Abstract
Organic electrodes are promising as next generation energy storage materials originating from their enormous chemical diversity and electrochemical specificity. Although organic synthesis methods have been extended to a broad range, facile and selective methods are still needed to expose the corners of chemical space. Herein, we report the organopolysulfide, 1,4-bis(diphenylphosphanyl)tetrasulfide, which is synthesized by electrochemical oxidation of diphenyl dithiophosphinic acid featuring the cleavage of a P–S single bond and a sulfur radical addition reaction. Density functional theory proves that the external electric field triggers the intramolecular rearrangement of diphenyl dithiophosphinic acid through dehydrogenation and sulfur migration along the P–S bond axis. Impressively, the Li/bis(diphenylphosphanyl)tetrasulfide cell exhibits the high discharge voltage of 2.9 V and stable cycling performance of 500 cycles with the capacity retention of 74.8%. Detailed characterizations confirm the reversible lithiation/delithiation process. This work demonstrates that electrochemical synthesis offers the approach for the preparation of advanced functional materials.
Highlights
Organic electrodes are promising as generation energy storage materials originating from their enormous chemical diversity and electrochemical specificity
The pentacoordinate phosphide of DPDTP was firstly dissolved in an undivided cell with lithium bis(trifluoromethanesulfonyl) imide (LiTFSI) and lithium nitrate (LiNO3) in the mixture of 1,3-dioxolane (DOL) and 1,2-dimethoxyethane (DME) as the electrolyte
We report the account of utilizing electrochemical oxidation to synthesize a organopolysulfide containing phosphorus heteroatoms that can be a promising cathode material for rechargeable lithium batteries
Summary
Organic electrodes are promising as generation energy storage materials originating from their enormous chemical diversity and electrochemical specificity. Radicals, and organosulfides possess redox-active sites and unique electrochemical properties, affording the potential for next-generation rechargeable lithium batteries[5,6,7,8,9]. The introduction of electronwithdrawing functional groups into the organic structures can generally increase the working voltage of the battery[16,17,18], organic structures containing multiple redox active sites can have high theoretical specific capacities[19,20]. Few organic thiophosphates containing redox-active sites such as P–S, S–S, and -Sn- (n > 2) are available Their electrochemical behavior in lithium batteries is still unknown. Researchers have extended traditional organic synthesis methods to a broad range, novel organosulfides compounds, and highly selective methods are still needed to expose the new corners of chemical space[34,35]
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