The role of solvent during solvothermal synthesis of amorphous SiOx anode materials for advanced Li-ion batteries

IF 5.3 3区材料科学 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY

Materials Research Bulletin Pub Date : 2025-06-10 DOI:10.1016/j.materresbull.2025.113613

Alla A. Pustovalova , Anatolii V. Morozov , Nikita M. Polivara , Yury Y. Dikhtyar , Alexey I. Nedoluzhko , Egor M. Pazhetnov , Artem M. Abakumov

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Abstract

Non-stoichiometric SiO_x (0 < x < 1.5) is promising anode active material for next-generation lithium-ion batteries. This work reports the amorphous SiO_x preparation via solvothermal reduction of SiCl₄ by Mg in tetrahydrofuran (THF) or dimethoxyethane (DME) solvents followed by annealing. We provide insights into the synthesis mechanism and solvent role. MgCl₂ is readily dissolved in THF, but not in DME where MgCl₂ remains bound to SiO_x particles. Hydration of MgCl₂ contributes to the SiO_x oxidation degree during washing. Thus, the solvent ability to dissolve and eliminate MgCl₂ by-product during the synthesis affects the сhemical composition and properties of SiO_x. The SiO_x–THF is less oxidized during washing compared with the SiO_x–DME. The electrochemical properties of SiO_x materials depend on their stoichiometry, which may be adjusted by the solvent used in the synthesis. The O/Si ratio increase in SiO_x decreases the reversible capacity and initial Coulombic efficiency but improves the cycling stability.

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溶剂热法合成先进锂离子电池非晶SiOx负极材料中的作用

非化学计量SiOx (0 <；x & lt;1.5)是下一代锂离子电池极有前途的负极活性材料。本文报道了在四氢呋喃（THF）或二甲氧基乙烷（DME）溶剂中用Mg溶剂热还原SiCl4，然后退火制备无定形SiOx的方法。对其合成机理和溶剂作用进行了深入研究。MgCl2很容易溶解在THF中，但不溶于二甲醚，在二甲醚中MgCl2仍然与SiOx颗粒结合。在洗涤过程中，MgCl2的水化作用有助于SiOx氧化程度的提高。因此，溶剂在合成过程中溶解和消除副产物MgCl2的能力影响了SiOx的化学组成和性能。与SiOx-DME相比，SiOx-THF在洗涤过程中氧化较少。SiOx材料的电化学性能取决于它们的化学计量，这可以通过合成中使用的溶剂来调节。SiOx中O/Si比的增加降低了可逆容量和初始库仑效率，但提高了循环稳定性。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Materials Research Bulletin 工程技术-材料科学：综合

CiteScore

9.80

自引率

5.60%

发文量

372

审稿时长

42 days

期刊介绍： Materials Research Bulletin is an international journal reporting high-impact research on processing-structure-property relationships in functional materials and nanomaterials with interesting electronic, magnetic, optical, thermal, mechanical or catalytic properties. Papers purely on thermodynamics or theoretical calculations (e.g., density functional theory) do not fall within the scope of the journal unless they also demonstrate a clear link to physical properties. Topics covered include functional materials (e.g., dielectrics, pyroelectrics, piezoelectrics, ferroelectrics, relaxors, thermoelectrics, etc.); electrochemistry and solid-state ionics (e.g., photovoltaics, batteries, sensors, and fuel cells); nanomaterials, graphene, and nanocomposites; luminescence and photocatalysis; crystal-structure and defect-structure analysis; novel electronics; non-crystalline solids; flexible electronics; protein-material interactions; and polymeric ion-exchange membranes.