Development of long lifespan high-energy aqueous organic||iodine rechargeable batteries

Abstract

Rechargeable aqueous metal||I2 electrochemical energy storage systems are a cost-effective alternative to conventional transition-metal-based batteries for grid energy storage. However, the growth of unfavorable metallic deposition and the irreversible formation of electrochemically inactive by-products at the negative electrode during cycling hinder their development. To circumvent these drawbacks, herein we propose 3,4,9,10-perylenetetracarboxylic diimide (PTCDI) as negative electrode active material and a saturated mixed KCl/I2 aqueous electrolyte solution. The use of these components allows for exploiting two sequential reversible electrochemical reactions in a single cell. Indeed, when they are tested in combination with an active carbon-enveloped I2 electrode in a glass cell configuration, we report an initial specific discharge capacity of 900 mAh g−1 (electrode mass of iodine only) and an average cell discharge voltage of 1.25 V at 40 A g−1 and 25$$\pm$$ ± 1 °C. Finally, we also report the assembly and testing of a PTCDI|KCl-I2|carbon paper multilayer pouch cell prototype with a discharge capacity retention of about 70% after 900 cycles at 80 mA and 25$$\pm$$ ± 1 °C.

Recent Development of Aqueous Multivalent‐Ion Batteries Based on Conversion Chemistry

“…Since ICl interhalogen displays the lowest dissociation energy, chloride ion‐containing electrolyte is considered as an ideal candidate to accelerate the I 0 /I + redox reaction. [ 84 ]…”

“…Since ICl interhalogen displays the lowest dissociation energy, chloride ion-containing electrolyte is considered as an ideal candidate to accelerate the I 0 /I + redox reaction. [84] Halogen ions (e.g., Cl − ) can be intercalated into nitrogendoped few-layered graphene by double-layer adsorption and ion insertion through a diffusion-controlled process. [85] More Interestingly, the interhalogens can also be intercalated into the layered materials, thus providing extra capacity at high voltage.…”

Perylenetetracarboxylic Diimide Composite Electrodes as Organic Cathode Materials for Rechargeable Sodium-Ion Batteries: A Joint Experimental and Theoretical Study

“…10 Organic molecules with carbonyl groups as their reactive moiety belong to this material class and have demonstrated great potential. 11,12 The charge storage is facilitated via an ion-coordination mechanism of the Na ion to the negatively charged oxygen atom of the electrochemically reduced carbonyl group and its reversible dissociation during the reverse oxidation, demonstrated for anthraquinone and its derivatives. 13,14 While most of these "carbonyl compounds" have fast Na-insertion kinetics and high capacities, they suffer from low electronic conductivity, high solubility in the electrolyte, and low potentials as cathodes.…”

“…Small organic semiconducting molecules, as the core element for low-cost and energy-efficient “green” electrodes, are a promising material class for such SIBs . Organic molecules with carbonyl groups as their reactive moiety belong to this material class and have demonstrated great potential. , The charge storage is facilitated via an ion-coordination mechanism of the Na ion to the negatively charged oxygen atom of the electrochemically reduced carbonyl group and its reversible dissociation during the reverse oxidation, demonstrated for anthraquinone and its derivatives. , While most of these “carbonyl compounds” have fast Na-insertion kinetics and high capacities, they suffer from low electronic conductivity, high solubility in the electrolyte, and low potentials as cathodes. A strategy to tackle these disadvantages is to modify the underlying framework of the molecule to tune properties like redox potential or solubility. , In 2015, Deng et al investigated the parent perylene diimide molecule, 3,4,9,10-perylenetetracarboxylic diimide (H 2 PTCDI), which has a hydrogen residual on the nitrogen atom of the imide moiety, as cathode material for SIBs.…”

Chaotropic Electrolyte Enabling Wide-Temperature Metal-Free Battery

“…). − However, limited resources, uncontrollable dendrite growth, and limitations of using a metal anode in an aqueous electrolyte have restricted their further development . Aqueous batteries based on nonmetallic charge carriers present a bright prospect in grid-scale energy storage due to the advantages of resource abundance, cost effectiveness, and fast kinetics. − Among them, the polyatomic NH 4 + charge carriers with a hydrated ionic radius (3.31 Å) and tetrahedral orientation structure exhibit small desolvation energy barriers, rapid diffusion kinetics, and distinct topotactic binding chemistry for available energy storage. − Furthermore, NH 4 + -containing electrolytes show weak corrosiveness and acidity, which can efficiently suppress the hydrogen evolution reaction (HER) and electrode material deterioration …”