A promising regeneration of waste carbon residue from spent Lithium-ion batteries via low-temperature fluorination roasting and water leaching
A promising regeneration of waste carbon residue from spent Lithium-ion batteries via low-temperature fluorination roasting and water leaching
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通过低温氟化焙烧和水浸法再生废旧锂离子电池废碳渣的前景广阔
DOI：
10.1016/j.cej.2021.132703
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发表时间：
2022-02
影响因子：
15.1
通讯作者：
Qifan Zhong
中科院分区：
文献类型：
--
作者：
Zhu Xiangdong;Jin Xiao;Qiuyun Mao;Zhenhua Zhang;You Zihan;Lei Tang;Qifan Zhong
摘要废旧锂离子电池残炭的回收利用对环境保护和经济发展具有重要意义。然而，目前国内外对西铁再生的研究报道较少。为此，提出了一种新的环保工艺-低温焙烧-水浸工艺，以实现对废铬渣的最佳净化。采用DFTB研究了水溶性络合离子在焙烧过程中的转化机理，表明NH 4F中的F与NH 4基团的离子键断裂，而与金属离子形成稳定的共价键。该工艺在最佳条件下，可去除WCR中99.59%、99.54%、99.82%、96.38%、98.41%、97.28%、99.23%和98.61%的钴、镍、锰、铝、硅、铁、锂和硫。同时，获得了纯度为99.98%的高纯石墨炭（PGC）产品。特别地，半电池中的PGC表现出340.9mAh/g的稳定比容量和92.13%的高ICE，并且在1C下100次循环后具有大于96%的容量保持率，比WCR好得多，并且与商业石墨相似。在0.2C倍率下，PGC的全电池放电容量为2302.82 mAh，ICE为87.3%。在1C/1C倍率下循环400次后，容量保持率保持在96%。然后用氨水作沉淀剂回收浸出液中的有价组分。Al、Co、Mn、Ni和Si的析出率分别为99.25%、81.74%、98.20%、62.43%和86.68%。此外，废气被含氟浸出液吸收，蒸发结晶回收氟化铵产品。该工艺具有循环经济和绿色化学的特点，有望在回收有价值组分的同时，应用于水氯再生。
Abstract Recycling and reusing the waste carbon residue (WCR) from spent lithium-ion batteries has substantial significance in environmental protection and economic growth. Nevertheless, research on the regeneration of WCR was seldom reported. Herein, a new environmentally friendly process of low-temperature fluorination roasting and water leaching technology were proposed to achieve optimal purification of WCR. And the transformation mechanism of water-soluble complex ions during fluorination roasting was investigated via DFTB indicating that the ionic bond of F and NH4 group in NH4F broken than form stable covalent bond with metal ions. This process showed that 99.59%, 99.54%, 99.82%, 96.38%, 98.41%, 97.28%, 99.23%, and 98.61% of cobalt, nickel, manganese, aluminum, silicon, iron, lithium, and sulfur in WCR could be removed under optimal conditions. Meanwhile, the high-purity graphite carbon (PGC) products with purity of 99.98% were obtained. In particular, PGC in half-cell exhibited a stable specific capacity of 340.9 mAh/g and high ICE of 92.13%, and with a more than 96% capacity retention after 100 cycles at 1C, much better performance than WCR and similarly to commercial graphite. Moreover, the discharge capacity of PGC in full-cell was 2302.82 mAh at 0.2C rate with 87.3% ICE. The capacity retention maintained at 96% after 400 cycles at 1C/1C rate. Subsequently, the valuable components in leaching solution were recovered with ammonia as precipitant. The precipitation rates of Al, Co, Mn, Ni, and Si were 99.25%, 81.74%, 98.20%, 62.43% and 86.68%, respectively. Besides, exhaust gas was absorbed in fluorine-containing leachate for recovery of ammonium fluoride products by evaporation crystallization. This proposed process with circular economy and green chemistry characteristics is expected to be employed in the regeneration of WCR while recovering valuable components.
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影响因子：
10.8
作者：
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通讯作者：
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影响因子：
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作者：
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作者：
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通讯作者：
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影响因子：
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作者：
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通讯作者：
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影响因子：
4.5
作者：
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