An All‐Solid‐State Fiber‐Shaped Aluminum–Air Battery with Flexibility,Stretchability, and High Electrochemical Performance

Owing to the high theoretical energy density of metal–air batteries, the aluminum–air battery has been proposed as a promising long‐term power supply for electronics. However, the available energy density from the aluminum–air battery is far from that anticipated and is limited by current electrode materials. Herein we described the creation of a new family of all‐solid‐state fiber‐shaped aluminum–air batteries with a specific capacity of 935 mAh g^?1 and an energy density of 1168 Wh kg^?1. The synthesis of an electrode composed of cross‐stacked aligned carbon‐nanotube/silver‐nanoparticle sheets contributes to the remarkable electrochemical performance. The fiber shape also provides the aluminum–air batteries with unique advantages; for example, they are flexible and stretchable and can be woven into a variety of textiles for large‐scale applications.     

An Ultraflexible Silicon–Oxygen Battery Fiber with High Energy Density

To satisfy the rapid development of portable and wearable electronics, it is highly desired to make batteries with both high energy densities and flexibility. Although some progress has been made in recent decades, the available batteries share critical problems of poor energy storage capacity and low flexibility. Herein, we have developed a silicon–oxygen battery fiber with high energy density and ultra‐high flexibility by designing a coaxial architecture with a lithiated silicon/carbon nanotube hybrid fiber as inner anode, a polymer gel as middle electrolyte and a bare carbon nanotube sheet as outer cathode. The fiber showed a high energy density of 512 Wh kg⁻¹ and could effectively work after bending for 20 000 cycles. These battery fibers have been further woven into flexible textiles for a large‐scale application.     

Flexible,Stretchable, and Rechargeable Fiber‐Shaped Zinc–Air Battery Based on Cross‐Stacked Carbon Nanotube Sheets

The fabrication of flexible, stretchable and rechargeable devices with a high energy density is critical for next‐generation electronics. Herein, fiber‐shaped Zn–air batteries, are realized for the first time by designing aligned, cross‐stacked and porous carbon nanotube sheets simultaneously that behave as a gas diffusion layer, a catalyst layer, and a current collector. The combined remarkable electronic and mechanical properties of the aligned carbon nanotube sheets endow good electrochemical properties. They display excellent discharge and charge performances at a high current density of 2 A g⁻¹. They are also flexible and stretchable, which is particularly promising to power portable and wearable electronic devices.     

A Low‐Cost Neutral Zinc–Iron Flow Battery with High Energy Density for Stationary Energy Storage

Flow batteries (FBs) are one of the most promising stationary energy‐storage devices for storing renewable energy. However, commercial progress of FBs is limited by their high cost and low energy density. A neutral zinc–iron FB with very low cost and high energy density is presented. By using highly soluble FeCl₂/ZnBr₂ species, a charge energy density of 56.30 Wh L⁻¹ can be achieved. DFT calculations demonstrated that glycine can combine with iron to suppress hydrolysis and crossover of Fe³⁺/Fe²⁺. The results indicated that an energy efficiency of 86.66 % can be obtained at 40 mA cm⁻² and the battery can run stably for more than 100 cycles. Furthermore, a low‐cost porous membrane was employed to lower the capital cost to less than $ 50 per kWh, which was the lowest value that has ever been reported. Combining the features of low cost, high energy density and high energy efficiency, the neutral zinc–iron FB is a promising candidate for stationary energy‐storage applications.     

A Sustainable Redox‐Flow Battery with an Aluminum‐Based,Deep‐Eutectic‐Solvent Anolyte

Nonaqueous redox‐flow batteries are an emerging energy storage technology for grid storage systems, but the development of anolytes has lagged far behind that of catholytes due to the major limitations of the redox species, which exhibit relatively low solubility and inadequate redox potentials. Herein, an aluminum‐based deep‐eutectic‐solvent is investigated as an anolyte for redox‐flow batteries. The aluminum‐based deep‐eutectic solvent demonstrated a significantly enhanced concentration of circa 3.2 m in the anolyte and a relatively low redox potential of 2.2 V vs. Li⁺/Li. The electrochemical measurements highlight that a reversible volumetric capacity of 145 Ah L⁻¹ and an energy density of 189 Wh L⁻¹ or 165 Wh kg⁻¹ have been achieved when coupled with a I₃⁻/I⁻ catholyte. The prototype cell has also been extended to the use of a Br₂‐based catholyte, exhibiting a higher cell voltage with a theoretical energy density of over 200 Wh L⁻¹. The synergy of highly abundant, dendrite‐free, multi‐electron‐reaction aluminum anodes and environmentally benign deep‐eutectic‐solvent anolytes reveals great potential towards cost‐effective, sustainable redox‐flow batteries.     

High‐Performance Lithium–Air Battery with a Coaxial‐Fiber Architecture

The lithium–air battery has been proposed as the next‐generation energy‐storage device with a much higher energy density compared with the conventional lithium‐ion battery. However, lithium–air batteries currently suffer enormous problems including parasitic reactions, low recyclability in air, degradation, and leakage of liquid electrolyte. Besides, they are designed into a rigid bulk structure that cannot meet the flexible requirement in the modern electronics. Herein, for the first time, a new family of fiber‐shaped lithium–air batteries with high electrochemical performances and flexibility has been developed. The battery exhibited a discharge capacity of 12 470 mAh g^?1 and could stably work for 100 cycles in air; its electrochemical performances were well maintained under bending and after bending. It was also wearable and formed flexible power textiles for various electronic devices.     

An Aligned and Laminated Nanostructured Carbon Hybrid Cathode for High‐Performance Lithium–Sulfur Batteries

An aligned and laminated sulfur‐absorbed mesoporous carbon/carbon nanotube (CNT) hybrid cathode has been developed for lithium–sulfur batteries with high performance. The mesoporous carbon acts as sulfur host and suppresses the diffusion of polysulfide, while the CNT network anchors the sulfur‐absorbed mesoporous carbon particles, providing pathways for rapid electron transport, alleviating polysulfide migration and enabling a high flexibility. The resulting lithium–sulfur battery delivers a high capacity of 1226 mAh g⁻¹ and achieves a capacity retention of 75 % after 100 cycles at 0.1 C. Moreover, a high capacity of nearly 900 mAh g⁻¹ is obtained for 20 mg cm⁻², which is the highest sulfur load to the best of our knowledge. More importantly, the aligned and laminated hybrid cathode endows the battery with high flexibility and its electrochemical performances are well maintained under bending and after being folded for 500 times.     

An Insoluble Benzoquinone‐Based Organic Cathode for Use in Rechargeable Lithium‐Ion Batteries

Application of organic electrode materials in rechargeable batteries has attracted great interest because such materials contain abundant carbon, hydrogen, and oxygen elements. However, organic electrodes are highly soluble in organic electrolytes. An organic electrode of 2,3,5,6‐tetraphthalimido‐1,4‐benzoquinone (TPB) is reported in which rigid groups coordinate to a molecular benzoquinone skeleton. The material is insoluble in aprotic electrolyte, and demonstrates a high capacity retention of 91.4 % (204 mA h g⁻¹) over 100 cycles at 0.2 C. The extended π‐conjugation of the material contributes to enhancement of the electrochemical performance (155 mA h g⁻¹ at 10 C). Moreover, density functional theory calculations suggest that favorable synergistic reactions between multiple carbonyl groups and lithium ions can enhance the initial lithium ion intercalation potential. The described approach may provide a novel entry to next‐generation organic electrode materials with relevance to lithium‐ion batteries.     

A Porphyrin Complex as a Self‐Conditioned Electrode Material for High‐Performance Energy Storage

The novel functionalized porphyrin [5,15‐bis(ethynyl)‐10,20‐diphenylporphinato]copper(II) (CuDEPP) was used as electrodes for rechargeable energy‐storage systems with an extraordinary combination of storage capacity, rate capability, and cycling stability. The ability of CuDEPP to serve as an electron donor or acceptor supports various energy‐storage applications. Combined with a lithium negative electrode, the CuDEPP electrode exhibited a long cycle life of several thousand cycles and fast charge–discharge rates up to 53 C and a specific energy density of 345 Wh kg⁻¹ at a specific power density of 29 kW kg⁻¹. Coupled with a graphite cathode, the CuDEPP anode delivered a specific power density of 14 kW kg⁻¹. Whereas the capacity is in the range of that of ordinary lithium‐ion batteries, the CuDEPP electrode has a power density in the range of that of supercapacitors, thus opening a pathway toward new organic electrodes with excellent rate capability and cyclic stability.     

Stabilizing Lithium into Cross‐Stacked Nanotube Sheets with an Ultra‐High Specific Capacity for Lithium Oxygen Batteries

Although lithium–oxygen batteries possess a high theoretical energy density and are considered as promising candidates for next‐generation power systems, the enhancement of safety and cycling efficiency of the lithium anodes while maintaining the high energy storage capability remains difficult. Here, we overcome this challenge by cross‐stacking aligned carbon nanotubes into porous networks for ultrahigh‐capacity lithium anodes to achieve high‐performance lithium–oxygen batteries. The novel anode shows a reversible specific capacity of 3656 mAh g^?1, approaching the theoretical capacity of 3861 mAh g^?1 of pure lithium. When this anode is employed in lithium–oxygen full batteries, the cycling stability is significantly enhanced, owing to the dendrite‐free morphology and stabilized solid–electrolyte interface. This work presents a new pathway to high performance lithium–oxygen batteries towards practical applications by designing cross‐stacked and aligned structures for one‐dimensional conducting nanomaterials.     

A Long Cycle Life,Self‐Healing Zinc–Iodine Flow Battery with High Power Density

A zinc–iodine flow battery (ZIFB) with long cycle life, high energy, high power density, and self‐healing behavior is prepared. The long cycle life was achieved by employing a low‐cost porous polyolefin membrane and stable electrolytes. The pores in the membrane can be filled with a solution containing I₃⁻ that can react with zinc dendrite. Therefore, by consuming zinc dendrite, the battery can self‐recover from micro‐short‐circuiting resulting from overcharging. By using KI, ZnBr₂, and KCl as electrolytes and a high ion‐conductivity porous membrane, a very high power density can be achieved. As a result, a ZIFB exhibits an energy efficiency (EE) of 82 % at 80 mA cm⁻², which is 8 times higher than the currently reported ZIFBs. Furthermore, a stack with an output of 700 W was assembled and continuously run for more than 300 cycles. We believe this ZIFB can lead the way to development of new‐generation, high‐performance flow batteries.     

Highly Rechargeable Lithium‐CO2 Batteries with a Boron‐ and Nitrogen‐Codoped Holey‐Graphene Cathode

Metal‐air batteries, especially Li‐air batteries, have attracted significant research attention in the past decade. However, the electrochemical reactions between CO₂ (0.04 % in ambient air) with Li anode may lead to the irreversible formation of insulating Li₂CO₃, making the battery less rechargeable. To make the Li‐CO₂ batteries usable under ambient conditions, it is critical to develop highly efficient catalysts for the CO₂ reduction and evolution reactions and investigate the electrochemical behavior of Li‐CO₂ batteries. Here, we demonstrate a rechargeable Li‐CO₂ battery with a high reversibility by using B,N‐codoped holey graphene as a highly efficient catalyst for CO₂ reduction and evolution reactions. Benefiting from the unique porous holey nanostructure and high catalytic activity of the cathode, the as‐prepared Li‐CO₂ batteries exhibit high reversibility, low polarization, excellent rate performance, and superior long‐term cycling stability over 200 cycles at a high current density of 1.0 A g⁻¹. Our results open up new possibilities for the development of long‐term Li‐air batteries reusable under ambient conditions, and the utilization and storage of CO₂.     

Mesoporous Carbon@Titanium Nitride Hollow Spheres as an Efficient SeS2 Host for Advanced Li–SeS2 Batteries

The introduction of a certain proportion of selenium into sulfur‐based cathodes is an effective strategy for enhancing the integrated battery performance. However, similar to sulfur, selenium sulfide cathodes suffer from poor cycling stability owing to the dissolution of reaction intermediate products. In this study, to exploit the advantages of SeS₂ to the full and avoid its shortcomings, we designed and synthesized a hollow mesoporous carbon@titanium nitride (HMC@TiN) host for loading 70 wt % of SeS₂ as a cathode material for Li–SeS₂ batteries. Benefiting from both physical and chemical entrapment by hollow mesoporous carbon and TiN, the HMC@TiN/SeS₂ cathode manifests high utilization of the active material and excellent cycling stability. Moreover, it exhibits promising areal capacity (up to 4 mAh cm⁻²) with stable cell performance in the high‐mass‐loading electrode.     

Nitrogen,Phosphorus, and Fluorine Tri‐doped Graphene as a Multifunctional Catalyst for Self‐Powered Electrochemical Water Splitting

Electrocatalysts are required for clean energy technologies (for example, water‐splitting and metal‐air batteries). The development of a multifunctional electrocatalyst composed of nitrogen, phosphorus, and fluorine tri‐doped graphene is reported, which was obtained by thermal activation of a mixture of polyaniline‐coated graphene oxide and ammonium hexafluorophosphate (AHF). It was found that thermal decomposition of AHF provides nitrogen, phosphorus, and fluorine sources for tri‐doping with N, P, and F, and simultaneously facilitates template‐free formation of porous structures as a result of thermal gas evolution. The resultant N, P, and F tri‐doped graphene exhibited excellent electrocatalytic activities for the oxygen reduction reaction (ORR), oxygen evolution reaction (OER), and hydrogen evolution reaction (HER). The trifunctional metal‐free catalyst was further used as an OER–HER bifunctional catalyst for oxygen and hydrogen gas production in an electrochemical water‐splitting unit, which was powered by an integrated Zn–air battery based on an air electrode made from the same electrocatalyst for ORR. The integrated unit, fabricated from the newly developed N, P, and F tri‐doped graphene multifunctional metal‐free catalyst, can operate in ambient air with a high gas production rate of 0.496 and 0.254 μL s⁻¹ for hydrogen and oxygen gas, respectively, showing great potential for practical applications.     

Superior Rechargeability and Efficiency of Lithium–Oxygen Batteries: Hierarchical Air Electrode Architecture Combined with a Soluble Catalyst

The lithium–oxygen battery has the potential to deliver extremely high energy densities; however, the practical use of Li‐O₂ batteries has been restricted because of their poor cyclability and low energy efficiency. In this work, we report a novel Li‐O₂ battery with high reversibility and good energy efficiency using a soluble catalyst combined with a hierarchical nanoporous air electrode. Through the porous three‐dimensional network of the air electrode, not only lithium ions and oxygen but also soluble catalysts can be rapidly transported, enabling ultra‐efficient electrode reactions and significantly enhanced catalytic activity. The novel Li‐O₂ battery, combining an ideal air electrode and a soluble catalyst, can deliver a high reversible capacity (1000 mAh g^?1) up to 900 cycles with reduced polarization (about 0.25 V).     

Full Dissolution of the Whole Lithium Sulfide Family (Li2S8 to Li2S) in a Safe Eutectic Solvent for Rechargeable Lithium–Sulfur Batteries

The lithium–sulfur battery is an attractive option for next‐generation energy storage owing to its much higher theoretical energy density than state‐of‐the‐art lithium‐ion batteries. However, the massive volume changes of the sulfur cathode and the uncontrollable deposition of Li₂S₂/Li₂S significantly deteriorate cycling life and increase voltage polarization. To address these challenges, we develop an ?‐caprolactam/acetamide based eutectic‐solvent electrolyte, which can dissolve all lithium polysulfides and lithium sulfide (Li₂S₈–Li₂S). With this new electrolyte, high specific capacity (1360 mAh g^?1) and reasonable cycling stability are achieved. Moreover, in contrast to conventional ether electrolyte with a low flash point (ca. 2 °C), such low‐cost eutectic‐solvent‐based electrolyte is difficult to ignite, and thus can dramatically enhance battery safety. This research provides a new approach to improving lithium–sulfur batteries in aspects of both safety and performance.     

A Rechargeable Li‐CO2 Battery with a Gel Polymer Electrolyte

The utilization of CO₂ in Li‐CO₂ batteries is attracting extensive attention. However, the poor rechargeability and low applied current density have remained the Achilles’ heel of this energy device. The gel polymer electrolyte (GPE), which is composed of a polymer matrix filled with tetraglyme‐based liquid electrolyte, was used to fabricate a rechargeable Li‐CO₂ battery with a carbon nanotube‐based gas electrode. The discharge product of Li₂CO₃ formed in the GPE‐based Li‐CO₂ battery exhibits a particle‐shaped morphology with poor crystallinity, which is different from the contiguous polymer‐like and crystalline discharge product in conventional Li‐CO₂ battery using a liquid electrolyte. Accordingly, the GPE‐based battery shows much improved electrochemical performance. The achieved cycle life (60 cycles) and rate capability (maximum applied current density of 500 mA g⁻¹) are much higher than most of previous reports, which points a new way to develop high‐performance Li‐CO₂ batteries.     

Mass‐Production of Mesoporous MnCo2O4 Spinels with Manganese(IV)‐ and Cobalt(II)‐Rich Surfaces for Superior Bifunctional Oxygen Electrocatalysis

A mesoporous MnCo₂O₄ electrode material is made for bifunctional oxygen electrocatalysis. The MnCo₂O₄ exhibits both Co₃O₄‐like activity for oxygen evolution reaction (OER) and Mn₂O₃‐like performance for oxygen reduction reaction (ORR). The potential difference between the ORR and OER of MnCo₂O₄ is as low as 0.83 V. By XANES and XPS investigation, the notable activity results from the preferred Mn^IV‐ and Co^II‐rich surface. The electrode material can be obtained on large‐scale with the precise chemical control of the components at relatively low temperature. The surface state engineering may open a new avenue to optimize the electrocatalysis performance of electrode materials. The prominent bifunctional activity shows that MnCo₂O₄ could be used in metal–air batteries and/or other energy devices.     

Realizing both High Energy and High Power Densities by Twisting Three Carbon‐Nanotube‐Based Hybrid Fibers

Energy storage devices, such as lithium‐ion batteries and supercapacitors, are required for the modern electronics. However, the intrinsic characteristics of low power densities in batteries and low energy densities in supercapacitors have limited their applications. How to simultaneously realize high energy and power densities in one device remains a challenge. Herein a fiber‐shaped hybrid energy‐storage device (FESD) formed by twisting three carbon nanotube hybrid fibers demonstrates both high energy and power densities. For the FESD, the energy density (50 mWh cm^?3 or 90 Wh kg^?1) many times higher than for other forms of supercapacitors and approximately 3 times that of thin‐film batteries; the power density (1 W cm^?3 or 5970 W kg^?1) is approximately 140 times of thin‐film lithium‐ion battery. The FESD is flexible, weaveable and wearable, which offers promising advantages in the modern electronics.     

A Versatile Halide Ester Enabling Li‐Anode Stability and a High Rate Capability in Lithium–Oxygen Batteries

Li‐O₂ batteries are promising candidates for next‐generation high‐energy‐density battery systems. However, the main problems of Li–O₂ batteries include the poor rate capability of the cathode and the instability of the Li anode. Herein, an ester‐based liquid additive, 2,2,2‐trichloroethyl chloroformate, was introduced into the conventional electrolyte of a Li–O₂ battery. Versatile effects of this additive on the oxygen cathode and the Li metal anode became evident. The Li–O₂ battery showed an outstanding rate capability of 2005 mAh g^?1 with a remarkably decreased charge potential at a large current density of 1000 mA g^?1. The positive effect of the halide ester on the rate capacity is associated with the improved solubility of Li₂O₂ in the electrolyte and the increased diffusion rate of O₂. Furthermore, the ester promotes the formation of a solid–electrolyte interphase layer on the surface of the Li metal, which restrains the loss and volume change of the Li electrode during stripping and plating, thereby achieving a cycling stability over 900 h and a Li capacity utilization of up to 10 mAh cm^?2.