Designing a Magnesium/Sodium Hybrid Battery Using Hierarchical Iron Selenide Architecture as Cathode Material and Modified Dual-Ion Salts in Ether as Electrolyte.

We developed a magnesium/sodium (Mg/Na) hybrid battery using a hierarchical disk-whisker FeSe2 architecture (HD-FeSe2) as the cathode material and a modified dual-ion electrolyte. The polarizable Se2- anion reduced the Mg2+ migration barrier, and the 3D configuration possessed a large surface area, which facilitated both Mg2+/Na+ cation diffusion and electron transport. The dual-ion salts with NaTFSI in ether reduced the Mg plating/stripping overvoltage in a symmetric cell. The hybrid battery exhibited an energy density of 260.9 Wh kg-1 and a power density of 600.8 W kg-1 at 0.2 A g-1. It showed a capacity retention of 154 mAh g-1 and a Coulombic efficiency of over 99.5% under 1.0 A g-1 after 800 long cycles. The battery also displayed outstanding temperature tolerance. The findings of 3D architecture as cathode material and hybrid electrolyte provide a pathway to design a highly reliable Mg/Na hybrid battery.

A Temperature-Tolerant Magnesium-Ion Battery Using Ball Cactus-like MgV2O4 as High-Performance Cathode.

Safe and high-performance secondary batteries using for all-climate conditions with different temperatures are highly required. Here, we develop a three-dimensional ball cactus-like MgV2O4 as cathode material for magnesium-ion (Mg-ion) batteries. After cycling 300 times, the capacity maintains 111.7 mAh g-1, while Coulombic efficiency stabilizes at about 100 %. Under temperatures of 45 °C and -5 °C, the capacities remain stable after 200 cycles. After three rounds of rate-performance tests, the capacity keeps quite stable. It is ascribed to the ball cactus-like morphology buffers the volumetric change during Mg2+ insertion/extraction, and provides sufficient pathways for ion diffusion, which has been verified by constant-current intermittent titration technology. It is believed that the good performance enables the Mg-ion batteries to have a all-climate capability.

A foldable self-healing rocking chair zinc-ion battery using a three-dimensional zinc metal-free anode.

We developed H2Ti5O11·xH2O on carbon cloth (HTO·xH2O/CC) as a binder-free Zn metal-free anode. This 'rocking chair' battery incorporated a ZnMn2O4/CC cathode, HTO·xH2O/CC anode, and a polyacrylamide-based electrolyte, and exhibited satisfactory flexibility and self-healing. It displayed recoverable capacities after four repetitions of cutting and healing, indicating a potential using as a foldable and wearable battery.

A Room-Temperature Self-Healing Liquid Metal-Infilled Microcapsule Driven by Coaxial Flow Focusing for High-Performance Lithium-Ion Battery Anode.

Liquid metals have attracted a lot of attention as self-healing materials in many fields. However, their applications in secondary batteries are challenged by electrode failure and side reactions due to the drastic volume changes during the "liquid-solid-liquid" transition. Herein, a simple encapsulated, mass-producible method is developed to prepare room-temperature liquid metal-infilled microcapsules (LMMs) with highly conductive carbon shells as anodes for lithium-ion batteries. Due to the reasonably designed voids in the microcapsule, the liquid metal particles (LMPs) can expand freely without damaging the electrode structure. The LMMs-based anodes exhibit superior capacity of rete-performance and ultra-long cycling stability remaining 413 mAh g-1 after 5000 cycles at 5.0 A g-1 . Ex situ X-ray powder diffraction (XRD) patterns and electrochemical impedance spectroscopy (EIS) reveal that the LMMs anode displays a stable alloying/de-alloying mechanism. DFT calculations validate the electronic structure and stability of the room-temperature LMMs system. These findings will bring some new opportunities to develop high-performance battery systems.

A metal organic framework-derived octahedral Cu1.95S@CoS2 for secondary batteries displaying long cycle life and stable temperature tolerance.

Low-cost and safe batteries are considered to be promising energy-storage systems. Here, a metal organic framework (MOF)-derived octahedral Cu1.95S@CoS2 composite is developed as a high-performance cathode of aluminium-ion (Al-ion) batteries. CoS2 nanoparticles on Cu1.95S provide active sites, making AlCl4- intercalation/deintercalation highly reversible, and reducing polarization. Cycling at 0.5 A g-1, Cu1.95S@CoS2 maintains stable capacities of 136.6 and 122.4 mA h g-1 after 200 cycles at room temperature and -10 °C, respectively. Stable rate-performance is also achieved. These findings will accelerate the application of Al-ion batteries and MOF-derived energy-storage composites.

Rational engineering NiMoO4nanosheets or Mn3O4nanowires on Fe2O3microdiscs as novel hierarchical anodes for high-performance lithium-ion batteries.

Since current graphite-based lithium-ion battery anode has a low theoretical capacity, the development of high-performance lithium-ion battery is severely restricted. Here, novel hierarchical composites composing of microdisc and the secondarily grown nanosheets and nanowires are developed, taking NiMoO4nanosheets and Mn3O4nanowires growing on Fe2O3microdiscs as demonstrating examples. The growth processes of the hierarchical structures have been investigated by adjusting a series of preparation conditions. The morphologies and structures have been characterized by using scanning electron microscopy, transmission electron microscope and x-ray diffraction. Fe2O3@Mn3O4composite-based anode displays a capacity of 713 mAh g-1after 100 cycles at 0.5 A g-1with a high Coulombic efficiency. A good rate-performance is also achieved. Fe2O3@NiMoO4anode delivers 539 mAh g-1after 100 cycles at 0.5 A g-1, which is obviously higher than that of pure Fe2O3. The hierarchical structure is conducive to improve the transport of electrons and ions, and provide numerous active sites, thus significantly enhancing the electrochemical performance. Moreover, the electron transfer performance is investigated by using density functional theory calculations. It is expected the findings presented here and the rational engineering of nanosheets/nanowires on microdiscs would be applicable for developing many other high-performance energy-storage composites.

A single-crystalline Co3O4 nanoparticle-assembled three-dimensional chain as an ultra-stable magnesium-ion battery cathode at different temperatures.

Engineering optimal cathode materials is significant for developing stable magnesium-ion (Mg-ion) batteries. Here, we present a single-crystalline Co3O4 nanoparticle-chain three-dimensional (3D) micro/nanostructure as an Mg-ion battery cathode. The hierarchical morphology is composed of radial nanochains self-assembled by single-crystalline nanoparticles, thus significantly facilitating the transfer of electrons and ions. 3D single-crystalline Co3O4 as an Mg-ion battery cathode displays a stable capacity of 111.7 mA h g-1 after 200 cycles with a decay rate per cycle as low as 0.037%. After four rounds of testing, the rate performance remains stable with a tiny decrease from 125.94 to 124.78 mA h g-1. At temperatures of 45 °C and -5 °C, the cathode still displays good stability and rate-performance. Galvanostatic intermittent titration technique (GITT) results verify a low energy barrier of the Co3O4 cathode. It is expected that the single-crystalline nanoparticle-assembled 3D structure and the stable Mg-storage performance will find broad applications for developing other stable energy-storage materials and their batteries.

A blade-like CoZn metal organic framework-based flexible quasi-solid Zn-ion battery.

Wearable flexible electronics has become more and more significant and popular in daily life. Here, a flexible quasi-solid Zn-ion battery consisting of CoZn-metal organic frameworks (MOFs) grown on carbon cloth as an all-in-one cathode working with a hydrogel electrolyte is developed. CoZn MOFs display a blade-like morphology, which is significant for rapid transfer of ions and electrons. The battery bending at angles from 0° to 180° displays high capacities and good capacity retention, and the capacity remains stable as the flexible battery twists to 90°. In addition, the capacity exceeds 101.4 mA h g-1 as the battery is folded to 180° for 30 times, which indicates that the developed Zn-ion batteries would be applicable for a large variety of wearable devices such as foldable cellphones and pads.

A Hierarchical SnO2@Ni6MnO8 Composite for High-Capacity Lithium-Ion Batteries.

Semiconductor-based composites are potential anodes for Li-ion batteries, owing to their high theoretical capacity and low cost. However, low stability induced by large volumetric change in cycling restricts the applications of such composites. Here, a hierarchical SnO2@Ni6MnO8 composite comprising Ni6MnO8 nanoflakes growing on the surface of a three-dimensional (3D) SnO2 is developed by a hydrothermal synthesis method, achieving good electrochemical performance as a Li-ion battery anode. The composite provides spaces to buffer volume expansion, its hierarchical profile benefits the fast transport of Li+ ions and electrons, and the Ni6MnO8 coating on SnO2 improves conductivity. Compared to SnO2, the Ni6MnO8 coating significantly enhances the discharge capacity and stability. The SnO2@Ni6MnO8 anode displays 1030 mAh g-1 at 0.1 A g-1 and exhibits 800 mAh g-1 under 0.5 A g-1, along with high Coulombic efficiency of 95%. Furthermore, stable rate performance can be achieved, indicating promising applications.

Highly-Efficient and Visible Light Photocatalytical Degradation of Organic Pollutants Using TiO2-Loaded on Low-Cost Biomass Husk.

A composite composing of TiO2 nanoparticles load on biomass rice husk (RH) is developed by directly growing TiO2 nanoparticles on RH. The in-situ growth of the nanocrystals on RH is achieved by a low-cost and one-step homogeneous precipitation. Rapid hydrolysis proceeds at 90 °C by using ammonium fluotitanate and urea to facilitate the selective growth of TiO2. The method provides an easy access to the TiO2-RH composite with a strong interaction between TiO2 nanoparticles and the underlying RH. The structure and composition of TiO2-RH are characterized by using X-ray diffraction, X-ray photoelectron spectroscopy, Fourier-transform infrared spectroscopy, and UV-vis absorption spectroscopy. TiO2 nanoparticles-RH exhibits a good photocatalytic degradation of methyl orange. The results show that 92% of methyl orange (20 mg L-1) can be degraded within three hours in visible light. The catalytic activity of the composite is not reduced after 6 cycles, and it still reaches 81% after 6 cycles. The enhanced performance is ascribed to the suitable particle size the good dispersibility. It is expected that the high photocatalytical performance and the cost-effective composite presented here will inspire the development of other high-performance photocatalysts.

Rational engineering of VS4 nanorod array on rose-shaped VS2 nanosheets for high-performance aluminium-ion batteries.

High performance aluminium-ion (Al-ion) batteries are of wide interest owing to the high theoretical capacity, abundance of Al metal and good safety. Here, we develop a hierarchical VS2@VS4 composed of a VS4 nanorod array in situ grown on VS2 rose-shaped nanosheets that displays a good electrochemical performance. The VS2@VS4 cathode displays a high capacity of 162.7 mA h g-1 after 200 cycles at -10 °C, and keeps 116.5 mA h g-1 after 500 cycles at room temperature. Rate-performance at -10 °C shows a capacity retention rate of 90%, which indicates the potential for engineering high-performance energy-storage composites.

A flexible self-healing Zn3V2O7(OH)2·2H2O-based Zn-ion battery under continuous folding and twisting.

Engineering flexible and self-healing batteries is significant for wearable electronics. Here, we develop a flexible self-healing Zn-ion battery with a Zn3V2O7(OH)2·2H2O cathode working with a polyvinyl alcohol hydrogel electrolyte. The battery achieves a high capacity and robust structure during switching and self-healing, and keeps a stable potential after cutting/healing several times. After being bent at 30°, 60°, 90°, 120° and 150°, the capacities remain stable, and the battery delivers 78.6 mA h g-1 when repeatedly folding at 90°, displaying the potential for various applications such as foldable cell phones.

A graphene oxide scaffold-encapsulated microcapsule for polysulfide-immobilized long life lithium-sulfur batteries.

Engineering high-performance cathodes for high energy-density lithium-sulfur (Li-S) batteries is quite significant to achieve commercialization. Here, we develop a graphene oxide scaffold/sulfur composite-encapsulated microcapsule (GSM) for high-performance Li-S batteries, which is prepared through the co-flow focusing (CFF) approach. The GSM-based cathode displays a high capacity of 1004 mA h g-1 at 0.2C after cycling 200 times, a long-term cycling stability after 1000 cycles at 2C, and a good rate-performance. At temperatures of -5 °C and 45 °C, the electrochemical performance is also excellent. The computational calculations based on density functional theory (DFT) verify the high adsorption energies of the microcapsules towards polysulfides, suppressing the shuttle effect efficiently. It is expected that the GSM system developed based on the CFF method here and its high electrochemical performance will enable it to be applicable for preparing many other emerging energy-storage materials and secondary batteries.

An Ensemble Learning Platform for the Large-Scale Exploration of New Double Perovskites.

Lead-free double perovskites are regarded as stable and green optoelectronic alternatives to single perovskites, but may exhibit indirect band gaps and high effective masses, thus limiting their maximum photovoltaic efficiency. Considering that the trial-and-error experimental and computational approaches cannot quickly identify ideal candidates, we propose an ensemble learning workflow to screen all suitable double perovskites from the periodic table, with a high predictive accuracy of 92% and a computed speed that is ∼108 faster than ab initio calculations. From ∼23 314 unexplored double perovskites, we successfully identify six candidates that exhibit suitable band gaps (1.0-2.0 eV), where two have direct band gaps and low effective masses. They all show good thermal stabilities that are hopefully able to be synthesized. The proposed ML workflow immensely shortens the screening cycle for double perovskites, which will greatly promote the development and application of photovoltaic devices.

A novel free-standing metal organic frameworks-derived cobalt sulfide polyhedron array for shuttle effect suppressive lithium-sulfur batteries.

Metal-organic-frameworks-derived nanostructures have received broad attention for secondary batteries. However, many strategies focus on the preparation of dispersive materials, which need complicated steps and some additives for making electrodes of batteries. Here, we develop a novel free-standing Co9S8polyhedron array derived from ZIF-67, which grows on a three-dimensional carbon cloth for lithium-sulfur (Li-S) battery. The polar Co9S8provides strong chemical binding to immobilize polysulfides, which enables efficiently suppressing of the shuttle effect. The free-standing S@Co9S8polyhedron array-based cathode exhibits ultrahigh capacity of 1079 mAh g-1after cycling 100 times at 0.1 C, and long cycling life of 500 cycles at 1 C, recoverable rate-performance and good temperature tolerance. Furthermore, the adsorption energies towards polysulfides are investigated by using density functional theory calculations, which display a strong binding with polysulfides.

General Liquid-Driven Coaxial Flow Focusing Preparation of Novel Microcapsules for Rechargeable Magnesium Batteries.

Magnesium batteries have been considered promising candidates for next-generation energy storage systems owing to their high energy density, good safety without dendrite formation, and low cost of magnesium resources. However, high-performance cathodes with stable capacity, good conductivity, and fast ions transport are needed, since many conventional cathodes possess a low performance and poor preparation controllability. Herein, a liquid-driven coaxial flow focusing (LDCFF) approach for preparing a novel microcapsule system with controllable size, high loading, and stable magnesium-storage performance is presented. Taking the MoS2-infilled microcapsule as a case study, the magnesium battery cathode based on the microcapsules displays a capacity of 100 mAh g-1 after 100 cycles. High capacity retention is achieved at both low and high temperatures of -10, ‒5, and 45 °C, and a stable rate-performance is also obtained. The influences of the liquid flow rates on the size and shell thickness of the microcapsules are investigated; and electron and ion diffusion properties are also studied by first-principle calculations. The presented LDCFF method is quite general, and the high performance of the microcapsules enables them to find broad applications for making emerging energy-storage materials and secondary battery systems.

An oriented laterally-growing NiCo2O4 nanowire array on a Fe2O3 microdisc as a high-capacity and excellent rate-performance secondary battery anode.

A novel hierarchical composite consisting of an ordered NiCo2O4 nanowire array growing on the lateral side of a Fe2O3 microdisc is presented, which was confirmed by X-ray holography technology on a synchrotron radiation station. The composite-based Li-ion battery anode exhibits a high capacity of 1528 mA h g-1 after 200 cycles at 0.2C, a recoverable rate-performance after repeated tests, and robust mechanical properties.

An artificial sea urchin with hollow spines: improved mechanical and electrochemical stability in high-capacity Li-Ge batteries.

Metallic germanium (Ge) as the anode can deliver a high specific capacity and high rate capability in lithium ion batteries. However, the large volume expansion largely restrains its further application. Herein, we constructed a three-dimensional sea urchin structure consisting of double layered Ge/TiO2 nanotubes as the spines via a ZnO template-removing method, which displays a capacity as high as 1060 mA h g-1 over 130 cycles. The robust, hollow oxide backbone serves as a strong support to accommodate the morphological change of Ge while the enhanced electron-transfer kinetics is attributed to the Ge content and the intimate contact between Ge and TiO2 during charging/discharging, which were confirmed using in situ transmission electronic microscopy observations and first-principles simulations. In addition, a high capacity retention of batteries using this hybrid composite as the anode was also achieved at low temperature.

A bee pupa-infilled honeycomb structure-inspired Li2MnSiO4 cathode for high volumetric energy density secondary batteries.

Emerging power batteries with both high volumetric energy density and fast charge/discharge kinetics are required for electric vehicles. The rapid ion/electron transport of mesostructured electrodes enables a high electrochemical activity in secondary batteries. However, the typical low fraction of active materials leads to a low volumetric energy density. Herein, we report a novel biomimetic "bee pupa infilled honeycomb"-structured 3D mesoporous cathode. We found previously the maximum active material filing fraction of an opal template before pinch-off was about 25%, whereas it could be increased to ∼90% with the bee pupa-infilled honeycomb-like architecture. Importantly, even with a high infilling fraction, fast Li+/e- transport kinetics and robust mechanical property were achievable. As the demonstration, a bee pupa infilled honeycomb-shaped Li2MnSiO4/C cathode was constructed, which delivered a high volumetric energy density of 2443 W h L-1. The presented biomimetic bee pupa infilled honeycomb configuration is applicable for a broad set of both cathodes and anodes in high energy density batteries.

A novel tin hybrid nano-composite with double nets of carbon matrixes as a stable anode in lithium ion batteries.

A novel battery hybrid composite anode consisting of tin nanoparticles encapsulated by double nets of carbon matrixes is presented. The improved electron transfer and volume change accommodation are confirmed via density functional theory modeling and in situ transmission electron microscopy observations, respectively.