Surface and grain boundary coating for stabilizing LiNi0.8Mn0.1Co0.1O2 based electrodes.

The widespread use of high-capacity Ni-rich layered oxides such as LiNi0.8Mn0.1Co0.1O2 (NMC811), in lithium-ion batteries is hindered due to practical capacity loss and reduced working voltage during operation. Aging leads to defective NMC811 particles, affecting electrochemical performance. Surface modification offers a promising approach to improve cycle life. Here, we introduce an amorphous lithium titanate (LTO) coating via atomic layer deposition (ALD), not only covering NMC811 surfaces but also penetrating cavities and grain boundaries. As NMC811 electrodes suffer from low structural stability during charge and discharge, We combined electrochemistry, operando X-ray diffraction (XRD), and dilatometry to understand structural changes and the coating protective effects. XRD reveals significant structural evolution during delithiation for uncoated NMC811. The highly reversible phase change in coated NMC811 highlights enhanced bulk structure stability. The LTO coating retards NMC811 degradation, boosting capacity retention from 86% to 93% after 140 cycles. This study underscores the importance of grain boundary engineering for Ni-rich layered oxide electrode stability and the interplay of chemical and mechanical factors in battery aging.

Robust method for uniform coating of carbon nanotubes with V2O5 for next-generation transparent electrodes and Li-ion batteries.

Composites comprising vanadium-pentoxide (V2O5) and single-walled carbon nanotubes (SWCNTs) are promising components for emerging applications in optoelectronics, solar cells, chemical and electrochemical sensors, etc. We propose a novel, simple, and facile approach for SWCNT covering with V2O5 by spin coating under ambient conditions. With the hydrolysis-polycondensation of the precursor (vanadyl triisopropoxide) directly on the surface of SWCNTs, the nm-thick layer of oxide is amorphous with a work function of 4.8 eV. The material recrystallizes after thermal treatment at 600 °C, achieving the work function of 5.8 eV. The key advantages of the method are that the obtained coating is uniform with a tunable thickness and does not require vacuuming or heating during processing. We demonstrate the groundbreaking results for two V2O5/SWCNT applications: transparent electrode and cathode for Li-ion batteries. As a transparent electrode, the composite shows stable sheet resistance of 160 Ω sq-1 at a 90% transmittance (550 nm) - the best performance reported for SWCNTs doped by metal oxides. As a cathode material, the obtained specific capacity (330 mA h g-1) is the highest among all the other V2O5/SWCNT cathodes reported so far. This approach opens new horizons for the creation of the next generation of metal oxide composites for various applications, including optoelectronics and electrochemistry.

Overcoming Voltage Losses in Vanadium Redox Flow Batteries Using WO3 as a Positive Electrode.

Vanadium redox flow batteries (VRFBs) are appealing large-scale energy storage systems due to their unique properties of independent energy/power design. The VRFBs stack design is crucial for technology deployment in power applications. Besides the design, the stack suffers from high voltage losses caused by the electrodes. The introduction of active sites into the electrode to facilitate the reaction kinetic is crucial in boosting the power rate of the VRFBs. Here, an O-rich layer has been applied onto structured graphite felt (GF) by depositing WO3 to increase the oxygen species content. The oxygen species are the active site during the positive reaction (VO2 +/VO2+) in VRFB. The increased electrocatalytic activity is demonstrated by the monoclinic (m)-WO3/GF electrode that minimizes the voltage losses, yielding excellent performance results in terms of power density output and limiting current density (556 mWcm-2@800 mAcm-2). The results confirm that the m-WO3/GF electrode is a promising electrode for high-power in VRFBs, overcoming the performance-limiting issues in a positive half-reaction.

Understanding the Stabilizing Effects of Nanoscale Metal Oxide and Li-Metal Oxide Coatings on Lithium-Ion Battery Positive Electrode Materials.

Nickel-rich layered oxides, such as LiNi0.6Co0.2Mn0.2O2 (NMC622), are high-capacity electrode materials for lithium-ion batteries. However, this material faces issues, such as poor durability at high cut-off voltages (>4.4 V vs Li/Li+), which mainly originate from an unstable electrode-electrolyte interface. To reduce the side reactions at the interfacial zone and increase the structural stability of the NMC622 materials, nanoscale (<5 nm) coatings of TiOx (TO) and LixTiyOz (LTO) were deposited over NMC622 composite electrodes using atomic layer deposition. It was found that these coatings provided a protective surface and also reinforced the electrode structure. Under high-voltage range (3.0-4.6 V) cycling, the coatings enhance the NMC electrochemical behavior, enabling longer cycle life and higher capacity. Cyclic voltammetry, X-ray photoelectron spectroscopy, and X-ray diffraction analyses of the coated NMC electrodes suggest that the enhanced electrochemical performance originates from reduced side reactions. In situ dilatometry analysis shows reversible volume change for NMC-LTO during the cycling. It revealed that the dilation behavior of the electrode, resulting in crack formation and consequent particle degradation, is significantly suppressed for the coated sample. The ability of the coatings to mitigate the electrode degradation mechanisms, illustrated in this report, provides insight into a method to enhance the performance of Ni-rich positive electrode materials under high-voltage ranges.