ABSTRACT
Li-air battery (LAB) technology is making continuous progress toward its theoretical capacity, which is comparable to gasoline. However, the sluggish reaction at the cathode is still a challenge. We propose a simple strategy to optimize the surface eg occupancy by adjusting the stoichiometric ratios of transition metal-based spinel structures through a controlled hydrothermal synthesis. Three distinct stoichiometries of Ni-Co oxides were used to demonstrate the direct correlation between stoichiometry and catalytic performance. The groundsel flower-like structure having a 1 : 1.4 Ni : Co atomic ratio with high surface area, high defect density, and an abundance of Ni3+ at the surface with semi-filled eg orbitals was found to benefit the structure promoting high catalytic activities in aqueous and aprotic media. The assembled LAB cells employing this cathode demonstrate an exceptional lifespan, operating for 3460 hours and completing 173 cycles while achieving the highest discharge capacity of 13 759 mA h g-1 and low charging overpotentials. The key to this prolonged performance lies in the full reversibility of the cell, attributed to its excellent OER performance. A well-surface adsorbed, amorphous LiO2/Li2O2 discharge product is found to possess high diffusivity and ease of decomposition, contributing significantly to the enhanced longevity of the cell.
ABSTRACT
The rational design of cost-effective and efficient electrocatalysts for electrochemical water splitting is essential for green hydrogen production. Utilizing nanocatalysts with abundant active sites, high surface area, and deliberate stacking faults is a promising approach for enhancing catalytic efficiency. In this study, we report a simple strategy to synthesize a highly efficient electrocatalyst for the hydrogen evolution reaction (HER) using carbonized luffa cylindrica as a conductive N-doped carbon skeleton decorated with Ag nanorings that are activated by introducing stacking faults. The introduction of stacking faults and the resulting tensile strain into the Ag nanorings results in a significant decrease in the HER overpotential, enabling the use of Ag as an efficient HER electrocatalyst. Our findings demonstrate that manipulating the crystal properties of electrocatalysts, even for materials with intrinsically poor catalytic activity such as Ag, can result in highly efficient catalysts. Further, applying a conductive carbon backbone can lower the quantities of metal needed without compromising the HER activity. This approach opens up new avenues for designing high-performance electrocatalysts with very low metallic content, which could significantly impact the development of sustainable and cost-effective electrochemical water-splitting systems.
ABSTRACT
Utilising the solid-state synthesis method is an easy and effective way to recycle spent lithium-ion batteries. However, verifying its direct repair effects on completely exhausting cathode materials is necessary. In this work, the optimal conditions for direct repair of completely failed cathode materials by solid-state synthesis are explored. The discharge capacity of spent LiCoO2 cathode material is recovered from 21.7 mAh g-1 to 138.9 mAh g-1 under the optimal regeneration conditions of 850 °C and n(Li)/n(Co) ratio of 1:1. The regenerated materials show excellent electrochemical performance, even greater than the commercial LiCoO2. In addition, based on the whole closed-loop recycling process, the economic and environmental effects of various recycling techniques and raw materials used in the battery production process are assessed, confirming the superior economic and environmental feasibility of direct regeneration method.
ABSTRACT
Nanocomposites with enhanced mechanical properties and efficient self-healing characteristics can change how the artificially engineered materials' life cycle is perceived. Improved adhesion of nanomaterials with the host matrix can drastically improve the structural properties and confer the material with repeatable bonding/debonding capabilities. In this work, exfoliated 2H-WS2 nanosheets are modified using an organic thiol to impart hydrogen bonding sites on the otherwise inert nanosheets by surface functionalization. These modified nanosheets are incorporated within the PVA hydrogel matrix and analyzed for their contribution to the composite's intrinsic self-healing and mechanical strength. The resulting hydrogel forms a highly flexible macrostructure with an impressive enhancement in mechanical properties and a very high autonomous healing efficiency of 89.92%. Interesting changes in the surface properties after functionalization show that such modification is highly suitable for water-based polymeric systems. Probing into the healing mechanism using advanced spectroscopic techniques reveals the formation of a stable cyclic structure on the surface of nanosheets, mainly responsible for the improved healing response. This work opens an avenue toward the development of self-healing nanocomposites where chemically inert nanoparticles participate in the healing network rather than just mechanically reinforcing the matrix by slender adhesion.
