Comparison of the Ammoniacal Leaching Behavior of Layered LiNi_xCo_yMn_1–x–yO₂ (x = 1/3, 0.5, 0.8) Cathode Materials

Abstract

Recycling of spent lithium-ion batteries has received widespread concern on account of the high content of hazardous and valuable metals contained therein. In this research, ammonia leaching process is adapted to extract valuable metals selectively from LiNi x Co y Mn1–x–y O2 (x = 1/3, 0.5, 0.8) cathode materials. By employing ammoniacal solution as the leaching agent and sodium sulfite as reductant, Ni, Co, and Li are leached from lixivium either as complexes or metallic ion. Manganese is first leached from lixivium as Mn2+ and subsequently deposited from Mn3O4 to (NH4)2Mn­(SO3)2·H2O as sodium sulfite is added. Compared with the agglomerated (NH4)2Mn­(SO3)2·H2O tightly wrapped on the surface of the unreacted material, loose and porous Mn3O4 is more favorable to ion diffusion and leaching reaction. Amounts of 93.3% Li, 98.2% Co, and 97.9% Ni can be leached from LiNi1/3Co1/3Mn1/3O2 material by the introduced two-step leaching process, much higher than that with the one-step process. Simultaneously, 94.4% Li, 99.7% Co, and 99.5% Ni can be leached from LiNi0.5Co0.2Mn0.3O2 material, while the leaching efficiency of Li, Ni, and Co reaches 95.0%, 98.4%, and 96.9% for LiNi0.8Co0.1Mn0.1O2 material by a one-step leaching process.

Recycling of mixed cathode lithium‐ion batteries for electric vehicles: Current status and future outlook

“…Several studies have noted that high leaching efficiencies (>95%) for all metals can be obtained using a two‐step process where the solid residue is filtered and leached again using identical conditions . Meng et al proposed that the second step is required due to the sluggish leaching kinetics caused by the formation of (NH 4 ) 2 Mn(SO 3 ) 2 ∙H 2 O/Mn 3 O 4 precipitate coated on the active material particles. To avoid the use of sodium sulfite and subsequent formation of Mn precipitate, Wang et al pretreated LiNi 0.5 Mn 0.3 Co 0.2 O 2 through a thermomechanochemical reduction reaction with graphite, similar to the approaches described previously.…”

“…As a result, selectivity against Mn was improved—the leachate purity comprised 98.6% Li + , Ni 2+ , and Co 2+ and only 1.4% Mn 2+ . Several studies have noted that high leaching efficiencies (>95%) for all metals can be obtained using a two‐step process where the solid residue is filtered and leached again using identical conditions . Meng et al proposed that the second step is required due to the sluggish leaching kinetics caused by the formation of (NH 4 ) 2 Mn(SO 3 ) 2 ∙H 2 O/Mn 3 O 4 precipitate coated on the active material particles.…”

Effect of Hydrogen Peroxide on the Recovery of Valuable Metals from Spent LiNi0.6Co0.2Mn0.2O2 Batteries

“…Lithium‐ion batteries (LIBs) have gained widespread use in energy storage tools because of excellent electrochemical attributes such as long life, high energy, power density, and minimal memory effect. [ 1,2 ] It is notable that the global LIB recycling market is expected to grow to $23.72 billion in 2030 from $1.78 billion in 2017. [ 3 ] In addition, spent LIBs can result in severe environmental pollution and have a threat to human health.…”

Recovering Lithium from the Cathode Active Material in Lithium-Ion Batteries via Thermal Decomposition

“…Numerous investigations on the resource recovery have focused on the cathode active material [12][13][14][15]. The proposed recovery methods include a wet process [16][17][18], a dry process [19][20][21], an electrochemical method [22][23][24], bioleaching [25][26][27], crushing and selection [28], and mechanochemical reactions [29]. At least 99% of the cobalt and nickel can be recovered by the wet process.…”