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A flexible and highly efficient air cathode is fabricated via a simple electro‐deposition approach. This cathode exhibits a series of considerable electrochemical performances, in particular a good cycling performance (more than 70 cycles with the capacity limited 1000 mA h g−1). Based on this flexible cathode, a Li–O2 battery with flexible properties is also assembled, which can power a commercial LED normally. [ABSTRACT FROM AUTHOR]

Ultralong cycle life, high energy, and power density rechargeable lithium-ion batteries are crucial to the ever-increasing large-scale electric energy storage for renewable energy and sustainable road transport. However, the commercial graphite anode cannot perform this challenging task due to its low theoretical capacity and poor rate-capability performance. Metal oxides hold much higher capacity but still are plagued by low rate capability and serious capacity degradation. Here, a novel strategy is developed to prepare binder-free and mechanically robust CoO/graphene electrodes, wherein homogenous and full coating of β-Co(OH)2 nanosheets on graphene, through a novel electrostatic induced spread growth method, plays a key role. The combined advantages of large 2D surface and moderate inflexibility of the as-obtained β-Co(OH)2/graphene hybrid enables its easy coating on Cu foil by a simple layer-by-layer stacking process. Devices made with these electrodes exhibit high rate capability over a temperature range from 0 to 55 °C and, most importantly, maintain excellent cycle stability up to 5000 cycles even at a high current density. [ABSTRACT FROM AUTHOR]

Abstract: Z-type ferrites doped with La3+, Ba3− x La x Co2Fe24O41 (x=0.00–0.30), were prepared by sol–gel method. The effect of the substitution La3+ rare-earth ions for Ba2+ ions on the microstructure, complex permeability, permittivity and microwave absorption of the samples was investigated. The results show that the major phase of the ferrites changed to Z-phase when sintering temperature was 1250°C for 5h. With the increase of the substitution ratio of La3+ ions from 0.0 to 0.3, the lattice parameters a and c increased gradually, which resulted in the change of the particle shape and size. The data of magnetism showed that the addition of La3+ ions make the ferrite a better soft magnetic material due to increase of magnetization (σ s) and decrease of coercivity (H c). The La3+ ions doped in the ferrite not only improved complex permeability and complex permittivity, but also microwave absorbency. [Copyright &y& Elsevier]

Generally, water displays a dominated impact on the solution growth mechanism of the aprotic lithium−oxygen (Li−O2) batteries, however, the high reaction activity and laborious secondary chemistry transformation process are associated with the irreversible utilization of water. In this paper, a substituted proton‐containing, highly dispersed and hydroxyl group (−OH)‐rich contained catalyst is employed in the Li−O2 battery chemistry, and lithium hydroxide (LiOH) is identified as the primary discharge product. Intriguingly, the hydrogen (H) in LiOH comes solely from the added −OH‐rich onion carbon (OLC), which is capable of building a high‐speed proton transfer bridge between the generated moieties of dual active intermediates superoxide species (O2−) and the moderate hydroperoxide (HO2−) over the platinum (Pt) active sites. The new mechanism involving the HO2− intermediate realizes a hydrogen transfer process via O2− nucleophilic attack toward OLC, which significantly suppresses the O2−‐related side reactions. Thereby, the batteries with Pt/OLC attain a high specific capacity of 12 500 mAh g−1 at a current density of 100 mA g−1, exceptional energy efficiency (100%), and remarkable rechargeability. In addition, the strong OLC‐DMSO interaction inhibits the lithium metal corrosion caused by the shuttle reactions and ensures favorable battery cycling stability. The promising results open up a new reaction pathway for Li−O2 battery electrochemistry. [ABSTRACT FROM AUTHOR]

Aqueous zinc ion batteries are promising candidates for large scale energy‐storage due to their combination of inherent security and abundant reserves. The Zn metal undergoes continuous plating and stripping during electrochemical cycling, accompanied by parasitic side reactions and dendrite growth, which severely impedes the commercialization of batteries. Here, an innovative strategy is introduced in electrolyte engineering, dedicated to enhancing the stability at the Zn/electrolyte interface. Theoretical calculations and in situ experimental analyses collectively demonstrate that methyl sulfonyl methane (MSM) additives are beneficial in jointly modulating the hydrogen bonding network and the Zn2+ solvation structure, which in turn restricts H2O activity at the interface. Concurrently, the preferential adsorption of MSM on the Zn surface facilitates the controlled growth of compact zinc layers while suppressing dendritic and parasitic reactions. By modulating the electrolyte and managing the electrode interface, the Zn||Zn symmetric battery can be reversibly cycled over 150 days at a current density of 2 mA cm−2, and the assembled Zn||Cu half‐batteries show impressive cycling stability over 3100 cycles. This study provides an in‐depth comprehension of the Zn2+ plating/stripping behavior, and the development of sophisticated electrolyte systems offers practical guidance for constructing high‐performance zinc‐based batteries. [ABSTRACT FROM AUTHOR]

Y. Zhang, X.‐B. Zhang, and co‐workers report on page 4345 an electrostatic‐induced spread‐growth method to homogeneously coat CoO on graphene. Binder‐free electrode with excellent structural stability can then be easily prepared by layer‐by‐layer stacking. As an anode for Li‐ion batteries, the asprepared electrode exhibits a high rate capability and excellent cycle stability up to 5000 cycles. This opens up a promising strategy to develop high‐performance anodes for next‐generation LIBs. [ABSTRACT FROM AUTHOR]

The issue of cathode passivation during cycling resulting in rapid capacity fading and premature battery death is a major challenge that hinders the applications of lithium–oxygen (Li–O 2) batteries. Here, a facile strategy of introducing a functional separator based on flexible amination SiO 2 /TiO 2 inorganic woven film (STON WF) is proposed to suppress the cathode passivation problem. The by-products, i.e. HCOOLi, CH 3 COOLi and Li 2 CO 3 can be selectively adsorbed on the STON WF separator preferably compared with the cathode and further proved by the density functional theory (DFT) calculations. Thus, benefiting from the separator, the Li–O 2 cells with super P carbon and catalyst-free cathode show enhanced electrochemical performance (5645 mA h g−1 at a current density of 200 mA g−1), good rate capability (discharge voltage of 2.43 V at a current density of 1.5 A g−1) and especially superior cycle stability up to 268 cycles. These findings present a promising approach to prevent the premature battery death. • STON WF separator is utilized as by-products scavenger for first time. • The cathode passivation can be effectively alleviated with STON WF separator. • Li+ ion diffusion and the cycling performance for Li–O 2 batteries are improved. • Recyclable and low-cost STON WF is expected to be applied industrialization. [ABSTRACT FROM AUTHOR]

The lack of stable solid-state electrolytes (SSEs) with high-ionic conductivity and the rational design of electrode/electrolyte interfaces remains challenging for solid-state lithium batteries. Here, for the first time, a high-performance solid-state lithium-oxygen (Li-O 2 ) battery is developed based on the Li-ion-conducted hydrogen-bonded organic framework (LHOF) electrolyte and the HOF-DAT@CNT composite cathode. Benefiting from the abundant dynamic hydrogen bonding network in the backbone of LHOF-DAT SSEs, fast Li + ion transport (2.2×10 -4  S cm -1 ), a high Li + transference number (0.88), and a wide electrochemical window of 5.05 V are achieved. Symmetric batteries constructed with LHOF-DAT SSEs exhibit a stably cycled duration of over 1400 h with uniform deposition, which mainly stems from the jumping sites that promote a uniformly high rate of Li + flux and the hydrogen-bonding network structure that can relieve the structural changes during Li + transport. LHOF-DAT SSEs-based Li-O 2 batteries exhibit high specific capacity (10335 mAh g -1 ), and stable cycling life up to 150 cycles. Moreover, the solid-state lithium metal battery with LHOF-DAT SSEs endow good rate capability (129.6 mAh g -1 at 0.5 C), long-term discharge/charge stability (210 cycles). The design of LHOF-DAT SSEs opens an avenue for the development of novel SSEs-based solid-state lithium batteries., (© 2024 Wiley-VCH GmbH.)

Uncontrollable interfacial side reactions generated from common aqueous electrolytes, just like the hydrogen evolution reaction (HER) and dendrite growth, have severely prevented the practical application of zinc-ion batteries (ZIBs). Solid-state ZIBs are considered to be an efficient strategy by adopting high-quality solid-state electrolytes (SSEs). Here, by confining deep eutectic electrolyte (DEE) into the nanochannels of metal-organic framework (MOF)-PCN-222, a stable DEE@PCN-222 SSE with internal Zn 2+ transport channels was obtained. A distinctive ion-transport network composed of DEE and PCN-222 in the interior of DEE@PCN-222 realizes the efficient Zn 2+ conduction, contributing to high ionic conductivity of 3.13×10 -4  S cm -1 at room temperature, low activation energy of 0.12 eV, and a high Zn 2+ transference number of 0.74. Furthermore, experimental and theoretical investigations demonstrate that DEE@PCN-222 with its unique channel structure could homogeneously regulate the Zn 2+ distribution and effectively alleviate the side reactions. Highly reversible Zn plating/stripping performance of 2476 h can be realized by the SSE. The solid-state ZIBs show a specific capacity of 306 mAh g -1 and display cycling stability of 517 cycles. This unique design concept provides a new perspective in realizing the high-safety and high-performance ZIBs., (© 2024 Wiley-VCH GmbH.)

Photo-assisted Zn-air batteries can accelerate the kinetics of oxygen reduction and oxygen evolution reactions (ORR/OER); however, challenges such as rapid charge carrier recombination and continuous electrolyte evaporation remain. Herein, for the first time, piezoelectric catalysis is introduced in a photo-assisted Zn-air battery to improve carrier separation capability and accelerate the ORR/OER kinetics of the photoelectric cathode. The designed microhelical catalyst exploits simple harmonic vibrations to regenerate the built-in electric field continuously. Specifically, in the presence of the low-frequency kinetic energy that occurs during water flow, the piezoelectric-photocoupling catalyst of poly(vinylidene fluoride-co-trifluoroethylene)@ferric oxide(Fe@P(V-T)) is periodically deformed, generating a constant reconfiguration of the built-in electric field that separates photogenerated electrons and holes continuously. Further, on exposure to microvibrations, the gap between the charge and discharge potentials of the Fe@P(V-T)-based photo-assisted Zn-air battery is reduced by 1.7 times compared to that without piezoelectric assistance, indicating that piezoelectric catalysis is highly effective for enhancing photocatalytic efficiency. This study provides a thorough understanding of coupling piezoelectric polarization and photo-assisted strategy in the field of energy storage and opens a fresh perspective for the investigation of multi-field coupling-assisted Zn-air batteries., (© 2024 Wiley‐VCH GmbH.)

Chemically self-recharging zinc ion batteries (ZIBs), which are capable of auto-recharging in ambient air, are promising in self-powered battery systems. Nevertheless, the exclusive reliance on chemical energy from oxygen for ZIBs charging often would bring some obstacles in charging efficiency. Herein, we develop photo-assisted chemically self-recharging aqueous ZIBs with a heterojunction of MoS2/SnO2 cathode, which are favorable to enhancing both the charging and discharging efficiency as well as the chemical self-charging capabilities under illumination. The photo-assisted process promotes the electron transfer from MoS2/SnO2 to oxygen, accelerating the occurrence of the oxidation reaction during chemical self-charging. Furthermore, the electrons within the MoS2/SnO2 cathode exhibit a low transfer impedance under illumination, which is beneficial to reducing the migration barrier of Zn2+ within the cathode and thereby facilitating the uniform inserting of Zn2+ into MoS2/SnO2 cathode during discharging. This photo-assisted chemical self-recharging mechanism enables ZIBs to attain a maximum self-charging potential of 0.95 V within 3 hours, a considerable self-charging capacity of 202.5 mAh g-1 and excellent cycling performance in a self-charging mode. This work not only provides a route for optimizing chemical self-charging energy storage, but also broadens the potential application of aqueous ZIBs., (© 2024 Wiley‐VCH GmbH.)

Solid-state lithium-oxygen (Li-O 2 ) batteries have been widely recognized as one of the candidates for the next-generation of energy storage batteries. However, the development of solid-state Li-O 2 batteries has been hindered by the lack of solid-state electrolyte (SSE) with high ionic conductivity at room temperature, high Li + transference number, and the high stability to air. Herein, the organic molecular porous solid cucurbit[7]uril (CB[7]) with one-dimensional (1D) ion migration channels is developed as the SSE for solid-state Li-O 2 batteries. Taking advantage of the 1D ion migration channel for Li + conduction, CB[7] SSE achieves high ionic conductivity (2.45 × 10 -4 S cm -1 at 25 °C). Moreover, the noncovalent interactions facilitated the immobilization of anions, realizing a high Li + transference number (t Li + = 0.81) and Li + uniform distribution. The CB[7] SSE also shows a wide electrochemical stability window of 0-4.65 V and high thermal stability and chemical stability, as well as realizes stable Li + plating/stripping (more than 1000 h at 0.3 mA cm -2 ). As a result, the CB[7] SSE endows solid-state Li-O 2 batteries with superior rate capability and long-term discharge/charge stability (up to 500 h). This design strategy of CB[7] SSE paves the way for stable and efficient solid-state Li-O 2 batteries toward practical applications., (© 2024 Wiley‐VCH GmbH.)

Li-CO 2 batteries have received significant attention owing to their advantages of combining greenhouse gas utilization and energy storage. However, the high kinetic barrier between gaseous CO 2 and the Li 2 CO 3 product leads to a low operating voltage (<2.5 V) and poor energy efficiency. In addition, the reversibility of Li 2 CO 3 has always been questioned owing to the introduction of more decomposition paths caused by its higher charging plateau. Here, a novel "trinity" Li-CO 2 battery system was developed by synergizing CO 2 , soluble redox mediator (2,2,6,6-tetramethylpiperidoxyl, as TEM RM), and reduced graphene oxide electrode to enable selective conversion of CO 2 to Li 2 C 2 O 4 . The designed Li-CO 2 battery exhibited an output plateau reaching up to 2.97 V, higher than the equilibrium potential of 2.80 V for Li 2 CO 3 , and an ultrahigh round-trip efficiency of 97.1 %. The superior performance of Li-CO 2 batteries is attributed to the TEM RM-mediated preferential growth mechanism of Li 2 C 2 O 4 , which enhances the reaction kinetics and rechargeability. Such a unique design enables batteries to cope with sudden CO 2 -deficient environments, which provides an avenue for the rationally design of CO 2 conversion reactions and a feasible guide for next-generation Li-CO 2 batteries., (© 2024 Wiley‐VCH GmbH.)

Applying solar energy into energy storage battery systems is challenging in achieving green and sustainable development, however, the efficient progress of photo-assisted metal-air batteries is restricted by the rapid recombination of photogenerated electrons and holes upon the photocathode. Herein, a 1D-ordered MoS 2 nanotube (MoS 2 -ONT) with confined mass transfer can be used to extend the lifetime of photogenerated carriers, which is capable of overcoming the challenge of rapid recombination of electron and holes. The tubular confined space cannot only promote the orderly separation and migration of charge carriers but also realize the accumulation of charge and the rapid activation of oxygen molecules. The concave surface of MoS 2 -ONT can improve the carrier separation ability and prolong the carrier lifetime. Meanwhile, the ordered tubular confined space can effectively realize the rapid transfer of charge, ion, and oxygen. Under light irradiation, a fast oxygen reduction reaction kinetics of 70 mW cm -2 for photo-assisted Zn-air battery is achieved, which is the highest value reported for photo-assisted Zn-air batteries. Significantly, the photo-assisted Li-O 2 battery based on MoS 2 -ONT also shows superior rate capability and other exciting battery performance. This work shows the universality of the confined carrier separation strategy in photo-assisted metal-air batteries., (© 2023 Wiley‐VCH GmbH.)

Li-N 2 batteries have received widespread attention for their potential to integrate N 2 fixation, energy storage, and conversion. However, because of the low activity and poor stability of cathode catalysts, the electrochemical performance of Li-N 2 batteries is suboptimal, and their electrochemical reversibility has rarely been proven. In this study, a novel bifunctional photo-assisted Li-N 2 battery system was established by employing a plasmonic Au nanoparticles (NPs)-modified defective carbon nitride (Au-N v -C 3 N 4 ) photocathode. The Au-N v -C 3 N 4 exhibits strong light-harvesting, N 2 adsorption, and N 2 activation abilities, and the photogenerated electrons and hot electrons are remarkably beneficial for accelerating the discharge and charge reaction kinetics. These advantages enable the photo-assisted Li-N 2 battery to achieve a low overpotential of 1.32 V, which is the lowest overpotential reported to date, as well as superior rate capability and prolonged cycle stability (≈500 h). Remarkably, a combination of theoretical and experimental results demonstrates the high reversibility of the photo-assisted Li-N 2 battery. The proposed novel strategy for developing efficient cathode catalysts and fabricating photo-assisted battery systems breaks through the overpotential bottleneck of Li-N 2 batteries, providing important insights into the mechanism underlying N 2 fixation and storage., (© 2024 Wiley-VCH GmbH.)

The use of light-assisted cathode is regarded as an effective approach to reduce the overpotential of lithium carbon dioxide (Li - CO 2 ) batteries. However, the inefficient electron-hole separation and the complex discharge-charge reactions hamper the efficiency of CO 2 photocatalytic reaction in battery. Herein, a highly reversible force-assisted Li - CO 2 battery has been established for the first time by employing a Bi 0.5 Na 0.5 TiO 3 nanorods piezoelectric cathode. The high-energy electron and holes generated by the piezoelectric cathode with ultrasonic force can effectively enhance the carbon dioxide reduction reaction (CDRR) and carbon dioxide evolution reaction (CDER) kinetics, thereby reducing the overpotentials during the discharge-charge processes. Moreover, the morphology of the discharge product (Li 2 CO 3 ) can be modified via the dense surface electrons of the piezoelectric cathode, resulting in the promoted decomposition kinetics of Li 2 CO 3 in charging progress. Thus, the force-assisted Li - CO 2 battery with the unique piezoelectric cathode can adjust the output and input energy by ultrasonic wave, and provides an ultra-low charging platform of 3.52 V, and exhibits excellent cycle stability (a charging platform of 3.42 V after 100 h cycles). The investigation of the force-assisted process described herein provides significant insights to solve overpotential in the Li - CO 2 batteries system., Competing Interests: Declaration of Competing Interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2023 Elsevier Inc. All rights reserved.)

Solid-state lithium (Li) batteries promise both high energy density and safety while existing solid-state electrolytes (SSEs) fail to satisfy the rigorous requirements of battery operations. Herein, novel polyoxometalate SSEs, Li 3 PW 12 O 40 and Li 3 PMo 12 O 40 , are synthesized, which exhibit excellent interfacial compatibility with electrodes and chemical stability, overcoming the limitations of conventional SSEs. A high ionic conductivity of 0.89 mS cm -1 and a low activation energy of 0.23 eV are obtained due to the optimized three-dimensional Li + migration network of Li 3 PW 12 O 40 . Li 3 PW 12 O 40 exhibits a wide window of electrochemical stability that can both accommodate the Li anode and high-voltage cathodes. As a result, all-solid-state Li metal batteries fabricated with Li/Li 3 PW 12 O 40 /LiNi 0.5 Co 0.2 Mn 0.3 O 2 display a stable cycling up to 100 cycles with a cutoff voltage of 4.35 V and an areal capacity of more than 4 mAh cm -2 , as well as a cost-competitive SSEs price of $5.68 kg -1 . Moreover, Li 3 PMo 12 O 40 homologous to Li 3 PW 12 O 40 was obtained via isomorphous substitution, which formed a low-resistance interface with Li 3 PW 12 O 40 . Applications of Li 3 PW 12 O 40 and Li 3 PMo 12 O 40 in Li-air batteries further demonstrate that long cycle life (650 cycles) can be achieved. This strategy provides a facile, low-cost strategy to construct efficient and scalable solid polyoxometalate electrolytes for high-energy solid-state Li metal batteries., (© 2023 Wiley-VCH GmbH.)

Aprotic lithium-oxygen (Li-O 2 ) batteries are considered to be a promising alternative option to lithium-ion batteries for high gravimetric energy storage devices. However, the sluggish electrochemical kinetics, the passivation, and the structural damage to the cathode caused by the solid discharge products have greatly hindered the practical application of Li-O 2 batteries. Herein, the nonsolid-state discharge products of the off-stoichiometric Li 1- x O 2 in the electrolyte solutions are achieved by iridium (Ir) single-atom-based porous organic polymers (termed as Ir/AP-POP) as a homogeneous, soluble electrocatalyst for Li-O 2 batteries. In particular, the numerous atomic active sites act as the main nucleation sites of O 2 -related discharge reactions, which are favorable to interacting with O 2 - /LiO 2 intermediates in the electrolyte solutions, owing to the highly similar lattice-matching effect between the in situ-formed Ir 3 Li and LiO 2 , achieving a nonsolid LiO 2 as the final discharge product in the electrolyte solutions for Li-O 2 batteries. Consequently, the Li-O 2 battery with a soluble Ir/AP-POP electrocatalyst exhibits an ultrahigh discharge capacity of 12.8 mAh, an ultralow overpotential of 0.03 V, and a long cyclic life of 700 h with the carbon cloth cathode. The manipulation of nonsolid discharge products in aprotic Li-O 2 batteries breaks the traditional growth mode of Li 2 O 2 , bringing Li-O 2 batteries closer to being a viable technology.

Rechargeable lithium-oxygen (Li-O 2 ) batteries with high theoretical energy density are considered as promising candidates for portable electronic devices and electric vehicles, whereas their commercial application is hindered due to poor cyclic stability caused by the sluggish kinetics and cathode passivation. Herein, the intrinsic stress originated from the growth and decomposition of the discharge product (lithium peroxide, Li 2 O 2 ) is employed as a microscopic pressure resource to induce the built-in electric field, further improving the reaction kinetics and interfacial Lithium ion (Li + ) transport during cycling. Piezopotential caused by the intrinsic stress-strain of solid Li 2 O 2 is capable of providing the driving force for the separation and transport of carriers, enhancing the Li + transfer, and thus improving the redox reaction kinetics of Li-O 2 batteries. Combined with a variety of in situ characterizations, the catalytic mechanism of barium titanate (BTO), a typical piezoelectric material, was systematically investigated, and the effect of stress-strain transformation on the electrochemical reaction kinetics and Li + interface transport for the Li-O 2 batteries is clearly established. The findings provide deep insight into the surface coupling strategy between intrinsic stress and electric fields to regulate the electrochemical reaction kinetics behavior and enhance the interfacial Li + transport for battery system., (© 2023 Wiley-VCH GmbH.)

Solid-state electrolytes (SSEs) with high ionic conductivity and superior stability are considered to be a key technology for the safe operation of solid-state lithium batteries. However, current SSEs are incapable of meeting the requirements for practical solid-state lithium batteries. Here we report a general strategy for achieving high-performance SSEs by engineering polymers of intrinsic microporosity (PIMs). Taking advantage of the interconnected ion pathways generated from the ionizable groups, high ionic conductivity (1.06×10 -3  S cm -1 at 25 °C) is achieved for the PIMs-based SSEs. The mechanically strong (50.0 MPa) and non-flammable SSEs combine the two superiorities of outstanding Li + conductivity and electrochemical stability, which can restrain the dendrite growth and prevent Li symmetric batteries from short-circuiting even after more than 2200 h cycling. Benefiting from the rational design of SSEs, PIMs-based SSEs Li-metal batteries can achieve good cycling performance and superior feasibility in a series of withstand abuse tests including bending, cutting, and penetration. Moreover, the PIMs-based SSEs endow high specific capacity (11307 mAh g -1 ) and long-term discharge/charge stability (247 cycles) for solid-state Li-O 2 batteries. The PIMs-based SSEs present a powerful strategy for enabling safe operation of high-energy solid-state batteries., (© 2023 Wiley-VCH GmbH.)

The design of highly efficient electrocatalysts is a promising strategy to improve the electrochemical kinetics of Li-CO 2 batteries. However, electrocatalysts usually aim to reduce the energetic barrier for the corresponding electrochemical reactions; little attention has been given to modulating the kinetics that directly determine the local concentration of reaction molecules surrounding catalysts. Herein, we present a systematic study on the role of Li + reunion on the improvement of reaction kinetics in Li-CO 2 batteries with a Cu cone cathode. Specifically, this local, geometry-driven tip effect can enrich the local electron concentration to facilitate Li + ions diffusion from the bulk electrolyte to the surface of catalyst, leading to boosted catalytic performance. Further studies demonstrate that Cu(II/I) as a solid redox mediator dominates the reversible bulk redox reactions in a Cu cone cathode, which acts as an electron-hole transfer agent and permits the efficient reduction and oxidation of solid Li 2 CO 3 , contributing to an accessible theoretical discharge voltage, low charge potential below 3.2 V, impressive rate capability, and a long cycling stability (333 days) for Li-CO 2 batteries. The exploitation of the sharp-tip enhancement effect and dynamic creation of catalytic active sites is expected to become routine practice in future mechanistic studies for metal-air batteries.

At present, photoassisted Li-air batteries are considered to be an effective approach to overcome the sluggish reaction kinetics of the Li-air batteries. And, the organic liquid electrolyte is generally adopted by the current conventional photoassisted Li-air batteries. However, the superior catalytic activity of photoassisted cathode would in turn fasten the degradation of the organic liquid electrolyte, leading to limited battery cycling life. Herein, we tame the above limitation of the traditional liquid electrolyte system for Li-CO 2 batteries by constructing a photoassisted all-solid-state Li-CO 2 battery with an integrated bilayer Au@TiO 2 /Li 1.5 Al 0.5 Ge 1.5 (PO 4 ) 3 (LAGP)/LAGP (ATLL) framework, which can essentially improve battery stability. Taking advantage of photoelectric and photothermal effects, the Au@TiO 2 /LAGP layer enables the acceleration of the slow kinetics of the carbon dioxide reduction reaction and evolution reaction processes. The LAGP layer could resolve the problem of liquid electrolyte decomposition under illumination. The integrated double-layer LAGP framework endows the direct transportation of heat and Li + in the entire system. The photoassisted all-solid-state Li-CO 2 battery achieves an ultralow polarization of 0.25 V with illumination, as well as a high round-trip efficiency of 92.4%. Even at an extremely low temperature of -73 °C, the battery can still deliver a small polarization of 0.6 V by converting solar energy into heat to achieve self-heating. This study is not limited to the Li-air batteries but can also be applied to other battery systems, constituting a significant step toward the practical application of all-solid-state photoassisted Li-air batteries.

The photoassisted lithium-oxygen (Li-O 2 ) system has emerged as an important direction for future development by effectively reducing the large overpotential in Li-O 2 batteries. However, the advancement is greatly hindered by the rapidly recombined photoexcited electrons and holes upon the discharging and charging processes. Herein, a breakthrough is made in overcoming these challenges by developing a new magnetic and optical field multi-assisted Li-O 2 battery with 3D porous NiO nanosheets on the Ni foam (NiO/FNi) as a photoelectrode. Under illumination, the photogenerated electrons and holes of the NiO/FNi photoelectrode play a key role in reducing the overpotential during discharging and charging, respectively. By introducing the external magnetic field, the Lorentz force acts oppositely on the photogenerated electrons and holes, thereby suppressing the recombination of charge carriers. The magnetic and optical field multi-assisted Li-O 2 battery achieves an ultralow charge potential of 2.73 V, a high energy efficiency of 96.7%, and good cycling stability. This external magnetic and optical field multi-assisted technology paves a new way of developing high-performance Li-O 2 batteries and other energy storage systems., (© 2021 Wiley-VCH GmbH.)

A photoinduced flexible Li-CO 2 battery with well-designed, hierarchical porous, and free-standing In 2 S 3 @CNT/SS (ICS) as a bifunctional photoelectrode to accelerate both the CO 2 reduction and evolution reactions (CDRR and CDER) is presented. The photoinduced Li-CO 2 battery achieved a record-high discharge voltage of 3.14 V, surpassing the thermodynamic limit of 2.80 V, and an ultra-low charge voltage of 3.20 V, achieving a round trip efficiency of 98.1 %, which is the highest value ever reported (<80 %) so far. These excellent properties can be ascribed to the hierarchical porous and free-standing structure of ICS, as well as the key role of photogenerated electrons and holes during discharging and charging processes. A mechanism is proposed for pre-activating CO 2 by reducing In 3+ to In + under light illumination. The mechanism of the bifunctional light-assisted process provides insight into photoinduced Li-CO 2 batteries and contributes to resolving the major setbacks of the system., (© 2020 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.)

The design of a nanoporous cathode for Li-O2 batteries that can achieve high chemical stability and superior electrochemical performance remains a formidable challenge. A novel approach for the fabrication of nanoengineered PdNi alloys directly coated onto Ni nonwoven fabric (PdNi/NiNF) obtained through electrospinning has been proposed. On the basis of the contributions of the porous structure, the prepared metal-based cathodes can exhibit high chemical and mechanical stabilities, high catalytic activity, and high conductivity. In this design, the major side reactions were excluded when compared with popularly used carbon cathodes, and excellent cycling stability (266 cycles) could be achieved. The proposed cathode exhibited a high discharge capacity of 15 700 mA h g-1 at 500 mA g-1, which was 5 times higher than those reported for carbon-free cathodes.

With the rising development of flexible and wearable electronics, corresponding flexible energy storage devices with high energy density are required to provide a sustainable energy supply. Theoretically, rechargeable flexible Li-O 2 batteries can provide high specific energy density; however, there are only a few reports on the construction of flexible Li-O 2 batteries. Conventional flexible Li-O 2 batteries possess a loose battery structure, which prevents flexibility and stability. The low mechanical strength of the gas diffusion layer and anode also lead to a flexible Li-O 2 battery with poor mechanical properties. All these attributes limit their practical applications. Herein, the authors develop an integrated flexible Li-O 2 battery based on a high-fatigue-resistance anode and a novel flexible stretchable gas diffusion layer. Owing to the synergistic effect of the stable electrocatalytic activity and hierarchical 3D interconnected network structure of the free-standing cathode, the obtained flexible Li-O 2 batteries exhibit superior electrochemical performance, including a high specific capacity, an excellent rate capability, and exceptional cycle stability. Furthermore, benefitting from the above advantages, the as-fabricated flexible batteries can realize excellent mechanical and electrochemical stability. Even after a thousand cycles of the bending process, the flexible Li-O 2 battery can still possess a stable open-circuit voltage, a high specific capacity, and a durable cycle performance., (© 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

An ultrathin, lightweight, and wearable Li-O 2 battery with a novel segmented structure is first fabricated by employing a "break up the whole into parts" strategy. Superior battery performance including low overpotential, high specific capacity, good rate capability, excellent cycle stability, and high gravimetric/volumetric energy density (294.68 Wh kg -1 /274.06 Wh L -1 ) is successfully achieved even under repeatedly various deformation., (© 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

The "nonsticky" surface of a highly stable RuO 2 /carbon nanotube cathode enhances the formation and decomposition of cathode surface-induced, solvation-mediated, micrometer-sized discharge products Li 2 O 2 in Li-O 2 batteries and thus significantly improves the specific capacity, overpotentials, and cycle life. These findings contribute to a new understanding how the cathode surface controls Li-O 2 electrochemistry., (© 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)