Ultramicroporous carbon aerogels encapsulating sulfur as the cathode for lithium–sulfur batteries

Nojabaee, Maryam; Sievert, Brigitta; Schwan, Marina; Schettler, Jessica; Warth, Frieder; Wagner, Norbert; Milow, Barbara; Friedrich, K. Andreas

doi:10.1039/d0ta11332h

Cited by 31 publications

(30 citation statements)

References 48 publications

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“…32 As expected, cathodes with C45-additive exhibit a similar self-discharge behavior (Figure S14) as C45 does not provide tailored pore sizes to incorporate sulfur. In general, the quasi-solid-state conceptknown to retain sulfur species in microporous carbons such as aerogels in the lithium−sulfur system 33 might not be applicable for magnesium cells as it relies on the solidstate diffusion of cations and the Mg 2+ diffusion is rather sluggish. A promising alternative strategy might be covalently bound sulfur in polymer chains (e.g., SPAN 34 ).…”

Section: ■ Self-dischargementioning

confidence: 99%

Operando UV/vis Spectroscopy Providing Insights into the Sulfur and Polysulfide Dissolution in Magnesium–Sulfur Batteries

et al. 2021

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The magnesium–sulfur battery represents a promising post-lithium system with potentially high energy density and improved safety. However, just as all metal–sulfur systems, it is plagued with the polysulfide shuttle leading to active material loss and surface layer formation on the anode. To gain further insights, the present study aims to shed light on the dissolution characteristics of sulfur and polysulfides in glyme-based electrolytes for magnesium–sulfur batteries. Therefore, operando UV/vis spectroscopy and imaging were applied to survey their concentration in solution and the separator coloration during galvanostatic cycling. The influence of conductive cathode additives (carbon black and titanium nitride) on the sulfur retention and cycling overpotentials were investigated. Thus, valuable insights into the system’s reversibility and the benefit of additional reaction sites are gained. On the basis of these findings, a reduction pathway is proposed with S8, S6 2–, and S4 2– being the present species in the electrolyte, while the dissolution of S8 2– and S3 •– is unfavored. In addition, the evolution of the sulfur species concentration during an extended rest at open-circuit voltage was investigated, which revealed a three-staged self-discharge.

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Section: ■ Self-dischargementioning

confidence: 99%

Operando UV/vis Spectroscopy Providing Insights into the Sulfur and Polysulfide Dissolution in Magnesium–Sulfur Batteries

et al. 2021

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“…The C 1s spectra of the CNT–biomass gel consists of four peaks at 284.6, 285.15, 287.0, and 288.5 eV, corresponding to sp 2 /sp 3 carbon, C–O species, CO species, and O–CO species, respectively (Figure b). , After 200 cycles at a 0.5C rate, the survey spectra of the CNT–biomass gel interlayer demonstrate the presence of C, O, Li, and S elements, as well as the F element (Figure c) originating from the LiTFSI electrolyte. Compared to the CNT–biomass gel interlayer before cycle, the C 1s spectrum is deconvoluted into three additional peaks at 289.9, 290.65, and 293.25 eV, corresponding to C–F, CF 2 CH 2 , and C 10 F 8 bonds, respectively. , Compared to the fresh sample, the sample after cycle has a new C–S bond, indicating that there is chemical adsorption between the biomass carbon and Li 2 S n . Furthermore, polysulfides adsorption is also investigated by the S 2p spectrum, as shown in Figure d.…”

Section: Resultsmentioning

confidence: 99%

Low-Cost Biomass-Gel-Induced Conductive Polymer Networks for High-Efficiency Polysulfide Immobilization and Catalytic Conversion in Li–S Batteries

Jiang

Guo

Tao

et al. 2022

ACS Appl. Energy Mater.

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Lithium−sulfur batteries are regarded as one of the most promising candidates for next-generation energy storage systems because of their high energy density and the low cost of sulfur. However, practical applications are still impeded by sluggish redox kinetics and the shuttling effect of soluble intermediate lithium polysulfides (LiPSs), which induces irreversible loss of active materials, self-discharge, and thus poor cycle stability. Herein, a polysulfide-anchored catalytic polymer is reported to solve the shuttling behavior and improve battery performance. Natural polymer xanthan gum and konjac gum with abundant polar oxygen-containing functional groups (−OH, CO, −COOH, and −O−) that induce strong binding interactions with lithium polysulfide and reduce the energy barrier of the reaction from S 8 to Li 2 S are entangled with a conductive carbon nanotube (CNT) skeleton as a polysulfide shielding interlayer. Combined with the highly conductive CNT porous network that facilitates Li + ion transportation, the CNT−biomass gel interlayer is endowed with great capability of adsorbing and catalyzing the active sulfur. Benefiting from these synergistic attributes, the as-obtained CNT−biomass gel composite interlayer can achieve excellent performance of a high initial capacity of 998.2 mA h g −1 at 0.2C and a slight capacity decay of 0.078% per cycle at 0.5C over 200 cycles. More importantly, the battery demonstrates a cycle stability at a high sulfur loading of 3.0 mg cm −2 . The proposed strategy will contribute to the design of biomass-derived materials for Li−S batteries. Natural polymer xanthan gum and konjac gum with abundant polar oxygen-containing functional groups that induce strong binding interactions with lithium polysulfide and reduce the energy barrier of the reaction from S 8 to Li 2 S are entangled with a conductive carbon nanotube skeleton as a polysulfide shielding interlayer. The CNT−biomass gel interlayer is endowed with a great capability of adsorbing and catalyzing the active sulfur.

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“…The results showed that with the increase in carbonization temperature, the ratios of the D peaks near 1343 cm –1 and the G peaks near 1592 cm –1 ( I D / I G ) for the three high carbonization temperature materials were all less than SSC-850. It is proved that a higher carbonization temperature would be beneficial for reducing the disorder degree and improve the conductivity of carbon hosts, so as to make up for the barrier of the electron–ion transport caused by the insulating property of active material sulfur. It is worth noting that the I D / I G value of SSC-1150 was the smallest among the four.…”

Section: Resultsmentioning

confidence: 99%

Self-supporting Biomass Li–S Cathodes Decorated with Metal Phosphides–Higher Sulfur Loading, Better Stability, and Longer Cycle Life

Liu

Xia

Wang

et al. 2022

ACS Appl. Energy Mater.

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Under the premise of high sulfur loading, how to solve the problems of low capacity, short cycle life, and poor rate performance caused by the dynamics of polysulfide and further exert the advantages of the excellent energy density of Li−S batteries is a hot topic nowadays. Herein, the high-S loading self-supporting biomass Li−S cathodes decorated with metal phosphides (MP x , M = Ni, Co, and Fe) were developed. The cattail, an aquatic plant, was employed as a raw material to prepare a three-dimensional self-supporting carbon matrix (SSC) with excellent flexibility. The complex and fluffy structure of the SSC carrier could effectively alleviate volume variation during the cycle of the battery while loading more sulfur, and its carbon nanotube network with favorable conductivity could also achieve rapid electron transfer. In addition, by combining the calculation results of density functional theory with electrochemical properties, we proved that all three phosphides have a strong adsorption and catalytic effect on polysulfides, while further elaborating the specific functions and behaviors of different metal phosphides in promoting polysulfide conversion. Finally, the MP x @SSC-1150 (M = Ni/ Co/Fe) not only possesses high initial discharge capacities (1236.96, 1398.45, and 1240.96 mA h g −1 , respectively) under a high load (5.5 mg cm −2 ) but also ensures excellent long-cycle stability. The work opens feasible avenues for the selection and preparation of compounds for the catalytic conversion of polysulfides in Li−S batteries with high-S loading.

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Ultramicroporous carbon aerogels encapsulating sulfur as the cathode for lithium–sulfur batteries

Abstract: In the presented study, a sulfur infiltrated ultra-microporous carbon aerogel as a composite cathode for lithium sulfur batteries is developed and investigated.

Cited by 31 publications

References 48 publications

Operando UV/vis Spectroscopy Providing Insights into the Sulfur and Polysulfide Dissolution in Magnesium–Sulfur Batteries

Operando UV/vis Spectroscopy Providing Insights into the Sulfur and Polysulfide Dissolution in Magnesium–Sulfur Batteries

Low-Cost Biomass-Gel-Induced Conductive Polymer Networks for High-Efficiency Polysulfide Immobilization and Catalytic Conversion in Li–S Batteries

Self-supporting Biomass Li–S Cathodes Decorated with Metal Phosphides–Higher Sulfur Loading, Better Stability, and Longer Cycle Life

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