Upcycling of spent LiCoO2/Graphite/Cu mixtures: Cu-doping with contrary gradient distribution towards high-rate and prolonged-cyclability

IF 18.9 1区 材料科学 Q1 CHEMISTRY, PHYSICAL
Hai Lei , Xinwei Cui , Jiexiang Li , Zihao Zeng , Chao Zhu , Xiaobo Ji , Wei Sun , Yue Yang , Peng Ge
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Abstract

Attracted by remarkable environmental/economic advantages, the direct regeneration of spent LiCoO2 (LCO) has been regarded as potential recycling method. However, limited by small-size and various designing-models, spent batteries are always industrially dismantled to obtain complex mixture, containing LCO, graphite, Cu-impurities, etc. Thus, exploring the synergetic effect of graphite removing and Cu-doping behaviors/threshold is crucial for the practical commercial production about spent mixture. Herein, spent mixtures are utilized to regenerate high-voltage LCO. Assisted by graphite self-heating and Li-vacancies, the doping-temperature and diffusion energy-barrier are lowering, facilitating Cu-atoms doping into bulk-phase. After optimizing Cu-content (0.7 wt.%), bulk-oriented doping at Li/Co sites is achieved with contrary gradient Cu-atoms distribution. Unique doping behaviors induce the evolution of morphology/lattice stability and the expanding of interlayer spacing. The as-optimized sample delivers a high capacity of 177.59 mAh g-1 at 0.2 C. Even at 5.0 C after 500 cycles, its capacity could reach up to 154.8 mAh g-1 with ∼82.4% retention. Supporting by electronic structure analysis, unique doping behaviors served as important roles in enhancing electronic conductivity and lowering O 2p band center. Given this, the work is expected to offer significant guidance of direct commercial regeneration, and shed light on the clear Cu-doping behaviors with threshold-value.

Abstract Image

Abstract Image

废旧钴酸锂(LiCoO2)/石墨/铜混合物的循环利用:以相反梯度分布掺入铜,实现高速率和长循环能力
废LiCoO2 (LCO)的直接再生因其显著的环境/经济优势而被认为是一种有潜力的回收方法。然而,由于废电池体积小,设计模型多,工业上往往将其拆解,得到复杂的混合物,其中含有LCO、石墨、cu杂质等。因此,探索石墨去除和cu掺杂行为/阈值的协同效应对于废混合料的实际商业化生产至关重要。在这里,废混合物被用来再生高压LCO。在石墨自热和锂空位的辅助下,掺杂温度和扩散能垒降低,有利于cu原子向体相掺杂。在优化cu含量(0.7 wt.%)后,在Li/Co位置实现了块体取向掺杂,并具有相反的梯度cu原子分布。独特的掺杂行为导致了形貌/晶格稳定性的演变和层间间距的扩大。优化后的样品在0.2℃下可提供177.59 mAh g-1的高容量,即使在5.0℃下循环500次,其容量也可达到154.8 mAh g-1,保留率为82.4%。电子结构分析表明,独特的掺杂行为对提高电子导电性和降低o2p带中心起着重要作用。因此,该工作有望为直接商业再生提供重要指导,并阐明具有阈值的cu掺杂行为。
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来源期刊
Energy Storage Materials
Energy Storage Materials Materials Science-General Materials Science
CiteScore
33.00
自引率
5.90%
发文量
652
审稿时长
27 days
期刊介绍: Energy Storage Materials is a global interdisciplinary journal dedicated to sharing scientific and technological advancements in materials and devices for advanced energy storage and related energy conversion, such as in metal-O2 batteries. The journal features comprehensive research articles, including full papers and short communications, as well as authoritative feature articles and reviews by leading experts in the field. Energy Storage Materials covers a wide range of topics, including the synthesis, fabrication, structure, properties, performance, and technological applications of energy storage materials. Additionally, the journal explores strategies, policies, and developments in the field of energy storage materials and devices for sustainable energy. Published papers are selected based on their scientific and technological significance, their ability to provide valuable new knowledge, and their relevance to the international research community.
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