The Li‐O2 batteries have attracted much attention due to their parallel theoretical energy density to gasoline. In the past 20 years, understanding and knowledge in Li‐O2 battery have greatly ...deepened in elucidating the relationship between structure and performance. Our group has been focusing on the cathode engineering and anode protection strategy development in the past years, trying to make full use of the superiority of metal‐air batteries towards applications. In this review, we aim to retrospect our efforts in developing practical, sustainable metal‐air batteries. We will first introduce the basic working principle of Li‐O2 batteries and our progresses in Li‐O2 batteries with typical cathode designs and anode protection strategies, which have together promoted the large capacity, long life and low charge overpotential. We emphasize the designing art of carbon‐based cathodes in this part along with a short talk on all‐metal cathodes. The following part is our research in Na‐O2 batteries including both cathode and anode optimizations. The differences between Li‐O2 and Na‐O2 batteries are also briefly discussed. Subsequently, our proof‐of‐concept work on Li‐N2 battery, a new energy storage system and chemistry, is discussed with detailed information on the discharge product identification. Finally, we summarize our designed models and prototypes of flexible metal‐air batteries that are promising to be used in flexible devices to deliver more power.
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SAZU, SBCE, SBMB, UL, UM, UPUK
The flexible Li‐O2 battery is suitable to satisfy the requirements of a self‐powered energy system, thanks to environmental friendliness, low cost, and high theoretical energy density. Herein, a ...flexible porous bifunctional electrode with both electrocatalytic and photocatalytic activity was synthesized and introduced as a cathode to assemble a high‐performance Li‐O2 battery that achieved an overpotential of 0.19 V by charging with the aid of solar energy. As a proof‐of‐concept application, a flexible Li‐O2 battery was constructed and integrated with a solar cell via a scalable encapsulate method to fabricate a flexible self‐powered energy system with excellent flexibility and mechanical stability. Moreover, by exploring the evolution of the electrode morphology and discharge products (Li2O2), the charging process of the Li‐O2 battery powered by solar energy and solar cell was demonstrated.
A flexible self‐powered energy system was fabricated by combining a flexible Li‐O2 battery with a flexible solar cell. By exploring the evolution of the electrode morphology and discharge products (Li2O2), the charging process of the Li‐O2 battery powered by solar energy and solar cell is demonstrated.
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SAZU, SBCE, SBMB, UL, UM, UPUK
Development of an efficient hydrogen evolution reaction (HER) catalyst composed of earth-abundant elements is scientifically and technologically important for the water splitting associated with the ...conversion and storage of renewable energy. Herein we report a new class of Co–C–N complex bonded carbon (only 0.22 at% Co) for HER with a self-supported and three-dimensional porous structure that shows an unexpected catalytic activity with low overpotential (212 mV at 100 mA cm–2) and long-term stability, better than that of most traditional-metal catalysts. Experimental observations in combination with density functional theory calculations reveal that C and N hybrid coordination optimizes the charge distribution and enhances the electron transfer, which synergistically promotes the proton adsorption and reduction kinetics.
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IJS, KILJ, NUK, PNG, UL, UM
To recycle rusty stainless‐steel meshes (RSSM) and meet the urgent requirement of developing high‐performance cathodes for potassium‐ion batteries (KIB), we demonstrate a new strategy to fabricate ...flexible binder‐free KIB electrodes via transformation of the corrosion layer of RSSM into compact stack‐layers of Prussian blue (PB) nanocubes (PB@SSM). When further coated with reduced graphite oxide (RGO) to enhance electric conductivity and structural stability, the low‐cost, stable, and binder‐free RGO@PB@SSM cathode exhibits excellent electrochemical performances for KIB, including high capacity (96.8 mAh g−1), high discharge voltage (3.3 V), high rate capability (1000 mA g−1; 42 % capacity retention), and outstanding cycle stability (305 cycles; 75.1 % capacity retention).
Turning waste into treasure: Rusty stainless steel meshes were utilized as solid‐state iron sources with excellent conductivity properties in order to fabricate stable, low‐cost, and flexible binder‐free potassium‐ion battery electrodes. When combined with unique structural design, the reduced graphite oxide‐coated electrodes exhibited high capacities, superior rate capabilities, and excellent cycle performance.
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The severe performance degradation of high‐capacity Li−O2 batteries induced by Li dendrite growth and concentration polarization from the low Li+ transfer number of conventional electrolytes hinder ...their practical applications. Herein, lithiated Nafion (LN) with the sulfonic group immobilized on the perfluorinated backbone has been designed as a soluble lithium salt for preparing a less flammable polyelectrolyte solution, which not only simultaneously achieves a high Li+ transfer number (0.84) and conductivity (2.5 mS cm−1), but also the perfluorinated anion of LN produces a LiF‐rich SEI for protecting the Li anode from dendrite growth. Thus, the Li−O2 battery with a LN‐based electrolyte achieves an all‐round performance improvement, like low charge overpotential (0.18 V), large discharge capacity (9508 mAh g−1), and excellent cycling performance (225 cycles). Besides, the fabricated pouch‐type Li–air cells exhibit promising applications to power electronic equipment with satisfactory safety.
A novel design principle of polymerization and fluorination for salt anions has been proposed and lithiated Nafion (LN) was suggested as a representative soluble lithium salt for the polyelectrolyte solution to improve the Li+ transfer number and produce a LiF‐rich solid electrolyte interface (SEI). Furthermore, the perfluorinated backbone of LN delivers the polyelectrolyte solution low flammability. Thus, making the Li−O2 batteries realize all‐round performance amelioration.
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SAZU, SBCE, SBMB, UL, UM, UPUK
With the rising demand for flexible and wearable electronic devices, flexible power sources with high energy densities are required to provide a sustainable energy supply. Theoretically, ...rechargeable, flexible Li‐O2/air batteries can provide extremely high specific energy densities; however, the high costs, complex synthetic methods, and inferior mechanical properties of the available flexible cathodes severely limit their practical applications. Herein, inspired by the structure of human blood capillary tissue, this study demonstrates for the first time the in situ growth of interpenetrative hierarchical N‐doped carbon nanotubes on the surface of stainless‐steel mesh (N‐CNTs@SS) for the fabrication of a self‐supporting, flexible electrode with excellent physicochemical properties via a facile and scalable one‐step strategy. Benefitting from the synergistic effects of the high electronic conductivity and stable 3D interconnected conductive network structure, the Li‐O2 batteries obtained with the N‐CNTs@SS cathode exhibit superior electrochemical performance, including a high specific capacity (9299 mA h g−1 at 500 mA g−1), an excellent rate capability, and an exceptional cycle stability (up to 232 cycles). Furthermore, as‐fabricated flexible Li‐air batteries containing the as‐prepared flexible super‐hydrophobic cathode show excellent mechanical properties, stable electrochemical performance, and superior H2O resistibility, which enhance their potential to power flexible and wearable electronic devices.
Inspired by blood capillary tissue, a self‐standing, flexible N‐CNTs@SS Li‐O2 battery cathode with an interpenetrative structure is fabricated via a facile and scalable one‐step strategy. The flexible Li‐O2 batteries with N‐CNTs@SS exhibit excellent mechanical properties, stable electrochemical performance, and superior H2O resistibility.
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FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SAZU, SBCE, SBMB, UL, UM, UPUK
A flexible and wearable lithium–oxygen (air) battery inspired by Chinese bamboo slips is constructed. In this novel battery, cathodes and anodes are woven without an air diffusion layer and any outer ...packaging; besides, the woven structure allows oxygen to access the cathodes from both sides freely, endowing the battery with a record energy density of over 523 W h kg−1.
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SAZU, SBCE, SBMB, UL, UM, UPUK
Arrays of aligned porous CuO nanorods are obtained by a facile and scalable method of engraving Cu foil in situ. Direct use of the arrays as a flexible and binder‐free sodium‐ion battery anode — ...without adding auxiliary materials — results in superior electrochemical performance, including cycle stability and rate capability, even at room temperature. This can be attributed to the unique array structure and the lack of binder in the electrode.
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SAZU, SBCE, SBMB, UL, UM, UPUK
Attractive hydrogen production? The amorphous Fe nanoparticles prepared following a simple but very efficient method possess high catalytic activity (see picture) for the generation of hydrogen from ...an aqueous solution of ammonia borane, even in air, and can readily be recycled with no obvious loss of catalytic activity.
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Electroreduction of CO2 into formic acid (HCOOH) is of particular interest as a hydrogen carrier and chemical feedstock. However, its conversion is limited by a high overpotential and low stability ...due to undesirable catalysts and electrode design. Herein, an integrated 3D bismuth oxide ultrathin nanosheets/carbon foam electrode is designed by a sponge effect and N‐atom anchor for energy‐efficient and selective electrocatalytic conversion of CO2 to HCOOH for the first time. Benefitting from the unique 3D array foam architecture for highly efficient mass transfer, and optimized exposed active sites, as confirmed by density functional theory calculations, the integrated electrode achieves high electrocatalytic performance, including superior partial current density and faradaic efficiency (up to 94.1 %) at a moderate overpotential as well as a high energy conversion efficiency of 60.3 % and long‐term durability.
Another dimension! An integrated 3D bismuth oxide ultrathin nanosheets/carbon foam electrode with a unique array foam architecture for highly efficient mass transfer and optimized exposed active sites has been designed by a sponge effect and N‐atom anchor for energy‐efficient, long‐term durable, and selective electrocatalytic conversion of CO2 to HCOOH (see figure).
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