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Pentafluorophenyl Isocyanate as an Effective Electrolyte Additive for Improved Performance of Silicon-Based Lithium-Ion Full Cells
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2018-07-25 00:00:00 , DOI: 10.1021/acsami.8b07683 Roman Nölle 1 , Andreas J. Achazi 2 , Payam Kaghazchi 2, 3 , Martin Winter 1, 4 , Tobias Placke 1
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2018-07-25 00:00:00 , DOI: 10.1021/acsami.8b07683 Roman Nölle 1 , Andreas J. Achazi 2 , Payam Kaghazchi 2, 3 , Martin Winter 1, 4 , Tobias Placke 1
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Due to its high specific and volumetric capacity and relatively low operation potential, silicon (Si) has attracted much attention to be utilized as a high-capacity anode material for lithium-ion batteries (LIBs) with increased energy density. However, the application of Si within commercial LIBs is still hindered by its poor cycling stability related to the huge volume changes of Si upon lithiation/delithiation, followed by continuous electrolyte decomposition and active lithium loss at the anode side. In this work, we present the application of pentafluorophenyl isocyanate (PFPI) as an effective electrolyte additive for lithium-ion full cells, containing a pure, magnetron-sputtered Si anode and a LiNi1/3Mn1/3Co1/3O2 (NMC-111) cathode. The performance of the Si/NMC-111 full cells is significantly improved in terms of capacity retention and Coulombic efficiency by the addition of 2 wt % PFPI to the baseline electrolyte and is compared to the well-known additives vinylene carbonate and fluoroethylene carbonate. Furthermore, it is revealed that the additive is able to reduce the active lithium losses by forming an effective solid–electrolyte interphase (SEI) on the Si anode. X-ray photoelectron spectroscopy investigations unveil that PFPI is a main part of the SEI layer, leading to less active lithium immobilized within the interphase. Overall, our results pave the path for a broad range of different isocyanate compounds, which have not been studied for Si-based anodes in lithium-ion full cells so far. These compounds can be easily adjusted by modifying the chemical structure and/or functional groups incorporated within the molecule, to specifically tailor the SEI layer for Si-based anodes in LIBs.
中文翻译：
五氟苯基异氰酸酯作为一种有效的电解质添加剂，可改善硅基锂离子完整电池的性能
由于其高的比容量和体积容量以及相对较低的工作电势，硅（Si）备受关注，被用作能量密度更高的锂离子电池（LIB）的高容量阳极材料。然而，Si在商业LIB中的应用仍然受到其循环稳定性差的阻碍，该循环稳定性与锂在锂化/脱锂时的巨大体积变化有关，随后在阳极侧连续电解质分解和活性锂损失。在这项工作中，我们介绍了五氟苯基异氰酸酯（PFPI）作为锂离子满电池的有效电解质添加剂的应用，其中包含纯的磁控溅射Si阳极和LiNi 1/3 Mn 1/3 Co 1/3 O 2个（NMC-111）阴极。通过在基线电解液中添加2 wt％PFPI，可在容量保持和库仑效率方面显着改善Si / NMC-111全电池的性能，并且与众所周知的碳酸亚乙烯酯和碳酸氟亚乙酯相比，Si / NMC-111全电池的性能得到了改善。此外，发现该添加剂能够通过在Si阳极上形成有效的固体电解质中间相（SEI）来减少活性锂的损失。X射线光电子能谱研究表明，PFPI是SEI层的主要部分，导致固定在相间的活性锂降低。总体而言，我们的结果为各种不同的异氰酸酯化合物铺平了道路，到目前为止，尚未针对锂离子满电池中的硅基阳极进行过研究。
更新日期：2018-07-25
中文翻译：
五氟苯基异氰酸酯作为一种有效的电解质添加剂，可改善硅基锂离子完整电池的性能
由于其高的比容量和体积容量以及相对较低的工作电势，硅（Si）备受关注，被用作能量密度更高的锂离子电池（LIB）的高容量阳极材料。然而，Si在商业LIB中的应用仍然受到其循环稳定性差的阻碍，该循环稳定性与锂在锂化/脱锂时的巨大体积变化有关，随后在阳极侧连续电解质分解和活性锂损失。在这项工作中，我们介绍了五氟苯基异氰酸酯（PFPI）作为锂离子满电池的有效电解质添加剂的应用，其中包含纯的磁控溅射Si阳极和LiNi 1/3 Mn 1/3 Co 1/3 O 2个（NMC-111）阴极。通过在基线电解液中添加2 wt％PFPI，可在容量保持和库仑效率方面显着改善Si / NMC-111全电池的性能，并且与众所周知的碳酸亚乙烯酯和碳酸氟亚乙酯相比，Si / NMC-111全电池的性能得到了改善。此外，发现该添加剂能够通过在Si阳极上形成有效的固体电解质中间相（SEI）来减少活性锂的损失。X射线光电子能谱研究表明，PFPI是SEI层的主要部分，导致固定在相间的活性锂降低。总体而言，我们的结果为各种不同的异氰酸酯化合物铺平了道路，到目前为止，尚未针对锂离子满电池中的硅基阳极进行过研究。
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