Fluoroethylene Carbonate Enabling a Robust LiF-rich Solid Electrolyte Interphase to Enhance the Stability of the MoS2 Anode for Lithium-Ion Storage

2018 ◽  
Vol 57 (14) ◽  
pp. 3656-3660 ◽  
Author(s):  
Zhiqiang Zhu ◽  
Yuxin Tang ◽  
Zhisheng Lv ◽  
Jiaqi Wei ◽  
Yanyan Zhang ◽  
...  
2018 ◽  
Vol 130 (14) ◽  
pp. 3718-3722 ◽  
Author(s):  
Zhiqiang Zhu ◽  
Yuxin Tang ◽  
Zhisheng Lv ◽  
Jiaqi Wei ◽  
Yanyan Zhang ◽  
...  

2016 ◽  
Vol 18 (12) ◽  
pp. 8643-8653 ◽  
Author(s):  
Yukihiro Okuno ◽  
Keisuke Ushirogata ◽  
Keitaro Sodeyama ◽  
Yoshitaka Tateyama

Additives in the electrolyte solution of lithium-ion batteries (LIBs) have a large impact on the performance of the solid electrolyte interphase (SEI) that forms on the anode and is a key to the stability and durability of LIBs.


2015 ◽  
Vol 27 (16) ◽  
pp. 5531-5542 ◽  
Author(s):  
Kjell Schroder ◽  
Judith Alvarado ◽  
Thomas A. Yersak ◽  
Juchuan Li ◽  
Nancy Dudney ◽  
...  

2019 ◽  
Author(s):  
Hezhen Xie ◽  
Sayed Youssef Sayed ◽  
W. Peter Kalisvaart ◽  
Simon Jakob Schaper ◽  
Peter Müller-Buschbaum ◽  
...  

<div>The formation of c-Li3.75Si is known to be detrimental to silicon anodes in lithium-ion batteries. To suppress the formation of this crystalline phase and improve the electrochemical performance of Sibased anodes, three approaches were amalgamated: addition of a nickel adhesion sublayer, alloying of the silicon with titanium, and the addition of either carbon or TiO2 as a capping layer. The silicon-based films were analyzed by a suite of methods, including scanning electron microscopy (SEM) and a variety of electrochemical methods, as well as X-ray photoelectron spectroscopy (XPS) to provide insights into the composition of the resulting solid electrolyte interphase (SEI). A nickel adhesion layer decreased the extent of delamination of the silicon from the underlying copper substrate, compared to Si deposited directly on Cu, which resulted in less capacity loss. Alloying of silicon with titanium (85% silicon, 15% titanium) further increased the stability. Finally, capping these multilayer electrodes with either a thin 10 nm layer of carbon or TiO2 resulted in the best electrode behavior, and lowest cumulative relative irreversible capacity. TiO2 is slightly more effective in enhancing the capacity retention, most likely due to differences in the resulting solid electrolyte interphase (SEI). The combination of an adhesion layer, alloying, and surface coatings shows a cumulative suppression of the formation of c-Li3.75Si and SEI, resulting in the greatest improvement of capacity retention when all three are incorporated together. However, these strategies appear to only delay the onset of the c-Li3.75Si phase; eventually, the c-Li3.75Si phase will form, and at that point, the rate of capacity degradation of all the electrodes becomes similar.</div>


2020 ◽  
Author(s):  
Nadia Intan ◽  
Jim Pfaendtner

The formation of a solid electrolyte interphase (SEI) at the electrode/electrolyte interface substantially affects the stability and lifetime of lithium-ion batteries (LIBs). One of the methods to improve the lifetime of LIBs is by the inclusion of additive molecules to stabilize the SEI. To understand the effect of additive molecules on the initial stage of SEI formation, we compare the decomposition and oligomerization reactions of a fluoroethylene carbonate (FEC) additive on a range of oxygen functionalized graphitic anode to those of an ethylene carbonate (EC) organic electrolyte. A series of density functional theory (DFT) calculations augmented by ab-initio molecular dynamics (AIMD) simulations reveal that EC decomposition on an oxygen functionalized graphitic (1120) edge facet through an SN2 mechanism is spontaneous, even in an uncharged cell. Decomposition of EC through an SN2 reaction pathway results in alkoxide species regeneration which is responsible for continual oligomerization along the graphitic surface. In contrast, FEC prefers to decompose through an SN1 pathway, which does not promote alkoxide regeneration. The ability of FEC as an additive to suppress alkoxide regeneration results in a smaller and thinner SEI layer that is more flexible towards lithium intercalation during the charging/discharging process. In addition, the presence of different oxygen functional groups at the surface of graphite dictates the oligomerization products and LiF formation in the SEI.


2019 ◽  
Author(s):  
Hezhen Xie ◽  
Sayed Youssef Sayed ◽  
W. Peter Kalisvaart ◽  
Simon Jakob Schaper ◽  
Peter Müller-Buschbaum ◽  
...  

<div>The formation of c-Li3.75Si is known to be detrimental to silicon anodes in lithium-ion batteries. To suppress the formation of this crystalline phase and improve the electrochemical performance of Sibased anodes, three approaches were amalgamated: addition of a nickel adhesion sublayer, alloying of the silicon with titanium, and the addition of either carbon or TiO2 as a capping layer. The silicon-based films were analyzed by a suite of methods, including scanning electron microscopy (SEM) and a variety of electrochemical methods, as well as X-ray photoelectron spectroscopy (XPS) to provide insights into the composition of the resulting solid electrolyte interphase (SEI). A nickel adhesion layer decreased the extent of delamination of the silicon from the underlying copper substrate, compared to Si deposited directly on Cu, which resulted in less capacity loss. Alloying of silicon with titanium (85% silicon, 15% titanium) further increased the stability. Finally, capping these multilayer electrodes with either a thin 10 nm layer of carbon or TiO2 resulted in the best electrode behavior, and lowest cumulative relative irreversible capacity. TiO2 is slightly more effective in enhancing the capacity retention, most likely due to differences in the resulting solid electrolyte interphase (SEI). The combination of an adhesion layer, alloying, and surface coatings shows a cumulative suppression of the formation of c-Li3.75Si and SEI, resulting in the greatest improvement of capacity retention when all three are incorporated together. However, these strategies appear to only delay the onset of the c-Li3.75Si phase; eventually, the c-Li3.75Si phase will form, and at that point, the rate of capacity degradation of all the electrodes becomes similar.</div>


2020 ◽  
Author(s):  
Nadia Intan ◽  
Jim Pfaendtner

The formation of a solid electrolyte interphase (SEI) at the electrode/electrolyte interface substantially affects the stability and lifetime of lithium-ion batteries (LIBs). One of the methods to improve the lifetime of LIBs is by the inclusion of additive molecules to stabilize the SEI. To understand the effect of additive molecules on the initial stage of SEI formation, we compare the decomposition and oligomerization reactions of a fluoroethylene carbonate (FEC) additive on a range of oxygen functionalized graphitic anode to those of an ethylene carbonate (EC) organic electrolyte. A series of density functional theory (DFT) calculations augmented by ab-initio molecular dynamics (AIMD) simulations reveal that EC decomposition on an oxygen functionalized graphitic (1120) edge facet through an SN2 mechanism is spontaneous, even in an uncharged cell. Decomposition of EC through an SN2 reaction pathway results in alkoxide species regeneration which is responsible for continual oligomerization along the graphitic surface. In contrast, FEC prefers to decompose through an SN1 pathway, which does not promote alkoxide regeneration. The ability of FEC as an additive to suppress alkoxide regeneration results in a smaller and thinner SEI layer that is more flexible towards lithium intercalation during the charging/discharging process. In addition, the presence of different oxygen functional groups at the surface of graphite dictates the oligomerization products and LiF formation in the SEI.


2021 ◽  
Vol 12 (1) ◽  
Author(s):  
Bing Han ◽  
Yucheng Zou ◽  
Zhen Zhang ◽  
Xuming Yang ◽  
Xiaobo Shi ◽  
...  

AbstractCryogenic transmission electron microscopy (cryo-TEM) is a valuable tool recently proposed to investigate battery electrodes. Despite being employed for Li-based battery materials, cryo-TEM measurements for Na-based electrochemical energy storage systems are not commonly reported. In particular, elucidating the chemical and morphological behavior of the Na-metal electrode in contact with a non-aqueous liquid electrolyte solution could provide useful insights that may lead to a better understanding of metal cells during operation. Here, using cryo-TEM, we investigate the effect of fluoroethylene carbonate (FEC) additive on the solid electrolyte interphase (SEI) structure of a Na-metal electrode. Without FEC, the NaPF6-containing carbonate-based electrolyte reacts with the metal electrode to produce an unstable SEI, rich in Na2CO3 and Na3PO4, which constantly consumes the sodium reservoir of the cell during cycling. When FEC is used, the Na-metal electrode forms a multilayer SEI structure comprising an outer NaF-rich amorphous phase and an inner Na3PO4 phase. This layered structure stabilizes the SEI and prevents further reactions between the electrolyte and the Na metal.


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