High-performance Rechargeable Batteries Research Articles

Enhanced electrochemical performance of garnet Li7La3Zr2O12 electrolyte by efficient incorporation of LiCl

Garnet-type Ta-doped Li7La3Zr2O12 (LLZO) lithium-ion-conducting ceramic electrolytes has become the promising and critical candidate for developing the high-energy-density all-solid-state lithium batteries, due to the satisfied Li+ conductivity, stability against metallic lithium anode, and the feasible preparation under ambient air. Here, to further increase the lithium-ion conductivity of LLZO comparable to that of the commercial organic liquid electrolytes, lithium chloride (LiCl) is effectively introduced to synthesize the garnet-type ceramic electrolytes with the nominal composition (Li6.5La3Zr1.5Ta0.5O12)1-x–(LiCl)x (x=0, 5mol%, 10mol%, 15mol%, 20mol%, and 25mol%) via high-temperature calcination process. The cubic structure with highly conductive performance is confirmed from X-ray diffraction measurement as well as Raman spectra analysis. Structural information is observed according to field emission scanning electron microscope equipped with energy dispersive spectrometer and density measurements. Among above investigated ceramic compositions, the prepared (Li6.5La3Zr1.5Ta0.5O12)0.85–(LiCl)0.15 ceramic electrolyte sheet sintered at 1200°C for 12h presents the room-temperature Li-ion conductivity of 1.22×10-3S·cm-1 by alternating current (AC) impedance analysis along with the corresponding activation energy of 0.262eV through Arrhenius equation calculation. The electronic conductivity measurements are also done by direct-current polarization to confirm the ionic nature for all investigated ceramics. Furthermore, the Li|(Li6.5La3Zr1.5Ta0.5O12)0.85–(LiCl)0.15 |Li symmetric batteries can possess the small interfacial resistance of 92.3 Ω·cm2 and stably run for 1000 h at 0.1 mA·cm−2 without a short circuit at room temperature. The hybridized lithium-sulfur battery with (Li6.5La3Zr1.5Ta0.5O12)0.85–(LiCl)0.15 electrolyte delivered excellent initial room-temperature discharge capacity of 1204mAh·g-1 and 1150mAh·g-1 under the current density of 0.1C and 0.2C respectively, large coulombic efficiency, and great cycling stability. Moreover, the lithium-sulfur batteries also can show excellent cycling performances under different current densities and a good capacity recoverability. The above investigation results suggest that the low-melting-point LiCl incorporation in Li6.5La3Zr1.5Ta0.5O12 electrolyte is an effective measurement to synthesize the cubic and dense Li-stuff garnet ceramic sheets for the high-performance rechargeable next-generation solid-state batteries.

Plasma-engineering of Pt-decorated NiCo2O4 nanowires with rich oxygen vacancies for enhanced oxygen electrocatalysis and zinc-air battery performance

The development of low-cost and efficient bifunctional catalysts is of great importance for the advancement of high-performance rechargeable zinc-air batteries. In this study, we present a composite material comprising Pt-decorated NiCo2O4 nanowires enriched with abundant oxygen vacancies, designed as an excellent bifunctional electrocatalyst for both the oxygen evolution reaction and the oxygen reduction reaction. The introduction of Pt atoms and oxygen vacancies onto the NiCo2O4 nanowires was achieved with the assistance of plasma treatment. This approach resulted in a catalyst with a greater number of active sites, enhanced surface conductivity and significantly improved electrocatalytic activity compared to the original NiCo2O4 nanowires. Moreover, the zinc-air battery based on this composite catalyst exhibits a narrow charge/discharge voltage gap and superior stability, which is better than batteries employing commercial noble-metal-based catalysts. This work provides a rational strategy for the construction of high-active and cost-effective Pt-based electrocatalysts.

Surface engineering of TiSiO4 nano-coating for high-voltage nickel-rich ternary cathodes: An approach to improve cyclic performance

In recent years, layered ternary transition metal oxides with a high nickel content have gained substantial attention as a potential positive electrode material for lithium-ion batteries. However, its poor rate capability, cyclability, and capacity retention at high working voltages limit its use in commercial lithium-ion batteries. To overcome these challenges, we synthesize a cost-effective wet-chemical deposition of novel TiSiO4 nano-coatings over the surface of LiNi0.83Mn0.06Co0.11O2 (NMC-83). X-ray diffraction and electron microscopy confirm the presence of a coating and verify that the deposition process did not alter the crystallinity and morphology of the NMC-83 particles. In addition, during cycling, it completely protects NMC-83 with enhancements in hexagonal phase transitions between H2 and H3, resulting in excellent cycling stability at upper cut-off voltages. Likewise, when the amount of coated material is equal to 1 wt%, it provides faster ion kinetics and a stable electrode-electrolyte interface. The 1 wt% TiSiO4 coating provides 35 % retention after 250 cycles at a 0.5C rate, while the pristine NMC-83 shows only 13.7 %. From postmortem analysis, the 1 wt% TiSiO4-coated NMC-83 cathode maintains its stable polycrystalline nature compared with pristine NMC-83. Thus, this novel TiSiO4 nanocoating has significant implications for developing high-performance rechargeable batteries for energy applications.

Anion vacancy engineering in carbon coating VS4 microspheres assembled by nanorod arrays for high-performance rechargeable Mg-Li hybrid batteries

Transition metal sulfides (TMSs) stand out as promising cathodes for rechargeable Mg-Li hybrid ion batteries (MLIBs) owing to their high theoretical capacity and rich redox chemistry. Nevertheless, it still faces great challenges involving the sluggish reaction kinetics and insufficient active sites, resulting in unsatisfactory stability and limited rate capability. And the role of anion vacancies on improving electrochemical properties of TMSs is still unclear. Herein, we have successfully designed an anion defect engineering strategy for the construction of carbon coating VS4 microspheres assembled by nanorod arrays (Sv-VS4@C-300) as the high-performance cathode for MLIBs. The systematic electrochemical tests together with theoretical calculations reveal that the sulfur vacancies simultaneously improve ion adsorption ability, facilitate charge transfer rate and boost reaction kinetics. Additionally, the open microsphere structure together with rich sulfur vacancies cooperatively provide more active sites and release the internal stress during cycling, thereby realizing the enhancement of capacity and structural stability. Consequently, these features enable Sv-VS4@C-300 with impressively high reversible capacity (485.1 mAh/g at 50 mA g−1) and exceptional long cycle lifespan (128.3 mAh/g at 2000 mA g−1 after 5000 cycles). This work implements an innovative strategy represented by anion vacancy engineering in the design of high-performance TMSs-based cathodes for rechargeable batteries.

Regulating the Double-Way Traffic of Cations and Anions in Ambipolar Polymer Cathodes for High-Performing Aluminum Dual-Ion Batteries.

The strong Coulombic interactions between Al3+ and traditional inorganic crystalline cathodes present a significant obstacle in developing high-performance rechargeable aluminum batteries (RABs) that hold promise for safe and sustainable stationary energy storage. While accommodating chloroaluminate ions (AlCl4 -, AlCl2+, etc.) in redox-active organic compounds offers a promising solution for RABs, the issues of dissolution and low ionic/electronic conductivities plague the development of organic cathodes. Herein, electron donors are synthetically connected with acceptors to create crosslinked, bipolar-conjugated polymer cathodes. These cathodes exhibit overlapped redox potential ranges for both donors and acceptors in highly concentrated AlCl3-based ionic liquid electrolytes. This approach strategically enables on-site doping of the polymer backbones during redox reactions involving both donor and acceptor units, thereby enhancing the electron/ion transfer kinetics within the resultant polymer cathodes. Based on the optimal donor/acceptor combination, the bipolar polymer cathodes can deliver a high specific capacity of 205mAhg-1 by leveraging the co-storage of AlCl4 - and AlCl2+. The electrodes exhibit excellent rate performance, a stable cycle life of 60000 cycles, and function efficiently at high mass loadings, i.e., 100mg cm-2, and at low temperatures, i.e., -30°C. The findings exemplify the exploration of high-performing conjugated polymer cathodes for RABs through rational structural design.

Facilitating charge transfer via a Semi-Coherent Fe(PO3)2-Co2P2O7 heterointerface for highly efficient Zn-Air batteries

Developing reversible oxygen electrodes for both the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) is crucial for achieving high-performance rechargeable Zn-air batteries (ZABs). This study introduced an nitrogen-doped carbon confined with a semi-coherent Fe(PO3)2-Co2P2O7 heterojunction for bifunctional oxygen electrocatalysis. This nanocomposite yielded an ORR half-wave potential of 0.908 V and an OER overpotential of 291 mV at 10 mA/cm2. ZABs incorporating this catalyst yielded impressive performance, including a peak power density of 203 mW/cm2, a specific capacity of 737 mAh/gZn, and promoted stability. Both experimental and theoretical simulations demonstrated that the unique electric field between Fe(PO3)2 and Co2P2O7 promoted efficient charge transport across the heterointerface. This interaction likely modulated the d-band center of the heterojunction, expedite the desorption of oxygen intermediates, thus improving oxygen catalysis and, consequently, ZAB performance. This work illustrates a significant design principle for creating efficient bifunctional catalysts in energy conversion technologies.

A Facile Strategy for Constructing High-Performance Polymer Electrolytes via Anion Modification and Click Chemistry for Rechargeable Magnesium Batteries.

Polymer electrolytes play a crucial role in advancing rechargeable magnesium batteries (RMBs) owing to their exceptional characteristics, including high flexibility, superior interface compatibility, broad electrochemical stability window, and enhanced safety features. Despite these advantages, research in this domain remains nascent, plagued by single preparation approaches and challenges associated with the compatibility between polymer electrolytes and Mg metal anode. In this study, we present a novel synthesis strategy to fabricate a glycerol α,α'-diallyl ether-3,6-dioxa-1,8-octanedithiol-based composite gel polymer electrolyte supported by glass fiber substrate (GDT@GF CGPE) through anion modification and thiol-ene click chemistry polymerization. The developed route exhibits novelty and high efficiency, leading to the production of GDT@GF CGPEs featuring exceptional mechanical properties, heightened ionic conductivity, elevated Mg2+ transference number, and commendable compatibility with Mg anode. The assembled modified Mo6S8||GDT@GF||Mg cells exhibit outstanding performance across a wide temperature range and address critical safety concerns, showcasing the potential for applications under extreme conditions. Our innovative preparation strategy offers a promising avenue for the advancement of polymer electrolytes in high-performance rechargeable magnesium batteries, while also opens up possibilities for future large-scale applications and the development of flexible electronic devices.

Tailored crystal planes of VO2 cathode power fast Zn2+ storage

Vanadium dioxide (VO2) cathode with specific tunnel structure and favorable specific capacity is critical for developing aqueous zinc-ion batteries (AZIBs) with excellent electrochemical performance. However, sluggish electrochemical kinetics hampered its development in burgeoning energy storage devices. Herein, we tailored VO2 material with different exposed crystal planes and employed as cathodes for AZIBs. The comprehensive analyses indicate the exposed (201) and (001) crystal planes are favorable for fast electrochemical kinetics, high capacitance storage, and the smallest diffusion energy barrier, which guarantee electrodes with high discharge capacity (367 mA h/g at 0.1 A/g), excellent rate capability (281 mA h/g at 4 A/g) and cycling stability over 800 cycles. Besides, Ex-situ characterizations manifest VO2 cathode with specific exposed crystal planes easily transformed to Zn3+x(OH)2V2O7·2H2O in the first discharge process, hence allowing continuous embedding of Zn2+ in this layered structure, and the ex-situ scanning electron microscopy (SEM) analysis confirms the morphology change matched well with the structural transformation. This study may enlighten and promote the role of exposed crystal plane to develop high-performance rechargeable batteries.

Cu Regulating the Bifunctional Activity of Co-O Sites for the High-Performance Rechargeable Zinc-Air Battery.

The rational design of cost-effective and highly active electrocatalysts becomes the crucial energy storage technology to boost the kinetics of the oxygen reduction reaction (ORR) and the oxygen evolution reaction (OER), which hinders the large-scale application of metal-air batteries under the situation of increasingly pressing energy anxiety. Herein, the Co-based ZIF introduced the moderate amount of Cu2+-derived Cu/Co metal nanoparticles (NPs) embedded in carbon frameworks after high-temperature calcination. The Co-O bond on the surface of Co nanoparticles is modulated by adjacent Cu nanoparticles with the surface Cu-O bonds. The resulted increase of the Co2+/Co3+ ratio in 0.1CuCo-NC enhances the ORR/OER bifunctional catalytic kinetics along with the ΔE of 0.639 V. In situ Raman spectra of the catalyst on the three-electrode system as well as in the driven zinc-air battery (ZAB) show that the Co-O active sites regulated by Cu nanoparticles with Cu-O bonds maintain a periodic lattice expansion and compression during discharging and charging. The zinc-air battery based on 0.1CuCo-NC has a peak power density of up to 198.3 mW cm-2, a mass-specific capacity of 798.2 mAh g-1, and a cycling stability of 923 h at room temperature. This work makes up the research gap of a Co-based metal-organic framework (MOF)-derived catalyst regulated by a transition metal.

High performance rechargeable aluminium ion batteries enabled by full utilization and understanding of polyaniline cathodes

As a renowned conductive polymer, polyaniline (PANI) shows remarkable potential in organic cathode materials for rechargeable aluminium ion batteries (RAIBs). However, existing research has not given sufficient understanding and explanation of the structure and states of PANI but failed to achieve ideal electrochemical performance. In this study, we differentiate and investigate for the first time its primary-doped (PANI-1), re-doped (PANI-Re), secondary-doped (PANI-2), and emeraldine based (PANI-EB) forms, meanwhile attempt to enhance the conductivity of PANI-EB using multi-walled carbon nanotubes (PANI-EB@C). Among them, the high-doped PANI-2 and non-doped PANI-EB exhibit theoretical capacity utilization far superior to lower doped PANI-1 and PANI-Re, with both specific capacities reaching approximately 225 mAh/g (full capacity utilization rate of 76.53 %) at a current density of 1 A/g, while maintaining capacity retention rates of 92.89 % after 2000 cycles and 92.44 % after 5000 cycles, respectively. Furthermore, the high-conductivity PANI-EB@C displays a discharge specific capacity of 284 mAh/g (full capacity utilization rate of 96.59 %), with a capacity retention rate of 91.19 % after 5000 cycles. Electrochemical analysis, Gaussian theoretical calculations, ex-situ characterization collectively indicate that the electrochemical performance of doped PANI is positively correlated with the degree of doping-induced conductivity changes, while the unique internal redox process of PANI-EB enhances the release of performance and could be further optimized by the assistant of conductivity medium. This work advances the classification of the electrochemical performance and structural understanding of PANI cathode materials to an extremely high stage, towards the practical application of a low-cost, high-performance, sustainable, and green cathode material in large-scale energy storage devices.

Three-dimensional mixed-valence polyoxovanadates@polyaniline architecture towards high-performance rechargeable aqueous zinc-ion batteries cathode

Aqueous zinc ion batteries (AZIBs) are toward promising candidates of energy storage systems for their low cost, high safety and eco-friendliness, whereas the sluggish reaction kinetics and unstable internal structure of cathode materials greatly limited the practical application of AZIBs. Herein, we employ the three-dimensional mixed-valance polyoxovanadates [Co3(H2O)12][VIV10VV8O42(SO4)]·24H2O (CoVO) coated with polyaniline (PANI) as stable zinc ion storage material (denoted as CoVO@PANI). The 3D highly porous CoVO framework constructs multidimensional interconnected Zn2+ migration channels, and the high conductivity of PANI facilitates the formation of oxygen defects during in-situ polymerization process and inhibits the polyoxovanadates dissolution. Density functional theory calculation reveals that PANI significantly regulates the electronic property of the CoVO host, further promoting the electron/ion transfer kinetics and thus contributing to high-effciency Zn2+ storage performance. As expected, the optimized as-fabricated CoVO@PANI60 cathode exhibits a high reversible capacity of 456.8 mAh g−1 at 0.1 A g−1 and long-term cyclability with capacity retention of 90.4 % after 1500 cycles at 10 A g−1.

Polyoxomolybdate-Based Metal-Organic Framework-Derived Cu-Embedded Molybdenum Dioxide Hybrid Nanoparticles as Highly Efficient Electrocatalysts for Al-S Batteries.

High-performance rechargeable aluminum-sulfur batteries (RASB) have great potential for various applications owing to their high theoretical capacity, abundant sulfur resources, and good safety. Nevertheless, the practical application of RASB still faces several challenges, including the polysulfide shuttle phenomenon and low sulfur utilization efficiency. Here, we first developed a synergistic copper heterogeneous metal oxide MoO2 derived from polymolybdate-based metal-organic framework as an efficient catalyst for mitigating polysulfide diffusion. This composite enhances sulfur utilization and electrical conductivity of the cathode. DFT calculations and experimental results reveal the catalyst Cu/MoO2@C not only effectively anchors aluminum polysulfides (AlPSs) to mitigate the shuttle effect, but also significantly promotes the catalytic conversion of AlPSs on the sulfur cathode side during charging and discharging. The unique nanostructure contains abundant electrocatalytic active sites of oxide nanoparticles and Cu clusters, resulting in excellent electrochemical performance. Consequently, the established RASB exhibits an initial capacity of 875 mAh g-1 at 500 mA g-1 and maintains a capacity of 967 mAh g-1 even at a high temperature of 50 °C.

Ternary Mg alloy-based artificial interphase enables high-performance rechargeable magnesium batteries

Rechargeable magnesium batteries (RMBs) provide potential advantages over lithium-ion batteries in terms of high volumetric capacity, natural abundance, and high safety. However, the rational design of high-performance magnesium-based metal anodes compatible with conventional electrolytes is a big challenge for the viability of RMBs. In this work, an in-situ formed ternary alloy-based artificial interphase layer on Mg foil as an anode was successfully prepared through a facile and universal electrodeposition strategy. The Mg-Sn-Bi@Mg anode provides high charge transfer dynamics for Mg deposition and constructs a reduced energy barrier for Mg2+ ions desolvation. Thanks to the unique Mg deposition behaviors, the Mg-Sn-Bi@Mg alloy anode demonstrates a low overpotential of 39.4 mV and a long cycle life of >2000 h. The transfer kinetics for RMBs can be largely improved due to the unique alloying reactions. Density functional theory (DFT) calculations demonstrate that the designed ternary alloy-based artificial interphase layer enables faster Mg2+ ion migration than the bare Mg electrode. Full cells with Mo6S8 cathode also show ultra-stable cycling performance over 2400 cycles at 1C in a conventional all-phenyl complex (APC) electrolyte. This facile interface modification strategy sheds light on the development of advanced RMBs and also provides a promising direction for the design of high-performance Mg-based alloy anodes for high-performance RMBs and beyond.

On the formation and properties of amorphous and crystalline Li3-yBay/2OCl electrolytes

All-solid-state batteries (ASSBs) have potential to provide higher specific energy, higher power, and longer cycle life than Li-ion batteries (LIBs) for continuously increasing demands of high-performance rechargeable batteries with intrinsic safety. However, one of the barriers for successful design and fabrication of ASSBs is the lack of solid-state electrolytes (SSEs) that can meet multi-functional requirements for ASSBs. To address this issue, the present study investigates hydrothermal synthesis of amorphous and crystalline Ba-doped Li3OCl solid electrolytes and develops the understanding of the relationships between the synthesis conditions and electrochemical properties of the products. It is shown that the formation of an amorphous/crystalline Ba-doped Li3OCl mixture with little hydroxide impurities depends strongly on the hydrothermal reaction temperature, drying temperature, Ba concentration, and rate of removing OH− and H+ ions as steam from water solvated Ba-doped Li3OCl. The key to generate amorphous Li3OCl-based electrolytes with high ionic conductivities (7.65 × 10−3 S/cm) at room temperature is to create non-equilibrium synthesis conditions such as the one identified in this study. The understanding developed in this study will offer critical guidelines for synthesizing amorphous and crystalline Li3OCl-based electrolytes with superior electrochemical properties for ASSBs reliably and reproducibly in the near future.

C3N4-digested intercalation MoS2 nano-flowers with expanded interlayer spacing towards high-performance rechargeable zinc-ion batteries

Molybdenum disulfide (MoS2) materials are very competitive cathode materials for aqueous zinc-ion batteries (AZIBs) due to their sandwich structure, large surface area and low cost. Also, the inherent low capacity and high energy barrier limit its further development. Here, the C3N4-digested intercalation MoS2 (MSCN) has been achieved via a hydrothermal strategy by using g-C3N4 nanosheets as a self-sacrificial template. The introduction of g-C3N4 greatly improves the MoS2 conductivity, which further enhances the Zn2+ diffusion dynamics, and succeeds in increasing the spacing between the layers. With a discharge capacity of 168 mAh g−1 at 5 A g−1, Zn-ion batteries based on the MSCN cathode assembly exhibit good cycle stability and excellent rate performance, under the same current density circulation capacity remain a rate of 92.9 % after 1000 cycles. And beyond that, flexible quasi-solid ZIBs with MSCN cathodes which have good Zn2+ storage properties and promising for future applications. The research in this article is of great significance for the design and development of AZIBs layered transition metal sulfide cathodes.

Tailoring Oxygen Reduction Reaction Kinetics of Fe-N-C Catalyst via Spin Manipulation for Efficient Zinc-Air Batteries.

The interaction between oxygen species and metal sites of various orbitals exhibits intimate correlation with the oxygen reduction reaction (ORR) kinetics. Herein, a new approach for boosting the inherent ORR activity of atomically dispersed Fe-N-C matrix is represented by implanting Featomic clusters nearby. The as-prepared catalyst delivers excellent ORR activity with half-wave potentials of 0.78 and 0.90V in acidic and alkaline solutions, respectively. The decent ORR activity can also be validated from the high-performance rechargeable Zn-air battery. The experiments and density functional theory calculations reveal that the electron spin-state of monodispersed Fe active sites is transferred from the low spin (LS, t2g 6 eg 0) to the medium spin (MS, t2g 5 eg 1) due to the involvement of Fe atomic clusters, leading to the spin electron filling in σ∗ orbit, by which it favors OH- desorption and in turn boosts the reaction kinetics of the rate-determining step. This work paves a solid way for rational design of high-performance Fe-based single atom catalysts through spin manipulation.

Thermoelectric generator powered timepiece circuit for rechargeable battery operation

The advent of digital technology has revolutionized the way we keep track of time. Digital watches have become an essential part of our daily lives and provide us with accurate and reliable time measurement. However, battery reliability is a long-standing issue in the digital watch industry. Batteries require frequent replacement and are a major source of waste. To solve this problem, a digital watch that runs on a lithium-polymer battery that is recharged by a voltage generated by a thermoelectric generator (TEG) placed on the hand. The proposed model uses TEG1-19913 that generates power in the range of 11.5 W to 14.5 W with hot end basking at 250 °C and a cold end between 30 °C and 50 °C. The TEG voltage is used to charge the lithium polymer battery, eliminating the need for conventional charging methods. The watch is designed to be compact and lightweight, so it can be worn comfortably for extended periods of time. The TEG is integrated into the watch strap and ensures that it is constantly in contact with the skin. The lithium-polymer battery used in the watch is a high-performance rechargeable battery that has high energy density and long life. In summary, the proposed digital watch is an innovative ecological solution to the problems associated with traditional battery-powered watches. The compact and light design of the watch combined with the energy-efficient display makes it a convenient and efficient timekeeping device.

Regulating the inner Helmholtz plane structure at the electrolyte-electrode interface for highly reversible aqueous Zn batteries

The development of aqueous Zn batteries is limited by parasitic water reactions, corrosion, and dendrite growth. To address these challenges, an inner Helmholtz plane (IHP) regulation method is proposed by employing low-cost, non-toxic maltitol as the electrolyte additive. The preferential adsorption behavior of maltitol can expel the water from the inner Helmholtz plane, and thus hinder the immediate contact between Zn metal and H2O. Meanwhile, strong interaction between maltitol and H2O molecules can restrain the activity of H2O. Besides, the “IHP adsorption effect” along with the low LUMO energy level of maltitol-CF3SO3- can promote the in-situ formation of an organic–inorganic complex solid electrolyte interface (SEI) layer. As a result, the hydrogen/oxygen evolution side reaction, corrosion, and dendrites issues are effectively suppressed, thereby leading to highly reversible and dendrite-free Zn plating/stripping. The Zn||I2 battery with hybrid electrolytes also demonstrates high electrochemical performance and ultralong cycling stability, showing a capacity retention of 75% over 20000 charge-discharge cycles at a large current density of 5 A g−1. In addition, the capacity of the device has almost no obvious decay over 20000 cycles even at −30 °C. This work offers a successful electrolyte regulation strategy via the IHP adsorption effect to design electrolytes for high-performance rechargeable Zn-ion batteries.

Theoretical prediction of two-dimensional CrSi2N4 as a potential anode material for Na-ion batteries

Efficient anode materials are critical for high-performance rechargeable lithium-ion batteries (LIBs) and sodium-ion batteries. This paper systematically investigates the potential of the CrSi2N4 monolayer as anode material for LIBs and sodium-ion batteries by first-principles density functional theory calculations. It was found that CrSi2N4 exhibits outstanding performance in sodium-ion batteries, with a low diffusion energy barrier of 0.10 eV and a high theoretical specific capacity of 490 mAh g−1. Meanwhile, the average open circuit voltage is 0.47 V, comparable to the typical anode materials. In addition, a small lattice constant change of 0.3%–3.1% ensures the cycling stability of CrSi2N4 in sodium-ion batteries. This work suggests a promising candidate anode material for sodium-ion batteries.

Unveiling Confinement Engineering for Achieving High-Performance Rechargeable Batteries.

The confinement effect, restricting materials within nano/sub-nano spaces, has emerged as an innovative approach for fundamental research in diverse application fields, including chemical engineering, membrane separation, and catalysis. This confinement principle recently presents fresh perspectives on addressing critical challenges in rechargeable batteries. Within spatial confinement, novel microstructures and physiochemical properties have been raised to promote the battery performance. Nevertheless, few clear definitions and specific reviews are available to offer a comprehensive understanding and guide for utilizing the confinement effect in batteries. This review aims to fill this gap by primarily summarizing the categorization of confinement effects across various scales and dimensions within battery systems. Subsequently, the strategic design of confinement environments is proposed to address existing challenges in rechargeable batteries. These solutions involve the manipulation of the physicochemical properties of electrolytes, the regulation of electrochemical activity, and stability of electrodes, and insights into ion transfer mechanisms. Furthermore, specific perspectives are provided to deepen the foundational understanding of the confinement effect for achieving high-performance rechargeable batteries. Overall, this review emphasizes the transformative potential of confinement effects in tailoring the microstructure and physiochemical properties of electrode materials, highlighting their crucial role in designing novel energy storage devices.