Mg batteries have the advantages of resource abundance, high volumetric energy density, and dendrite-free plating/stripping of Mg anodes. However the injection of highly polar Mg cannot maintain the structural integrity of intercalation-type cathodes even for open framework prototypes. The lack of high-voltage electrolytes and sluggish Mg diffusion in lattices or through interfaces also limit the energy density of Mg batteries. Mg-S system based on moderate-voltage conversion electrochemistry appears to be a promising solution to high-energy Mg batteries. However, it still suffers from poor capacity and cycling performances so far. Here, a ZIF-67 derivative carbon framework codoped by N and Co atoms is proposed as effective S host for highly reversible Mg-S batteries even under high rates. The discharge capacity is as high as ≈600 mA h g at 1 C during the first cycle, and it is still preserved at ≈400 mA h g after at least 200 cycles. Under a much higher rate of 5 C, a capacity of 300-400 mA h g is still achievable. Such a superior performance is unprecedented among Mg-S systems and benefits from multiple factors, including heterogeneous doping, Li-salt and Cl addition, charge mode, and cut-off capacity, as well as separator decoration, which enable the mitigation of electrode passivation and polysulfide loss.
Water electrolysis is a sustainable technology for hydrogen production since this process can utilize the intermittent electricity generated by renewable energy such as solar, wind, and hydro. However, the large‐scale application of this process is restricted by the high electricity consumption due to the large potential gap (>1.23 V) between the anodic oxygen evolution reaction and the cathodic hydrogen evolution reaction (HER). Herein, a novel and efficient hydrogen production system is developed for coupling glucose‐assisted Cu(I)/Cu(II) redox with HER. The onset potential of the electrooxidation of Cu(I) to Cu(II) is as low as 0.7 VRHE (vs reversible hydrogen electrode). In situ Raman spectroscopy, ex situ X‐ray photoelectron spectroscopy, and density functional theory calculation demonstrates that glucose in the electrolyte can reduce the Cu(II) into Cu(I) instantaneously via a thermocatalysis process, thus completing the cycle of Cu(I)/Cu(II) redox. The assembled electrolyzer only requires a voltage input of 0.92 V to achieve a current density of 100 mA cm−2. Consequently, the electricity consumption for per cubic H2 produced in the system is 2.2 kWh, only half of the value for conventional water electrolysis (4.5 kWh). This work provides a promising strategy for the low‐cost, efficient production of high‐purity H2.
A magnesium battery is a promising candidate for large-scale transportation and stationary energy storage due to the security, low cost, abundance, and high volumetric energy density of a Mg anode. But there are still some obstacles retarding the wide application of Mg batteries, including poor kinetics of Mg-ion transport in lattices and low theoretical capacity in inorganic frameworks. A Mg-Li dual-salt electrolyte enables kinetic activation by dominant intercalation of Li-ions instead of Mg-ions in cathode lattices without the compromise of a stable Mg anode process. Here we propose a Mg-organic battery based on a renewable rhodizonate salt ( e. g., NaCO) activated by a Mg-Li dual-salt electrolyte. The nanostructured organic system can achieve a high reversible capacity of 350-400 mAh/g due to the existence of high-density carbonyl groups (C═O) as redox sites. Nanocrystalline NaCO wired by reduced graphene oxide enables a high-rate performance of 200 and 175 mAh/g at 2.5 (5 C) and 5 A/g (10 C), respectively, which also benefits from a high intrinsic diffusion coefficient (10-10 cm/s) and pesudocapacitance contribution (>60%) of NaCO for Li-Mg co-intercalation. The suppressed exfoliation of CO layers by a firmer non-Li pinning via Na-O-C or Mg-O-C and a dendrite-resistive Mg anode lead to a long-term cycling for at least 600 cycles. Such an extraordinary capacity/rate performance endows the Mg-NaCO system with high energy and power densities up to 525 Wh/kg and 4490 W/kg (based on active cathode material), respectively, exceeding the level of high-voltage insertion cathodes with typical inorganic structures.
Large-capacity conversion electrodes are highly required to raise the energy density of batteries. However, their undesired phase segregation and volume expansion during cycling lead to the motivation for nanofabrication and nanochemistry of active species in order to decrease "dead mass" and promote better construction of conductive networks. However, the inactivity of the conductive skeleton and loose nanostructure would compromise the energy density of the electrode. The integration of large-sized (high-density) grains into an electroactive conductive network in a compact way is still a big challenge. Here we report a proof-of-concept prototype consisting of unusual MoS solid bubbles of hundreds of nanometers in size, which are conformally encapsulated by thin-layer carbon. The seamless welding between this carbon coating and the surrounding broader carbon substrate can effectively avoid the peel-off of active species and breakage of the conductive network. This MoS-C composite is achieved by simultaneous self-sulfuration and self-carbonization of a polyoxometalate (POM)-based chelate, and its Li-storage performance is superior to most MoS-based anodes even with ultrathin 2D nanosheets. Partially benefiting from the electroactivity of a dithiooxamide (DTO)-derivate carbon network, the reversible capacity of MoS-C by pyrolyzing the POM-DTO chelate can reach 1500-2000 mAh/g at 0.5-1 A/g even after 700 cycles and be maintained around 1000 mAh/g under as high as 10-20 A/g.
Lithium metal batteries (LMBs) containing S, O, and fluoride cathodes are attracting increasing attention owing to their much higher energy density than that of Li-ion batteries. However, current limitation for the progress of LMBs mainly comes from the uncontrolled formation and growth of Li dendrites at the anode side. In order to suppress dendrite growth, exploring novel nanostructured electrolyte of high modulus without degradation of Li-electrolyte interface appears to be a potential solution. Here we propose a lightweight polymer-reinforced electrolyte based on graphitic carbon nitride (g-CN) mesoporous microspheres as electrolyte filler [bis(trifluoromethanesulfonimide) lithium salt/di(ethylene glycol) dimethyl ether mixed with g-CN, denoted as LiTFSI-DGM-CN] for the first time. This nanostructured electrolyte can effectively suppress lithium dendrite growth during cycling, benefiting from the high mechanical strength and nanosheet-built hierarchical structure of g-CN. The Li/Li symmetrical cell based on this slurrylike electrolyte enables long-term cycling of at least 120 cycles with a high capacity of 6 mA·h/cm and small plating/stripping overpotential of ∼100 mV at a high current density of 2 mA/cm. g-CN filling also enables a separator(Celgard)-free Li/FeS cell with at least 400 cycles. The 3D geometry of g-CN shows advantages on interfacial resistance and Li plating/stripping stability compared to its 2D geometry.
Li dendrite suppression enables a highly reversible Li-metal battery. However the strategy to smooth Li surface, especially under long-term cycling and high current density, is still a big challenge. Here, we propose a facile additive strategy to reinforce Li dendrite inhibition in a range of ether and carbonate electrolytes. Dissoluble Mg(TFSI) is employed as a degradable electrolyte additive, leading to in situ plating of porous Mg network when contacting reductive Li atoms. Mg adatoms with extremely low diffusion energy barrier as lithiophilic sites enable a smooth or flaky morphology of Li surface even under a high current density of 2 mA/cm and high capacity of 6 mAh/cm. Mg-salt additive significantly extends the cycling life of Li||Cu asymmetric cells up to 240 and 200 cycles for carbonate and ether electrolytes, respectively. Under a current density as high as 5 mA/cm, the Li||Cu cell based on ether system can still survive up to 140 cycles with a small voltage hysteresis close to 60 mV. The hysteresis can be reduced to below 25 mV for lasting 200 cycles at 1 mA/cm. This additive strategy provides a facile solution to in situ construction of conductive anode-electrolyte interface with low interface resistance for alleviating uneven Li nucleation.
As a green and eco-friendly technology, triboelectric nanogenerator (TENG) can harvest energy from human motion to generate electricity, so TENGs have been widely applied in wearable electronic devices to replace traditional batteries. However, the surface of these TENGs is easily contaminated and breeds bacteria, which is a threat to human health. Here, we report an antibacterial composite film-based triboelectric nanogenerator (ACF-TENG) that uses Ag-exchanged zeolite (Ag-zeolite) and polypropylene (PP) composite film as the triboelectric layer. Adding a small amount of Ag-zeolite with excellent antibacterial properties can increase the dielectric permittivity and improve the surface charge density of composite films, which enhances the output performance of the ACF-TENG. The open-circuit voltage (V), short-circuit current (I), and transferred charge (Q) of the ACF-TENG are about 193.3, 225.4, and 233.3% of those of a pure PP film-based TENG, respectively. Because of the silver in the Ag-zeolite, the ACF-TENG can effectively kill Escherichia coli and fungi. When used in insoles, the ACF-TENG can resist the athlete's foot fungus effectively and work as a power source to light up light-emitting diodes and charge capacitors. The ACF-TENG has wide application prospects in self-powered medical and healthcare electronics.
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