通过低温熔盐工艺与还原环境直接再生废磷酸铁锂,Industrial & Engineering Chemistry Research

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通过低温熔盐工艺与还原环境直接再生废磷酸铁锂
Industrial & Engineering Chemistry Research ( IF 3.8 ) Pub Date : 2022-03-08 , DOI: 10.1021/acs.iecr.1c05034
Xiang Liu _{1,

2} , Mengmeng Wang ₁ , Longping Deng _{1,

3} , Ya-Jun Cheng ₁ , Jie Gao ₁ , Yonggao Xia _{1,

4}

Affiliation

大量废旧锂离子电池（LIB）造成了资源浪费和环境污染等严重问题。磷酸铁锂（LFP）是废锂离子电池的主要正极材料之一。迫切需要开发一种安全、环保且具有成本竞争力的方法来再生从用过的 LIB 中收集的 LFP 正极。硝酸盐熔盐工艺已被用于再生层状阴极材料，但与 LFP 再生工艺不兼容。LFP 晶格将在熔盐过程中被氧化环境破坏，其中 Fe(II) 被氧化为 Fe(III)。在这项工作中提出了一种新方法来解决这个问题，其中低温熔盐工艺与还原环境相结合以抑制 Fe(II) 的氧化。具体而言，硝酸锂同时用作熔盐介质和锂源。蔗糖用作碳源以提供还原环境。通过在 300 °C 下进行短时间的熔盐再锂化步骤和在 650 °C 下进一步退火过程，可以成功回收具有缺锂和损坏结构的 LFP 颗粒。快速的锂补充过程暴露了更多的（101）晶面，促进了锂离子的传输。因此，再生 LFP 的比容量为 145 mAh g 可以成功回收具有缺锂和损坏结构的 LFP 颗粒。快速的锂补充过程暴露了更多的（101）晶面，促进了锂离子的传输。因此，再生 LFP 的比容量为 145 mAh g 可以成功回收具有缺锂和损坏结构的 LFP 颗粒。快速的锂补充过程暴露了更多的（101）晶面，促进了锂离子的传输。因此，再生 LFP 的比容量为 145 mAh g^{在 0.5C 时为–1}，相对于用过的 LFP 增加了 13% 以上，并且比在 5C 时的原始 LFP 具有更好的倍率性能。此外，我们还指出随着锂源的增加和处理时间的延长， LFP转化为Li ₃ PO _{4 。}这项工作为再生废 LFP 阴极提供了一种新的有前途的方法。

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Direct Regeneration of Spent Lithium Iron Phosphate via a Low-Temperature Molten Salt Process Coupled with a Reductive Environment

A huge number of spent lithium-ion batteries (LIBs) have caused serious problems such as resource waste and environmental pollution. Lithium iron phosphate (LFP) is one of the major cathode materials in the spent LIBs. It is urgently needed to develop a safe, environmentally friendly, and cost competitive approach to regenerate the LFP cathode collected from the spent LIBs. The nitrate molten salt process has been utilized to regenerate layered cathode materials, which are nevertheless non-compatible with the LFP regeneration process. The LFP crystal lattice will be destroyed during the molten salt process by the oxidative environment, where Fe(II) is oxidized to Fe(III). A new approach is proposed in this work to tackle this issue, where a low-temperature molten salt process is coupled with a reductive environment to suppress oxidation of Fe(II). In detail, lithium nitrate is used as a molten salt medium and lithium source simultaneously. Sucrose is used as a carbon source to provide a reductive environment. Through a short molten-salt relithiation step at 300 °C and further annealing process at 650 °C, LFP particles with a lithium-deficient and damaged structure can be successfully recovered. The rapid lithium replenishment process exposes more (101) crystal planes facilitating lithium-ion transportation. As a result, the regenerated LFP delivers a specific capacity of 145 mAh g^–1 at 0.5C, which is more than a 13% increase relative to the spent LFP and has a better rate performance than pristine LFP at 5C. In addition, we also point out that the LFP is converted to Li₃PO₄ with the increase in lithium source and the extension of treatment time. This work provides a new promising way to regenerate spent LFP cathodes.

更新日期：2022-03-08

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