<p>Silicon (Si) is widely regarded as a highly attractive anode material for lithium-ion batteries (LIBs) because of its intrinsically high theoretical capacity; however, its practical implementation is severely hindered by large volume changes, mechanical instability, and limited charge-transport efficiency during repeated cycling. Alloying Si with metallic elements has been investigated as an effective strategy to mitigate these issues, yet conventional low-complexity alloys often fail to provide sufficient long-term stability. In this work, we introduce a high-entropy Si alloy (HESiA) anode concept based on equiatomic multi-element alloying, designed to fundamentally regulate Si lithiation behavior. The HESiA, consisting of multiple metallic elements homogeneously incorporated into a Si-rich matrix, is synthesized via a mechanical alloying process. Compared with single-element Si alloys, the high-entropy architecture enables more uniform stress distribution and improved electrochemical durability. To further enhance electronic connectivity and mechanical robustness, the HESiA is integrated with a hybrid reduced graphene oxide/carbon nanotube (rGO/CNT) conductive framework through a spray-drying process, forming a conformal carbon-encapsulated composite. Furthermore, graphite–HESiA composite electrodes demonstrate enhanced capacity utilization, improved rate performance, and stable cycling behavior compared with pristine graphite electrodes, while preserving structural integrity under high-rate operation. These results highlight that high-entropy alloying, combined with hierarchical carbon encapsulation, provides a versatile and potentially scalable materials-design strategy for overcoming the long-standing capacity–stability trade-off of Si anodes, offering a viable pathway toward next-generation high-energy-density LIBs.</p> Graphic abstract <p></p>

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Stabilizing silicon anodes via high-entropy alloying and hierarchical carbon encapsulation for high-performance lithium-ion batteries

  • Jung-Hyeok Park,
  • Byeong Guk Kim,
  • Jungdong Shin,
  • Jaeik Hyun,
  • Seung Yol Jeong,
  • Je In Lee,
  • Sunhye Yang,
  • Ki-Hun Nam

摘要

Silicon (Si) is widely regarded as a highly attractive anode material for lithium-ion batteries (LIBs) because of its intrinsically high theoretical capacity; however, its practical implementation is severely hindered by large volume changes, mechanical instability, and limited charge-transport efficiency during repeated cycling. Alloying Si with metallic elements has been investigated as an effective strategy to mitigate these issues, yet conventional low-complexity alloys often fail to provide sufficient long-term stability. In this work, we introduce a high-entropy Si alloy (HESiA) anode concept based on equiatomic multi-element alloying, designed to fundamentally regulate Si lithiation behavior. The HESiA, consisting of multiple metallic elements homogeneously incorporated into a Si-rich matrix, is synthesized via a mechanical alloying process. Compared with single-element Si alloys, the high-entropy architecture enables more uniform stress distribution and improved electrochemical durability. To further enhance electronic connectivity and mechanical robustness, the HESiA is integrated with a hybrid reduced graphene oxide/carbon nanotube (rGO/CNT) conductive framework through a spray-drying process, forming a conformal carbon-encapsulated composite. Furthermore, graphite–HESiA composite electrodes demonstrate enhanced capacity utilization, improved rate performance, and stable cycling behavior compared with pristine graphite electrodes, while preserving structural integrity under high-rate operation. These results highlight that high-entropy alloying, combined with hierarchical carbon encapsulation, provides a versatile and potentially scalable materials-design strategy for overcoming the long-standing capacity–stability trade-off of Si anodes, offering a viable pathway toward next-generation high-energy-density LIBs.

Graphic abstract