Lithium dynamics in carbon-rich polymer-derived SiCN ceramics probed by nuclear magnetic resonance

Baek, S.‐H.; Reinold, Lukas Mirko; Graczyk‐Zajac, Magdalena; Riedel, Ralf; Hammerath, Franziska; Büchner, B.; Grafe, H.-J.

doi:10.1016/j.jpowsour.2013.12.065

Cited by 25 publications

(18 citation statements)

References 30 publications

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“…Within the work of Reinold et al [12], the excellent performance of carbon-rich SiCN materials with outstanding stability and capacities up to 600 mAh g −1 has been demonstrated, including the discussion of the influence of the molecular polymer structure on the resulting ceramic microstructure and in consequence on the electrochemical performance of the material. By means of solid state NMR of lithiated and delithiated SiCN carbon phase was identified as a major lithium storage site [13], this finding being in agreement with the work of Fukui et al on SiOC materials [14]. Within our previous studies, we have also shown that composite anode materials comprised of SiCN/graphite [15] and SiCN/silicon [16] exhibit enhanced electrochemical properties compared to that of pure graphite and silicon, respectively.…”

Section: Introductionsupporting

confidence: 90%

Lithium intercalation into SiCN/disordered carbon composite. Part 1: influence of initial carbon porosity on cycling performance/capacity

Graczyk‐Zajac

Wimmer

Neumann

et al. 2015

J Solid State Electrochem

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Within this work, we investigate the structural and electrochemical properties of new composite materials based on disordered carbons embedded into a polymer-derived silicon carbonitride matrix. In particular, we focus on the relationship between the initial characteristic of disordered carbon, that is its microstructure and porosity with the lithiumions storage properties of the composite. Although there is almost no difference between composites found by means of Raman spectroscopy and X-ray powder diffraction, it is demonstrated that the pore volume of the carbon is of significant importance, i.e., volume of the preceramic polymer must be matched with pore volume of the carbon in order to ensure the optimal electrochemical performance. Thus, it is possible to synthesize a composite containing only 50 % of external carbon, which recovers the capacity comparable to that of pure carbon.

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Section: Introductionsupporting

confidence: 90%

Lithium intercalation into SiCN/disordered carbon composite. Part 1: influence of initial carbon porosity on cycling performance/capacity

Graczyk‐Zajac

Wimmer

Neumann

et al. 2015

J Solid State Electrochem

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“…After etching polymer-derived silicon-oxycarbide ceramics with hydrofluoric acid, silica domains are removed and the remaining structure is postulated to consist of a scaffolding of graphene networks with their surfaces decorated with mixed bonds of tetrahedral silicon bonded to both oxygen and carbon (Peña-Alonso et al, 2006). In Baek's study using SiCN as candidate for anode of Li-ion batteries to replace graphite anodes (Baek et al, 2014), the mixed bond tetrahedra of Si in SiCN is believed to act as an additional lithiation site. …”

Section: Resultsmentioning

confidence: 99%

Predicting structural properties of amorphous silicon carbonitride by atomistic simulation

Liao

Zhang

Raj

et al. 2016

IJMSI

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Silicon carbonitride (SiCN) has superior mechanical properties at high temperature, but its structural properties in molecular scale are not clear. In this study, atomistic simulations were applied to study the molecular structure of amorphous SiCN. The atomistic structures obtained by large-scale molecular dynamics simulations agree with current experimental results, and moreover, provide more details on molecular structure. The Si-C bonds generally keep stable proportion for all the three cases, which means the additional carbon tends to form free carbon network rather than Si-C bonds. Si-CN 3 is dominant inSi-C/N tetrahedron, and as expected the increase of C content in SiCN tends to form more Si-C 2 N 2 and Si-C 3 N tetrahedra.

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“…Within recent years, anode materials based on carbon-rich SiOC and SiCN PDCs have been widely investigated for their lithium storage properties [13][14][15][16][17][18][19][20][21][22][23][24][25][26][27][28]. It has been reported that carbon-rich silicon carbonitride (SiCN) recovers capacities as high as 600 mAh¨g´1 [25] while storing lithium mostly in the carbon phase [23,28]. The composite materials consisting of graphite/carbon-poor SiCN or precursor-derived Si(B)CN coated-multiwalled carbon nanotube (CNT) composite exceed by far the sum of the capacities of the single components [27,29,30].…”

Section: Introductionmentioning

confidence: 99%

“…It signifies that more ordered carbon (higher La) might also enhance lithium storage performance. However, we assume that a decreased carbon content, which serves as the major active phase for reversible Li insertion in polymer-derived SiCN and SiOC ceramics [14,15,23,26], is the main reason for diminished electrochemical performance of BC 2 N.…”

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confidence: 99%

Electrochemical Li Storage Properties of Carbon-Rich B–C–N Ceramics

Bhat

Sasikumar

Molina‐Luna

et al. 2016

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Amorphous BCN ceramics were synthesized via a thermal conversion procedure of piperazine-borane and pyridine-borane. The synthesized BC 2 N and BC 4 N ceramics contained, in their final amorphous structure, 45 and 65 wt % of carbon, respectively. Elemental analysis revealed 45 and 65 wt % of carbon for BC 2 N and BC 4 N, respectively. Transmission electron microscopy (TEM) and X-ray diffraction (XRD) confirmed the amorphous nature of studied compounds. Lateral cluster size of carbon crystallites of 7.43 and 10.3 nm for BC 2 N and BC 4 N, respectively, was calculated from Raman spectroscopy data. This signified a higher order of the carbon phase present in BC 4 N. The electrochemical investigation of the low carbon BC 2 N composition as anodes for Li-ion batteries revealed initial capacities of 667 and 235 mAh¨g´1 for lithium insertion/extraction, respectively. The material with higher carbon content, BC 4 N, disclosed better reversible lithium storage properties. Initial capacities of 1030 and 737 mAh¨g´1 for lithium insertion and extraction were recovered for carbon-rich BC 4 N composition. Extended cycling with high currents up to 2 C/2 D revealed the cycling stability of BC 4 N electrodes. Cycling for more than 75 cycles at constant current rates showed a stable electrochemical behavior of BC 4 N anodes with capacities as high as 500 mAh¨g´1.

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Lithium dynamics in carbon-rich polymer-derived SiCN ceramics probed by nuclear magnetic resonance

Cited by 25 publications

References 30 publications

Lithium intercalation into SiCN/disordered carbon composite. Part 1: influence of initial carbon porosity on cycling performance/capacity

Lithium intercalation into SiCN/disordered carbon composite. Part 1: influence of initial carbon porosity on cycling performance/capacity

Predicting structural properties of amorphous silicon carbonitride by atomistic simulation

Electrochemical Li Storage Properties of Carbon-Rich B–C–N Ceramics

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