通过镍金属催化表面转化石墨晶体提高硬碳的电化学性能

Junsheng Yuan, Muxuan Li, Mengjing Jin, Yanting Wang, Guowen Sun, Jianqiao Song, Jinyuan Zhou, Xia Ni, Xiaojun Pan
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摘要

硬碳表面有丰富的微孔、无序石墨烯层、缺陷和各种可作为反应位点的官能团。然而,这些反应位点在电子和几何上都是非等价位点。因此,硬碳电极上形成的固体电解质界面(SEI)在有机电解质体系中表现出不稳定性,导致电解质中的 LiPF6 不断耗竭,从而影响其循环稳定性。在此,通过调节硬碳纤维的表面结构,诱导形成稳定的 SEI。利用过渡金属镍在高温下将硬碳纤维表面的无序结构转化为石墨结晶。这也减少了硬碳纤维表面的官能团、微孔、缺陷和无序石墨烯层,使活性位点等效。同时,高活性石墨烯边缘作为成核点均匀地暴露在纤维表面,从而诱导形成均匀致密的 SEI,抑制 LiPF6 的持续分解,从而提高硬碳的速率性能和循环稳定性。
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Enhanced Electrochemical Performances of Hard Carbon via Nickel‐Metal Catalyzed Surface Conversion Graphitic Crystallites
The surface of hard carbon is rich in micropores, disordered graphene layers, defects, and various functional groups that can serve as reactive sites. However, these reaction sites are non‐equivalent sites both electronically and geometrically. Consequently, the solid electrolyte interface (SEI) formed on the hard carbon electrode exhibits instability in the organic electrolyte system, resulting in a continuous depletion of LiPF6 within the electrolyte, thereby compromising its cycling stability. Herein, the formation of stable SEI is induced by modulating the surface structure of hard carbon fibers. The transition metal nickel is utilized to convert the disordered structure on the surface of hard carbon fibers into graphitic crystallites at high temperatures. This also reduces the functional groups, micropores, defects, and disordered graphene layers on the surface of the hard carbon fibers, making the active sites equiv. Meanwhile, the highly active graphene edges are uniformly exposed as nucleation sites on the fibers surface, which induces the formation of a uniform and dense SEI and inhibits the continuous decomposition of LiPF6, thus improving the rate performance and cycling stability of the hard carbon.
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