Conversion Mechanisms of Selective Extraction of Lithium from Spent Lithium-Ion Batteries by Sulfation Roasting

Abstract

With the undergoing unprecedented development of lithium-ion batteries (LIBs), the recycling of end-of-life batteries has become an urgent task considering the demand for critical materials, environmental pollution, and ecological impacts. Selective recovery of targeted element(s) is becoming a topical field that enables metal recycling in a short path with highly improved material efficiencies. This research demonstrates a process of selective recovery of spent Ni–Co–Mn (NCM)-based lithium-ion battery by systematically understanding the conversion mechanisms and controlling the sulfur behavior during a modified-sulfation roasting. As a result, Li from complex cathode components can be selectively extracted with high efficiency by only using water. Notably, the sulfur driven recovery processes can be divided into two stages: (i) part of the structure of NCM523 was destroyed, and Ni, Co, and Mn were reduced to divalent in different degrees to form sulfate (NiSO4, CoSO4, MnSO4) when reacting with H2SO4 at ambient temperature; (ii) with increasing temperature, Li ions in the unstable layered structure are released and combined with SO4 2– in the transition metal sulfate to form Li2SO4, and the sulfates of transition metals react to form Ni0.5Co0.2Mn0.3O1.4. Studies have shown sulfur can be recirculated thoroughly in the form of SO4 2–, which in principle avoids secondary pollutions. By controlling the appropriate conversion temperature, we envisage that the sulfation selective roasting recovery technology could be easily applied to other spent lithium-ion battery materials. Besides, this work may also provide a unique platform for further study on the efficient extracting of other mineral resources.

Sustainable Recycling of Cathode Scrap towards High‐Performance Anode Materials for Li‐Ion Batteries

“…The C peak corresponded to C 1s and originated from the carbon used for system calibration (Figure 1h,i). [ 10 ] The O peak corresponded to O 1s and can be fitted by two peaks (Figure 1j,k), one for the metal–oxygen bond, corresponding to the peak of 529.8 eV, and the other for the chemisorbed oxygen species, corresponding to the peak of 531.3–531.6 eV. [ 11 ]…”

Technologies of lithium recycling from waste lithium ion batteries: a review

“…Pyrometallurgy uses high temperatures to remove organic material via evaporation and causes reactions in the cathode and anode to make lithium soluble in water. [66][67][68][69][70][71][72][73][74][75][76] Lithium was then recycled from the aqueous solution. The pre-treated active materials were powdered and subjected to calcination.…”

“…73 Li et al used sulfation roasting to recycle Li 2 SO 4 from NCM523 material by using H 2 SO 4 with the process of roasting and water leaching. 76 Chlorination roasting is also used in pyrometallurgy, which uses sintered lithium slag (xLi 2 OÁyCaOÁzAl 2 O 3 ÁnSiO 2 ) with chlorine donor to form LiCl after the roasting. Chang et al used CaCl 2 and roasted it at 1000 1C for 90 min with LiAl(SiO 3 ) 2 to transform it into LiCl 71 (eqn ( 7)).…”

A unique co-recovery strategy of cathode and anode from spent LiFePO4 battery

“…Pyrometallurgy primarily smelts valuable metals into new alloys at high temperatures, consuming extremely high energy. Furthermore, anodes and electrolytes are oxidized and provide energy for the smelting process [16,17]. Moreover, the process emits a considerable amount of polluting greenhouse gases and exerting massive pressure on the environment.…”