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At least 181 records · Page 10

Model-Instructed Design of Novel Charging Protocols for the Extreme Fast Charging of Lithium-Ion Batteries Without Lithium Plating

Relatively long recharge time of high-energy density lithium-ion batteries (LIBs) is one of the major obstacles to the widespread deployment of electric vehicles (EVs). Excessive fast charge of LIBs can cause severe safety issues, the most significant of which is lithium plating. In addition to the consumption of cyclable lithium, dendrite-like lithium plating can cause short-circuiting within the cell, which could lead to catastrophic failure. In addition to the developments of advanced electrolytes, active materials and electrodes, the fast charging capability of LIBs can be improved by using optimized charging protocol. In this paper, the Pseudo2D battery model is first used to screen some conventional charging protocols proposed for fast charging, including the constant-current constant-voltage charging (CCCV), constant-power constant-voltage charging (CPCV), multi-stage constant-current charging, and pulse current charging. A semi-optimal charging protocol is then developed by automatically modifying the charge current such that the cell is charged at close-to-maximum current without lithium plating. Based on the features of the semi-optimal protocol, two practical novel fast charging protocols are proposed which allow charging the cell at a higher rate without lithium plating. Through simulation, we show that the no-plating capacity after 10 min charge can be improved by up to ~10.7% compared to CCCV charging for a 2.5 mAh cm -2 cell and ~18.8% for a 4 mAh cm -2 cell, when the proposed charging protocols are used.

25 ENERGY STORAGE↗

Scalable Metal Phosphides as a Dual-Function Catalyst and Lithium–Metal Stabilizer for Lithium–Sulfur Batteries

Although lithium-sulfur batteries are a promising approach for achieving high energy density, their commercial viability is limited by poor sulfur redox kinetics, polysulfide shuttling, and lithium metal instability. To resolve these issues concurrently, we utilize titanium phosphides (TiP x ) as dual-function materials to catalyze the sulfur redox kinetics at the cathode and stabilize the lithium metal at the anode. Importantly, these phosphides are synthesized via a facile, highly scalable one-step mechanochemical ball-milling process that does not generate toxic phosphine gas as a byproduct, making it more viable compared to traditional synthesis routes. At the cathode, we find that higher phosphorus contents in the phosphide as in TiP 2 leads to superior redox kinetics and reduced polysulfide shuttling due to improved polysulfide adsorption ability. Meanwhile, at the anode, TiP 2 acts as a lithiophilic seed in a 3-dimensional carbonaceous host that can be lithiated to form a Li-TiP 2 /C composite. This composite alleviates the volume changes of lithium metal while utilizing TiP 2 to form a more favorable solid-electrolyte interface (SEI). Full coin cells employing TiP 2 in the cathode and anode were assembled with a sulfur loading of 4 mg cm -2 and a negative to positive capacity (N/P) ratio of 6. After 50 cycles, the TiP 2 full cells retain a higher capacity of 643 mA h g -1 compared to 422 mA h g -1 for the conventional cell, despite the higher N/P ratio of 12 for the conventional cell. Altogether, we showcase the viability of employing metal phosphides as catalysts in practical lithium-sulfur batteries.

25 ENERGY STORAGE↗

Stable Lithium Plating in “Lithium Metal-Free” Solid-State Batteries Enabled by Seeded Lithium Nucleation

In the “Li 0 -free” architecture, cells are manufactured with a bare anode current collector and the Li metal anode is plated in situ during the first charging step. While this architecture has many attractive qualities from manufacturing and energy density perspectives, stable Li plating in solid-state “Li 0 -free” cells can be challenging. It is generally accepted that the Li overpotential affects Li homogeneity in “Li 0 -free” cells. We demonstrate that the nucleation overpotential for Li plating in solid-state “Li 0 -free” cells using commercial current collectors can be eliminated by introducing metal clusters that guide Li nucleation. Au is used as model alloying metal cluster. Here, we demonstrate stable Li plating with thickness 16.5 μ m (3.3 mAh cm −2 ) in oxide solid-state electrolyte “Li 0 -free” cells enabled by Au metal clusters. It is shown that 97% of the in situ plated Li can be reversibly stripped at 60 °C and 2.5 MPa. Conversely, Au interlayers which are flat and continuous instead of clustered in morphology consistently showed short-circuiting during in situ Li plating, limiting Li electrodeposition to <0.1 mAh cm −2 . These results can help guide future studies of Li nucleation and growth at solid/solid interfaces, as well as offer alternative manufacturing pathways for “Li 0 -free” solid-state batteries.

25 ENERGY STORAGE↗

Developing an In-situ Formed Dynamic Protection Layer to Mitigate Lithium Interface Shifting: Preventing Dendrite Formation on Metallic Lithium Surface to Facilitate Long Cycle Life of Lithium Solid-State Batteries

After extensive research on various system, a fully lithiated Si anode material (Li 3.75 Si) was synthesized. The high energy density, long cycle life anode demonstrated no apparent dendrite growth in an all-solid-state Li battery. A flexible solid-state electrolyte film with a thickness less than 50 μm was developed. All-solid-state Li full batteries were built and tested with NMC811, organic, organosulfide and sulfur cathode. Energy density of 1140 Wh/Kg at material level and 376 Wh/Kg at electrode level were demonstrated for over 500 cycles and with no apparent dendrite formation on the Li anode.

25 ENERGY STORAGE↗

Anode‐Free Lithium–Sulfur Cells Enabled by Rationally Tuning Lithium Polysulfide Molecules

Abstract The two major barriers of practical lithium–sulfur batteries are the poor reversibility of lithium‐metal anode and sluggish kinetics of sulfur cathode. Here, we report a simple yet cogent, molecular tailoring approach for lithium polysulfides, enabling a synergistic enhancement of anode reversibility and cathode kinetics. We show that SnI 4 coordinates with lithium polysulfides to form soluble complexes, resulting in a Li 2 SnS 3 ‐rich anode interphase layer. As Li 2 SnS 3 is stable against parasitic reactions and has a lower ionic resistance over cycling, the Li plating/stripping efficiency is greatly improved. In addition, the formation of soluble complexes between SnI 4 and lithium polysulfides play a non‐negligible role in suppressing the clustering behavior of lithium polysulfide molecules, resulting in a significant enhancement in sulfur conversion kinetics under lean electrolyte conditions. The synergistic improvement is validated in anode‐free, lean‐electrolyte pouch cells with a Li 2 S cathode that displays capacity retention of 78 % after 100 cycles.

Ren, Yuxun↗

Anode-Free Lithium–Sulfur Cells Enabled by Rationally Tuning Lithium Polysulfide Molecules

The two major barriers of practical lithium–sulfur batteries are the poor reversibility of lithium-metal anode and sluggish kinetics of sulfur cathode. Here, we report a simple yet cogent, molecular tailoring approach for lithium polysulfides, enabling a synergistic enhancement of anode reversibility and cathode kinetics. In this study, we show that SnI 4 coordinates with lithium polysulfides to form soluble complexes, resulting in a Li 2 SnS 3 -rich anode interphase layer. As Li 2 SnS 3 is stable against parasitic reactions and has a lower ionic resistance over cycling, the Li plating/stripping efficiency is greatly improved. In addition, the formation of soluble complexes between SnI 4 and lithium polysulfides play a non-negligible role in suppressing the clustering behavior of lithium polysulfide molecules, resulting in a significant enhancement in sulfur conversion kinetics under lean electrolyte conditions. The synergistic improvement is validated in anode-free, lean-electrolyte pouch cells with a Li 2 S cathode that displays capacity retention of 78 % after 100 cycles.

25 ENERGY STORAGE↗

Self-Healing Lithium Dendrites through Spontaneous Passivating Layer Formation for Stable Solid-State Lithium–Metal Batteries

All-solid-state lithium–metal batteries have attracted significant attention, owing to their high energy density and superior safety. However, lithium–metal penetration through the solid electrolyte, leading to short-circuiting, remains a critical failure mode that demands comprehensive mitigation strategies. Most existing strategies are effective only prior to the initiation of lithium-dendrite formation and fail once dendrites begin to propagate through the electrolyte. In this study, we propose a self-healing mechanism in which the penetrated lithium reacts with a self-healing agent to form a passivating layer along the particle boundaries. Lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) was incorporated into a Li 6 PS 5 Cl solid electrolyte as the self-healing agent to suppress lithium-dendrite propagation even after dendrite formation initiated under high current densities. The self-healing induced by LiTFSI was verified through comprehensive experimental analyses and was further demonstrated in a full-cell configuration. Moreover, LiTFSI incorporation plays an important role in increasing the critical current density by reducing the overall electronic conductivity of the solid electrolyte and facilitating the formation of a robust LiF-containing solid-electrolyte interphase.

25 ENERGY STORAGE↗

Lithium titanate hydrates with superfast and stable cycling in lithium ion batteries

Lithium titanate and titanium dioxide are two best-known high-performance electrodes that can cycle around 10,000 times in aprotic lithium ion electrolytes. Here we show there exists more lithium titanate hydrates with superfast and stable cycling. That is, water promotes structural diversity and nanostructuring of compounds, but does not necessarily degrade electrochemical cycling stability or performance in aprotic electrolytes. As a lithium ion battery anode, our multi-phase lithium titanate hydrates show a specific capacity of about 130 mA h g –1 at ~35 C (fully charged within ~100 s) and sustain more than 10,000 cycles with capacity fade of only 0.001% per cycle. In situ synchrotron diffraction reveals no 2-phase transformations, but a single solid-solution behavior during battery cycling. Here, so instead of just a nanostructured intermediate to be calcined, lithium titanate hydrates can be the desirable final destination.

25 ENERGY STORAGE↗

Flexible and stable high-energy lithium-sulfur full batteries with only 100% oversized lithium

Lightweight and flexible energy storage devices are urgently needed to persistently power wearable devices, and lithium-sulfur batteries are promising technologies due to their low mass densities and high theoretical capacities. Here we report a flexible and high-energy lithium-sulfur full battery device with only 100% oversized lithium, enabled by rationally designed copper-coated and nickel-coated carbon fabrics as excellent hosts for lithium and sulfur, respectively. These metallic carbon fabrics endow mechanical flexibility, reduce local current density of the electrodes, and, more importantly, significantly stabilize the electrode materials to reach remarkable Coulombic efficiency of >99.89% for a lithium anode and >99.82% for a sulfur cathode over 400 half-cell charge-discharge cycles. Furthermore, the assembled lithium-sulfur full battery provides high areal capacity (3 mA h cm –2 ), high cell energy density (288 W h kg –1 and 360 W h L –1 ), excellent cycling stability (260 cycles), and remarkable bending stability at a small radius of curvature (<1 mm).

25 ENERGY STORAGE↗

Lithium anode stable in air for low-cost fabrication of a dendrite-free lithium battery

Lithium metal, the ideal anode material for rechargeable batteries, suffers from the inherent limitations of sensitivity to the humid atmosphere and dendrite growth. Herein, low-cost fabrication of a metallic-lithium anode that is stable in air and plated dendrite-free from an organic-liquid electrolyte solves four key problems that have plagued the development of large-scale Li-ion batteries for storage of electric power. Replacing the low-capacity carbon anode with a safe, dendrite-free lithium anode provides a fast charge while reducing the cost of fabrication of a lithium battery, and increasing the cycle life of a rechargeable cell by eliminating the liquid-electrolyte ethylene-carbonate additive used to form a solid-electrolyte interphase passivation layer on the anode that is unstable during cycling. This solution is accomplished by formation of a hydrophobic solid-electrolyte interphase on a metallic-lithium anode that allows for handling of the treated lithium anode membrane in a standard dry room during cell fabrication.

25 ENERGY STORAGE↗