Chemically tailoring the nanostructure of graphenenanosheets to confine sulfur for high-performance lithium-sulfur batteries

Ding, Bing; Yuan, Changzhou; Shen, Laifa; Xu, Guiyin; Nie, Ping; Lai, Qingxue; Zhang, Xiaogang

doi:10.1039/c2ta00396a

Cited by 183 publications

(129 citation statements)

References 42 publications

(52 reference statements)

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“…Thus, one of the main mechanisms for capacity fade is associated with the shuttling process. Consequently, devising ways to prevent the polysulfide shuttling process through the use of additives, 19 modification of the cathode structure, [20][21][22][23][24][25][26][27][28][29][30][31][32] modification of the electrolyte, 33,34 and by other methods [35][36][37] has been the focus of the recent research efforts in the area of lithium-sulfur batteries.…”

Section: Summary Of Technical Challenges With Lithium-sulfur Batteries-mentioning

confidence: 99%

Direct Measurement of Polysulfide Shuttle Current: A Window into Understanding the Performance of Lithium-Sulfur Cells

Moy

Manivannan

Narayanan

2014

J. Electrochem. Soc.

234

232

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The shuttling of polysulfide ions between the electrodes in a lithium-sulfur battery is a major technical issue limiting the self-discharge and cycle life of this high-energy rechargeable battery. Although there have been attempts to suppress the shuttling process, there has not been a direct measurement of the rate of shuttling. We report here a simple and direct measurement of the rate of the shuttling (that we term "shuttle current"), applicable to the study of any type of lithium-sulfur cell. We demonstrate the effectiveness of this measurement technique using cells with and without lithium nitrate (a widely-used shuttle suppressor additive). We present a phenomenological analysis of the shuttling process and simulate the shuttle currents as a function of the state-of-charge of a cell. We also demonstrate how the rate of decay of the shuttle current can be used to predict the capacity fade in a lithium-sulfur cell due to the shuttle process. We expect that this new ability to directly measure shuttle currents will provide greater insight into the performance differences observed with various additives and electrode modifications that are aimed at suppressing the rate of shuttling of polysulfide ions and increasing the cycle life of lithium-sulfur cells. The rechargeable lithium-sulfur battery is of great interest due to its high theoretical specific energy of 2600 Wh/kg and also the relatively low cost of sulfur. However, large-scale deployment of lithium-sulfur batteries has been limited by several performance issues relating to power density and cycle life. [1][2][3][4][5][6][7][8][9] With sulfur at the positive electrode and lithium metal at the negative electrode, the lithium-sulfur battery operates over a voltage range of 1.5 to 2.8 V. The reactions at the positive and negative electrode during charge and discharge are shown schematically in Figure 1. During discharge, sulfur at the positive electrode is reduced progressively to various polysulfides and eventually to the sulfide, while lithium metal at the negative electrode is oxidized to lithium ions. During charge, the lithium ions are reduced to lithium at the negative electrode, and the sulfide is re-oxidized at the positive electrode to the higher-order polysulfides. The organic electrolyte is a 0.5 M solution of lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) in a 1:1 mixture by volume of dioxolane (DOL) and dimethoxyethane (DME). A "solid electrolyte interphase" (SEI) protects the lithium anode from reacting freely with the organic electrolyte. The polysulfides produced during discharge are usually soluble in the battery electrolyte. Summary of technical challenges with lithium-sulfur batteries.-The principal challenge for the realization of a practical lithium-sulfur battery with long cycle life arises from the solubility of the higherorder polysulfides (S 8 2− , S 6 2− , S 4 2− ) in the electrolyte. These polysulfides, generated at the positive electrode during discharge, diffuse to the negative lithium electrode where they are reduced to...

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Section: Summary Of Technical Challenges With Lithium-sulfur Batteries-mentioning

confidence: 99%

Direct Measurement of Polysulfide Shuttle Current: A Window into Understanding the Performance of Lithium-Sulfur Cells

Moy

Manivannan

Narayanan

2014

J. Electrochem. Soc.

234

232

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“…6 shows the CV curves of S/PPy cathode between 1.5 V and 3 V vs. Li þ /Li for initial two cycles at a scan rate of 0.1 mV s À1 . The sharp redox peaks with stable overlapping features confirm high reversibility and an excellent stability of the composite electrode upon operation in lithium battery [28]. In the cathodic (reduction) sweep, the peaks at 2.4 and 2.0 V can be observed, which are assigned to the reduction of element sulfur (S 8 ) to soluble lithium polysulfides (Li 2 S n , 4 n 8) and further conversion of these lithium polysulfides into insoluble Li 2 S 2 and Li 2 S, respectively [29].…”

Section: Resultsmentioning

confidence: 85%

Well-dispersed sulfur anchored on interconnected polypyrrole nanofiber network as high performance cathode for lithium-sulfur batteries

Yin

Liu

Zhang

et al. 2017

Solid State Sciences

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a b s t r a c tPreparation of novel sulfur/polypyrrole (S/PPy) composite consisting well-dispersed sulfur particles anchored on interconnected PPy nanowire network was demonstrated. In such hybrid structure, the asprepared PPy clearly displays a three-dimensionally cross-linked and hierarchical porous structure, which was utilized in the composite cathode as a conductive network trapping soluble polysulfide intermediates and enhancing the overall electrochemical performance of the system. Benefiting from this unique structure, the S/PPy composite demonstrated excellent cycling stability, resulting in a discharge capacity of 931 mAh g À1 at the second cycle and retained about 54% of this value over 100 cycles at 0.1 C. Furthermore, the S/PPy composite cathode exhibits a good rate capability with a discharge capacity of 584 mAh g À1 at 1 C.

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“…Three peaks positioned at 288.3, 284.9, and 283.7 eV are observed from the C1s spectrum, which could be attributed to the C=O, C-O, and C=C/C-C groups [34,35], respectively, indicating that C still retains some oxygen-containing groups from the carbonization process of the carbon precursor. The S 2p spectrum exhibits two peaks at 164.8 and 163.7 eV, corresponding to the resolved S 2p 1/2 and S 2p 3/2 peaks.…”

Section: Resultsmentioning

confidence: 93%

TiO 2 coated three-dimensional hierarchically ordered porous sulfur electrode for the lithium/sulfur rechargeable batteries

Wang

et al. 2014

Energy

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Guo, Z. (2014). TiO2 coated three-dimensional hierarchically ordered porous sulfur electrode for the lithium/sulfur rechargeable batteries. Energy, 75 597-602.TiO2 coated three-dimensional hierarchically ordered porous sulfur electrode for the lithium/sulfur rechargeable batteries AbstractA three-dimensional (3D) hierarchically ordered mesoporous carbon-sulfur composite slice coated with a thin TiO2 layer has been synthesized by a low-cost process and investigated as a cathode for the lithium-sulfur batteries. The TiO2 coated carbon sulfur composite thin slice works as a binder-free cathode without any current collectors for lithium-sulfur batteries. The hierarchical architecture provides a 3D conductive network for electron transfer, open channels for ion diffusion and strong confinement of soluble polysulfides. Meanwhile, TiO2 (titanium dioxide) coating layer could further effectively prevent the dissolution of polysulfides and also improve the strength of the entire electrode, thereby enhancing the electrochemical performance. As a result, after TiO2 coating, the electrode demonstrates excellent cycling performance, with a discharge capacity of 608 mAh/g at 0.2 C current rate and 500 mAh/g at 1 C current rate after 120 cycles, respectively. ABSTRACT: A three-dimensional (3D) hierarchically ordered mesoporous carbon-sulfur composite slice coated with a thin TiO 2 layer has been synthesized by a low-cost process and investigated as a cathode for the lithium-sulfur batteries. The TiO 2 coated carbon sulfur composite thin slice works as a binder-free cathode without any current collectors for lithium-sulfur batteries. The hierarchical architecture provides a 3D conductive network for electron transfer, open channels for ion diffusion and strong confinement of soluble polysulfides. Meanwhile, TiO 2 coating layer could further effectively prevent the dissolution of polysulfides and also improve the strength of the entire electrode, thereby enhancing the electrochemical performance. As a result, after TiO 2 coating, the electrode demonstrates excellent cycling performance, with a discharge capacity of 608 mAh/g at 0.2 C current rate and 500 mAh/g at 1 C current rate after 120 cycles, respectively.

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Chemically tailoring the nanostructure of graphenenanosheets to confine sulfur for high-performance lithium-sulfur batteries

Cited by 183 publications

References 42 publications

Direct Measurement of Polysulfide Shuttle Current: A Window into Understanding the Performance of Lithium-Sulfur Cells

Direct Measurement of Polysulfide Shuttle Current: A Window into Understanding the Performance of Lithium-Sulfur Cells

Well-dispersed sulfur anchored on interconnected polypyrrole nanofiber network as high performance cathode for lithium-sulfur batteries

TiO 2 coated three-dimensional hierarchically ordered porous sulfur electrode for the lithium/sulfur rechargeable batteries

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