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Download fileUpcycling Real Waste Mixed Lithium-Ion Batteries by Simultaneous Production of rGO and Lithium-Manganese-Rich Cathode Material
journal contribution
posted on 2021-09-24, 15:36 authored by Pier Giorgio Schiavi, Robertino Zanoni, Mario Branchi, Camilla Marcucci, Corrado Zamparelli, Pietro Altimari, Maria Assunta Navarra, Francesca PagnanelliThe direct synthesis
of high-value products from end-of-life Li-ion
batteries (LIBs), avoiding the complex and costly separation of the
different elements, can be reached through a competitive recycling
strategy. Here, we propose the simultaneous synthesis of reduced graphene
oxide (rGO) and lithium-manganese-rich (Li1.2Mn0.55Ni0.15Co0.1O2 - LMR) cathode material
from end-of-life LIBs. The electrode powder recovered after LIBs mechanical
pretreatment was directly subjected to the Hummers’ method.
This way, quantitative extraction of the target metals (Co, Ni, Mn)
and oxidation of graphite to graphene oxide (GO) were simultaneously
achieved, and a Mn-rich metal solution resulted after GO filtration,
owing to the use of KMnO4 as an oxidizing agent. This solution,
which would routinely constitute a heavy-metal liquid waste, was directly
employed for the synthesis of Li1.2Mn0.55Ni0.15Co0.1O2 cathode material. XPS measurements
demonstrate the presence in the synthesized LMR of Cu2+, SO42–, and SiO44– impurities, which were previously proposed as effective doping species
and can thus explain the improved electrochemical performance of recovered
LMR. The GO recovered by filtration was reduced to rGO by using ascorbic
acid. To evaluate the role of graphite lithiation/delithiation during
battery cycling on rGO production, the implemented synthesis procedure
was replicated starting from commercial graphite and from the graphite
recovered by a consolidated acidic–reductive leaching procedure
for metals extraction. Raman and XPS analysis disclosed that cyclic
lithiation/delithiation of graphite during battery life cycle facilitates
the graphite exfoliation and thus significantly increases conversion
to rGO.
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xps measurements demonstratexps analysis disclosedwould routinely constituteusing ascorbic acidmetal liquid wasteimproved electrochemical performancehummers ’ methodeffective doping speciescompetitive recycling strategylibs mechanical pretreatmentlibs ), avoiding55 sub4 sub2 sub15 subelectrode powder recoveredimplemented synthesis procedure4 – sup1 subrich cathode materialreduced graphene oxidegraphene oxidecathode materiallife libsgraphite recoveredvalue productsthus explaintarget metalssimultaneously achievedsimultaneous synthesissimultaneous productionreplicated startingquantitative extractionpreviously proposedoxidizing agentmetals extractionion batteriesdirectly subjecteddirectly employeddirect synthesisdifferent elementscyclic lithiationcostly separationbattery cycling