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1.
Nanoscale ; 16(16): 7937-7950, 2024 Apr 25.
Artigo em Inglês | MEDLINE | ID: mdl-38545684

RESUMO

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.

2.
ACS Appl Mater Interfaces ; 16(5): 5847-5856, 2024 Feb 07.
Artigo em Inglês | MEDLINE | ID: mdl-38284621

RESUMO

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.

4.
J Colloid Interface Sci ; 640: 1080-1088, 2023 Jun 15.
Artigo em Inglês | MEDLINE | ID: mdl-36931011

RESUMO

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.

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