To achieve a high reversibility and long cycle life for lithium-oxygen (Li-O) batteries, the irreversible formation of LiO, inevitable side reactions, and poor charge transport at the cathode interfaces should be overcome. Here, we report a rational design of air cathode using a cobalt nitride (CoN) functionalized carbon nanofiber (CNF) membrane as current collector-catalyst integrated air cathode. Brush-like CoN nanorods are uniformly anchored on conductive electrospun CNF papers via hydrothermal growth of Co(OH)F nanorods followed by nitridation step. CoN-decorated CNF (CoN/CNF) cathode exhibited excellent electrochemical performance with outstanding stability for over 177 cycles in Li-O cells. During cycling, metallic CoN nanorods provide sufficient accessible reaction sites as well as facile electron transport pathway throughout the continuously networked CNF. Furthermore, thin oxide layer (<10 nm) formed on the surface of CoN nanorods promote reversible formation/decomposition of film-type LiO, leading to significant reduction in overpotential gap (∼1.23 V at 700 mAh g). Moreover, pouch-type Li-air cells using CoN/CNF cathode stably operated in real air atmosphere even under 180° bending. The results demonstrate that the favorable formation/decomposition of reaction products and mediation of side reactions are hugely governed by the suitable surface chemistry and tailored structure of cathode materials, which are essential for real Li-air battery applications.
Wireless electronic devices require small, rechargeable batteries that can be rapidly designed and fabricated in customized form factors for shape conformable integration. Here, we demonstrate an integrated design and manufacturing method for aqueous zinc-ion batteries composed of polyaniline (PANI)-coated carbon fiber (PANI/CF) cathodes, laser micromachined zinc (Zn) anodes, and porous separators that are packaged within three-dimensional printed geometries, including rectangular, cylindrical, H-, and ring-shapes. The PANI/CF cathode possesses high surface area and conductivity giving rise to high rate (∼600 C) performance. Due to outstanding stability of Zn-PANI batteries against oxygen and moisture, they exhibit long cycling stability in an aqueous electrolyte solution. As exemplar, we demonstrated rechargeable battery packs with tunable voltage and capacity using stacked electrodes that are integrated with electronic components in customized wearable devices.
Electrode materials with three-dimensional (3D) mesoporous structures possess superior features, such as shortened solid-phase lithium diffusion distance, large pore volume, full lithium ion accessibility, and a high specific area, which can facilitate fast lithium ion transport and electron transfer between solid/electrolyte interfaces. In this work, we introduce a facile synthesis route for the preparation of a 3D nanoarchitecture of Ge coated with carbon (3D-Ge/C) via a carbothermal reduction method in an inert atmosphere. The 3D-Ge/C showed excellent cyclability: almost 86.8% capacity retention, corresponding to a charge capacity of 1216 mAh g -1 even after 1000 cycles at a 2 C-rate. Surprisingly, the high average reversible capacity of 1122 mAh g -1 was maintained at a high charge rate of 100 C (160 A g -1 ). Even at an ultrahigh charge rate of 400 C (640 A g -1 ), an average capacity of 429 mAh g -1 was attained. Further, the full cell composed of 3D-Ge/C anode and LiCoO2 cathode exhibited excellent rate capability and cyclability with 94.7% capacity retention over 50 cycles. 3D-Ge/C, which offers a high energy density like batteries as well as a high power density like supercapacitors, is expected to be used in a wide range of electrochemical devices.A novel, facile synthetic route has been proposed to prepare a 3D nanoarchitecture Ge coated with carbon (3D-Ge/C) via a carbothermal reduction. The GeO 2 /PVP composite was carbonized in an argon atmosphere at 775 °C for 1 h to carbonize the PVP. During carbonization, the carbothermal reduction of GeO 2 occurred and simultaneously formed Ge within a 3D structure.
The combination of high-capacity and long-term cyclability has always been regarded as the first priority for next generation anode materials in lithium-ion batteries (LIBs). To meet these requirements, the Ag nanoparticle decorated mesoporous SnO/NiO nanotube (m-SNT) anodes were synthesized via an electrospinning process, followed by fast ramping rate calcination and subsequent chemical reduction in this work. The one-dimensional porous hollow structure effectively alleviates a large volume expansion during cycling as well as provides a short lithium-ion duffusion length. Furthermore, metallic nickel (Ni) nanoparticles converted from the NiO nanograins during the lithiation process reversibly decompose LiO during delithiation process, which significantly improves the reversible capacity of the m-SNT anodes. In addition, Ag nanoparticles uniformly decorated on the m-SNT via a simple chemical reduction process significantly improve rate capability and also contribute to long-term cyclability. The m-SNT@Ag anodes exhibited excellent cycling stability without obvious capacity fading after 500 cycles with a high capacity of 826 mAh g at a high current density of 1000 mA g. Furthermore, even at a very high current density of 5000 mA g, the charge-specific capacity remained as high as 721 mAh g, corresponding to 60% of its initial capacity at a current density of 100 mA g.
Chronic problems of zinc (Zn) metal anodes, such as notorious zinc dendrite growth and continuous side and corrosion reactions, hamper the commercialization of aqueous zinc-ion batteries (ZIBs). Herein, we have demonstrated the significance of surface properties of Zn anodes for suppressing parasitic side reactions and zinc dendrite growth. On the basis of the findings, we have successfully stabilized Zn anodes by building a thin and hydrophilic artificial solid electrolyte interphase (SEI) layer via a simple dip-coating method. The artificial SEI layer effectively inhibits the parasitic side reactions and guarantees uniform Zn stripping/plating for dendrite-free Zn anodes. As a result, durable cycle stability (3000 cycles at 1 A g −1 ) is achieved. More importantly, the artificial SEI layer is easily adapted for enlarged Zn anodes (176 cm 2 ) and highly stable cell operation is observed. This strategy can provide a more practical path and significant advances for developing aqueous ZIBs for large-scale ESSs.
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