Large‐Area Rolled‐Up Nanomembrane Capacitor Arrays for Electrostatic Energy Storage

The fabrication, characterization, and optimization of large area rolled‐up ultracompact nanomembrane‐based capacitor arrays is demonstrated by combining bottom‐up and top‐down fabrication methods. The scalability of the process is tested on a 4‐inch wafer platform where 1600 devices are manufactured in parallel. By using a hybrid dielectric layer consisting of HfO₂ and TiO₂ incorporated into an Al₂O₃ matrix, rolled‐up ultracompact capacitors can have their capacitance per footprint area increased by over two orders of magnitude. Their electrical properties can be precisely controlled by adjusting the oxide composition. Furthermore, the rolling of large‐area nanomembrane‐based structures naturally results in a substantial decrease of the occupied footprint area. Such electrostatic rolled‐up ultracompact energy‐storage elements have a large potential in powering various autonomous microsystems.     

Quantifying the Usefulness of Oxide-Encapsulated Silver Nanoparticles in Semiconducting Films

Incorporating plasmonic nanoparticles (NPs) in an organic solar cell (OSC) can improve device performance. In our simulation studies, at NP resonance, absorption in poly(3-hexythiophene)/phenyl-C61-butyric acid methyl ester (P3HT/PCBM) can be increased by encapsulating 50 nm Ag NPs with Al₂O₃, HfO₂, MoO₃, and SiO₂. At Ag NP resonance, when the oxide thickness is significant enough, oxides with high relative permittivity induces a higher electric field enhancement at the metal/dielectric interface. This is translated to improved absorption in the polymer layer. By integrating against AM1.5G, overall absorption in P3HT/PCBM is improved when incorporating Ag NPs encapsulated with a thin oxide shell into the polymer film. However, polymeric absorption loss is induced for oxide-encapsulated Ag NPs if MoO₃ and SiO₂ shells are more than 5 nm. For Al₂O₃ and HfO₂, Ag NPs should not be encapsulated with shells thicker than 10 nm. Modeling studies are also extended to absorption in a CH₃NH₃PbI₃ perovskite layer. It is revealed that both Al₂O₃ and HfO₂ have an optimal shell thickness of about 20 nm to ensure maximum absorption in CH₃NH₃PbI₃. The results can be utilized as a useful guideline when designing photovoltaics from an optical point of view.     

Improved Functionality of Lithium‐Ion Batteries Enabled by Atomic Layer Deposition on the Porous Microstructure of Polymer Separators and Coating Electrodes

Atomic layer deposition (ALD) of Al₂O₃ is applied on a polypropylene separator for lithium‐ion batteries. A thin Al₂O₃ layer (<10 nm) is coated on every surface of the porous polymer microframework without significantly increasing the total separator thickness. The thin Al₂O₃ ALD coating results in significantly suppressed thermal shrinkage, which may lead to improved safety of the batteries. More importantly, the wettability of Al₂O₃ ALD‐coated separators in an extremely polar electrolyte based on pure propylene carbonate (PC) solvent is demonstrated, without any decrease in electrochemical performances such as capacity, rate capability, and cycle life. Finally, a LiCoO₂/natural graphite full cell is demonstrated under extremely severe conditions (pure PC‐based electrolyte and high (4.5 V) upper cut‐off potential), which is enabled by the Al₂O₃ ALD coating on all three components (cathode, anode, and separator).     

Significantly Enhanced Electrostatic Energy Storage Performance of Flexible Polymer Composites by Introducing Highly Insulating‐Ferroelectric Microhybrids as Fillers

A hybrid nanoparticle, consisting of BaTiO₃ nanoparticles tightly embedded in bronnitride (BN) nanosheets, has been fabricated based on a daring supposition that BN may act as a host to incorporate ferroelectric nanoparticles to improve insulation and polarization under a high electric field. Using the hybrids as fillers in poly(vinylidene fluoride) (PVDF) composites, a high electric breakdown strength (E_b ≈580 kV/mm), which is 1.76 times of the PVDF film, is obtained when the filler content is 5 wt%. A large displacement (9.3 µC/cm² under 580 kV/mm) is observed so as to obtain a high discharged energy density (U_d ≈17.6 J/cm³) of the BT@BN/PVDF composites, which is 2.8 times of the PVDF film. The enhancement ratio of E_b achieved in this study demonstrates the highest among the reported results. This hybrid structure of fillers provides an effective way to adjust and improve the energy storage properties of the polymer‐based dielectrics.     

Flexible,Scalable, and Highly Conductive Garnet‐Polymer Solid Electrolyte Templated by Bacterial Cellulose

Solid‐state electrolytes are a promising candidate for the next‐generation lithium‐ion battery, as they have the advantages of eliminating the leakage hazard of liquid solvent and elevating stability. However, inherent limitations such as the low ionic conductivity of solid polymer electrolytes and the high brittleness of inorganic ceramic electrolytes severally impede their practical application. Here, an inexpensive, facile, and scalable strategy to fabricate a hybrid Li₇La₃Zr₂O₁₂ (LLZO) and poly(ethylene oxide)‐based electrolyte by exploiting bacterial cellulose as a template is reported. The well‐organized LLZO network significantly enhances the ionic conductivity by extending long transport pathways for Li ions, exhibiting an elevated conductivity of 1.12 × 10^?4 S cm^?1. In addition, the hybrid electrolyte presents a structural flexibility, with minor impedance increase after bending. The facile and applicable approach establishes new principles for the strategy of designing scalable and flexible hybrid polymer electrolytes that can be utilized for high‐energy‐density batteries.     

Metal-Dielectric-Graphene Hybrid Heterostructures with Enhanced Surface Plasmon Resonance Sensitivity Based on Amplitude and Phase Measurements

Metal-dielectric-graphene hybrid heterostructures based on oxides Al₂O₃, HfO₂, and ZrO₂ as well as on complementary metal–oxide–semiconductor compatible dielectric Si₃N₄ covering plasmonic metals Cu and Ag have been fabricated and studied. We show that the characteristics of these heterostructures are important for surface plasmon resonance biosensing (such as minimum reflectivity, sharp phase changes, resonance full width at half minimum and resonance sensitivity to refractive index unit (RIU) changes) can be significantly improved by adding dielectric/graphene layers. We demonstrate maximum plasmon resonance spectral sensitivity of more than 30,000 nm/RIU for Cu/Al₂O₃ (ZrO₂, Si₃N₄), Ag/Si₃N₄ bilayers and Cu/dielectric/graphene three-layers for near-infrared wavelengths. The sensitivities of the fabricated heterostructures were?~?5–8 times higher than those of bare Cu or Ag thin films. We also found that the width of the plasmon resonance reflectivity curves can be reduced by adding dielectric/graphene layers. An unexpected blueshift of the plasmon resonance spectral position was observed after covering noble metals with high-index dielectric/graphene heterostructures. We suggest that the observed blueshift and a large enhancement of surface plasmon resonance sensitivity in metal-dielectric-graphene hybrid heterostructures are produced by stationary surface dipoles which generate a strong electric field concentrated at the very thin top dielectric/graphene layer.

     

Plasmachemical and heterogeneous processes in ozonizers with oxygen activation by a dielectric barrier discharge

Plasmachemical and heterogeneous processes of generation and loss of ozone in the atmosphericpressure dielectric barrier discharge in oxygen are studied theoretically. Plasmachemical and electronic kinetics in the stage of development and decay of a single plasma filament (microdischarge) are calculated numerically with and without allowance for the effects of ozone vibrational excitation and high initial ozone concentration. The developed analytical approach is applied to determine the output ozone concentration taking into account ozone heterogeneous losses on the Al₂O₃ dielectric surface. Using the results of quantummechanical calculations by the method of density functional theory, a multistage catalytic mechanism of heterogeneous ozone loss based on the initial passivation of a pure Al₂O₃ surface by ozone and the subsequent interaction of O₃ molecules with the passivated surface is proposed. It is shown that the conversion reaction 2O₃ → 3O₂ of a gas-phase ozone molecule with a physically adsorbed ozone molecule can result in the saturation of the maximum achievable ozone concentration at high specific energy depositions, the nonstationarity of the output ozone concentration, and its dependence on the prehistory of ozonizer operation.     

Inverted Tandem Polymer Solar Cells with Polyethylenimine‐Modified MoOX/Al2O3:ZnO Nanolaminate as the Charge Recombination Layers

A new charge recombination layer for inverted tandem polymer solar cells is reported. A bilayer of MoO_X/Al₂O₃:ZnO nanolaminate is shown to enable efficient charge recombination in inverted tandem cells. A polymer surface modification on the MoO_X/Al₂O₃:ZnO nanolaminate bilayer increases the work function contrast between the two outward surfaces of the charge recombination layer, further improving the performance of tandem solar cells. An analysis of the electrical, optical, and surface properties of the charge recombination layer is presented. Inverted tandem polymer solar cells, with two photoactive layers comprising poly (3‐hexylthiophene) (P3HT):indene‐C₆₀ bisadduct (IC₆₀BA) for the bottom cell and poly[(4,8‐bis‐(2‐ethylhexyloxy)‐benzo[1,2‐b:4,5‐b']dithiophene)‐2,6‐diyl‐alt‐(4‐(2‐ethylhexanoyl)‐thieno[3,4‐b]thiophene))‐2,6‐diyl] (PBDTTT‐C):[6,6]‐phenyl C₆₁ butyric acid methyl ester (PC₆₀BM) for the top cell, yield an open‐circuit voltage of 1481 mV ± 15 mV, a short‐circuit current density of 7.1 mA cm^?2 ± 0.1 mA cm^?2, and a fill factor of 0.62 ± 0.01, resulting in a power conversion efficiency of 6.5% ± 0.1% under simulated AM 1.5G, 100 mW cm^?2 illumination.     

Flexible Lead‐Free Perovskite Oxide Multilayer Film Capacitor Based on (Na0.8K0.2)0.5Bi0.5TiO3/Ba0.5Sr0.5(Ti0.97Mn0.03)O3 for High‐Performance Dielectric Energy Storage

Flexible thin film dielectric capacitors with high energy storage density and a fast charging–discharging rate have attracted increasing attention as the development of microelectronics progresses toward flexibility and miniaturization. In this work, an all‐inorganic thin film dielectric capacitor with a multilayer structure based on (Na_0.8K_0.2)_0.5Bi_0.5TiO₃ and Ba_0.5Sr_0.5(Ti_0.97Mn_0.03)O₃ is designed and synthesized on a mica substrate. By optimizing the periodic number (N), concomitantly enhanced breakdown strength and large polarization difference are achieved in the film with N = 6, which contributes to the large energy density (W_rec) of 91 J cm^?3, high efficiency (η) of 68%, and fast discharging rate of 47.6 µs. The obtained energy density is the highest value up to now in flexible dielectric capacitors, including lead‐free and lead‐based inorganic films as well as organic dielectric films. Moreover, no obvious deterioration of the energy storage performance is observed in the wide ranges of working temperature (?50–200 °C), operating frequency (500 Hz to 30 kHz), and fatigue cycles (1–10⁸). Besides, the W_rec and η are ultra‐stable under various bending radii (R = 12–2 mm) and even after 10⁴ bending cycles at R = 4 mm, demonstrating an outstanding mechanical bending endurance. This excellent performance will allow the capacitor thrive in flexible microenergy storage systems.     

The Prospects of Metal Oxide Nanoradiosensitizers: The Effect of the Elemental Composition of Particles and Characteristics of Radiation Sources on Enhancement of the Adsorbed Dose

Nanoparticles with a high atomic number are of interest as radiosensitizers for radiation therapy of cancer. A variety of nanoparticles and radiation sources makes the challenge of selecting their optimal combinations to achieve maximum irradiation efficacy relevant. In this work, we calculated the values of the dose enhancement factors of elemental compositions of metal oxide nanoparticles (Al₂O₃, TiO₂, MnO₂, Fe₂O₃ and Fe₃O₄, NiO, GeO₂, ZrO₂, CeO₂, Gd₂O₃, Tm₂O₃, HfO₂, Ta₂O₅, and Bi₂O₃), as well as GeO₂ and HfO₂ doped with the rare-earth elements lanthanum or ytterbium in combination with monochromatic photons (1–500 keV) and X-ray radiation corresponding to the radiation of kilovoltage X-ray therapy machines. At a nanoparticle concentration of 10 mg/mL, the maximum values of the dose enhancement factors were from 1.03 to 2.55 for monochromatic radiation and from 1.01 to 2.33 for the studied X-ray spectra. Doping GeO₂ with 20% lanthanum or ytterbium led to an increase in the maximum value of dose enhancement factors by ~10%. Doping HfO₂ did not lead to significant changes in the value of dose-enhancement factors. Thus, all studied elemental compositions of nanoparticles, with the exception of Al₂O₃ (a dose enhancement factor ~1.02), are promising for application in kilovoltage X-ray radiotherapy. At the same time, the complex dependence of dose enhancement factors on the spectral composition of X-ray radiation requires detailed studies of the impact of irradiation conditions on the magnitude of the radiomodifying effect of nanoparticles.

     

Medium Bandgap Polymer Donor Based on Bi(trialkylsilylthienyl‐benzo[1,2‐b:4,5‐b′]‐difuran) for High Performance Nonfullerene Polymer Solar Cells

A new 2D‐conjugated medium bandgap donor–acceptor copolymer, J81 , based on benzodifuran with trialkylsilyl thiophene side chains as donor unit and fluorobenzothiazole as acceptor, is synthesized and successfully used in nonfullerene polymer solar cells (PSCs) with low bandgap n‐type organic semiconductor (n‐OS) 3,9‐bis(2‐methylene‐ (3‐(1,1‐dicyanomethylene)‐indanone)‐5,5,11,11‐tetrakis(4‐ hexylphenyl)‐dithieno[2,3‐d:2′,3′‐d′]‐s‐indaceno[1,2‐b:5,6‐b′]‐ dithiophene (ITIC) and m ‐ITIC as acceptor. J81 possesses a lower‐lying highest occupied molecular orbital (HOMO) energy level of ?5.43 eV and medium bandgap of 1.93 eV with complementary absorption in the visible–near infrared region with the n‐OS acceptor. The PSCs based on J81 :ITIC and J81 :m ‐ITIC yield high power conversion efficiency of 10.60% and 11.05%, respectively, with high V _oc of 0.95–0.96 V benefit from the lower‐lying HOMO energy level of J81 donor. The work indicates that J81 is another promising polymer donor for the nonfullerene PSCs.     

Exploiting the Condensation Reactions of Acetophenone to Engineer Carbon‐Encapsulated Nb2O5 Nanocrystals for High‐Performance Li and Na Energy Storage Systems

Efficient synthetic methods to produce high‐performance electrode‐active materials are crucial for developing energy storage devices for large‐scale applications, such as hybrid supercapacitors (HSCs). Here, an effective approach to obtain controllable carbon‐encapsulated T‐Nb₂O₅ nanocrystals (NCs) is presented, based on the solvothermal treatment of NbCl₅ in acetophenone. Two separate condensation reactions of acetophenone generate an intimate and homogeneous mixture of Nb₂O₅ particles and 1,3,5‐triphenylbenzene (TPB), which acts as a unique carbon precursor. The electrochemical performance of the resulting composites as anode electrode materials can be tuned by varying the Nb₂O₅/TPB ratio. Remarkable performances are achieved for Li‐ion and Na‐ion energy storage systems at high charge–discharge rates (specific capacities of ≈90 mAh g^?1 at 100 C rate for lithium and ≈125 mAh g^?1 at 20 C for sodium). High energy and power densities are also achieved with Li‐ and Na‐ion HSC devices constructed by using the Nb₂O₅/C composites as anode and activated carbon (YPF‐50) as cathode, demonstrating the excellent electrochemical properties of the materials synthesized with this approach.     

Eu3+–Eu2+‐doped xAl2O3–ySiO2 and xAl2O3–zMgO composites phosphors

In this paper, the Eu³⁺–Eu²⁺ (4%, molar ratio)‐doped xAl₂O₃–ySiO₂ (x = 0–2.5, y = 1–5) and xAl₂O₃–zMgO (x = 0–1.5, z = 0–3) composites phosphors with different Al₂O₃ to SiO₂ (A/S) and Al₂O₃ to MgO (A/M) ratios were prepared using a high‐temperature solid‐state reaction under air atmosphere. The effects of the A/S and A/M on luminescence properties, crystal structure, electron spin resonance, and Commission Internationale de l’Eclairage chromaticity coordinates of the samples were systematically analyzed. These results indicated that the different A/S and A/M ratios in the matrix effectively affected the crystal phase, degrees of self‐reduction of Eu³⁺, and led the relative emission intensity of Eu²⁺/Eu³⁺ to change and adjust.     

Slow Organic‐to‐Inorganic Sub‐Lattice Thermalization in Methylammonium Lead Halide Perovskites Observed by Ultrafast Photoluminescence

Carrier dynamics in methylammonium lead halide (CH₃NH₃PbI_3–xCl_x) perovskite thin films, of differing crystal morphology, are examined as functions of temperature and excitation wavelength. At room temperature, long‐lived (>nanosecond) transient absorption signals indicate negligible carrier trapping. However, in measurements of ultrafast photoluminescence excited at 400 nm, a heretofore unexplained, large amplitude (50%–60%), 45 ps decay process is observed. This feature persists for temperatures down to the orthorhombic phase transition. Varying pump photon energy reveals that the fast, band‐edge photoluminescence (PL) decay only appears for excitation ≥2.38 eV (520 nm), with larger amplitudes for higher pump energies. Lower photon‐energy excitation yields slow dynamics consistent with negligible carrier trapping. Further, sub‐bandgap two‐photon pumping yields identical PL dynamics as direct absorption, signifying sensitivity to the total deposited energy and insensitivity to interfacial effects. Together with first principles electronic structure and ab initio molecular dynamics calculations, the results suggest the fast PL decay stems from excitation of high energy phonon modes associated with the organic sub‐lattice that temporarily enhance wavefunction overlap within the inorganic component owing to atomic displacement, thereby transiently changing the PL radiative rate during thermalization. Hence, the fast PL decay relates a characteristic organic‐to‐inorganic sub‐lattice equilibration timescale at optoelectronic‐relevant excitation energies.     

Pb‐Reduced CsPb0.9Zn0.1I2Br Thin Films for Efficient Perovskite Solar Cells

Fabrication of efficient Pb reduced inorganic CsPbI₂Br perovskite solar cells (PSC) are an important part of environment‐friendly perovskite technology. In this work, 10% Pb reduction in CsPb_0.9Zn_0.1I₂Br promotes the efficiency of PSCs to 13.6% (AM1.5, 1sun), much higher than the 11.8% of the pure CsPbI₂Br solar cell. Zn²⁺ has stronger interaction with the anions to manipulate crystal growth, resulting in size‐enlarged crystallite with enhanced growth orientation. Moreover, the grain boundaries (GBs) are passivated by the Cs‐Zn‐I/Br compound. The high quality CsPb_0.9Zn_0.1I₂Br greatly diminishes the GB trap states and facilitates the charge transport. Furthermore, the Zn4s‐I5p states slightly reduce the energy bandgap, accounting for the wider solar spectrum absorption. Both the crystalline morphology and energy state change benefit the device performance. This work highlights a nontoxic and stable Pb reduction method to achieve efficient inorganic PSCs.     

Luminescence of Eu3+ ions in hybrid polymer‐inorganic composites based on poly(methyl methacrylate) and zirconia nanoparticles

Spherical nanoparticles of ZrO₂ with 2 and 10 mol% EuO_1.5 up to 20 nm size were prepared by the method of hydrothermal synthesis for luminescent functionalization of the polymer–inorganic nanocomposites based on poly(methyl methacrylate). Surface modification of oxide nanoparticles was carried out by 3‐(trimethoxysilyl)propyl methacrylate, dimethoxymethylvinyl silane and 2‐hydroxyethyl methacrylate to provide uniform distribution and to prevent agglomeration of nanosized filler in the polymer matrix. Polymer–inorganic composites were synthesized by in situ free radical polymerization in bulk. Structuring of ZrO₂‐EuO_1.5 nanoparticles in the poly(methyl methacrylate) was studied by very‐small‐angle neutron scattering. According to the results, the dependence of photoluminescent properties of ZrO₂‐EuO_1.5 nanoparticles on the content of lanthanide, the symmetry of the crystal field, surface treatment and the polymer matrix were established. A correlation was shown between Stark splitting in luminescence spectra of ZrO₂‐EuO_1.5 nanoparticles and their phase composition. Using MMT‐assay it was shown that composites based on poly(methyl methacrylate) and ZrO₂‐EuO_1.5 nanoparticles do not have cytotoxic properties, which makes it possible to use them as prosthesis materials with contrasted and luminescent imaging properties.     

Influence of Electrical Resistivity and Machining Parameters on Electrical Discharge Machining Performance of Engineering Ceramics

Engineering ceramics have been widely used in modern industry for their excellent physical and mechanical properties, and they are difficult to machine owing to their high hardness and brittleness. Electrical discharge machining (EDM) is the appropriate process for machining engineering ceramics provided they are electrically conducting. However, the electrical resistivity of the popular engineering ceramics is higher, and there has been no research on the relationship between the EDM parameters and the electrical resistivity of the engineering ceramics. This paper investigates the effects of the electrical resistivity and EDM parameters such as tool polarity, pulse interval, and electrode material, on the ZnO/Al₂O₃ ceramic''s EDM performance, in terms of the material removal rate (MRR), electrode wear ratio (EWR), and surface roughness (SR). The results show that the electrical resistivity and the EDM parameters have the great influence on the EDM performance. The ZnO/Al₂O₃ ceramic with the electrical resistivity up to 3410 Ω·cm can be effectively machined by EDM with the copper electrode, the negative tool polarity, and the shorter pulse interval. Under most machining conditions, the MRR increases, and the SR decreases with the decrease of electrical resistivity. Moreover, the tool polarity, and pulse interval affect the EWR, respectively, and the electrical resistivity and electrode material have a combined effect on the EWR. Furthermore, the EDM performance of ZnO/Al₂O₃ ceramic with the electrical resistivity higher than 687 Ω·cm is obviously different from that with the electrical resistivity lower than 687 Ω·cm, when the electrode material changes. The microstructure character analysis of the machined ZnO/Al₂O₃ ceramic surface shows that the ZnO/Al₂O₃ ceramic is removed by melting, evaporation and thermal spalling, and the material from the working fluid and the graphite electrode can transfer to the workpiece surface during electrical discharge machining ZnO/Al₂O₃ ceramic.     

Thermally Durable Lithium‐Ion Capacitors with High Energy Density from All Hydroxyapatite Nanowire‐Enabled Fire‐Resistant Electrodes and Separators

The reliability and durability of lithium‐ion capacitors (LICs) are severely hindered by the kinetic imbalance between capacitive and Faradaic electrodes. Efficient charge storage in LICs is still a huge challenge, particularly for thick electrodes with high mass loading, fast charge delivery, and harsh working conditions. Here, a unique thermally durable, stable LIC with high energy density from all‐inorganic hydroxyapatite nanowire (HAP NW)‐enabled electrodes and separators is reported. Namely, the LIC device is designed and constructed with the electron/ion dual highly conductive and fire‐resistant composite Li₄Ti₅O₁₂‐based anode and activated carbon‐based cathode, together with a thermal‐tolerant HAP NW separator. Despite the thick‐electrode configuration, the as‐fabricated all HAP NW‐enabled LIC exhibits much enhanced electrochemical kinetics and performance, especially at high current rates and temperatures. Long cycling lifetime and state‐of‐the‐art areal energy density (1.58 mWh cm^?2) at a high mass loading of 30 mg cm^?2 are achieved. Benefiting from the excellent fire resistance of HAP NWs, such an unusual LIC exhibits high thermal durability and can work over a wide range of temperatures from room temperature to 150 °C. Taking full advantage of synergistic configuration design, this work sets the stage for designing advanced LICs beyond the research of active materials.     

Enhanced Energy Storage in Nanocomposite Capacitors through Aligned PZT Nanowires by Uniaxial Strain Assembly

The design of nanocomposite capacitors poses certain challenges due to the reduced dielectric strength resulting from the integration of typically high dielectric fillers into the polymer. In prior efforts it was demonstrated that increasing of the filler could lead to energy‐storage densities up to 19.3% above the neat polymer. To further enhance the energy density, a novel strategy is developed to align nanowires in a thermoplastic matrix by uniaxial stretching assembly. It is demonstrated that the energy‐storage capability of the nanocomposite can be enhanced through the alignment of lead zirconate titanate (PZT) nanowires (NWs) in the direction of the applied electric field compared to randomly oriented samples. The maximum energy density of the nanocomposites is as high as 1.28 J cm^?3 at a volume fraction of 40% PZT NWs (aspect ratio around 14) with axis of alignment in the direction of the electric field. The findings of this research could lead to broader interest due to development of the piezoceramic nanocomposites with enhanced dielectric properties for use in next‐generation energy‐storage and conversion devices.     

Ethylene Carbonate‐Free Electrolytes for High‐Nickel Layered Oxide Cathodes in Lithium‐Ion Batteries

Layered lithium nickel oxide (LiNiO₂) can provide very high energy density among intercalation cathode materials for lithium‐ion batteries, but suffers from poor cycle life and thermal‐abuse tolerance with large lithium utilization. In addition to stabilization of the active cathode material, a concurrent development of electrolyte systems of better compatibility is critical to overcome these limitations for practical applications. Here, with nonaqueous electrolytes based on exclusively aprotic acyclic carbonates free of ethylene carbonate (EC), superior electrochemical and thermal characteristics are obtained with an ultrahigh‐nickel cathode (LiNi_0.94Co_0.06O₂), capable of reaching a 235 mA h g^?1 specific capacity. Pouch‐type graphite|LiNi_0.94Co_0.06O₂ cells in EC‐free electrolytes withstand several hundred charge–discharge cycles with minor degradation at both ambient and elevated temperatures. In thermal‐abuse tests, the cathode at full charge, while reacting aggressively with EC‐based electrolytes below 200 °C, shows suppressed self‐heating without EC. Through 3D chemical and structural analyses, the intriguing impact of EC is visualized in aggravating unwanted surface parasitic reactions and irreversible bulk structural degradation of the cathode at high voltages. These results provide important insights in designing high‐energy electrodes for long‐lasting and reliable lithium‐ion batteries.