueous electrolyte. Highly concentrated electrolytes can improve electrochemical stability but lead to higher costs and increased hydrolysis of NH4+. In this work ethylene glycol (EG) is proposed as co‐solvent, which can act as H‐bond modulating agent, to increase the stability of AAIBs with diluted electrolytes. The perturbation of water H‐bond network regulated by EG is proved by spectroscopic methods, while the suppressed HER is confirmed by differential electrochemical mass spectrometry (DEMS) results. As a result, full cells with 3,4,9,10‐perylenebis(dicarboximide) (PTCDI) anode and FeFe(CN)6 (FeHCF) cathode and EG‐added electrolyte exhibit stable cycling performance with capacity retention of 77% after 1950 cycles.