Yao Yang

Tuning the Morphology and Crystal Structure of Li2O2: A Graphene Model Electrode Study for Li–O2 Battery

The performance and the cyclability of the Li-O2 batteries are strongly affected by the morphology and crystal structure of Li2O2 produced during discharge. In order to explore the details of growth and electrochemical decomposition of Li2O2, and its relationship with the cell performance, graphene films were used as model carbon electrodes and compared with electrodeposited Pd nanoparticles (NPs) on graphene. Multiple methods, including transmission/scanning electron microscopy (TEM/SEM), Raman spectroscopy, electrochemical impedance spectroscopy (EIS), and coin cell charge/discharge test, were employed for material characterization and reaction monitoring. The results showed that the presence of Pd NPs significantly changed the growth, morphology, and crystal structure of Li2O2 and reduced the charge overpotential by 1060 mV. All of these changes are ascribed to the stronger binding energy between LiO2 and the Pd surface, resulting in the generation of amorphous Li2O2 with higher ionic conductivity of Li(+) and O2(2-), which in turn improve the cell charging performance.

Tuning the Morphology of Li2O2 by Noble and 3d metals: A Planar Model Electrode Study for Li–O2 Battery

In this work, a planar model electrode method has been used to investigate the structure-activity relationship of multiple noble and 3d metal catalysts for the cathode reaction of Li-O2 battery. The result shows that the battery performance (discharge/charge overpotential) strongly depends not only on the type of catalysts but also on the morphology of the discharge product (Li2O2). Specifically, according to electrochemical characterization and scanning electron microscopy (SEM) observation, noble metals (Pd, Pt, Ru, Ir, and Au) show excellent battery performance (smaller discharge/charge overpotential), with wormlike Li2O2 particles with size less than 200 nm on their surfaces. On the other hand, 3d metals (Fe, Co, Ni, and Mn) offered poor battery performance (larger discharge/charge overpotential), with much larger Li2O2 particles (1 μm to a few microns) on their surfaces after discharging. Further research shows that a volcano plot is found by correlating the discharging/charging plateau voltage with the adsorption energy of LiO2 on different metals. The metals with better battery performance and worm-like-shaped Li2O2 are closer to the top of the volcano, indicating adsorption energy of LiO2 is one of the key characters for the catalyst to reach a good performance for the oxygen electrode of Li-O2 battery, and it has a strong influence on the morphology of the discharge product on the electrode surface.

Systematic Optimization of Battery Materials: Key Parameter Optimization for the Scalable Synthesis of Uniform, High-Energy, and High Stability LiNi0.6Mn0.2Co0.2O2 Cathode Material for Lithium-Ion Batteries

Ni-rich LiNixMnyCo1-x-yO2 (x > 0.5) (NMC) materials have attracted a great deal of interest as promising cathode candidates for Li-ion batteries due to their low cost and high energy density. However, several issues, including sensitivity to moisture, difficulty in reproducibly preparing well-controlled morphology particles and, poor cyclability, have hindered their large scale deployment; especially for electric vehicle (EV) applications. In this work, we have developed a uniform, highly stable, high-energy density, Ni-rich LiNi0.6Mn0.2Co0.2O2 cathode material by systematically optimizing synthesis parameters, including pH, stirring rate, and calcination temperature. The particles exhibit a spherical morphology and uniform size distribution, with a well-defined structure and homogeneous transition-metal distribution, owing to the well-controlled synthesis parameters. The material exhibited superior electrochemical properties, when compared to a commercial sample, with an initial discharge capacity of 205 mAh/g at 0.1 C. It also exhibited a remarkable rate capability with discharge capacities of 157 mAh/g and 137 mAh/g at 10 and 20 C, respectively, as well as high tolerance to air and moisture. In order to demonstrate incorporation into a commercial scale EV, a large-scale 4.7 Ah LiNi0.6Mn0.2Co0.2O2 Al-full pouch cell with a high cathode loading of 21.6 mg/cm2, paired with a graphite anode, was fabricated. It exhibited exceptional cyclability with a capacity retention of 96% after 500 cycles at room temperature. This material, which was obtained by a fully optimized scalable synthesis, delivered combined performance metrics that are among the best for NMC materials reported to date.

SnS/C nanocomposites for high-performance sodium ion battery anodes

Sodium-ion batteries have been considered as one of the most promising types of batteries, beyond lithium-ion batteries, for large-scale energy storage applications. However, their deployment hinges on the development of new anode materials, since it has been shown that many important anode materials employed in lithium ion batteries, such as graphite and silicon, are inadequate for sodium-ion batteries. We have simply prepared novel SnS/C nanocomposites through a top-down approach as anode materials for sodium-ion batteries. Their electrochemical performance has been significantly improved when compared to bare SnS, especially in terms of cycling stability and rate capabilities. SnS/C nanocomposites exhibit excellent capacity retention, at various current rates, and deliver capacities as high as 400 mA h g−1 even at the high current density of 800 mA g−1 (2C). Ex situ transmission electron microscopy, X-ray diffraction and operando X-ray absorption near edge structure studies have been performed in order to unravel the reaction mechanism of the SnS/C nanocomposites.

Pt-Decorated Composition-Tunable Pd–Fe@Pd/C Core–Shell Nanoparticles with Enhanced Electrocatalytic Activity toward the Oxygen Reduction Reaction

Design of electrocatalysts with both a high-Pt-utilization efficiency and enhanced electrochemical activity is still the key challenge in the development of proton exchange membrane fuel cells. In the present work, Pd-Fe/C bimetallic nanoparticles (NPs) with an optimal Fe composition and decorated with Pt are introduced as promising catalysts toward the oxygen reduction reaction. These bimetallic nanoparticles have a Pd-Fe@Pd core-shell structure with a surface Pt decoration as established through the use of electron energy loss spectroscopy (EELS) and energy-dispersive X-ray (EDX) spectroscopy. These catalysts exhibit excellent electrocatalytic activity ( E1/2 = 0.866 V vs RHE), increasing the mass activity by more than 70% over that of Pt/C in terms of the total mass of Pt and Pd and by 14 times if only Pt is considered. Simple geometrical calculations, based on spherical core-shell models, indicate that Pd-Fe@Pt has a surface Pt decoration rather than a complete Pt monolayer. Such calculations applied to other examples in the literature point out the need for careful and rigorous arguments about claimed Pt monolayer/multilayers. Such calculations must be based on not only elemental mapping data but also on the Pt/Pd and other metal atomic ratios in the precursors. Our analysis predicts a minimal Pt/Pd atomic ratio in order to achieve a complete Pt monolayer on the surface of the core materials.

High-Performance Ga2O3 Anode for Lithium-Ion Batteries

There is a great deal of interest in developing battery systems that can exhibit self-healing behavior, thus enhancing cyclability and stability. Given that gallium (Ga) is a metal that melts near room temperature, we wanted to test if it could be employed as a self-healing anode material for lithium-ion batteries (LIBs). However, Ga nanoparticles (NPs), when directly applied, tended to aggregate upon charge/discharge cycling. To address this issue, we employed carbon-coated Ga2O3 NPs as an alternative. By controlling the pH of the precursor solution, highly dispersed and ultrafine Ga2O3 NPs, embedded in carbon shells, could be synthesized through a hydrothermal carbonization method. The particle size of the Ga2O3 NPs was 2.6 nm, with an extremely narrow size distribution, as determined by high-resolution transmission electron microscopy and Brunauer-Emmett-Teller measurements. A lithium-ion battery anode based on this material exhibited stable charging and discharging, with a capacity of 721 mAh/g after 200 cycles. The high cyclability is due to not only the protective effects of the carbon shell but also the formation of Ga0 during the lithiation process, as indicated by operando X-ray absorption near-edge spectroscopy.