As a promising lithium‐ion battery anode materials, silicon suboxides (SiO_x) exhibit elusive microstructure with atomic‐scale disproportionation which reveals a strong relation to performance. Generally, the structure of SiO_x could be tuned via high‐temperature treatment. In this work, disproportionated SiO_x are prepared to systematically discuss the internal relationship among microstructure, physicochemical properties and electrochemical performance. After annealing, amorphous SiO₂ and nanocrystalline Si appear, and the SiO₂ accumulating on the surface results in large resistance and low Li‐ion diffusivity, which leads to large overpotential and poor performance. If mechanical milling is employed followed by annealing, the SiO₂ layer can be crushed, SiO_x and Si with electrochemical activity are uncovered. Further research on the SiO_x with diverse degrees of disproportionation indicates that proper amount of Si and SiO₂ determines the optimal electrochemical performance. This result gives an in‐depth understanding and probable guidance to the modification investigation of SiO_x anode for Li‐ion batteries.

中文翻译：

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揭示表面和本体结构对歧化SiOx阳极电化学性能的影响

作为一种有前途的锂离子电池负极材料，次氧化硅（SiO _x）表现出难以捉摸的微观结构，且原子级歧化，这与性能密切相关。通常，可以通过高温处理来调整SiO _x的结构。在这项工作中，制备歧化的SiO _x以便系统地讨论微观结构，理化性质和电化学性能之间的内部关系。退火后，出现无定形SiO ₂和纳米晶Si，且SiO ₂积聚在表面上会导致较大的电阻和较低的锂离子扩散率，从而导致较大的超电势和较差的性能。如果采用机械研磨然后退火，则可以将SiO ₂层压碎，发现具有电化学活性的SiO _x和Si。对具有不同歧化度的SiO _x的进一步研究表明，适量的Si和SiO ₂决定了最佳的电化学性能。该结果为锂离子电池用SiO _x阳极的改性研究提供了深入的理解和可能的指导。