Analysis of the Sulfur Cathode Capacity Fading Mechanism and Review of the Latest Development for Li-S Battery

Diao, Yan; Xie, Kai; Hong, Xiaobin; Xiong, Shizhao

doi:10.6023/a12121024

Cited by 26 publications

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“…The long-chain lithium polysulfi des such as Li 2 S 8 and Li 2 S 6 are highly dissoluble in ether-based electrolytes, which can cause rapid capacity fading during cell cycling. The conversion from Li 2 S 4 to Li 2 S and/or the redeposition of Li 2 S from polysulfi des in the electrolyte takes place in the voltage range between ≈2.2 and 1.7 V. [39][40][41][42][43][44][45][46][47][48] The capacity at this stage (≈75% of the total capacity) is relatively stable as the short-chain lithium polysulfi des have low solubility in the electrolyte. Therefore, we take two approaches to achieve long cycle-life Li/S cells: one is increasing the number of active sites for redepositing Li 2 S from polysulfi des in the electrolyte (see Figure 3 d), the other is limiting the charge voltage range for inhibiting the dissolution of longchain lithium polysulfi des in the electrolyte.…”

Section: Shown Inmentioning

confidence: 99%

“…The long‐chain lithium polysulfides such as Li 2 S 8 and Li 2 S 6 are highly dissoluble in ether‐based electrolytes, which can cause rapid capacity fading during cell cycling. The conversion from Li 2 S 4 to Li 2 S and/or the redeposition of Li 2 S from polysulfides in the electrolyte takes place in the voltage range between ≈2.2 and 1.7 V . The capacity at this stage (≈75% of the total capacity) is relatively stable as the short‐chain lithium polysulfides have low solubility in the electrolyte.…”

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confidence: 99%

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Highly Nitridated Graphene–Li₂S Cathodes with Stable Modulated Cycles

Qiu

Rong

Yang

et al. 2015

Advanced Energy Materials

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an effective strategy for the redeposition of lithium polysulfi des due to their affi nities for these materials, which leads to significant improvement of corresponding Li/S cells.Li 2 S is a promising prelithiated cathode material with a high theoretical capacity of 1166 mA h g −1 . Unlike conventional sulfur cathode, Li 2 S cathode shrinks as it delithiates initially, producing voids for subsequent lithiation/delithiation cycling, hence protecting the electrode structure from damage. More importantly, Li 2 S can be matched with lithium metal-free anodes (such as silicon and tin), thus eliminating serious safety issues associated with the formation of "dendrites." Despite of these merits, the performance of Li 2 S-based cathode significantly lags behind its sulfur counterpart. [ 9,10,30,31 ] A key issue for the Li 2 S material seems to be in its ineffi cient activation and redeposition process. [ 32,33 ] To understand the actual electrochemical activation processes, we fi rst developed in situ scanning electron microscopy (SEM) and transmission electron microscopy (TEM) techniques to study the cathode material structural changes on delithiation. The newly developed in situ SEM set-up is shown in Figure 1 a,b. A liquid cell contains one electrode with graphene and Li 2 S particles on a 50 nm thick SiN x window, and the other electrode with Li metal on Cu foil. The cell is fi lled by a liquid electrolyte (see the Experimental Section). When charged at 3.5 V, the conversion reaction from Li 2 S to polysulfi des occurs fi rst at their surfaces (Figure 1 c and Figure S1 and Movie 1, Supporting Information). We see that the Li 2 S particles on graphene become smaller and smaller upon charging due to gradual dissolution of lithium polysulfi des into the electrolyte. The phenomenon is also supported by in situ Raman spectroscopy (see Figure S2, Supporting Information). The observed phenomenon could be explained by that Li 2 S was chemically converted to soluble lithium polysulfi des upon charging. The process was further examined by in situ TEM study. A newly designed in situ TEM microchip (Figure 1 d) was fabricated and schematically shown in Figure 1 e. The main part is an Au wire, of which one end was connected to one electrode of the chip by silver paste, and the other end was glued with the graphene− Li 2 S sample. The surface of the other electrode of the chip was deposited by Li metal. The graphene−Li 2 S sample and Li metal were connected via an ionic liquid electrolyte. When charged at 3.5 V, Li 2 S particles encapsulated in the graphene gradually disappeared (Figure 1 f and Movie 2, Supporting Information). The processes could be explained by the dissolution of the generated lithium polysulfi des in the ionic liquid electrolyte. The observed The development of high-capacity cathode materials is critical for applications such as mobile devices and electric vehicles. Li/S batteries represent a promising system based on sulfurconductive additive composite as the cathode. [1][2][3][4][5] However, various factors ...

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Section: Shown Inmentioning

confidence: 99%

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Highly Nitridated Graphene–Li₂S Cathodes with Stable Modulated Cycles

Qiu

Rong

Yang

et al. 2015

Advanced Energy Materials

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“…If the soluble polysulfide diffuses outside of the cathode region, it would not be recycled, lead-ing to a permanent decline in capacity. Basically, the shuttle process of the soluble polysulfides lead to a severe decrease in LSB performance [45,46]. The delay in liquid-to-liquid polysulfide conversion would result in its accumulation in the electrolyte and the subsequent shuttle effect.…”

Section: Intermediator Conversion Reaction Between Long-chain and Shomentioning

confidence: 99%

Catalyzing the polysulfide conversion for promoting lithium sulfur battery performances: A review

Niu

Guo

et al. 2021

Journal of Energy Chemistry

166

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“…S 8 ?Li 2 S 2 /Li 2 S. However, the conversion process of active sulfur materials is not strictly following the above equation step by step, and the specific reaction is more complicated. For instance, longchain lithium polysulfide can not only react with metal lithium, but also react with insoluble Li 2 S 2 and Li 2 S, as well as the lithium polysulfide will undergo a disproportionation reaction [6]. The long-chain lithium polysulfide generated by the cathode diffuses to metal lithium anode due to the existence of concentration gradient and reacts with metal lithium, forming low-order lithium polysulfide.…”

Section: Introductionmentioning

confidence: 99%

A review on electronically conducting polymers for lithium-sulfur battery and lithium-selenium battery: Progress and prospects

Xiang

Deng

Zhao

et al. 2021

Journal of Energy Chemistry

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Analysis of the Sulfur Cathode Capacity Fading Mechanism and Review of the Latest Development for Li-S Battery

Cited by 26 publications

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Highly Nitridated Graphene–Li₂S Cathodes with Stable Modulated Cycles

Highly Nitridated Graphene–Li₂S Cathodes with Stable Modulated Cycles

Catalyzing the polysulfide conversion for promoting lithium sulfur battery performances: A review

A review on electronically conducting polymers for lithium-sulfur battery and lithium-selenium battery: Progress and prospects

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Analysis of the Sulfur Cathode Capacity Fading Mechanism and Review of the Latest Development for Li-S Battery

Cited by 26 publications

References 0 publications

Highly Nitridated Graphene–Li2S Cathodes with Stable Modulated Cycles

Highly Nitridated Graphene–Li2S Cathodes with Stable Modulated Cycles

Catalyzing the polysulfide conversion for promoting lithium sulfur battery performances: A review

A review on electronically conducting polymers for lithium-sulfur battery and lithium-selenium battery: Progress and prospects

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Product

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Highly Nitridated Graphene–Li₂S Cathodes with Stable Modulated Cycles

Highly Nitridated Graphene–Li₂S Cathodes with Stable Modulated Cycles