Publications by authors named "Devaraj Shanmukaraj"

The effective flow of electrons through bulk electrodes is crucial for achieving high-performance batteries, although the poor conductivity of homocyclic sulfur molecules results in high barriers against the passage of electrons through electrode structures. This phenomenon causes incomplete reactions and the formation of metastable products. To enhance the performance of the electrode, it is important to place substitutable electrification units to accelerate the cleavage of sulfur molecules and increase the selectivity of stable products during charging and discharging.

View Article and Find Full Text PDF

Li metal secondary batteries known for their high energy and power density are the much-awaited energy storage systems owing to the high specific capacity of Li metal. However, due to the instability of Li metal with common Li-ion battery electrolytes, a combination with a polymer electrolyte seems to be an effective strategy to alleviate the safety issues of employing Li metal and provide design conformity to the system. Current trends show improvements in different aspects, such as improving ionic conductivity, single-ion conductivity, mechanical stability, and electrochemical stability.

View Article and Find Full Text PDF

Recycling lithium from spent batteries is challenging because of problems with poor purity and contamination. Here, we propose a green and sustainable lithium recovery strategy for spent batteries containing LiFePO, LiCoO, and LiNiCoMnO electrodes. Our proposed configuration of "lithium-rich electrode || LLZTO@LiTFSI+P3HT || LiOH" system achieves double-side and roll-to-roll recycling of lithium-containing electrode without destroying its integrity.

View Article and Find Full Text PDF

The current Li-based battery technology is limited in terms of energy contents. Therefore, several approaches are considered to improve the energy density of these energy storage devices. Here, we report the combination of a heteroatom-based gel polymer electrolyte with a hybrid cathode comprising of a Li-rich oxide active material and graphite conductive agent to produce a high-energy "shuttle-relay" Li metal battery, where additional capacity is generated from the electrolyte's anion shuttling at high voltages.

View Article and Find Full Text PDF

The abundance of the available sodium sources has led to rapid progress in sodium-ion batteries (SIBs), making them potential candidates for immediate replacement of lithium-ion batteries (LIBs). However, commercialization of SIBs has been hampered by their fading efficiency due to the sodium consumed in the formation of solid-electrolyte interphase (SEI) when using hard carbon (HC) anodes. Herein, NaCO sodium salt is introduced as a highly efficient, cost-effective, and safe cathode sodiation additive.

View Article and Find Full Text PDF

The practical applications of lithium metal anodes in high-energy-density lithium metal batteries have been hindered by their formation and growth of lithium dendrites. Herein, we discover that certain protein could efficiently prevent and eliminate the growth of wispy lithium dendrites, leading to long cycle life and high Coulombic efficiency of lithium metal anodes. We contend that the protein molecules function as a "self-defense" agent, mitigating the formation of lithium embryos, thus mimicking natural, pathological immunization mechanisms.

View Article and Find Full Text PDF

Rechargeable sodium batteries are a promising technology for low-cost energy storage. However, the undesirable drawbacks originating from the use of glass fiber membrane separators have long been overlooked. A versatile grafting-filtering strategy was developed to controllably tune commercial polyolefin separators for sodium batteries.

View Article and Find Full Text PDF

All-organic batteries are a promising sustainable energy storage technology owing to the wide availability, flexibility, and recyclability of organic/polymeric compounds. The development of all-organic or polymer batteries is still a challenge, as both electrode materials need to be carefully optimized to have a wide difference of redox potential and compatibility with the electrolyte. Herein, dual redox-active polyimides based on phenothiazine and naphthalene tetracarboxylic dianhydride units are presented.

View Article and Find Full Text PDF

The low Coulombic efficiency and serious safety issues resulting from uncontrollable dendrite growth have severely impeded the practical applications of lithium (Li) metal anodes. Herein we report a stable quasi-solid-state Li metal battery by employing a hierarchical multifunctional polymer electrolyte (HMPE). This hybrid electrolyte was fabricated via in situ copolymerizing lithium 1-[3-(methacryloyloxy)propylsulfonyl]-1-(trifluoromethanesulfonyl)imide (LiMTFSI) and pentaerythritol tetraacrylate (PETEA) monomers in traditional liquid electrolyte, which is absorbed in a poly(3,3-dimethylacrylic acid lithium) (PDAALi)-coated glass fiber membrane.

View Article and Find Full Text PDF

Due to the high theoretical specific energy, the lithium-oxygen battery has been heralded as a promising energy storage system for applications such as electric vehicles. However, its large over-potentials during discharge-charge cycling lead to the formation of side-products, and short cycle life. Herein, we report an ionic liquid bearing the redox active 2,2,6,6-tetramethyl-1-piperidinyloxy moiety, which serves multiple functions as redox mediator, oxygen shuttle, lithium anode protector, as well as electrolyte solvent.

View Article and Find Full Text PDF

Cation-deficient two-dimensional (2D) materials, especially atomically thin nanosheets, are highly promising electrode materials for electrochemical energy storage that undergo metal ion insertion reactions, yet they have rarely been achieved thus far. Here, we report a Ti-deficient 2D unilamellar lepidocrocite-type titanium oxide (TiO) nanosheet superlattice for sodium storage. The superlattice composed of alternately restacked defective TiO and nitrogen-doped graphene monolayers exhibits an outstanding capacity of ∼490 mA h g at 0.

View Article and Find Full Text PDF

High-temperature sodium-sulfur batteries operating at 300-350 °C have been commercially applied for large-scale energy storage and conversion. However, the safety concerns greatly inhibit their widespread adoption. Herein, we report a room-temperature sodium-sulfur battery with high electrochemical performances and enhanced safety by employing a "cocktail optimized" electrolyte system, containing propylene carbonate and fluoroethylene carbonate as co-solvents, highly concentrated sodium salt, and indium triiodide as an additive.

View Article and Find Full Text PDF

The development of sodium-ion batteries has been hindered so far by the large irreversible capacity of hard carbon anodes and other anode materials in the initial few cycles, as sodium ions coming from cathode materials is consumed in the formation of the solid-electrolyte interface (SEI) and irreversibly trapped in anodes. Herein, the successful synthesis of an environmentally benign and cost-effective sodium salt (Na C O ) is reported that could be applied as additive in cathodes to solve the irreversible-capacity issues of anodes in sodium-ion batteries. When added to Na (VO) (PO ) F cathode, the cathode delivered a highly stable capacity of 135 mAh g and stable cycling performance.

View Article and Find Full Text PDF

Ambient-temperature sodium-sulfur (Na-S) batteries are considered a promising energy storage system due to their high theoretical energy density and low costs. However, great challenges remain in achieving a high rechargeable capacity and long cycle life. Herein we report a stable quasi-solid-state Na-S battery enabled by a poly(S-pentaerythritol tetraacrylate (PETEA))-based cathode and a (PETEA-tris[2-(acryloyloxy)ethyl] isocyanurate (THEICTA))-based gel polymer electrolyte.

View Article and Find Full Text PDF

Two new cathode materials based on redox organosulfur polymers were synthesized and investigated for rechargeable lithium batteries as a proof-of-concept study. These cathodes offered good cycling performance owing to the absence of polysulfide solubility, which plagues Li/S systems. Herein, an aliphatic polyamine or a conjugated polyazomethine was used as the base to tether the redox-active species.

View Article and Find Full Text PDF

The development of new redox polymers is being boosted by the increasing interest in the area of energy and health. The development of new polymers is needed to further advance new applications or improve the performance of actual devices such as batteries, supercapacitors, or drug delivery systems. Here we show the synthesis and characterization of a new polymer which combines the present most successful conjugated polymer backbone and the most successful redox active side group, i.

View Article and Find Full Text PDF

Organic carbonate mixtures are used almost exclusively as lithium battery electrolyte solvents. The linear compounds (dimethyl carbonate, diethyl carbonate, ethyl methyl carbonate) act mainly as thinner for the more viscous and high-melting ethylene carbonate but are the least stable component and have low flash points; these are serious handicaps for lifetime and safety. Polyethers (glymes) are useful co-solvents, but all formerly known representatives solvate Li(+) strongly enough to co-intercalate in the graphite negative electrode and exfoliate it.

View Article and Find Full Text PDF

Compounds like LiF, Li(2)O, and Li(2)O(2) have considerable importance in batteries; the first two are ubiquitous in the protective SEI at the negative electrode, or the result of conversion reactions with fluorides and oxides. The latter, Li(2)O(2,) forms from oxygen reduction in the much vaunted Li/air batteries. Mastering their solubility in Li-based electrolytes is viewed as essential for further progress in battery safety, lifetime, or capacity.

View Article and Find Full Text PDF