Intrinsic lithium storage mechanisms and superior electrochemical behaviors of monodispersed hierarchical CoCO3 sub-microspheroids as a competitive anode towards Li-ion batteries
Intrinsic lithium storage mechanisms and superior electrochemical behaviors of monodispersed hierarchical CoCO3 sub-microspheroids as a competitive anode towards Li-ion batteries
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单分散分级 CoCO3 亚微球作为锂离子电池竞争性阳极的固有锂存储机制和优异的电化学行为
DOI：
10.1016/j.electacta.2019.03.171
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发表时间：
2019-06
期刊：
影响因子：
--
通讯作者：
Changzhou Yuan
中科院分区：
文献类型：
--
作者：
Zhiwei Zhao;Zhengluo Wang;Dienguila Kionga Denis;Xuan Sun;Jinyang Zhang;Linrui Hou;Xiaogang Zhang;Changzhou Yuan
近年来，CoCO 3作为锂离子电池负极材料，因其容量大、合成简单而受到广泛关注。然而，其适度的电化学行为和模糊的锂存储机制仍然需要很好地解决。在此，我们设计了一种可扩展的自下而上的溶剂热方法来制造单分散的松果状CoCO 3亚微球构建的纳米片亚单位。当作为LIB的有吸引力的阳极进行评估时，所得CoCO 3阳极表现出高达75.2%的初始库仑效率，以及在200 mA g − 1的速率下高达1008 mAh g− 1的大可逆容量，甚至在2 A g−1下高达663 mAh g−1，这有利于其分层的微米/纳米结构。此外，CoCO 3亚微球的界面电荷储存能力随着循环而增强，在500次连续循环中，其长期容量保持率为138%。更重要的是，全面的锂存储机制的CoCO 3，包括传统的转换反应，可逆的低价C/C（IV）的氧化还原反应，并首次观察到可逆的Co（II）/Co（III）的转变，提出了in-situandex-situphysical和电化学研究。此外，还组装了CoCO 3//LiNi0.8Co0.15Al0.05O2全电池，并提供了出色的电化学性能，极大地突出了我们的CoCO 3亚微球体在下一代LIB中作为竞争性阳极的巨大潜力。
Recently, CoCO3is attracting extensive interests as a promising anode for Li-ion batteries (LIBs) thanks to its large capacities and simple synthesis. However, its modest electrochemical behaviors and ambiguous lithium storage mechanisms still need to be well addressed. Herein, we devise a scalable bottom-up solvothermal methodology to fabricate monodispersed pinecone-like CoCO3sub-microspheroids constructed with nanosheet subunits. When evaluated as appealing anode for LIBs, the resultant CoCO3anode exhibits high initial Coulombic efficiency of ∼75.2%, and large reversible capacity of ∼1008 mAh g−1at a rate of 200 mA g−1, and even ∼663 mAh g−1at 2 A g−1, benefiting its hierarchical micro-/nanostructures. Besides, the enhanced interfacial charge-storage capability of the CoCO3sub-microspheroids with cycling accounts for the long-duration capacity retention of ∼138% over 500 consecutive cycles. More significantly, comprehensive lithium storage mechanism of the CoCO3, involving conventional conversion reactions, reversible redox reaction of low-valence C/C(IV), and debut observation of reversible Co(II)/Co(III) transition, is proposed within-situandex-situphysicochemical and electrochemical investigations. Furthermore, a CoCO3//LiNi0.8Co0.15Al0.05O2full battery is assembled and delivers prominent electrochemical properties, hugely highlighting the enormous potential of our CoCO3sub-microspheroids in next-generation LIBs as competitive anodes.
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