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High-voltage initial anode-free lithium metal batteries (AFLMBs) promise the maximized energy densities of rechargeable lithium batteries. However, the reversibility of the high-voltage cathode and lithium metal anode is unsatisfactory in sustaining their long lifespan. In this research, a concentrated electrolyte comprising dual salts of LiTFSI and LiDFOB dissolved in mixing solvents of dimethyl carbonate (DMC) and fluoroethylene carbonate (FEC) with a LiNO3 additive was formulated to address this challenge. FEC and LiNO3 regulate the anion-rich solvation structure and help form a LiF, Li3N-rich solid electrolyte interphase (SEI) with a high lithium plating/stripping Coulombic efficiency of 98.3%. LiDFOB preferentially decomposes to effectively suppress the side reaction at the high-voltage operation of the Li-rich Li1.2Mn0.54Ni0.13Co0.13O2 cathode. Moreover, the large irreversible capacity during the initial charge/discharge cycle of the cathode provides supplementary lithium sources for cycle life extension. Owing to these merits, the as-fabricated AFLMBs can operate stably for 80 cycles even at an ultrahigh voltage of 4.6 V. This study sheds new insights on the formulation of advanced electrolytes for highly reversible high-voltage cathodes and lithium metal anodes and could facilitate the practical application of AFLMBs. [ABSTRACT FROM AUTHOR]

Small molecule quinone compounds are attractive cathode materials for rechargeable aqueous zinc‐organic batteries (AZOBs) because of their structural diversity and low‐cost merits. Among them, nonpolar quinones are dominant given the relatively low solubilities in aqueous electrolytes. However, their poor electronic conductivity and accumulated Coulombic repulsion lead to underutilized active sites and sluggish redox kinetics. Here, polar 2,6‐dimethoxy‐1,4‐benzoquinone (m‐DMBQ) works as an advanced AZOB cathode with unexpectedly superior performance over the nonpolar isomer of 2,5‐dimethoxy‐1,4‐benzoquinone (p‐DMBQ). The asymmetric charge distribution of active centers in the p−π conjugated backbone of m‐DMBQ induces reduced bandgap with improved electronic conductivity and redox activity, thus achieving a high specific capacity of 312 mAh g−1 approaching the theoretical limit. Additionally, the lowest unoccupied molecular orbital energy level is lowered for an increased average discharge voltage of 0.88 V. Characterizations and computational studies revealed boosted competitiveness of H+ relative to Zn2+ for significantly enhanced charge transfer kinetics and reversibility. As a result, the as‐fabricated AZOB achieves a high energy density of 275 Wh kg−1 based on m‐DMBQ along with high‐rate capability and long‐term cycling stability. This work provides a new molecular engineering strategy through regulating charge distribution symmetry for boosting charge storage in organic cathodes. [ABSTRACT FROM AUTHOR]

A supercapacitor that possesses excellent performance in a wide temperature range is constructed with a partially graphitized porous carbon (PGPC) as the electrode material and tetraethylammonium tetrafluoroborate/propylene carbonate (Et4NBF4/PC) as the electrolyte. The PGPC-based electrode shows a very consistent performance in a wide temperature range of −20 to 50 °C. At working temperatures as high as 50 °C and as low as −20 °C, it delivers specific capacitances of ∼148 and ∼135 F g−1, respectively, and the supercapacitors exhibit high energy densities of ∼46 and ∼43 W h kg−1. In particular, the low-temperature capacitive performance and rate capability of PGPC are much better than those of the normally used activated carbon and among the best ones ever-reported for carbon-based supercapacitors. More significantly, the PGPC-based supercapacitor shows excellent cycling performance at all tested working temperatures, with a capacitance retention of ∼98% after 1000 cycles at 5 A g−1 even when the working temperature decreases to −20 °C. [ABSTRACT FROM AUTHOR]

Magnesium citrate and potassium citrate are two commonly used food additives in our daily life. Herein, we prepared nitrogen-doped hierarchical porous carbon nanosheets (N-HPCNSs) through direct pyrolysis of their mixtures and subsequent NH3 treatment. The as-prepared N-HPCNS shows hierarchical porosity (specific surface area of 1735 m2 g−1 and pore volume of 1.71 cm3 g−1), and a moderate nitrogen doping of 1.7%. Moreover, it can be effectively applied in various energy storage/conversion systems. When used as supercapacitor electrodes, it shows a high specific capacitance of 128 F g−1 in organic electrolytes and retains 45% of the original capacitance even at an ultrahigh current density of 100 A g−1. It can also serve as an effective sulfur carrier in lithium–sulfur batteries. The N-HPCNS/sulfur cathode shows high discharge capacities of 1209 mA h g−1 at 0.2C and 493 mA h g−1 even at 4C. Over 500 charge/discharge cycles at 1C, it still retains a high discharge capacity of 486 mA h g−1 with an ultralow capacity loss of 0.051% per cycle and a high average coulombic efficiency of 99.4%. [ABSTRACT FROM AUTHOR]

Lithium-ion hybrid capacitors (LICs) are regarded as one of the most promising next generation energy storage devices. Commercial activated carbon materials with low cost and excellent cycling stability are widely used as cathode materials for LICs, however, their low energy density remains a significant challenge for the practical applications of LICs. Herein, Na0.76V6O15 nanobelts (NaVO) were prepared and combined with commercial activated carbon YP50D to form hybrid cathode materials. Credit to the synergism of its capacitive effect and diffusion-controlled faradaic effect, NaVO/C hybrid cathode displays both superior cyclability and enhanced capacity. LICs were assembled with the as-prepared NaVO/C hybrid cathode and artificial graphite anode which was pre-lithiated. Furthermore, 10-NaVO/C//AG LIC delivers a high energy density of 118.9 Wh kg−1 at a power density of 220.6 W kg−1 and retains 43.7 Wh kg−1 even at a high power density of 21,793.0 W kg−1. The LIC can also maintain long-term cycling stability with capacitance retention of approximately 70% after 5000 cycles at 1 A g−1. Accordingly, hybrid cathodes composed of commercial activated carbon and a small amount of high energy battery-type materials are expected to be a candidate for low-cost advanced LICs with both high energy density and power density. [ABSTRACT FROM AUTHOR]