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3D ordered Mesoporous Si/C Sphere Arrays as High‐Volumetric‐Capacity and Durable Anode for Lithium‐ion Batteries

Qunyi WangThe Belt and Road Initiative Advanced Materials International Joint Research Center of Hebei Province School of Materials Science and Engineering Hebei University of Technology Tianjin 300130 ChinaYaduo JiaThe Belt and Road Initiative Advanced Materials International Joint Research Center of Hebei Province School of Materials Science and Engineering Hebei University of Technology Tianjin 300130 ChinaYutai WangThe Belt and Road Initiative Advanced Materials International Joint Research Center of Hebei Province School of Materials Science and Engineering Hebei University of Technology Tianjin 300130 ChinaPuguang JiWorld‐Class Research Center Advanced Digital Technologies State Marine Technical University Saint‐Petersburg 190121 RussiaChengwei ZhangThe Belt and Road Initiative Advanced Materials International Joint Research Center of Hebei Province School of Materials Science and Engineering Hebei University of Technology Tianjin 300130 ChinaHuiyang GouCenter for High Pressure Science and Technology Advanced Research Beijing 100094 ChinaMirtemir Shodievich KurbanovArifov Institute of Ion‐Plasma and Laser Technologies Academy of Sciences of the Republic of Uzbekistan Tashkent 100077 UzbekistanGongkai WangThe Belt and Road Initiative Advanced Materials International Joint Research Center of Hebei Province School of Materials Science and Engineering Hebei University of Technology Tianjin 300130 China
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ABI

Abstract

Abstract Micro‐nanostructured Si/C composites are recognized as promising anode materials for high‐performance lithium‐ion batteries (LIBs), but such anodes often result in suboptimal volumetric capacities. Herein, a novel 3D ordered mesoporous Si/N‐doped carbon (Si/NC) sphere array (M‐Si/NC‐SA) as the anode material is introduced. The M‐Si/NC‐SA anode is designed to address these challenges by combining high compacted density and a mesoporous structure that provides efficient pathways for electrolyte and Li + diffusion, while also accommodating the volume expansion of silicon during cycling. The mesopores within the Si/NC spheres and macropores between the spheres act as buffer zones, preventing pulverization and minimizing particle‐level expansion. The optimal M‐Si/NC‐SA demonstrates outstanding electrochemical performance, delivering a high compacted density of 0.78 mg cm −3 , an impressive volumetric capacity of 2275 mAh cm −3 at 0.1 A g −1 , and a capacity of 1011 mAh g −1 at 1 A g −1 after 1000 cycles. The full‐cells paired with lithium iron phosphate cathode can achieve practically relevant attributes. This work provides a kilogram‐scale method for producing high‐performance Si‐based anodes with enhanced volumetric capacity and superior cycling stability, offering a promising approach for next‐generation LIBs.

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