Effect of morphology of C-rich silicon carbonitride ceramic on electrochemical properties of sulfur cathode for Li-S battery

Qu, Fangmu; Graczyk‐Zajac, Magdalena; Vranković, Dragoljub; Chai, Nan; Yu, Zhaoju; Riedel, Ralf

doi:10.1016/j.electacta.2021.138265

Cited by 16 publications

(20 citation statements)

References 61 publications

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“…Although the SSA of the sample SiCN-900 is lower, its total pore volume V t changed little, in comparison with the sample SiCN-800, and it reveals more mesopores, in comparison to SiCN-1100 (results of BET). The presence of mesopores is of advantage for stabilization of sulfur electrochemical behavior [27,40,41], which can explain the best electrochemical performance of SiCN-S-900 among measured samples. Even though SiCN-S-1100 contains more organized free carbon phase and thus reveals higher electronic conductivity, SiCN-S-900 outperforms it in prolonged cycles stability.…”

Section: Extended Cycling Performancementioning

confidence: 88%

“…All samples show characteristic D band and G band peaks of carbon at around 1345 cm −1 and 1583 cm −1 , as well as a broad peak between 2500 cm −1 and 3000 cm −1 , corresponding to the 2D and D + G band of carbon, respectively. The sulfur-free SiCN ceramics show decreased ratio of I (A D )/I (A G ) and increased crystallite size (L a ), with increasing pyrolysis temperature (Figure 3a and Table 1) [27]. The I (A D )/I (A G ) ratio of all samples indicate that the carbon inside the SiCN ceramics exhibits amorphous structure originating from disordered sp 2 -hybridized carbon.…”

Section: Raman Spectroscopymentioning

confidence: 95%

“…Cross-linking reactions of commercial perhydropolysilazane (PHPS, DURAZANE 2250, Merck Performance Materials GmbH, Wiesbaden, Germany) with divinylbenzene (DVB, 80%, mixture of isomers, Sigma-Aldrich, Burlington, MA, USA) in Di-n-butylether (DBE, Merck Performance Materials GmbH, Wiesbaden, Germany) as the solvent and catalyzed by platinum (0)-1,3-divinyl-1,1,3,3-tetramethyldisiloxane complex solution (~Pt 2% in xylene, Sigma-Aldrich, Burlington, MA, USA) were performed via the same method, as described in our previous work-reference [27]. The obtained colorless solid precursors were then pyrolyzed in a Schlenk tube under argon flow at 800 • C, 900…”

Section: Synthesis Of C-rich Sicn Ceramicsmentioning

confidence: 99%

“…In addition, their porous property makes it possible to load sulfur and to realize physical adsorption barrier for polysulfides to hamper the "shuttle effect" [23][24][25][26]. Our previous work showed that porous C-rich SiCN ceramics pyrolyzed at temperatures between 1000 • C and 1600 • C can stabilize the electrochemical behaviour of sulfur [27]. It has been also demonstrated that the morphology of C-rich SiCN ceramics significantly affects the electrochemical performance of the S/SiCN composites and nitrogen contained in the ceramic matrix has a stabilizing effect for the electrochemical performance.…”

Section: Introductionmentioning

confidence: 99%

“…Thus, in this work, we further investigate the electrochemical stability of SiCN-S composites containing C-rich SiCN ceramics pyrolyzed at temperatures below 1000 • C in more detail. The C-rich SiCN-S composites are synthesized using a scalable melting-diffusion method [27]. After the melting-diffusion procedure, sulfur is introduced and embedded into the C-rich SiCN ceramic.…”

Section: Introductionmentioning

confidence: 99%

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Electrochemical Performance of Carbon-Rich Silicon Carbonitride Ceramic as Support for Sulfur Cathode in Lithium Sulfur Battery

Król

et al. 2022

Nanomaterials

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As a promising matrix material for anchoring sulfur in the cathode for lithium-sulfur (Li-S) batteries, porous conducting supports have gained much attention. In this work, sulfur-containing C-rich SiCN composites are processed from silicon carbonitride (SiCN) ceramics, synthesized at temperatures from 800 to 1100 °C. To embed sulfur in the porous SiCN matrix, an easy and scalable procedure, denoted as melting-diffusion method, is applied. Accordingly, sulfur is infiltrated under solvothermal conditions at 155 °C into pores of carbon-rich silicon carbonitride (C-rich SiCN). The impact of the initial porosity and microstructure of the SiCN ceramics on the electrochemical performance of the synthesized SiCN-sulfur (SiCN-S) composites is analysed and discussed. A combination of the mesoporous character of SiCN and presence of a disordered free carbon phase makes the electrochemical performance of the SiCN matrix obtained at 900 °C superior to that of SiCN synthesized at lower and higher temperatures. A capacity value of more than 195 mAh/g over 50 cycles at a high sulfur content of 66 wt.% is achieved.

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Section: Extended Cycling Performancementioning

confidence: 88%

Section: Raman Spectroscopymentioning

confidence: 95%

Section: Synthesis Of C-rich Sicn Ceramicsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

See 3 more Smart Citations

Electrochemical Performance of Carbon-Rich Silicon Carbonitride Ceramic as Support for Sulfur Cathode in Lithium Sulfur Battery

Król

et al. 2022

Nanomaterials

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Harnessing Regenerated Graphite from Spent Lithium‐Ion Batteries to Enhance the Performance of Sulfur Cathode in Lithium‐Sulfur Batteries

Sheng,

Graczyk‐Zajac,

Tian

et al. 2024

Batteries & Supercaps

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In this work, a facile hydrometallurgical approach combined with heat treatment has been adopted to recycle spent graphite from retired lithium‐ion battery cells. Graphite regenerated with 18 M H2SO4 leaching leads to a high specific surface area, significant porosity and small crystallite size. The regenerated graphite has been infiltrated with sulfur under solvothermal conditions at 160 oC. The sample containing 68 wt% of sulfur recovers a capacity of 224 mAh/g after 100 cycles. Furthermore, the electrode with a higher sulfur content of 84 wt%, recuperates the specific discharging capacity of 207 mAh/g after 100 cycles. After the initial fading during the first 5‐10 cycles, the cathodes based on regenerated graphite demonstrate stable cycling behavior. This research not only offers an accessible and scalable method for regenerating graphite from spent LIBs but also demonstrates a new application of the regenerated graphite in LSBs, showcasing outstanding electrochemical performance.

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Unraveling Na‐Ion Insertion Mechanisms in Polymer‐Derived SiCN(O) Ceramic via Operando Raman Spectroscopy

Melzi d'Eril,

Kempf,

De Carolis

et al. 2024

Batteries & Supercaps

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In this study we investigate the Na insertion process occurring in the “free carbon” phase embedded in two different SiCN(O) matrices with operando Raman spectroscopy. The two SiCN(O) samples have been prepared using two different thermal treatments carried out at 1000 °C (SiCN(O)1000) and 1400 °C (SiCN(O)1400). X‐ray diffraction as well as argon adsorption reveal significant structural and morphological differences between the materials. SiCN(O)1000 shows an amorphous nature whereas SiCN(O)1400 reveals the presence of crystalline β‐SiC, accompanied by a notable increase in surface area (from 56.7 m2/g to 331 m2/g) and micropore volume (from 0.02 cm3/g to 0.12 cm3/g). These alterations in the ceramic matrix due to thermal treatment affect significantly the electrochemical performance with initial de‐sodiation capacities of 112.4 mAh/g and 52.3 mAh/g for SiCN(O)1000 and SiCN(O)1400, respectively. Operando Raman spectroscopy, carried out during the sodiation and de‐sodiation of the SiCN(O) ceramics, reveals the microstructural changes occurring to the “free carbon” phase during the storage of sodium ions. As sodium is inserted, a shift in the G‐band position is observed in both the samples from about 1600 cm−1 to 1555 cm−1, with a concomitant decrease of the D‐band intensity and the distance between defects (LD) growing from 7.5 nm to 17.5 nm. Upon de‐sodiation, SiCN(O)1400 exhibits an inferior storage reversibility compared to SiCN(O)1000. This may be attributed to the irreversible sodium trapping occurring in SiCN(O)1400, highlighted by the reduced efficiency of the electrochemical process.

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Effect of morphology of C-rich silicon carbonitride ceramic on electrochemical properties of sulfur cathode for Li-S battery

Cited by 16 publications

References 61 publications

Electrochemical Performance of Carbon-Rich Silicon Carbonitride Ceramic as Support for Sulfur Cathode in Lithium Sulfur Battery

Electrochemical Performance of Carbon-Rich Silicon Carbonitride Ceramic as Support for Sulfur Cathode in Lithium Sulfur Battery

Harnessing Regenerated Graphite from Spent Lithium‐Ion Batteries to Enhance the Performance of Sulfur Cathode in Lithium‐Sulfur Batteries

Unraveling Na‐Ion Insertion Mechanisms in Polymer‐Derived SiCN(O) Ceramic via Operando Raman Spectroscopy

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