Lithium-ion batteries (LIBs) play a significant role in our highly electrified world and will continue to lead technology innovations. Millions of vehicles are equipped with or directly powered by LIBs, mitigating environmental pollution and reducing energy use. This rapidly increasing use of LIBs in vehicles will introduce a large quantity of spent LIBs within an 8-10-year span. Proper handling of endof-life (EOL) vehicle LIBs is required, and multiple options should be considered. This paper demonstrates that the necessity for EOL recycling is underpinned by leveraging fluctuating material costs, uneven distribution and production, and the transport situation. From a life-cycle perspective, remanufacturing and repurposing extend the life of LIBs, and industrial demonstrations indicate that this is feasible. Recycling is the ultimate option for handling EOL LIBs, and recent advancements both in research and industry regarding pyrometallurgical, hydrometallurgical, and direct recycling are summarized. Currently, none of the current battery recycling technologies is ideal, and challenges must be overcome. This article is anticipated as a starting point for a more sophisticated study of recycling, and it suggests potential improvements in the process through mutual efforts from academia, industry, and governments.

We report the first cradle-to-gate emissions assessment for a mass-produced battery in a commercial battery electric vehicle (BEV); the lithium-ion battery pack used in the Ford Focus BEV. The assessment was based on the bill of materials and primary data from the battery industry, that is, energy and materials input data from the battery cell and pack supplier. Cradle-to-gate greenhouse gas (GHG) emissions for the 24 kWh Ford Focus lithium-ion battery are 3.4 metric tonnes of CO2-eq (140 kg CO2-eq per kWh or 11 kg CO2-eq per kg of battery). Cell manufacturing is the key contributor accounting for 45% of the GHG emissions. We review published studies of GHG emissions associated with battery production to compare and contrast with our results. Extending the system boundary to include the entire vehicle we estimate a 39% increase in the cradle-to-gate GHG emissions of the Focus BEV compared to the Focus internal combustion engine vehicle (ICEV), which falls within the range of literature estimates of 27-63% increases for hypothetical nonproduction BEVs. Our results reduce the uncertainties associated with assessment of BEV battery production, serve to identify opportunities to reduce emissions, and confirm previous assessments that BEVs have great potential to reduce GHG emissions over the full life cycle and provide local emission free mobility.

Slurry making is a critical step that can irrevocably affect the subsequent steps in battery manufacturing. Many experimental parameters, including the mixing sequence, must be considered in making the slurry. In this work, we investigated the effects of the two main industry-used mixing sequences on the rheological behavior of the slurry, and the relation of the slurry rheology to structural, mechanical, and electrochemical performance of LiNi 0.33 Mn 0.33 Co 0.33 O 2 (NMC) electrodes. We show that: (1) mixing carbon black (CB) with polyvinylidene fluoride (PVDF) solution before adding NMC can facilitate the formation of a gel-like slurry; (2) porous clusters of CB/PVDF can form around NMC after drying the gel-like slurry, providing a high C-rate capability;(3) dry powder mixing of CB and NMC can facilitate the binding of the CB to the NMC surfaces, reducing the amount of CB in the PVDF and resulting in a liquid-like slurry; (4) after drying of the liquid-like slurry, a dense CB/PVDF layer can form on the NMC surfaces; and (5) this dense layer can provide high binding strength but may block ionic transport and weaken the electronic connection, reducing the C-rate capability. Thus, it is critically important to understand the effects of mixing sequence in electrode manufacturing.

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The lithium-ion battery (LIB) recycling market is becoming increasingly important because of the widespread use of LIBs in every aspect of our lives. Mobile devices and electric cars represent the largest application areas for LIBs. Vigorous innovation in these sectors is spurring continuous deployment of LIB powered devices, and consequently more and more LIBs will become waste as they approach end of life. Considering the significant economic and environmental impacts, recycling is not only necessary, but also urgent. The WPI group has successfully developed a closed-loop recycling process, and has previously demonstrated it on a relatively small scale 1 kg spent batteries per experiment. Here, we show that the closed-loop recycling process can be successfully scaled up to 30 kg of spent LIBs from electric vehicle recycling streams, and the recovered cathode powder shows similar (or better) performance to equivalent commercial powder when evaluated in both coin cells and single layer pouch cells. All of these results demonstrate the closed-loop recycling process has great adaptability and can be further developed into industrial scale.