The increasing usage of electrical drive systems and stationary energy storage worldwide lead to a high demand of raw materials for the production of lithium-ion batteries. To prevent further shortage of these crucial materials, ecological and efficient recycling processes of lithium-ion batteries are needed. Nowadays industrial processes are mostly pyrometallurgical and as such energy and cost intensive. The LithoRec projects, funded by the Federal Ministry for the Environment, Nature Conservation, Building and Nuclear Safety (BMUB), aimed at a realization of a new energy-efficient recycling process, abstaining high temperatures and tracing mechanical process-steps. The conducted mechanical processes were thoroughly investigated by experiments in a laboratory and within technical scale, describing gas release of aged and non-aged lithium-ion batteries during dry crushing, intermediates, and products of the mechanical separation. Conclusively, we found that applying a second crushing step increases the yield of the coating materials, but also enables more selective separation. This work identifies the need for recycling of lithium-ion batteries and its challenges and hazard potential in regards to the applied materials. The outlined results show a safe and ecological recycling process with a material recycling rate of at least 75%.

This work demonstrates the feasibility of a novel solvent‐free anode production for lithium‐ion batteries. It combines a modified dry‐mixing procedure with an innovative electrostatic coating process. The mixing is divided into two steps. At first, carbon black and binder are deagglomerated and recombined to a matrix structure by intensive mixing. In a second less intensive step, this matrix is blended with graphite. The powder mixture is fluidized and then transferred to the current collector by inducing a high voltage. After a subsequent hot pressing step, the powder coating is permanently fixed on the current collector. This procedure is presented with three different fluorinated binders. Furthermore, effects of different mixing intensities on the powder and electrode properties are examined. The electrodes are investigated in the three‐electrode T‐cell setup versus lithium metal to examine their C‐rates and cycle stabilities. The produced anodes offer comparable electrochemical performance to conventional wet‐coated ones on electrode and cell levels. Overall, this new process is a suitable alternative to the conventional electrode production techniques.

Nowadays recycling processes for lithium-ion batteries focus on the recovery of nickel and cobalt. These processes are mainly pyro-metallurgical and as such energy and cost intensive. The project LithoRec, sponsored by the German Federal Ministry for the Environment, Nature Conservation, Building and Nuclear Safety (BMUB), aims at a realization of a new ecological recycling process tracing mechanical process-steps and considering recycling of lithium. This work presents the main challenges of the recycling of battery systems of electric and hybrid electric vehicles and the developed process chain, as well as the influence of a second crushing step on the yield and purity of the separated black mass containing the aged active materials.

Climate change is part of today's most complex global challenges. Social efforts to achieve sustainable and CO 2 -neutral ways to provide mobility as well as for electrical energy production, induce ambitious challenges to energy storage. In the field of rechargeable batteries, the lithium-ion-battery (LIB) is today's most promising approach, to match all energy storage requirements of electric vehicles (mobile energy storage) as well as for grid stabilization (stationary energy storage). Since their first commercialization by Sanyo, Sony, and Matsuhita in the early 1990ies, [1] LIBs enabled a wide range of portable electronics. Nevertheless, LIBs still require further improvements in terms of energy density, power density, lifetime, safety, and cost reduction, which presently drives enormous research efforts to focus on these topics. Typical research fields cover the advancement of active and inactive electrode materials, separators, electrolytes, as well as manufacturing techniques. Simulation approaches for characterization of fundamental physical and chemical processes during LIB operation highlighted surfaces and interfaces to have a substantial influence on LIB kinetics, in terms of electrolyte mass transport, charge-transfer (CT) reactions at anodic and cathodic active material (AM) particles, and electronic resistance at the electrode--current collector interface. Significant improvements to battery performance by surface/interface modification were yet demonstrated by calendering [2,3] or laser structuring [4][5][6][7][8] of electrodes, lamination of electrodes and separator, [9] or by enlargement of the current collector micro-surface. [10][11][12][13][14] Plasma-processes are well-known as a helpful tool in the field of LIBs. [15] Plasma-processes enable the production of nanosized AM particles, [16][17][18] carbon-based conductive AM coatings, [19] specialized 3D architectures for electrode nanowires, [20,21]