Unveiling Sodium Ion Pollution in Spray-Dried Precursors and Its Implications for the Green Upcycling of Spent Lithium-Ion Batteries.

Unclear impurity pollution is one of the key scientific problems that limit the large-scale production of new lithium-ion batteries (LIBs) from spent LIBs. This work is the first to report the pollution path, pollution degree, and solution method of sodium ions in the recycling process of spent LIBs in the real world. The results show that sodium ions can intrude into the precursor particles to form crystalline salts with the anion of the leaching acid that cover the transition metal elements, thereby resulting in a failed precursor. Specifically, the intrusion of sodium ions will produce a variety of pollutants containing metal oxide bonds, such as Na-O, NaO, and Na-O, on the precursor surface. These active lattice oxygen will further adsorb or react to form organic oxygen, chemical oxygen, and free oxygen, which will highly deteriorate the surface cleanliness. Strictly controlling the consumption of sodium salt in each step and using ammonia instead of NaOH for pH regulation can effectively solve sodium ion pollution to prepare high-quality battery precursors. It reveals that for the green upcycling of spent LIBs, we should strengthen the design of the recycling process to reduce the consumption of chemical reagents, which will produce unexpected secondary pollution.