Molecular Engineered Safer Organic Battery through the Incorporation of Flame Retarding Organophosphonate Moiety.

Here, we report the first electrochemical assessment of organophosphonate-based compound as a safe electrode material for lithium-ion batteries, which highlights the reversible redox activity and inherent flame retarding property. Dinickel 1,4-benzenediphosphonate delivers a high reversible capacity of 585 mA h g-1 with stable cycle performance. It expands the scope of organic batteries, which have been mainly dominated by the organic carbonyl family to date. The redox chemistry is elucidated by X-ray absorption spectroscopy and solid-state 31P NMR investigations. Differential scanning calorimetry profiles of the lithiated electrode material exhibit suppressed heat release, delayed onset temperature, and endothermic behavior in the elevated temperature zone.

Synergistic Effect of Partially Fluorinated Ether and Fluoroethylene Carbonate for High-Voltage Lithium-Ion Batteries with Rapid Chargeability and Dischargeability.

The roles of a partially fluorinated ether (PFE) based on a mixture of 1,1,1,2,2,3,3,4,4-nonafluoro-4-methoxybutane and 2-(difluoro(methoxy)methyl)-1,1,1,2,3,3,3-heptafluoropropane on the oxidative durability of an electrolyte under high-voltage conditions, the rate capability of the graphite and 5 V-class LiNi0.4Mn1.6O4 (LNMO) electrodes, and the cycling performance of graphite/LNMO full cells are examined. Our findings indicate that the use of PFE as a cosolvent in the electrolyte yields thermally stable electrolytes with self-extinguishing ability. Electrochemical tests confirm that the PFE combined with fluoroethylene carbonate (FEC) effectively alleviates the oxidative decomposition of the electrolyte at the high-voltage LNMO cathode and enables reversible electrochemical reactions of the graphite anodes and LNMO cathodes at high rates. Moreover, the combination of PFE, which mitigates electrolyte decomposition at high voltages, and FEC, which stabilizes the anode-electrolyte interface, enables the reversible cycling of high-voltage full cells (graphite/LNMO) with a capacity retention of 70.3% and a high Coulombic efficiency of 99.7% after 100 cycles at 1C rate at 30 °C.

Amphiphilic Graft Copolymers as a Versatile Binder for Various Electrodes of High-Performance Lithium-Ion Batteries.

It is known that grafting one polymer onto another polymer backbone is a powerful strategy capable of combining dual benefits from each parent polymer. Thus amphiphilic graft copolymer precursors (poly(vinylidene difluoride)-graft-poly(tert-butylacrylate) (PVDF-g-PtBA)) have been developed via atom transfer radical polymerization, and demonstrated its outstanding properties as a promising binder for high-performance lithium-ion battery (LIB) by using in situ pyrolytic transformation of PtBA to poly(acrylic acid) segments. In addition to its superior mechanical properties and accommodation capability of volume expansion, the Si anode with PVDF-g-PtBA exhibits the excellent charge and discharge capacities of 2672 and 2958 mAh g(-1) with the capacity retention of 84% after 50 cycles. More meaningfully, the graft copolymer binder shows good operating characteristics in both LiN0.5 M1.5 O4 cathode and neural graphite anode, respectively. By containing such diverse features, a graft copolymer-loaded LiN0.5 M1.5 O4 /Si-NG full cell has been successfully achieved, which delivers energy density as high as 546 Wh kg(-1) with cycle retention of ≈70% after 50 cycles (1 C). For the first time, this work sheds new light on the unique nature of the graft copolymer binders in LIB application, which will provide a practical solution for volume expansion and low efficiency problems, leading to a high-energy-density lithium-ion chemistry.