Organic Thiocarboxylate Electrodes for a Room‐Temperature Sodium‐Ion Battery Delivering an Ultrahigh Capacity

Abstract

Organic room-temperature sodium-ion battery electrodes with carboxylate and carbonyl groups have been widely studied. Herein, for the first time, we report a family of sodium-ion battery electrodes obtained by replacing stepwise the oxygen atoms with sulfur atoms in the carboxylate groups of sodium terephthalate which improves electron delocalization, electrical conductivity and sodium uptake capacity. The versatile strategy based on molecular engineering greatly enhances the specific capacity of organic electrodes with the same carbon scaffold. By introducing two sulfur atoms to a single carboxylate scaffold, the molecular solid reaches a reversible capacity of 466 mAh g at a current density of 50 mA g . When four sulfur atoms are introduced, the capacity increases to 567 mAh g at a current density of 50 mA g , which is the highest capacity value reported for organic sodium-ion battery anodes until now.

Electrochromic Poly(chalcogenoviologen)s as Anode Materials for High‐Performance Organic Radical Lithium‐Ion Batteries

“…[7] Theexcellent redox properties and unique radical states of viologens make them exceptional electrode candidates for an ew generation of energy-storage devices,s uch as inorganic/organic Li/Na/ Mg ion batteries, [8] aqueous organic redox flow batteries, [9] organic radical batteries, [10] lithium-oxygen batteries, [11] and others. [18] Furthermore, we synthesizedas eries of novelc halcogenoviologens by introducing different chalcogen atoms( S, Se,a nd Te ). [16] Reported ORBs suffered from poor performance,f or example,l ow cell capacity and stability, owing to fewer redox states and low specific energy.T herefore,t he development of novel viologen derivatives with multiple stable redox centers and higher specific energy could dramatically enhance the performance and expand the limits of ORBs.…”

“…[8c] Thei ntroduction of chalcogen atoms into organic conjugated scaffolds could enhance the electron mobility of the compounds in terms of greater mass and polarizability. [18] Furthermore, we synthesizedas eries of novelc halcogenoviologens by introducing different chalcogen atoms( S, Se,a nd Te ). The development of novel chalcogenides with low toxicity,l ow chalcogen content, and high energy density through the modification of functional groups is necessary to balance the problems of toxicity and shortage.R ecently,o ur group developed thiocarboxylate compounds for organic sodiumion battery electrodes and observed high capacity and stability when four sulfur atoms were introduced, which demonstrated theb enefit of the atom-substitutiona pproach foro rganic batteries.…”

“…[17] However,t he inherent toxicity and shortage of heavychalcogenide resources may limit their application. [18] Furthermore, we synthesizedas eries of novelc halcogenoviologens by introducing different chalcogen atoms( S, Se,a nd Te ). [18] Furthermore, we synthesizedas eries of novelc halcogenoviologens by introducing different chalcogen atoms( S, Se,a nd Te ).…”

Organic Carbonyl Compounds for Sodium‐Ion Batteries: Recent Progress and Future Perspectives

“…[17b] These resultsc an be attributed to the reasonst hat the extension of the p-conjugated system not only improves the charge transport and stabilizes the charged/discharged states, but also enhances the intermolecular interactions and facilitates the insertion/extraction of the Na ions. [18] Interestingly,t he substitution of oxygen in the carboxylate group by sulfur can also improve electron delocalization and sodium uptake capacity.T herefore, al arger capacity of 567 mAh g À1 can be obtained when four sulfur atoms are introduced (8). [18] Interestingly,t he substitution of oxygen in the carboxylate group by sulfur can also improve electron delocalization and sodium uptake capacity.T herefore, al arger capacity of 567 mAh g À1 can be obtained when four sulfur atoms are introduced (8).…”

Accurate Control Multiple Active Sites of Carbonaceous Anode for High Performance Sodium Storage: Insights into Capacitive Contribution Mechanism

“…Hence, the attentions are gradually diverted to heteroatom doping owing to multiple heteroatom can effectively regulate the physicochemical properties of carbonaceous anodes, including electronegativity, electronic conductivity, and hydrophilicity . Nitrogen is the most commonly investigated heteroatom owing to their significant improvement of conductivity and surface wettability between electrode interface and electrolyte, while sulfur doping especially in amorphous carbon prominently enhances sodium storage capacity due to its considerable faraday behavior . Additionally, sulfur doping can also slightly expand the interlayer distances, which is of great assistance for sodium insertion behavior .…”