Abstract

High-energy battery systems are gaining attention in the frame of global demands for electronic devices and vehicle electrification. This context leads to higher demands in terms of battery system properties, such as cycle stability and energy density. Here, Lithium–Sulfur (Li–S) batteries comprise an alternative to conventional Li-Ion battery (LIB) systems and can be asserted to next-generation electric storage systems. They offer a promising solution for contemporary needs, especially for applications requiring a higher energy density. In a global environment with increasing sustainable economics and ambitions towards commodity recirculation, the establishing of new technologies should also be evaluated in terms of their recycling potential. In this sense, innovative recycling considers highly valuable metals but also mobilizes all technologically relevant materials for reaching a high Recycling Efficiency (RE). This study uses an approach in which the recycling of Li–S batteries is addressed. For this purpose, a holistic recycling process using both thermal and hydrometallurgical steps is suggested for a safe treatment in combination with a maximum possible recycling efficiency. According to the batteries’ chemical composition, the containing elements are recovered separately, while a multi-step treatment is chosen. Hence, a thermal treatment in combination with a subsequent mechanical comminution separates a black mass powder containing all recoverable resources from the metal casing. The black mass is then treated further in an aqueous solution using different solid/liquid ratios: 1:20, 1:50, 1:55, and 1:100. Different basic and acidic leaching solutions are compared with one another: sulfuric acid (H2SO4), nitric acid (HNO3), hydrochloric acid (HCl), and NaOH. For further precipitation steps, different additives for a pH adjustment are also contrasted: sodium hydroxide (NaOH) and potassium hydroxide (KOH). The results are evaluated by both purity and yield; chemical analysis is performed by ICP-OES (inductively coupled plasma optical emission spectrometry). The aim of this recycling process comprises a maximum yield for the main Li–S battery fractions: Li, S, C, and Al. The focal point for the evaluation comprises lithium yields, and up to 93% of lithium could be transferred to a solid lithium carbonate product.

Highlights

  • Looking at today’s society, it can be observed that the demand and desire of greenhouse gas saving and sustainable technologies is higher than ever before

  • The focus is based on lithium yields, since lithium is the key driver for the recycling of lithium–sulfur batteries (LSBs), especially by value

  • The lithium yields were calculated by summing up the lithium mass in every filter cake (C-fc, Al(OH)3 fc and Li2 CO3 fc), and the mass of lithium in the residual filtrate after filtration IV(Lifiltrate, IV )

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Summary

Introduction

Looking at today’s society, it can be observed that the demand and desire of greenhouse gas saving and sustainable technologies is higher than ever before. As a result of this social rethinking, numerous branches of industry are being affected, including the automotive industry. This has led to a rapid change in drive technology from the combustion to electric engine [1,2,3]. Metals 2020, 10, 1513 small electronics sector (smartphones, laptops, etc.), are lithium batteries [2,4]. In this context, sales of one million electric vehicles per year were already recorded worldwide in 2017, which represents an increase of 56% compared to the previous year, 2016 [5,6]. Despite the constant development and different forms (NMC, NCA, LMO, LFP, etc.), the most modern LIBs reach a physical limit at a specific gravimetric energy density of

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