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, NaO2, and Na+–O2, 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.