Cascade Defluorination of Perfluoroalkylated Catholytes Unlocks High Lithium Primary Battery Capacities

نویسندگان

چکیده

Exceeding the energy density of lithium−carbon monofluoride (Li−CFx), today's leading Li primary battery, requires an increase in fluorine content (x) that determines theoretical capacity available from C−F bond reduction. However, high F-content carbon materials face challenges such as poor electronic conductivity, low reduction potentials (<1.3 V versus Li/Li+), and/or utilization. This study investigates molecular structural design principles for a new class fluoroalkyl-aromatic catholytes address these challenges. A polarizable conjugated system—an aromatic ring with alkene linker—functions electron acceptor and redox initiator, enabling cascade defluorination adjacent perfluoroalkyl chain (RF = −CnF2n+1). The synthesized molecules successfully overcome premature deactivation observed previously studied achieve close-to-full (up to 15/17 F), yielding gravimetric capacities 748 mAh g−1fluoroalkyl-aromatic energies 1785 Wh kg−1fluoroalkyl-aromatic. voltage compatibility between fluoroalkyl-aromatics CFx enables hybrid cells containing activity both solid liquid phases, projected enhancement Li–CFx by 35% based on weight electrodes+electrolyte. With further improvement cathode architecture, “liquid CFx” analogues are strong candidates exceeding limitations chemistries.

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ژورنال

عنوان ژورنال: Advanced Energy Materials

سال: 2023

ISSN: ['1614-6832', '1614-6840']

DOI: https://doi.org/10.1002/aenm.202301751