Designing Host Materials for Sulfur Cathodes: From Physical Confinement to Surface Chemistry

Peng, Hong‐Jie; Zhang, Qiang

doi:10.1002/anie.201505444

Cited by 235 publications

(139 citation statements)

References 34 publications

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“…It is generally believed that the dissolution of these polysulfide species into the electrolyte, and their subsequent diffusion away from electrochemically active surfaces, contribute to a major degradation mechanism as well as sulfur-utilization limitation [4,5]. In light of this loss mechanism, numerous strategies have been proposed to encapsulate polysulfides in the cathode, including optimization of the cathode nanomorphology (as reviewed in [6,7]), doping of polysulfide-adsorption sites [8,9], and coating of polysulfide blocking or adsorption layers [10,11]. However, most of these experimental studies are carried out with vast excess of electrolyte [12], not taking into account the fact that the electrolyte-to-sulfur mass ratio has a major influence on the sulfur utilisation [13,14,15].…”

Section: Introductionmentioning

confidence: 99%

Modelling transport-limited discharge capacity of lithium-sulfur cells

Zhang

Marinescu

Waluś

et al. 2016

Electrochimica Acta

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Lithium-sulfur (Li-S) battery could bring a step-change in battery technology with a potential specific energy density of 500 -600 Wh/kg. A key challenge for further improving the specific energy-density of Li-S cells is to understand the mechanisms behind reduced sulfur utilisation at low electrolyte loadings and high discharge currents. While several Li-S models have been developed to explore the discharge mechanisms of Li-S cells, they so far fail to capture the discharge profiles at high currents. In this study, we propose that the slow ionic transport in concentrated electrolyte is limiting the rate capability of Li-S cells. This transport-limitation mechanism is demonstrated through a one-dimensional Li-S model which qualitatively captures the discharge capacities of a sulfolane-based Li-S cell at different currents. Furthermore, our model predicts that a discharged Li-S cell is able regain some capacity with a short period of relaxation. This capacity recovery phenomenon is validated experimentally for different discharge currents and relaxation durations. The transport-limited discharge behavior of Li-S cells highlights the importance of optimizing the electrolyte loading and electrolyte transport property in Li-S cells.

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Section: Introductionmentioning

confidence: 99%

Modelling transport-limited discharge capacity of lithium-sulfur cells

Zhang

Marinescu

Waluś

et al. 2016

Electrochimica Acta

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“…Once LiPSs are solvated, they can easily dissolve into the organic electrolyte from the electrode surface and diffuse away. Subsequent reutilization of LiPSs for capacity contribution will become very difficult due to the repulsion between the polar reactants and the nonpolar conductive surface24.…”

mentioning

confidence: 99%

“…Recently, it has been realized that polar functional groups/surfaces can significantly increase the chemical interaction between polysulfides and the substrates2324, and many efforts have been expended to develop sulfur hosts with strong chemical adsorption capability for LiPSs. For instance, heteroatom doping252627 and surfaces functionalization282930 of carbon materials lead to significant improvement of chemical adsorption of LiPSs.…”

mentioning

confidence: 99%

A sulfur host based on titanium monoxide@carbon hollow spheres for advanced lithium–sulfur batteries

et al. 2016

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Lithium–sulfur batteries show advantages for next-generation electrical energy storage due to their high energy density and cost effectiveness. Enhancing the conductivity of the sulfur cathode and moderating the dissolution of lithium polysulfides are two key factors for the success of lithium–sulfur batteries. Here we report a sulfur host that overcomes both obstacles at once. With inherent metallic conductivity and strong adsorption capability for lithium-polysulfides, titanium monoxide@carbon hollow nanospheres can not only generate sufficient electrical contact to the insulating sulfur for high capacity, but also effectively confine lithium-polysulfides for prolonged cycle life. Additionally, the designed composite cathode further maximizes the lithium-polysulfide restriction capability by using the polar shells to prevent their outward diffusion, which avoids the need for chemically bonding all lithium-polysulfides on the surfaces of polar particles.

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“…Since the carbon is non-polar whereas Li polysulfides are inherently polar molecules, the cathodes which make up this non-polar host still face fast capacity decay over long-term cycling because it can only permit adsorption of polysulfides up to diffusion limitations [71,72]. Surface properties of the porous carbon can be altered by functionalization such as doping with N or B. Doping carbon with N or B is an effective way to enhance the intrinsic properties of porous carbon materials as it may facilitate the chemisorption of Li polysulfides at the surface [16,[73][74][75][76].…”

Section: Bio-derived Microporous Carbonmentioning

confidence: 99%

“…A new strategy is to design a sulfur host that can utilize chemisorption and thus prevent lithium polysulfides from shuttling (Fig. 7) [71,72,115]. The surface chemistry of carbon can be modified by functionalization by heteroatom-doping.…”

Section: Conclusion and Remarksmentioning

confidence: 99%

Biomass-derived nanostructured porous carbons for lithium-sulfur batteries

et al. 2016

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Biomass has been utilized as an energy source for thousands of years typically in the form of wood and charcoal. Technological advances create new methodologies to extract energy and chemicals from biomass. The biomass-derived nanostructured porous carbons (BDNPCs) are the most promising sulfur hosts and interlayers in rechargeable lithium-sulfur (Li-S) batteries. In this article, a comprehensive review is provided in the synthesis of nanostructured porous carbon materials for high-performance rechargeable Li-S batteries by using biomass. The performances of the Li-S batteries dependent on the porous structures (micro, meso and hierarchical) from BDNPCs are discussed, which can provide an in-depth understanding and guide rational design of high-performance cathode materials by using low-cost, sustainable and natural bio-precursors. Furthermore, the current existing challenges and the future research directions for enhancing the performance of Li-S batteries by using natural biomass materials are also addressed.

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Designing Host Materials for Sulfur Cathodes: From Physical Confinement to Surface Chemistry

Cited by 235 publications

References 34 publications

Modelling transport-limited discharge capacity of lithium-sulfur cells

Modelling transport-limited discharge capacity of lithium-sulfur cells

A sulfur host based on titanium monoxide@carbon hollow spheres for advanced lithium–sulfur batteries

Biomass-derived nanostructured porous carbons for lithium-sulfur batteries

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