power density, [1] especially for electronic devices, electric vehicles (EVs), and grid storage systems. As a result, the global market of LIBs is expected to follow a rapid upward trend, projected to reach US$56 billion by 2024. [1c] The primary growth will be triggered by the massive EV production, which is expected to reach $253 million by 2030. [1c] The rising LIB utilization has increased the demand for critical raw materials such as lithium (Li), nickel (Ni), and cobalt (Co). However, most of these essential materials are regulated by specific countries. More than half of cobalt ore is mined in the Democratic Republic of Congo and refined in China, and about 80% of lithium is controlled by Australia and Chile. [2] This uneven distribution of raw materials and production areas has raised concerns about the global supply chain. As a result, lithium and cobalt prices are rising and fluctuating, and in the meantime, the geopolitics could lead to a monopoly of raw material supply by local governments. [3] Therefore, from a sustainability perspective, it is essential to establish a secondary supply of critical materials recovered from spent LIBs (from EVs, stationary storage batteries, and home appliances) and from the manufacturing wastes (trimming, end products, off-spec products, etc.) to mitigate the severity of this potential shortage.On the other hand, since LIBs can usually be used for 10 years on average, [3,4] the amount of spent LIBs is expected to reach more than 5 million tons by 2030. [5] The main components of LIBs are cathode materials (LiNi x Co y Mn z O 2 (0 < x, y, z <1, x + y + z = 1, known as NCM), LiCoO 2 (LCO), LiFePO 4 (LFP), etc.), anode materials (graphite), current collectors (aluminum (Al) and copper (Cu)), electrolyte salts such as lithium hexafluorophosphate (LiPF 6 ), organic solvents (ethylene carbonate (EC), diethyl carbonate (DEC), ethyl methyl carbonate (EMC), dimethyl carbonate (DMC), etc.). All these different components contain hazardous materials and result in metal, dust, organic, and fluorine contaminations. [6] Landfilling or incineration can harm ecosystems. For example, once the electrode materials enter the environment, metal ions from the cathode, carbon dust from the anode, strong alkali, and heavy metal ions from the electrolyte may cause severe environmental pollutions, hazards, etc., including raising the pH value of the soil, [7] and producing the toxic gases (HF, HCl, etc.). In addition, the metals and electrolytes in batteries can harm human health. For example, the cobalt may get into the human body via underground water and other channels, causing Li-ion battery (LIB) recycling has become an urgent need with rapid prospering of the electric vehicle (EV) industry, which has caused a shortage of material resources and led to an increasing amount of retired batteries. However, the global LIB recycling effort is hampered by various factors such as insufficient logistics, regulation, and technology readiness. Here, the challenges associated with LIB recycling...
Despite significant progress in energy retention, lithium‐ion batteries (LIBs) face untenable reductions in cycle life under extreme fast‐charging (XFC) conditions, which primarily originate from a variety of kinetic limitations between the graphite anode and the electrolyte. Through quantitative Li+ loss accounting and comprehensive materials analyses, it is directly observed that the operation of LIB pouch cells at 4 C||C/3 (charging||discharging) results in Li plating, disadvantageous solid‐electrolyte‐interphase formation, and solvent co‐intercalation leading to interstitial decomposition within graphite layers. It is found that these failure modes originate from the insufficient properties of conventional electrolytes, where employing a designed ester‐based electrolyte improved the capacity retention of these cells from 55.9% to 88.2% after 500 cycles when operated at the aforementioned conditions. These metrics are the result of effective mitigation of the aforementioned failure modes due to superior Li+ transport and desolvation characteristics demonstrated through both experimental and computational characterization. This work reveals the vital nature of electrolyte design to XFC performance.
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