In Situ AFM Imaging of Solid Electrolyte Interfaces on HOPG with Ethylene Carbonate and Fluoroethylene Carbonate-Based Electrolytes

2015 ◽  
Vol 7 (45) ◽  
pp. 25441-25447 ◽  
Author(s):  
Cai Shen ◽  
Shuwei Wang ◽  
Yan Jin ◽  
Wei-Qiang Han
2017 ◽  
Vol 10 (05) ◽  
pp. 1750052 ◽  
Author(s):  
Lingpiao Lin ◽  
Kai Yang ◽  
Haibiao Chen ◽  
Feng Pan

We used in situ atomic force microscope to observe the evolution of the solid-electrolyte interphase (SEI) layer on the graphite surface during the initial lithium intercalation process. We found that 1% vinylene carbonate (VC) in the electrolyte can promote the formation of an initial SEI at a higher potential by VC reduction. VC also restrained the reduction of ethylene carbonate (EC) and as a consequence, it can affect the morphology of the SEI formed.


2020 ◽  
Vol 8 (35) ◽  
pp. 18388-18388
Author(s):  
Anna B. Gunnarsdóttir ◽  
Sundeep Vema ◽  
Svetlana Menkin ◽  
Lauren E. Marbella ◽  
Clare P. Grey

Correction for ‘Investigating the effect of a fluoroethylene carbonate additive on lithium deposition and the solid electrolyte interphase in lithium metal batteries using in situ NMR spectroscopy’ by Anna B. Gunnarsdóttir et al., J. Mater. Chem. A, 2020, 8, 14975–14992, DOI: 10.1039/D0TA05652A


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.


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):  
Wei Guo ◽  
Wanying Zhang ◽  
Yubing Si ◽  
Donghai Wang ◽  
Yongzhu Fu ◽  
...  

AbstractThe interfacial instability of the lithium-metal anode and shuttling of lithium polysulfides in lithium-sulfur (Li-S) batteries hinder the commercial application. Herein, we report a bifunctional electrolyte additive, i.e., 1,3,5-benzenetrithiol (BTT), which is used to construct solid-electrolyte interfaces (SEIs) on both electrodes from in situ organothiol transformation. BTT reacts with lithium metal to form lithium 1,3,5-benzenetrithiolate depositing on the anode surface, enabling reversible lithium deposition/stripping. BTT also reacts with sulfur to form an oligomer/polymer SEI covering the cathode surface, reducing the dissolution and shuttling of lithium polysulfides. The Li–S cell with BTT delivers a specific discharge capacity of 1,239 mAh g−1 (based on sulfur), and high cycling stability of over 300 cycles at 1C rate. A Li–S pouch cell with BTT is also evaluated to prove the concept. This study constructs an ingenious interface reaction based on bond chemistry, aiming to solve the inherent problems of Li–S batteries.


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