Effect of Dual‐Salt Concentrated Electrolytes on the Electrochemical Performance of Silicon Nanoparticles

Chang, Zenghua; Li, Xiang; Yun, Fengling; Shao, Zechao; Wu, Zhaohui; Wang, Jiantao; Lu, Shigang

doi:10.1002/celc.201901906

Cited by 20 publications

(19 citation statements)

References 69 publications

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“…The same group demonstrated a capacity of 2000 mAhg −1 after 100 cycles with an initial capacity of 3300 mAhg −1 , in a concentrated dual salt electrolyte composed of LiFSI and LiDFOB (lithium difluoro(oxalato)borate) in PC, also at room temperature. 40 Even though these various electrolytes cannot be compared directly to those investigated here, we can expect the continuous degradation of carbonate -based electrolytes in contact with the silicon surface to still occur and to be exacerbated at 50 °C. It is then possible that a slightly longer cycle life could be obtained with highly concentrated LiPF 6 in EC:DMC electrolyte compared to state of the art LP30.…”

Section: Resultsmentioning

confidence: 81%

Editors’ Choice—Understanding the Superior Cycling Performance of Si Anode in Highly Concentrated Phosphonium-Based Ionic Liquid Electrolyte

Araño

Mazouzi

Kerr

et al. 2020

J. Electrochem. Soc.

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Considerable effort has been devoted to improving the cyclability of silicon (Si) negative electrodes for lithium-ion batteries because it is a promising high specific capacity alternative to graphite. In this work, the electrochemical behaviour of Si in two ionic liquid (IL) electrolytes, triethyl(methyl)phosphonium bis(fluorosulfonyl)imide (P 1222 FSI) and N-propyl-Nmethylpyrrolidinium-FSI (C 3 mpyrFSI) with high and low lithium (Li) salt content is investigated at 50 °C. Results highlight that higher capacity and better cycling stability are achieved over 50 2 cycles with high salt concentration, the first time for a pyrrolidinium-based electrolyte in the area of Si negative electrodes. However, the Si cycling performance was far superior in the P 1222 FSIbased high salt content electrolyte compared to that of the C 3 mpyrFSI. To understand this unexpected result, diffusivity measurements of the IL-based electrolytes were performed using PFG-NMR, while their stability was probed using MAS-NMR and XPS after long-term cycling. A higher apparent transport number for Li ions in highly concentrated ILs, combined with a significantly lower extent of electrolyte degradation explains the superior cycle life of the highly concentrated phosphonium-based system. Si/concentrated P 1222 FSI-LiFSI/lithium nickel cobalt aluminum oxide (NCA) full cells with more than 3 mAh cm-2 nominal capacity deliver a promising cycle life and good rate capability.

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Section: Resultsmentioning

confidence: 81%

Editors’ Choice—Understanding the Superior Cycling Performance of Si Anode in Highly Concentrated Phosphonium-Based Ionic Liquid Electrolyte

Araño

Mazouzi

Kerr

et al. 2020

J. Electrochem. Soc.

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“…The strong band located at 720 cm −1 suggests that most of the FSI − anions remain at their free state. [ 19,22,23 ] By increasing the salt concentration to 3.0 m LiFSI/0.125 m LiDFOB in DME/FEC (3:1 by vol) (denoted as H‐DF), which is in consistence with the local salt concentration in N‐DHF, the corresponding peaks of the free solvent molecules got profoundly weakened. The new bands emerged at 839, 873 cm −1 and 739, 869 cm −1 are attributed to the coordinated DME and FEC molecules, respectively, indicating more solvent molecules have participated in the Li + solvation.…”

Section: Resultsmentioning

confidence: 99%

Electrolyte Design Enabling a High‐Safety and High‐Performance Si Anode with a Tailored Electrode–Electrolyte Interphase

et al. 2021

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Silicon (Si) anodes are advantageous for application in lithium‐ion batteries in terms of their high theoretical capacity (4200 mAh g−1), appropriate operating voltage (<0.4 V vs Li/Li+), and earth‐abundancy. Nevertheless, a large volume change of Si particles emerges with cycling, triggering unceasing breakage/re‐formation of the solid‐electrolyte interphase (SEI) and thereby the fast capacity degradation in traditional carbonate‐based electrolytes. Herein, it is demonstrated that superior cyclability of Si anode is achievable using a nonflammable ether‐based electrolyte with fluoroethylene carbonate and lithium oxalyldifluoroborate dual additives. By forming a high‐modulus SEI rich in fluoride (F) and boron (B) species, a high initial Coulombic efficiency of 90.2% is attained in Si/Li cells, accompanied with a low capacity‐fading rate of only 0.0615% per cycle (discharge capacity of 2041.9 mAh g−1 after 200 cycles). Full cells pairing the unmodified Si anode with commercial LiFePO4 (≈13.92 mg cm−2) and LiNi0.5Mn0.3Co0.2O2 (≈17.9 mg cm−2) cathodes further show extended service life to 150 and 60 cycles, respectively, demonstrating the superior cathode‐compatibility realized with a thin and F, B‐rich cathode electrolyte interface. This work offers an easily scalable approach in developing high‐performance Si‐based batteries through Si/electrolyte interphase regulation.

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“…Significant progress has been made via functional additives, highly concentrated electrolytes, Li salt, and solvent optimization to further improve the properties of SEI [161][162][163][164][165][166]. However, the lack of an SEI design principle for alloying anodes inhibits success.…”

Section: Design Of Electrolytesmentioning

confidence: 99%

The pursuit of commercial silicon-based microparticle anodes for advanced lithium-ion batteries: A review

Liu

et al. 2022

Nano Research Energy

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Silicon (Si) is one of the most promising anode materials for high-energy lithium-ion batteries. However, the widespread application of Si-based anodes is inhibited by large volume change, unstable solid electrolyte interphase, and poor electrical conductivity. During the past decade, significant efforts have been made to overcome these major challenges toward industrial applications. This review summarizes the recent development of microscale Si-based electrodes fabricated by Si microparticles or other industrial bulk materials from the perspective of industrialization. First, the challenges for microscale Si anodes are clarified. Second, structural design strategies of stable micro-sized Si materials are discussed. Third, other critical practical metrics, such as robust binder construction and electrolyte design, are also highlighted. Finally, future trends and perspectives on the commercialization of Si-based anodes are provided. KEYWORDSsilicon, micro-sized particles, lithium-ion batteries, porous structures, polymer binder, electrolyte design Figure 1 Overview of Si-based anodes for LIBs: (a) merits and (b) fundamental challenges. Reproduced with permission from Ref. [16], © Wiley-VCH GmbH 2021.

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Effect of Dual‐Salt Concentrated Electrolytes on the Electrochemical Performance of Silicon Nanoparticles

Cited by 20 publications

References 69 publications

Editors’ Choice—Understanding the Superior Cycling Performance of Si Anode in Highly Concentrated Phosphonium-Based Ionic Liquid Electrolyte

Editors’ Choice—Understanding the Superior Cycling Performance of Si Anode in Highly Concentrated Phosphonium-Based Ionic Liquid Electrolyte

Electrolyte Design Enabling a High‐Safety and High‐Performance Si Anode with a Tailored Electrode–Electrolyte Interphase

The pursuit of commercial silicon-based microparticle anodes for advanced lithium-ion batteries: A review

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