High-rate lithium (Li) ion batteries that can be charged in minutes and store enough energy for a 350-mile driving range are highly desired for all-electric vehicles. A high charging rate usually leads to sacrifices in capacity and cycling stability. We report use of black phosphorus (BP) as the active anode for high-rate, high-capacity Li storage. The formation of covalent bonds with graphitic carbon restrains edge reconstruction in layered BP particles to ensure open edges for fast Li+ entry; the coating of the covalently bonded BP-graphite particles with electrolyte-swollen polyaniline yields a stable solid–electrolyte interphase and inhibits the continuous growth of poorly conducting Li fluorides and carbonates to ensure efficient Li+ transport. The resultant composite anode demonstrates an excellent combination of capacity, rate, and cycling endurance.
Lithium metal batteries (LMB) are vital devices for high-energy-density energy storage, but Li metal anode is highly reactive with electrolyte and forms uncontrolled dendrite that can cause undesirable parasitic reactions thus poor cycling stability and raise safety concerns. Despite remarkable progress made to partly solve these issues, the Li metal still plate at the electrode/electrolyte interface where the parasitic reactions and dendrite formation invariably occur. Here we demonstrate the inwardgrowth plating of Li into a metal foil while avoiding surface deposition, which is driven by the reversible solid-solution based alloy phase change. Lithiation of the solid solution alloy phase facilitates the freshly generated Li atoms at the surface to sink into the foil, while the reversible alloy phase change is companied by the dealloying reaction during delithiation, which extracts Li atoms from inside of the foil. The yielded dendrite free Li anode produces an enhanced Coulombic efficiency of 99.5 0.2% with a reversible capacity of 1660 mA h g -1 (3.3 mA h cm -2 ).
Few-layer black phosphorus (BP) with an anisotropic two-dimensional (2D)-layered structure shows potential applications in photoelectric conversion and photocatalysis, but is easily oxidized under ambient condition preferentially at its edge sites. Improving the ambient stability of BP nanosheets has been fulfilled by chemical functionalization, however this functionalization is typically non-selective. Here we show that edge-selective functionalization of BP nanosheets by covalently bonding stable C60 molecules leads to its significant stability improvement. Owing to the high stability of the hydrophobic C60 molecule, C60 functions as a sacrificial shield and effectively protects BP nanosheets from oxidation under ambient condition. C60 bonding leads to a rapid photoinduced electron transfer from BP to C60, affording enhanced photoelectrochemical and photocatalytic activities. The selective passivation of the reactive edge sites of BP nanosheets by sacrificial C60 molecules paves the way toward ambient processing and applications of BP.
The rechargeable aluminum-sulfur (Al-S) battery is a promising next generation electrochemical energy storage system owing to its high theoretical capacity of 1672 mAh g −1 and in combining low-cost and naturally abundant elements, Al and S. However, to date, its poor reversibility and low lifespan have limited its practical application. In this paper, a composite cathode is reported for Al-S batteries based on S anchored on a carbonized HKUST-1 matrix (S@HKUST-1-C). The S@HKUST-1-C composite maintains a reversible capacity of 600 mAh g −1 at the 75th cycle and a reversible capacity of 460 mAh g −1 at the 500th cycle under a current density of 1 A g −1 , with a Coulombic efficiency of around 95%. X-ray diffraction and Auger spectrum results reveal that the Cu in HKUST-1 forms S-Cu ionic clusters. This serves to facilitate the electrochemical reaction and improve the reversibility of S during charge/discharge. Additionally, Cu increases the electron conductivity at the carbon matrix/S interface to significantly decrease the kinetic barrier for the conversion of sulfur species during battery operation.
There has been a renewed interest in using lithium (Li) metal as an anode material for rechargeable batteries owing to its high theoretical capacity of 3860 mA h g . Despite extensive research, modifications to effectively inhibit Li dendrite growth still result in decreased Li loading and Li utilization. As a result, real capacities are often lower than values expected, if the total mass of the electrode is taken into consideration. Herein, a lightweight yet mechanically robust carbon nanotube (CNT) paper is demonstrated as a freestanding framework to accommodate Li metal with a Li mass fraction of 80.7 wt%. The highly conductive network made of sp2-hybridized carbon effectively inhibits formation of Li dendrites and affords a favorable coulombic efficiency of >97.5%. Moreover, the Li/CNT electrode retains practical areal and gravimetric capacities of 10 mA h cm and 2830 mA h g (vs the mass of electrode), respectively, with 90.9% Li utilization for 1000 cycles at a current density of 10 mA cm . It is demonstrated that the robust and expandable nature is a distinguishing feature of the CNT paper as compared to other 3D scaffolds, and is a key factor that leads to the improved electrochemical performance of the Li/CNT anodes.
Black phosphorus (BP) is a desirable anode material for alkali metal ion storage owing to its high electronic/ionic conductivity and theoretical capacity. In‐depth understanding of the redox reactions between BP and the alkali metal ions is key to reveal the potential and limitations of BP, and thus to guide the design of BP‐based composites for high‐performance alkali metal ion batteries. Comparative studies of the electrochemical reactions of Li+, Na+, and K+ with BP were performed. Ex situ X‐ray absorption near‐edge spectroscopy combined with theoretical calculation reveal the lowest utilization of BP for K+ storage than for Na+ and Li+, which is ascribed to the highest formation energy and the lowest ion diffusion coefficient of the final potassiation product K3P, compared with Li3P and Na3P. As a result, restricting the formation of K3P by limiting the discharge voltage achieves a gravimetric capacity of 1300 mAh g−1 which retains at 600 mAh g−1 after 50 cycles at 0.25 A g−1.
Lithium-sulfur batteries are widely seen as a promising next-generation energy-storage system owing to their ultrahigh energy density. Although extensive research efforts have tackled poor cycling performance and self-discharge, battery stability has been improved at the expense of energy density. We have developed an interlayer consisting of two-layer chemical vapor deposition (CVD)-grown graphene supported by a conventional polypropylene (PP) separator. Unlike interlayers made of discrete nano-/microstructures that increase the thickness and weight of the separator, the CVD-graphene is an intact film with an area of 5 × 60 cm and has a thickness of ∼0.6 nm and areal density of ∼0.15 μg cm, which are negligible to those of the PP separator. The CVD-graphene on PP separator is the thinnest and lightest interlayer to date and is able to suppress the shuttling of polysulfides and enhance the utilization of sulfur, leading to concurrently improved specific capacity, rate capability, and cycle stability and suppressed self-discharge when assembled with cathodes consisting of different sulfur/carbon composites and electrolytes either with or without LiNO additive.
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