A closed-loop regeneration of LiNi0.6Co0.2Mn0.2O2 and graphite from spent batteries via efficient lithium supplementation and structural remodelling,Sustainable Energy & Fuels

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A closed-loop regeneration of LiNi0.6Co0.2Mn0.2O2 and graphite from spent batteries via efficient lithium supplementation and structural remodelling
Sustainable Energy & Fuels ( IF 5.0 ) Pub Date : 2021-08-20 , DOI: 10.1039/d1se01114f
Qinwen Zhou ₁ , Zixuan Huang ₁ , Jianwen Liu _{1,

2} , Yufeng Zhao ₃ , Joey Chung-Yen Jung ₃ , Jiujun Zhang ₃ , Shengming Xu ₄

Affiliation

The recycling and regeneration of spent lithium nickel cobalt manganese oxides (NCMs) are highly valued, due to the scarcity of raw materials and high cost of the synthetic process. Nevertheless, most current investigations are mainly focused on the recycling of NCMs with low nickel content (e.g. NCM111 or NCM 523), and there are hardly any reports on the corresponding research on high nickel NCMs. Herein, we report a novel closed-loop method to realize the simultaneous regeneration of LiNi_0.6Co_0.2Mn_0.2O₂ (NCM622) and graphite electrode materials from spent batteries. By adding an appropriate amount of lithium sources and designing a segmental calcination process, the depleted lithium in the spent NCM622 material is efficiently supplemented, and the collapsed structure of NCM622 is simultaneously remodelled. The spent graphite is also reconstructed by pretreatment and annealing at the same time. The regenerated NCM622 and graphite used in a new full cell deliver a reversible capacity of 151.4 mA h g⁻¹ after 100 cycles at 0.2C with a capacity retention of 95.6% and gradually improved coulombic efficiency, exhibiting battery performance comparable to that of new commercial batteries. The solid phase regeneration method proposed in this paper will provide strong support for the sustainable development of power lithium ion batteries, especially in industrial applications.

中文翻译：

通过有效的锂补充和结构重塑从废电池中闭环再生 LiNi0.6Co0.2Mn0.2O2 和石墨

由于原材料稀缺和合成过程成本高，废锂镍钴锰氧化物 (NCM) 的回收和再生受到高度重视。然而，目前大多数研究主要集中在低镍含量的NCMs （如NCM111或NCM 523）的回收利用，而对高镍NCMs的相应研究几乎没有报道。在此，我们报道了一种新的闭环方法来实现 LiNi _0.6 Co _0.2 Mn _0.2 O ₂的同步再生(NCM622) 和来自废电池的石墨电极材料。通过添加适量的锂源和设计分段煅烧工艺，有效补充废NCM622材料中耗尽的锂，同时重塑NCM622的坍塌结构。废石墨也通过预处理和退火同时进行再造。用于新型全电池的再生 NCM622 和石墨提供 151.4 mA hg ^-1的可逆容量0.2C循环100次后容量保持率为95.6%，库仑效率逐渐提高，电池性能可与新型商用电池相媲美。本文提出的固相再生方法将为动力锂离子电池的可持续发展，尤其是工业应用提供有力支持。

更新日期：2021-09-06

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