Material–electrolyte interfacial interaction enabling the formation of an inorganic-rich solid electrolyte interphase for fast-charging Si-based lithium-ion batteries

Cheng, Kai; Tu, Shuibin; Zhang, Bao; Wang, Wenyu; Wang, Xiaohong; Tan, Yucheng; Chen, Xiaoxue; Li, Chunhao; Li, Chenhui; Wang, Li; Sun, Yongming

doi:10.1039/d4ee00407h

Energy Environ. Sci.

2024

DOI: 10.1039/d4ee00407h

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Material–electrolyte interfacial interaction enabling the formation of an inorganic-rich solid electrolyte interphase for fast-charging Si-based lithium-ion batteries

Kai Cheng,

Shuibin Tu,

Bao Zhang

et al.

Abstract: Solid-electrolyte interphase (SEI) with high stability and high Li+ conductivity is highly desirable for Si-based lithium-ion batteries with high energy density and superior fast charging capability. Here, we proposed constructing...

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Cited by 6 publications

References 51 publications

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Element Screening Engineering for High‐Entropy Alloy Anodes: Achieving Fast and Robust Li‐Storage With Optimal Working Potential

Li,

Wang,

Yang

et al. 2024

Advanced Materials

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While the high‐entropy strategy is highly effective in enhancing the performance of materials across various fields, an optimal methodology for selecting component elements for performance optimization is still lacking. Here the findings on uncovering the element selection rules for rational design of high‐entropy alloy anodes with exceptional lithium storage performance are reported. It is investigated high‐entropy element screening rules by modifying stable diamond‐structured Ge with P to induce a tetrahedrally coordinated sphalerite structure for enhanced metallic conductivity, further stabilized by incorporating Zn and other elements. Moreover, both theoretical and experimental results confirm that Li‐storage performance improves with increasing atomic number: BZnGeP3 < AlZnGeP3 < GaZnGeP3 < InZnGeP3. InZnGeP3‐based electrodes demonstrate the highest Li‐ion affinity, fastest electronic and Li‐ion transport, largest Li‐storage capacity and reversibility, and best mechanical integrity. Further element screening based on the above criteria leads to high entropy alloy anodes with metallic conductivity like GaCuSnInZnGeP6, GaCu(or Sn)InZnGeP5, CuSnInZnGeP5, InZnGePSeS(or Te), InZnGeP2S(or Se) which show superior Li‐storage performances. The excellent phase stability is attributed to their high configurational entropy. This study offers profound insights into element screening for high‐entropy alloy‐based anodes in Li‐ion batteries, providing guidance and reference for the element combination and screening of other high‐entropy functional materials.

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Element Screening Engineering for High‐Entropy Alloy Anodes: Achieving Fast and Robust Li‐Storage With Optimal Working Potential

Li,

Wang,

Yang

et al. 2024

Advanced Materials

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Enhancing Rate Capability, Capacity, and Durability of Co‐Doped Germanium Phosphide Anodes for Li‐Ion Batteries

Li,

Wang,

Yen

et al. 2024

Advanced Energy Materials

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While germanium‐based anodes for Li‐ion batteries (LIBs) have potential to offer high energy density, their commercialization is impeded by low ionic and electronic conductivity and poor tolerance to volume change during cycling. Here a new quaternary CuGeSiP3 anode is reported to simultaneously overcome these limitations. Synthesized via ball milling process, CuGeSiP3 displays high ionic and electronic conductivity and excellent flexibility to accommodate volume change, attributed to increased structural entropy and reversible formation of favorable intermediates of both electronic and Li ion conductors, as confirmed by experimental measurements and theoretical calculations. When used as an LIB anode, CuGeSiP3 demonstrates large reversible capacity, high Coulombic efficiency, robust cycling stability, and high‐rate capability because it undergoes a reversible lithiation process that involves intercalation and conversion reaction. When composited with layered graphite, the electrode demonstrates exceptional cycling stability (1 261 mA h g−1 after 600 cycles at 400 mA g−1 and 861 mA h g−1 after 1 450 cycles at 20 00 mA g−1) and ultrahigh rate capability (448 mA h g−1 at 20 000 mA g−1). Further, the quaternary, pentanary, and hexanary cation‐disordered phosphides are also synthesized, all having similar Li‐storage superiority, implying the multiple co‐doping strategy is applicable to other material systems.

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Performance Degradation Mechanism of the Si@N, S‐Doped Carbon Anode in Sulfide‐Based All‐Solid‐State Batteries

Sun,

Ma,

Xin

et al. 2024

Small

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Silicon (Si) anode is a promising anode material for all‐solid‐state lithium batteries with ultra‐high theoretical specific capacity and low lithium dendrite risk. However, the inevitable vast volume expansion of Si anode during charge/discharge is recognized as a major limitation preventing its commercial application. Herein, an N, S self‐doped amorphous carbon layer coated on porous micron‐sized Si (p‐mSi@C) is designed to construct an electron/ion conducting network while ensuring structural and interfacial stability. Uneven distribution of von mises stresses during p‐mSi lithiation leads to irregular volume expansion and even fragmentation. Meanwhile, the growth of by‐products at the interface between p‐mSi and electrolyte contact leads to a rapid capacity decay. Compared to p‐mSi anode, p‐mSi@C reduces the risk of fragmentation thanks to the stress‐absorbing effect of amorphous carbon, delivering excellent electrochemical performance (2679.65 mAh g−1 at 0.2 mA cm−2 with initial coulombic efficiency of 84%). More importantly, the chemical failure mechanisms of p‐mSi and p‐mSi@C composite anodes are revealed through structural characterization, chemical analysis, and simulation, which provides the necessary theoretical guidance for practicalization.

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Material–electrolyte interfacial interaction enabling the formation of an inorganic-rich solid electrolyte interphase for fast-charging Si-based lithium-ion batteries

Abstract: Solid-electrolyte interphase (SEI) with high stability and high Li+ conductivity is highly desirable for Si-based lithium-ion batteries with high energy density and superior fast charging capability. Here, we proposed constructing...

Cited by 6 publications

References 51 publications

Element Screening Engineering for High‐Entropy Alloy Anodes: Achieving Fast and Robust Li‐Storage With Optimal Working Potential

Element Screening Engineering for High‐Entropy Alloy Anodes: Achieving Fast and Robust Li‐Storage With Optimal Working Potential

Enhancing Rate Capability, Capacity, and Durability of Co‐Doped Germanium Phosphide Anodes for Li‐Ion Batteries

Performance Degradation Mechanism of the Si@N, S‐Doped Carbon Anode in Sulfide‐Based All‐Solid‐State Batteries

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