High Open Voltage Research Articles

Exploring the Mechanisms of LiNiO2 Cathode Degradation by the Electrolyte Interfacial Deprotonation Reaction.

Nickel-rich layered oxides stand as ideal cathode candidates for high specific capacity and energy density next-generation lithium-ion batteries. However, increasing the Ni content significantly exacerbates structural degradation under high operating voltage, which greatly restricts large-scale commercialization. While strategies are being developed to improve cathode material stability, little is known about the effects of electrolyte-electrode interaction on the structural changes of cathode materials. Here, using LiNiO2 in contact with electrolytes with different proton-generating levels as model systems, we present a holistic picture of proton-induced structural degradation of LiNiO2. Through ab initio molecular dynamics calculations based on density functional theory, we investigated the mechanisms of electrolyte deprotonation, protonation-induced Ni dissolution, and cathode degradation and the impacts of dissolved Ni on the Li metal anode surfaces. We show that the proton-transfer reaction from electrolytes to cathode surfaces leads to dissolution of Ni cations in the form of NiOOHx, which stimulates cation mixing and oxygen loss in the lattice accelerating its layered-spinel-rock-salt phase transition. Migration of dissolved Ni2+ ions to the anode side causes their reduction into the metallic state and surface deposition. This work reveals that interactions between the electrolyte and cathode that result in protonation can be a dominant factor for the structural stability of Ni-rich cathodes. Considering this factor in electrolyte design should be of benefit for the development of future batteries.

High-voltage aqueous supercapacitors enabled by polysiloxane passivation coating-modified carbon cloth electrode

The voltage window plays a crucial role in determining the energy density of supercapacitors. The limited energy density of carbon-based supercapacitors poses a significant challenge to their widespread adoption. Here, we propose a novel approach to modify carbon cloth by implementing a polysiloxane (PSiO) passivation coating. This forms an ion-conductive and electron-insulating thin film on the surface, effectively impeding electron conduction from electrode surface to electrode/electrolyte interface and suppressing electrolyte electrolysis. Consequently, an expanded voltage window is realized, thereby enhancing the energy density of aqueous carbon-based supercapacitors. The carbon cloth electrode modified with the PSiO passivation coating (CC-A-KH560) exhibits exceptional electrochemical performance, with a significantly increased 78.6 % widened applicable potential range compared to the activated carbon cloth electrode (CC-A). In a two-electrode configuration, the voltage window is broadened from 0.8 V for CC-A to 1.4 V for CC-A-KH560, and the energy density based on CC-A-KH560 is 8 times that based on CC-A. The good stability and durability are also obtained for the firm C–O–Si bonds during PSiO modification. More importantly, this design provides a generic solution of PSiO passivation coating-modified carbon electrode, applicable for diversified silicane couple agents, to realize a high-voltage energy storage performance for aqueous supercapacitors.

Enhanced electrochemical performance of K0.67[Ni0.3Mn0.6Co0.1] O2 as a cathode material for secondary K-Ion batteries: Improved K-Ion insertion and reduced charge transfer barrier

Potassium-ion batteries, with their high operating voltage and cost-efficiency, emerged as promising contenders for large-scale energy storage system. Nevertheless, the practical application is hindered by the significant challenges of achieving high capacity and good rate capability in cathodes. Herein, a novel layered oxide cathode, K0.67[Ni0.3Mn0.6Co0.1] O2 (KNMCO), has been synthesized via solid-state (S-KNMCO) and co-precipitation (C-KNMCO) routes. The X-Ray diffraction (XRD) peaks of KNMCO are identified in R3 m space group and well-indexed to hexagonal unit cell. The FE-SEM shows non-spherical morphologies for both samples. Additionally, high-resolution transmission electron microscopy (HR-TEM) images of the synthesized cathode materials shows the interlayer spacing of S-KNMCO is higher than that of C-KNMCO. Furthermore, the electrochemical performance of S-KNMCO and C-KNMCO is characterized using K-metal as anode and electrolyte KPF6 in EC/DEC (1:1, v/v). The S-KNMCO and C-KNMCO exhibit the maximum specific discharge capacity of ∼101 mAhg-1 and ∼66 mAhg-1 at the current rate of C/20 respectively. Additionally, these cells show the good rate capability and coulombic efficiency (∼94%). This research offers novel perspectives on the development of cathode substances for KIBs.

Beam energy recovery in Neutral Beam Injections and related simulations

The Neutral Beam Injectors (NBI) will be used to further increase the plasma temperature for the ignition of the fusion reactions in the ITER project. For future applications of electric energy production, the NBI efficiency is crucial. Since the gas neutralizer gives large residual ion fractions of D+ and D-, adequate energy recovery systems may be necessary. Recently a conceptually simple beam energy recovery based on space charge effects has been proposed; it can also work as an ion dump device, with advantages in removing the residual ions with reduced power dissipation. Preliminary simulation results were evidence of that the proposed device can remove all the residual ions by collecting them at very low energy on proper electrodes. In this contribution, further simulations with more accurate space charge calculations are reported to mostly confirm the high residual ion collection efficiency obtained in the preliminary simulations. The simulated operation voltage is also increased from 20 kV to 500 kV in steps. Higher efficiencies require some increase of the collector length, especially at higher operation voltage, as here discussed. Some design detailed features are also updated.

Dual-Salts Localized High-Concentration Electrolyte for Li- and Mn-Rich High-Voltage Cathodes in Lithium Metal Batteries.

Limited electrochemical stability windows of conventional carbonate-based electrolytes pose a challenge to support the Lithium (Li)- and manganese (Mn)-rich (LMR) high-voltage cathodes in rechargeable Li-metal batteries (LMBs). To address this issue, a novel localized high-concentration electrolyte (LHCE) composition incorporating LiPF6 and LiTFSI as dual-salts (D-LHCE), tailored for high-voltage (>4.6Vvs.Li) operation of LMR cathodes in LMBs is introduced. 7Li nuclear magnetic resonance and Raman spectroscopy revealed the characteristics of the solvation structure of D-LHCE. The addition of LiPF6 provides stable Al-current-collector passivation while the addition of LiTFSI improves the stability of D-LHCE by producing a more robust cathode-electrolyte interphase (CEI) on LMR cathode and solid-electrolyte interphase (SEI) on Li-metal anode. As a result, LMR/Li cell, using the D-LHCE, achieved 72.5% capacity retention after 300 cycles, a significant improvement compared to the conventional electrolyte (21.9% after 100 cycles). The stabilities of LMR CEI and Li-metal SEI are systematically analyzed through combined applications of electrochemical impedance spectroscopy and distribution of relaxation times techniques. The results present that D-LHCE concept represents an effective strategy for designing next-generation electrolytes for high-energy and high-voltage LMB cells.

The novel methods of insulation detection based on Adaptive Levenberg–Marquardt algorithm and Third-Order Variable Forgetting Factor Recursive Least Squares-Decouple algorithm

Electric vehicles (EVs) are central to the future of automotive development, with high-voltage insulation performance critical for operational safety. Existing insulation detection methods face challenges such as limited scope, low accuracy, poor interference resistance, and slow response. This study introduces two insulation detection models based on the unbalanced bridge method and low-frequency signal injection, analyzing their theoretical effectiveness and confirming superior detection capability in the unbalanced bridge method. Furthermore, to address feedback voltage waveform issues in this method, an adaptive Levenberg–Marquardt (ALM) algorithm is proposed to prevent the divergence typically seen in traditional approaches. Additionally, a decoupling algorithm utilizing a Third-order Variable Forgetting Factor Recursive Least Squares (TVFF-Decouple) simplifies algorithm complexity significantly while enabling anomaly detection. Finally, AEKF and SRCKF algorithms were used for observation, identifying an optimal combination that reduces noise interference effectively. Simulations and bench tests demonstrate that the proposed methods swiftly and accurately detect positive and negative insulation resistances and equivalent Y capacitance under various conditions.

Effect of surface alignment on electric-field-induced phase transitions in blue phases

This study investigates the critical electric field thresholds required for phase transitions in the blue phases of liquid crystals (BPs) confined within vertical field switching cells. BPs are attractive for electro-optical applications due to their polarization-independent response and fast switching times; however; challenges remain regarding their limited temperature stability and previously reported high operational voltages. We employ a combined approach of polarized optical microscopy and electrical impedance analysis to identify the electric field thresholds triggering BP transitions to focal conic domains in cells with and without planar polyimide alignment layers. We show that surface alignment layers stabilize the blue phases and allow for higher applied electric fields before transitioning into the focal conic state. This suggests the possibility of a wider operational voltage range in thinner cells with alignment layers. These findings significantly improve our understanding of BPs, addressing key challenges and paving the way for their integration into advanced photonic devices, based on the CMOS technology.

Simultaneous structure and surface engineering of metal-organic framework derived LiNi0.5-xFe2xMn1.5-xO4 cathode material for improving high voltage performance of lithium-ion batteries

This study presents a novel material synthesis approach utilizing a terephthalic acid-based metal-organic framework as a precursor and employing an ethanol-assisted hydrothermal treatment to produce high-performance Fe-doped LiNi0.5Mn1.5O4 (LNMO) cathode material. This strategy yields a well-crystallized spinel structure with uniformly distributed transition metal ions. Additionally, the appropriate quantity of Fe dopant can achieve the desired Mn3+/Mn4+ ratio, level of structural disordering, and crystal phase purity for Fe-doped LNMO. The synthesis process also aids in forming an amorphous Li2CO3 surface layer, approximately 1 nm thick, which protects the active material from excessive reaction with electrolyte. The typical Fe-doped LNMO cathode (S-05) exhibits superior performance compared to a commercialized LNMO counterpart. It delivers an initial discharge capacity of 135 mAh g-1 at 1 C with exceptional cycling stability over 500 cycles (capacity retention of 90%) under high voltage (5.0 V vs. Li+/Li). Furthermore, its rate capability significantly improves, with a capacity retention of 85% (5 C/0.2 C). This enhanced performance aligns with evidence of activated Ni2+/Ni3+/Ni4+ redox reactions and suppressed cathode electrolyte interphase resistance, leading to promoted Li+ diffusion. Moreover, it is found the cathode helps alleviate electrolyte degradation at high voltages by inhibiting the formation of singlet oxygen in the electrolyte.

Nickel‐Manganese‐Based Layered Oxide for Sodium Ion Battery Cathode Materials

Sodium‐ion batteries (SIBs) have demonstrated significant potential as alternatives to conventional lithium‐ion batteries (LIBs) for modern grid and mobile energy storage applications, due to the abundant natural resources and low cost of sodium. Layered transition metal oxides (LTMOs) have attracted focused research attentions due to their high specific capacities, energy densities as well as the compatible preparation processes with those of LIBs cathode materials. Among these, Ni/Mn‐based LTMOs (NMLOs) are particularly noteworthy for their cost‐effectiveness and superior electrochemical performance, such as excellent capacity retention, voltage stability, high operating voltage and rate capability. In this review, we briefly introduce the synthesis methods of NMLOs, discuss the challenges, and summarize the solutions. The insights presented may contribute to the development of NMLOs based SIBs.

A high-capacity and stable dual-ion battery based on an ultra-large lattice-spacing amorphous carbon anode

Compared with traditional lithium-ion batteries (LIBs), dual-ion batteries (DIBs) offer advantages such as high operating voltage, good safety performance, and low cost. However, DIBs often suffer from challenges such as low specific capacity and poor cycling performance in practical applications. Here, a layered nitrogen-doped carbon anode has been prepared using a one-step pyrolysis method with excellent Li+ storage sites. The large lattice spacing of 0.55 nm provides more space for the storage and migration of active ions. Concurrently, the utilization of concentrated electrolyte facilitated the electrochemical window and the restrained solvation of ions, which helps to boost ion transport and improve the stability of the electrolyte and the operating voltage of DIBs. The assembled DIBs exhibit a high specific discharge capacity of 179.27 mA h g−1, within a 2.5–4.8 V voltage range, and excellent cycling stability of 3500 cycles without degradation. Specifically, the structural evolution of the electrodes during charging and discharging and the working mechanism of the DIBs are also explored. The DIBs system designed in this paper provides a facile and scalable approach to promote the development of DIBs with low-cost and high-performance.

Potential difference-induced electrodeposition of defect-rich α-cobalt hydroxide on porous copper (PCu): High-voltage performance of supercapacitor

Designing electrode materials for aqueous battery-type supercapacitors to extend the operating voltage window remains a significant challenge to increase the energy density of aqueous supercapacitors. In this work, a directional electrodeposition method without any additives was employed to deposit α-Co(OH)2 onto a porous copper (PCu) current collector substrate, which involves the fabrication of a supercapacitor electrode material with a cross-linked network structure named α-Co(OH)2@PCu900. The potential difference between copper and cobalt facilitated the formation of a larger interlayer spacing for α-Co(OH)2. In addition, crystals of α-Co(OH)2 with different orientations exert stress on one another, leading to lattice distortion and vacancy formation. The morphology and microstructure of materials were analyzed through techniques such as SEM, HRTEM, XRD, and XPS, confirming the validity of the experimental design. This defect-rich, large interlayer spacing structure facilitates ion intercalation and deintercalation during the charge-discharge process, thereby expanding the operating voltage window. In a three-electrode system, α-Co(OH)2@PCu900 exhibited a potential range from −0.45 V to 0.55 V and demonstrated an areal capacitance of 2580 mF cm−2 and specific capacitance of 600 A g−1 at 2 mA cm−2. The α-Co(OH)2@PCu900 was used as the cathode material and commercial reduced graphene oxide (rGO) was used as the anode material in an asymmetric supercapacitor, and the ASC device exhibited an areal capacitance of 295.3 mF cm−2 and a specific capacitance of 87.89 F g−1. Notably, it retained a high energy density of 0.12 mW h cm−2 (35.27 Wh kg−1) at a power density of 1.7 mW cm−2 (505.95 W kg−1). This method established α-Co(OH)2@PCu900 as a promising supercapacitor electrode material, providing a viable strategy for designing and fabricating functional electrode materials.

High rate capability and ultra‐long cycling life: Electrochemical synthesis of PEDOT based electrode material doped with AMPS and its supercapacitor application

AbstractPoly(3,4‐ethylene dioxythiophene) (PEDOT) is a conducting polymer that can be used in flexible bioelectronic devices. The electrode/electrolyte interface interaction is one of the most important factors in improving the electrochemical performance of energy storage materials, and these polymers are often combined with a negatively charged poly(styrene sulfonate) (PSS) chain to improve their interaction with alkali metal cations such as sodium and potassium. In this work, we performed a one‐step electrochemical synthesis of PEDOT on carbon fabric using the molecule 2‐acrylamido‐2‐methyl‐1‐propane sulfonic acid (AMPS) to create highly effective materials for supercapacitor electrodes. The electrode had a significant increase in capacitance value, measured 16.4 times higher than that of the PEDOT electrode. The 2‐electrode system exhibited a specific capacitance value of 495.2 F g−1 at a scan rate of 5 mV s−1. It exhibited a high operating voltage of 2.3 V in aqueous electrolyte system. It showed a significant energy density of 109.0 Wh kg−1 when operating at 6.1 kW kg−1 power density and 85.2 Wh kg−1 when operating at 30.6 kW kg−1 power density. Recent findings reveal that the capacitance retention performance value of the device increased significantly to 113.9% after 25,000 cycles in 3.0 M NaCl aqueous electrolyte, demonstrating its outstanding long‐term durability. Thus, the creation of the synthesized supercapacitor electrode is a significant advance in the study of conducting polymers, which often have a limited lifetime in real‐world electronic applications.

Enhancing the performance of LiNi0.8Mn0.1Co0.1O2-based pouch cells through advanced electrolyte additive systems for high-temperature lithium-ion batteries

Next-generation lithium-ion batteries, which achieve high energy densities and prolonged cycle performance, require cathode materials with high operating voltages and specific capacities. Because of their high capacity and operating voltage, nickel-rich layered oxides like LiNi0.8Mn0.1Co0.1O2 (NMC811) are attractive cathodes; nevertheless, they have drawbacks such capacity loss, poor cycle performance, structural instability, and thermal instability. Enhancing the stability of the NMC811 cathode-electrolyte interphase demands improvements in both cathode materials and electrolytes. This study explores the enhancement of NMC811-based battery systems through electrolyte modification, focusing on mixed additive combinations to evaluate their synergistic effects at elevated temperatures, relevant for tropical climates. A ternary additive system comprising vinylene carbonate (VC), lithium difluorophosphate (LiPO2F2), and p-toluenesulfonyl isocyanate (PTSI) in a LiPF6-based electrolyte showed significant improvements. This system mitigated capacity fading for cells cycled over 3 V–4.2 V at both 25 °C and 45 °C, outperforming the baseline electrolyte. The designed electrolyte stabilized the electrode-electrolyte interface, enhancing cell performance and the cathode's structural integrity. Notably, the graphite/NMC811 pouch cell's cycling performance showed an increase in capacity retention from 82.4% to 90.2% after 150 cycles at C/2 at 45 °C. Moreover, the deactivation of PF5 by PTSI can help to suppress the side reaction from the instability of LiPF6-based electrolytes, especially at elevated temperatures. These findings carried out from this strategic electrolyte additive system can substantially improve nickel-rich LIBs, especially in challenging thermal environments.

A low redox potential and long life organic anode material for sodium-ion batteries

Sodium-ion batteries (SIBs) with organic electrodes are an emerging research direction due to the sustainability of organic materials based on elements like C, H, O, and sodium ions. Currently, organic electrode materials for SIBs are mainly used as cathodes because of their relatively high redox potentials (>1 V). Organic electrodes with low redox potential that can be used as anode are rare. Herein, a novel organic anode material (tetrasodium 1,4,5,8-naphthalenetetracarboxylate, Na4TDC) has been developed with low redox potential (<0.7 V) and excellent cyclic stability. Its three-sodium storage mechanism was demonstrated with various in-situ/ex-situ spectroscopy and theoretical calculations, showing a high capacity of 208 mAh/g and an average decay rate of merely 0.022% per cycle. Moreover, the Na4TDC-hard carbon composite can further acquire improved capacity and cycling stability for 1200 cycles even with a high mass loading of up to 20 mg cm−2. By pairing with a thick Na3V2(PO4)3 cathode (20.6 mg cm−2), the as-fabricated full cell exhibited high operating voltage (2.8 V), excellent rate performance and cycling stability with a high capacity retention of 88.7% after 200 cycles, well highlighting the Na4TDC anode material for SIBs.

One-step surface-to-bulk modification of single-crystalline Ni-rich Co-poor cathodes for high-rate and long-life Li-ion batteries at high-voltage operations

Single-crystalline Ni-rich Co-poor cathodes operating at high-voltage are attractive owing to their higher energy density for meeting the requirements of next-generation Li-ion batteries, yet they usually suffer from sluggish Li-ion diffusion kinetics and serious Li/Ni disordering. Herein, an in-situ co-precipitation strategy is implemented to achieve the novel In-doped and Li3InO3 coated single-crystalline LiNi0.90Co0.05Mn0.05O2 cathodes with a highly ordered layered structure. The In-doping facilitates grain growth by decreasing the surface energy of crystal faces, reducing the synthesis temperature by about 20 °C, which thus drastically suppresses Li/Ni disordering and lattice oxygen loss. Furthermore, the pillar effect of In-ion doping and the in-situ formation of the ultrafast Li-ion conductive Li3InO3 coating synergistically enhance the Li-ion diffusion kinetics. These merits enable the as-obtained Ni-rich Co-poor cathodes with a high reversible capacity of 229.4 mAh g−1 at 0.1C and 124.6 mAh g−1 at 7C. In a pouch-type full cell, 93.9 % of the initial capacity is still maintained after 500 cycles at 1C within 2.7–4.5 V. This finding opens up a new path for improving the rate performance and cycle life of single-crystalline Ni-rich cathodes for high-voltage Li-ion batteries.

Surface Reconstruction of High-Voltage LiNi0.5Mn1.5O4 Cathode via the Sculpture Method toward Enhanced Stability.

High-voltage LiNi0.5Mn1.5O4 (LNMO) cathodes suffer from severe capacity degradation during long-term cycling due the manganese dissolution and their high operating voltage (∼4.95 V), which pose serious challenges at the surface or interface. Moreover, both traditional ion-doping and passivation layer coating are difficult to apply consistently to LNMO cathode because of their complicated procedures, especially in large-scale production. To address these issues, a strategy employing HNO3/H2O2 leaching in synergy with a sintering process at a mid-temperature of 700 °C was used to achieve selective surface reconstruction. An optimal ratio of reactants was applied to balance the capacity and the cyclic stability of the LNMO cathode. The optimized valence composition of Mn on the material surface mitigates the occurrence of Jahn-Teller distortion, accompanied by a reasonable ratio of ordered and disordered phases and the concentration of oxygen vacancies after sintering, which improves the interface behavior between the electrode and electrolyte. This method delivers a high reversible capacity of 116.5 mAh g-1 after 200 cycles at 0.5 C (1 C = 147 mAh g-1) with a capacity retention of 91.30% and 110 mAh g-1 with a remarkably high capacity retention of 86.85% after 500 cycles at 2 C. This balanced approach, utilizing the protective effects of oxidation (O22-) and the erosive action of acid (H+), is proposed to achieve regional surface reconstruction of advanced LNMO cathode. This opens up a strategy for improving oxide-based cathode materials with low cost and mass production capability, especially favoring high consistency.

"Water-in-Salt" Electrolyte Suppressed MnVOPO4·2H2O Cathode Dissolution for Stable High-Voltage Platform and Cycling Performance for Aqueous Zinc Metal Battery.

Vanadium-based materials have the advantages of abundant valence states and stable structures, having great application potential as cathode materials in metal-ion batteries. However, their low voltage and vanadium dissolution in traditional water-based electrolytes greatly limit their application and development in aqueous zinc metal batteries (AZMBs). Herein, phosphate- and vanadium-based cathode materials (MnVOPO4·2H2O) with stacked layers and few defects were prepared via a condensation reflux method and then combined with a high-concentration electrolyte (21 m LiTFSI + 1 M Zn(CF3SO3)2) to address these limitations. The specific capacity and cycle stability accompanying the stable high voltage of 1.39 V were significantly enhanced compared with those for the traditional electrolyte of 3 M Zn(CF3SO3)2, benefiting from the suppressed vanadium dissolution. The cathode materials of MnVOPO4·2H2O achieved a high specific capacity of 152 mAh g-1 at 0.2 A g-1, with a retention rate of 86% after 100 cycles for AZMBs. A high energy density of 211.78 Wh kg-1 was also achieved. This strategy could illuminate the significance of electrolyte modification and provide potential high-voltage cathode materials for AZMBs and other rechargeable batteries.

Effects of multi-element composition regulation on the structure and electrochemistry of P2-type layered cathode materials

P2-type Mn-based oxides are promising cathode materials for sodium-ion batteries due to their low cost and high capacity virtue. However, the irreversible phase transition and unstable anion redox at high operating voltages (∼4.2 V) will cause structural distortions, leading to slow sodium-ion diffusion kinetics and severe capacity degradation. Herein, a multi-elemental composition regulation strategy is proposed to enhance the structural stability of P2-type cathode by optimizing the structure and modulating the irreversible oxygen redox during high-voltage cycling. A series of multi-element cathodes Na0.67(Fe1/4Co1/4Ni1/4Ti1/4)1-xMnxO2 (x = 0.4,0.5,0.6,0.7,0.8,0.9) are designed and the effects of component modulation on their structure and electrochemical behavior are systematically investigated. Especially, the optimized Na0.67Fe0.05Co0.05Ni0.05Ti0.05Mn0.8O2 cathode maintains P2 phase during the initial charging/discharging between 1.5 V and 4.5 V, inhibits irreversible oxygen redox, and exhibits small lattice expansion. Impressively, the above optimized cathode exhibits superior cycling stability with capacity retention of nearly 90 % and reversible capacity of 130.1 mAhg−1 after 100 cycles at 1C rate. Furthermore, the optimized cathode also displays an excellent rate capability (capacity of 108.2 mAh g−1 at 5 C rate) due to the enhanced Na+ diffusion kinetics. This work provides new insight into developing high-stable Mn-based oxide cathodes operating at high voltage for sodium-ion batteries.

Cation-inspired polyhedral distortion boosting moisture/electrolyte stability of iron sulfate cathode for durable high-temperature sodium-ion storage

Alluaudite-type iron-based sulfates are prospective positive-electrode active materials for sodium-ion batteries given their low-cost and high operation voltage, yet suffer from poor intrinsic ionic conductivity and (electro)chemical instability at high temperatures. Herein, a cation-modified Na2.466Fe1.724Mg0.043(SO4)3 with micron-sized spherical structure was reported. The substitutive MgO6 octahedron featured stronger covalent bonding interactions and enriched the ion transfer pathways within the crystals, facilitating the ionic kinetics in bulk. Using in situ mass spectrometry and quartz crystal microbalance techniques, Mg cations were demonstrated to lower the electron density around O atoms and surficial nucleophilicity of materials, which effectively suppressed their side reactions with H2O in air and active ester molecule in electrolyte. This interaction enables an inorganic-rich and uniform interphase to stabilize the cathode/electrolyte interface at high voltage (4.5 V vs. Na+/Na). The as-prepared cathode exhibits a high discharge capacity of 102.2 mAh g−1 (voltage platform at 3.74 V), remarkable reaction reversibility (average Coulomb efficiency of 99.3% over 300 cycles) at high loading (9.0 − 9.6 mg cm−2) and temperature (60 °C), as well as long-lasting cyclability (70.8%, 5000 cycles). Its application was verified in assembled sodium-ion full cells with a hard carbon negative electrode, showing a long cycling lifetime over 190 cycles.

Bipolar Textile Composite Electrodes Enabling Flexible Tandem Solid-State Lithium Metal Batteries.

A majority of flexible and wearable electronics require high operational voltage that is conventionally achieved by serial connection of battery unit cells using external wires. However, this inevitably decreases the energy density of the battery module and may cause additional safety hazards. Herein, a bipolar textile composite electrode (BTCE) that enables internal tandem-stacking configuration to yield high-voltage (6 to 12V class) solid-state lithium metal batteries (SSLMBs) is reported. BTCE is comprised of a nickel-coated poly(ethylene terephthalate) fabric (NiPET) core layer, a cathode coated on one side of the NiPET, and a Li metal anode coated on the other side of the NiPET. Stacking BTCEs with solid-state electrolytes alternatively leads to the extension of output voltage and decreased usage of inert package materials, which in turn significantly boosts the energy density of the battery. More importantly, the BTCE-based SSLMB possesses remarkable capacity retention per cycle of over 99.98% over cycling. The composite structure of BTCE also enables outstanding flexibility; the battery keeps stable charge/discharge characteristics over thousands of bending and folding. BTCE shows great promise for future safe, high-energy-density, and flexible SSLMBs for a wide range of flexible and wearable electronics.