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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. [ABSTRACT FROM AUTHOR]

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. [ABSTRACT FROM AUTHOR]

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. [ABSTRACT FROM AUTHOR]

Graphical abstract Highlights • A biomimetic composite cathode is fabricated. • The cathode shows high capacity and good low-temperature performance. • Enhanced electron transfer is confirmed by first-principle modeling. • Highly-stable large capacity battery is achievable. Abstract High capacity and good safety secondary batteries are desired for portable electronics and electric vehicles. Currently, an effective method for simultaneously improving the intrinsically poor conductivity and the low capacity of cathodes remains a challenge. Here we present a biomimetic composite consisting of novel litchi-like LiFePO 4 spheres assembled by 20 nm nanoparticles and reduced graphene oxides (rGO). In particular, this biomimetic cathode provides short electron transfer pathways inside the LiFePO 4 spheres (through the hierarchical structure) and on the surface (by the interconnected rGO scaffold). The composite shows a high capacity of 161 mAh g−1 after 200 cycles, accompanying with a good Coulombic efficiency of about 100%. In addition, the composite retains a capacity of 93 mAh g−1 after cycling for 400 times, and shows a good capacity retention when cycling at −5 °C. [ABSTRACT FROM AUTHOR]

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. [ABSTRACT FROM AUTHOR]

[Display omitted] • A novel coral-like LiMn 2 O 4 cathode is prepared. • Biomimetic LiMn 2 O 4 displays stable energy-storage. • Coral-like nanostructure improves rate-performance. • A stable LiMn 2 O 4 cathode for Li-ion battery is achievable. Lithium-ion battery has been widely used in many fields; however, a good energy–density along with a high working voltage cathode is highly required. Here, a three-dimensional coral-like LiMn 2 O 4 nanostructure is developed by annealing a precursor synthesized through a hydrothermal approach, which displays a stable electrochemical performance as Li-ion battery cathode. The coral-like LiMn 2 O 4 cathode exhibits a capacity exceeds 118 mAh/g when cycling at 0.2C, and a Coulombic efficiency of 98.3%. When cycling at a relatively high rate of 0.5C, the electrochemical performance remains stable after 150 cycles. Moreover, good performances are achieved when cycling at different charge/discharge rates, which are ascribed to the biomimetic coral-like structure facilitates the transport of electrons and ions. The general preparation approach and the stable performance of the coral-like cathode would find broad applications for developing many other emerging energy-storage materials. [ABSTRACT FROM AUTHOR]

Despite extensive studies, the development of solid-state batteries (SSBs) has not yet met expectations, owing mainly to the lack of suitable solid electrolytes (SEs) that exhibit low electronic conductivity (σ e), high ionic conductivity (σ i), and good stability. Here, we propose an effective target-driven framework for holistic identifying promising garnet-type SEs. Using artificial intelligence (AI) technologies, we accurately predict the σ e with a mean absolute error of 0.25 eV, achieving a computed speed that is ~109 faster than ab initio calculations. Successfully, from 29,008 garnets, we discovered 12 promising super Li-ion conductors for SEs with σ e < 3.6 × 10−30 S cm−1, σ i > 10−4 S cm−1 (up to 3.24 S cm−1), and good thermal stability at room temperature and high temperature based on rigorous ab initio validation. These emerging SEs are expected to be used in Li-ion SSBs, thus improving the safety, performance, and lifetime of state-of-the-art energy storage technology. This approach directly cuts across at least 95 years of computational cycles to screen SEs, resulting in significant cost savings and helping us enter an electrified future that relies less on fossil fuels. The data that support the machine learning model of this study are available at: https://www.materialsproject.org. [Display omitted] • We successfully discover 12 promising super-ion conductors from 29,008 garnet materials. • The AI model for electronic conductivity prediction with high accuracy, achieving a computed speed that is ~109 times faster than using DFT calculations. • Our method spans ~95-year computational cycle for screening solid electrolytes. [ABSTRACT FROM AUTHOR]

A sandwich-structured NiMn 2 O 4 @reduced graphene oxide (NiMn 2 O 4 @rGO) nanocomposite consisting of ultrathin NiMn 2 O 4 sheets uniformly anchored on both sides of a three-dimensional (3D) porous rGO is presented. The NiMn 2 O 4 @rGO nanocomposites prepared through a dipping process combining with a hydrothermal method show a good electrochemical performance including a high reversible capability of 1384 mAh g −1 at 1000 mA g −1 over 1620 cycles, and an superior rate performance. Thus, a full cell consisting of a commercial LiCoO 2 cathode and the NiMn 2 O 4 @rGO anode delivers a stable capacity of about 1046 mAh g −1 (anode basis) after cycling at 50 mA g −1 for 60 times. It is demonstrated that the 3D porous composite structure accommodates the volume change during the Li + insertion/extraction process and facilitates the rapid transport of ions and electrons. The high performance would enable the presented NiMn 2 O 4 @rGO nanocomposite a promising anode candidate for practical applications in Li-ion batteries. [ABSTRACT FROM AUTHOR]

Engineering highly-stable and high-capacity energy-storage materials are significant for secondary batteries. Here, a multi-layered yolk-shell in yolk-shell microcapsule composing of yolk-shell Si@void@SnO 2 nanospheres packaged inside a microcapsule is developed through a microfluidic co-flow focusing approach. The multi-layered microcapsules-based Li-ion battery anode displays 1005 mAh g−1 after 200 cycles and a 99.9% Coulombic efficiency; and the capacity remains 752 mAh g−1 after charging-discharging 900 times at −10 °C. In addition, a stable rate-performance is achieved, and the cycling performance keeps well at different charging/discharging speeds. It is considered that the voids inside the microcapsules could accommodate the volumetric change of Si nanoparticles during cycling; and the porous morphology improves the transport of ions, which has been verified by a series of galvanostatic intermittent titration technique investigations. The high electrochemical performance indicates a good potential for practical applications at real environments, and the engineering of microcapsule would be applicable for developing other energy-storage composites. • A porous yolk-shell in yolk-shell microcapsule is developed for energy-storage. • Microcapsule is prepared through a microfluidic co-flow focusing approach. • The Li-ion battery exhibits long cycling life at low temperature. • Rapid ion diffusion is achievable in a porous microcapsule system. [ABSTRACT FROM AUTHOR]

Many binary metal oxides possess poor conductivity and ion diffusion efficiency, even though they have a high theoretical capacity as secondary battery anodes. Herein, we present a double binary metal sulfide composing of ZnCo 2 S 4 /NiCo 2 S 4 growing on carbon cloth, which was derived from a Zn–Co–Ni metal organic foam. Compared to the ZnCo 2 O 4 /NiCo 2 O 4 , the ZnCo 2 S 4 /NiCo 2 S 4 anodes exhibit an obviously improved electrochemical performance including a high areal capacity of 2.4 mAh cm−2 after cycling for 100 times at 0.36 mA cm−2, and a Coulombic efficiency of 99.9%. A well-recoverable rate-performance is also presented. In addition, the enhancement mechanism is investigated by using density functional theory simulations, which show the density of states and Li ion diffusion energies of the ZnCo 2 S 4 /NiCo 2 S 4 are improved compared to ZnCo 2 O 4 /NiCo 2 O 4. It is expected that the high-performance hybrid and the theoretical enhancement mechanism would enable them to find important applications for developing emerging energy-storage materials. A fast electron-transfer and ion-diffusion binary metal sulfide hybrid anode consisting of ZnCo 2 S 4 /NiCo 2 S 4 derived from MOFs was presented. Image 1 • A novel binary metal sulfide hybrid is reported. • Binary metal sulfides derived from MOFs are achieved. • Sulfide hybrid anodes exhibit a high lithium-storage performance. • DFT simulations confirm improvement of electron and ion transportation. [ABSTRACT FROM AUTHOR]

[Display omitted] • A free-standing NiCo 2 O 4 nanowires/ginkgo biloba composite is developed for Li-ion battery anode. • Surface growth on biomass achieves a low interfacial reaction barrier for energy-storage. • Nanowires/ginkgo biloba composite displays high performance at different temperatures. • The developed composite system is applicable for other metal oxide nanomaterials. The low cost and special structure of biomass materials enable them to be applicable for many energy-storage systems. Here, we develop NiCo 2 O 4 nanowires growing on carbonized ginkgo biloba to form free-standing anodes of Li-ion battery. The porous NiCo 2 O 4 nanowires have a high capacity, and they are able to accommodate the expansion of volume in cycling. Low surface reaction barrier of the NiCo 2 O 4 /ginkgo biloba anode is confirmed by galvanostatic intermittent titration technique analysis. The NiCo 2 O 4 /ginkgo biloba anode displays recoverable rate-performance and good stability when cycling at different current densities, which remains 2.6 mAh cm−2 after 350 cycles at room temperature. The Coulombic efficiency is about 99 % under −10 °C at 1 mA cm−2, and the capacity remains 1.28 mAh cm−2 after cycling 200 times. Capacity keeps 1.83 mA cm−2 under 45 °C, exhibiting a good Li-storage performance. The NiCo 2 O 4 /ginkgo biloba anode displays a better cycling performance than NiCo 2 O 4 /nickel foam and NiCo 2 O 4 /carbon cloth. The cost-effective synthesis strategy provides extensible applications for metal oxide/ginkgo biloba-based composites. Growing other binary metal oxides on the carbonized ginkgo biloba is also achievable such as ZnCo 2 O 4 , indicating the developed composite system is promising for preparing other free-standing energy-storage composites. [ABSTRACT FROM AUTHOR]

[Display omitted] • In-situ growing nickel cobalt layered double hydroxide on MOFs is developed for Li-ion batteries. • Surface growth on MOFs achieves a low interfacial reaction barrier for energy-storage. • Hierarchical nanocubes display high capacity and rate-performance at different temperatures. • Promising potential for real applications of nanocubes-based batteries is achievable. Binary transition metal oxides have attracted broad interests as promising Li-ion battery anode candidates because of high capacity and low cost. However, the poor cycling stability and severe volumetric expansion limit their practical applications. Herein, we develop a novel metal-organic-framework (MOF) derived hierarchical nanostructure composing of hollow NiFe 2 O 4 nanocube in-situ growing with nickel cobalt layered double hydroxide (NiCo-LDH) nanosheets. The NiFe 2 O 4 @NiCo-LDH nanocube anode delivers a specific capacity of 636.9 mAh g−1 after 100 cycles, high Coulombic efficiency and good rate-performance recoverability, which are much better compared to pristine NiFe 2 O 4. In addition, the developed nanocube composites display stable energy-storage properties at both low and high temperatures, indicating a promising potential for applications. In-situ monitoring on the interfacial reaction resistance of the NiFe 2 O 4 @NiCo-LDH at different charge–discharge stages proves its high conductivity and low interfacial resistance barrier. These findings enable the hierarchical nanocubes to be applicable for engineering many other energy-storage composites. [ABSTRACT FROM AUTHOR]

[Display omitted] • A Ga-Sn liquid alloy-encapsulated microcapsule is developed as self-healing Li-ion battery anode. • The liquid alloy microcapsules are prepared by using an oil-in-water emulsion. • Liquid alloy-encapsulated microcapsules exhibit high capacity and rate-performance. • Promising applications of Ga-Sn liquid alloy-encapsulated microcapsules is achievable. Engineering emerging anodes for lithium-ion batteries is of great significance. Here, we develop a self-healing anode composing of Ga-Sn liquid alloy infilling in a microcapsule. The microcapsules are prepared by using an oil-in-water emulsion. Liquid state of the Ga-Sn alloy in microcapsules is able to reduce structural failure on the basis of a self-healing mechanism during long-term cycling; the voids of microcapsules alleviate volumetric change of Ga-Sn alloy upon charge–discharge; and carbon shell improves the conductivity. The liquid alloy-encapsulated microcapsule anode exhibits a capacity of 711.6 mA h g−1 after 500 cycles and an ultrahigh Coulombic efficiency of 99.9 %. Moreover, the microcapsules present a recoverable rate-performance. Those properties enable the self-healing Ga-Sn liquid alloy-encapsulated microcapsules developed here to have a good potential for practical applications. [ABSTRACT FROM AUTHOR]

Bio-inspired materials have received broad attention for energy-storage systems owing to their special properties and low cost. Here, a cost-effective and general strategy is developed for preparing nanocluster arrays on leaves as three-dimensional free-standing Li-ion battery anodes. As a demonstrating case study, an FeCo 2 O 4 nanocluster array is constructed on lotus leaf, which displays a high areal capacity of 2.4 mAh cm−2 after cycling 100 times, and a stable Coulombic efficiency of 99.9%. After long-term 900 cycles at 10 ºC, capacity remains 1.15 mAh cm−2. At a high temperature of 45 ºC, capacity keeps 1.95 mAh cm−2 after cycling 150 times. A recoverable rate-performance after three-rounds measurements is also achieved, enabling the anode to be potentially used at different conditions. In addition, the preparation approach is successfully used for making many other composites including ZnCo 2 O 4 , NiCo 2 O 4 , CuCo 2 O 4 nanocluster arrays on lotus leaves, and ZnCo 2 O 4 , NiCo 2 O 4 , CuCo 2 O 4 , FeCo 2 O 4 nanocluster arrays on bamboo leaves, displaying a good applicability. [Display omitted] • A cost-effective and general bio-inspired approach for preparing nanocluster array on lotus leaf is presented. • 3D nanocluster array as free-standing anode shows a high areal capacity. • High performance during long-term 900 cycles at 10 ºC is achieved. • Several nanocluster arrays on leaves are prepared successfully. [ABSTRACT FROM AUTHOR]