Search for: All records

All-climate temperature operation capability and increased energy density have been recognized as two crucial targets, but they are rarely achieved together in rechargeable lithium (Li) batteries. Herein, we demonstrate an electrolyte system by using monodentate dibutyl ether with both low melting and high boiling points as the sole solvent. Its weak solvation endows an aggregate solvation structure and low solubility toward polysulfide species in a relatively low electrolyte concentration (2 mol L −1 ). These features were found to be vital in avoiding dendrite growth and enabling Li metal Coulombic efficiencies of 99.0%, 98.2%, and 98.7% at 23 °C, −40 °C, and 50 °C, respectively. Pouch cells employing thin Li metal (50 μm) and high-loading sulfurized polyacrylonitrile (3.3 mAh cm −2 ) cathodes (negative-to-positive capacity ratio = 2) output 87.5% and 115.9% of their room temperature capacity at −40 °C and 50 °C, respectively. This work provides solvent-based design criteria for a wide temperature range Li-sulfur pouch cells. 

Lithium metal batteries are capable of pushing cell energy densities beyond what is currently achievable with commercial Li-ion cells and are the ideal technology for supplying power to electronic devices at low temperatures (≤−20 °C). To minimize the thermal management requirements of these devices, batteries capable of both charging and discharging at these temperatures are highly desirable. Here, we report >4 V Li metal full cell batteries (N/P = 2) capable of hundreds of stable cycles down to −40 °C, unambiguously enabled by the introduction of cation/anion pairs in the electrolyte. Via controlled experimental and computational investigations in electrolytes employing 1,2-dimethoxyethane as the solvating solvent, we observed distinct performance transitions in low temperature electrochemical performance, coincident with a shift in the Li + binding environment. The performance advantages of heavily ion-paired electrolytes were found to apply to both the cathode and anode, providing Li metal Coulombic efficiencies of 98.9, 98.5, and 96.9% at −20, −40, and −60 °C, respectively, while improving the oxidative stability in support of >4 V cathodes. This work reveals a strong correlation between ion-pairing and low-temperature performance while providing a viable route to Li metal full batteries cycling under extreme conditions. 

As lithium-ion batteries (LIBs) become vital energy source for daily life and industry applications, a large volume of spent LIBs will be produced after their lifespan. Recycling of LIBs has been considered as an effective closed-loop solution to mitigate both environmental and economic issues associated with spent LIBs. While reclaiming of transition metal elements from LIB cathodes has been well established, recycling of graphite anodes has been overlooked. Here, we show an effect upcycling method involving both healing and doping to directly regenerate spent graphite anodes. Specifically, using boric acid pretreatment and short annealing, our regeneration process not only heals the composition/structure defects of degraded graphite but also creates functional boron-doping on the surface of graphite particles, providing high electrochemical activity and excellent cycling stability. The efficient direct regeneration of spent graphite by using low cost, non-volatile and non-caustic boric acid with low annealing temperature provides a more promising direction for green and sustainable recycling of spent LIB anodes.

 

A low‐carbon future demands more affordable batteries utilizing abundant elements with sustainable end‐of‐life battery management. Despite the economic and environmental advantages of Li‐MnO₂batteries, their application so far has been largely constrained to primary batteries. Here, we demonstrate that one of the major limiting factors preventing the stable cycling of Li‐MnO₂batteries, Mn dissolution, can be effectively mitigated by employing a common ether electrolyte, 1 mol/L lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) in 1,3‐dioxane (DOL)/1,2‐dimethoxyethane (DME). We discover that the suppression of this dissolution enables highly reversible cycling of the MnO₂cathode regardless of the synthesized phase and morphology. Moreover, we find that both the LiPF₆salt and carbonate solvents present in conventional electrolytes are responsible for previous cycling challenges. The ether electrolyte, paired with MnO₂cathodes is able to demonstrate stable cycling performance at various rates, even at elevated temperature such as 60°C. Our discovery not only represents a defining step in Li‐MnO₂batteries with extended life but provides design criteria of electrolytes for vast manganese‐based cathodes in rechargeable batteries.

 

Achieving increased energy density under extreme operating conditions remains a major challenge in rechargeable batteries. Herein, we demonstrate an all‐fluorinated ester‐based electrolyte comprising partially fluorinated carboxylate and carbonate esters. This electrolyte exhibits temperature‐resilient physicochemical properties and moderate ion‐paired solvation, leading to a half solvent‐separated and half contact‐ion pair in a sole electrolyte. As a result, facile desolvation and preferential reduction of anions/fluorinated co‐solvents for LiF‐dominated interphases are achieved without compromising ionic conductivity (>1 mS cm⁻¹even at −40 °C). These advantageous features were found to apply to both lithium metal and sulfur‐based electrodes even under extreme operating conditions, allowing stable cycling of Li || sulfurized polyacrylonitrile (SPAN) full cells with high SPAN loading (>3.5 mAh cm⁻²) and thin Li anode (50 μm) at −40, 23 and 50 °C. This work offers a promising path for designing temperature‐resilient electrolytes to support high energy density Li metal batteries operating in extreme conditions.

 

Achieving increased energy density under extreme operating conditions remains a major challenge in rechargeable batteries. Herein, we demonstrate an all‐fluorinated ester‐based electrolyte comprising partially fluorinated carboxylate and carbonate esters. This electrolyte exhibits temperature‐resilient physicochemical properties and moderate ion‐paired solvation, leading to a half solvent‐separated and half contact‐ion pair in a sole electrolyte. As a result, facile desolvation and preferential reduction of anions/fluorinated co‐solvents for LiF‐dominated interphases are achieved without compromising ionic conductivity (>1 mS cm⁻¹even at −40 °C). These advantageous features were found to apply to both lithium metal and sulfur‐based electrodes even under extreme operating conditions, allowing stable cycling of Li || sulfurized polyacrylonitrile (SPAN) full cells with high SPAN loading (>3.5 mAh cm⁻²) and thin Li anode (50 μm) at −40, 23 and 50 °C. This work offers a promising path for designing temperature‐resilient electrolytes to support high energy density Li metal batteries operating in extreme conditions.

 

As the dominant means of energy storage technology today, the widespread deployment of lithium‐ion batteries (LIBs) would inevitably generate countless spent batteries at their end of life. From the perspectives of environmental protection and resource sustainability, recycling is a necessary strategy to manage end‐of‐life LIBs. Compared with traditional hydrometallurgical and pyrometallurgical recycling methods, the emerging direct recycling technology, rejuvenating spent electrode materials via a non‐destructive way, has attracted rising attention due to its energy efficient processes along with increased economic return and reduced CO₂footprint. This review investigates the state‐of‐the‐art direct recycling technologies based on effective relithiation through solid‐state, aqueous, eutectic solution and ionic liquid mediums and thoroughly discusses the underlying regeneration mechanism of each method regarding different battery chemistries. It is concluded that direct regeneration can be a more energy‐efficient, cost‐effective, and sustainable way to recycle spent LIBs compared with traditional approaches. Additionally, it is also identified that the direct recycling technology is still in its infancy with several fundamental and technological hurdles such as efficient separation, binder removal and electrolyte recovery. In addressing these remaining challenges, this review proposes an outlook on potential technical avenues to accelerate the development of direct recycling toward industrial applications.

 

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 and their possible solutions are summarized. Different aspects such as recycling/upcycling techniques, worldwide government policies, and the economic and environmental impacts are discussed, along with some practical suggestions to overcome these challenges for a promising circular economy for LIB materials. Some potential strategies are proposed to convert such challenges into opportunities to maintain the global expansion of the EV and other LIB‐dependent industries.