High-yield and scalable synthesis of a Silicon/Aminosilane-functionalized Carbon NanoTubes/Carbon (Si/A-CNT/C) composite as a high-capacity anode for lithium-ion batteries

Sehlleier, Yee Hwa; Dobrowolny, Sascha; Plümel, Ingo; Xiao, Lisong; Mahlendorf, Falko; Heinzel, Angelika; Schulz, Christof; Wiggers, Hartmut

doi:10.1007/s10800-015-0897-x

Cited by 15 publications

(9 citation statements)

References 36 publications

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“…Si NPs were synthesized in N 2 using a tubular hot-wall reactor (HWR, inner diameter 14 cm) and pure monosilane (SiH 4 , quality EHP, Air Liquide) as the precursor. The experimental procedure was described in our previous work. , In brief, SiH 4 gas was fed into the reaction-tube through a concentric nozzle that is mounted at the top of the HWR. A coaxial H 2 gas flow (quality 5.0, Air Liquide) served as a sheath gas to prevent the decomposition of SiH 4 on the reactor-wall.…”

Section: Methodsmentioning

confidence: 99%

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Parasitic Reactions in Nanosized Silicon Anodes for Lithium-Ion Batteries

et al. 2017

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When designing nano-Si electrodes for lithium-ion batteries, the detrimental effect of the c-LiSi phase formed upon full lithiation is often a concern. In this study, Si nanoparticles with controlled particle sizes and morphology were synthesized, and parasitic reactions of the metastable c-LiSi phase with the nonaqueous electrolyte was investigated. The use of smaller Si nanoparticles (∼60 nm) and the addition of fluoroethylene carbonate additive played decisive roles in the parasitic reactions such that the c-LiSi phase could disappear at the end of lithiation. This suppression of c-LiSi improved the cycle life of the nano-Si electrodes but with a little loss of specific capacity. In addition, the characteristic c-LiSi peak in the differential capacity (dQ/dV) plots can be used as an early-stage indicator of cell capacity fade during cycling. Our findings can contribute to the design guidelines of Si electrodes and allow us to quantify another factor to the performance of the Si electrodes.

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Section: Methodsmentioning

confidence: 99%

“…The experimental procedure was described in our previous work. 31,32 In brief, SiH 4 gas was fed into the reaction-tube through a concentric nozzle that is mounted at the top of the HWR. A coaxial H 2 gas flow (quality 5.0, Air Liquide) served as a sheath gas to prevent the decomposition of SiH 4 on the reactor-wall.…”

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confidence: 99%

Parasitic Reactions in Nanosized Silicon Anodes for Lithium-Ion Batteries

et al. 2017

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“…The Raman spectra of the tested electrodes indicates the existence of Si and carbon as the Zn 2+ (Figure A,B) and Al 3+ ions (Figure C,D), are adsorbed on the surface of the electrodes. The Raman spectra of untreated 1.1 Si/MWCNT composites show peaks centered at 480 cm –1 , assigned to the phonon vibration of crystalline Si. ,, Regarding the cycled state in both Zn 2+ and Al 3+ ions aqueous electrolytes, the peaks related to Si are shifted, indicating a decrease in crystallite size . Furthermore, the non-existence of peaks in the region of 890–950 cm –1 , verifies the absence of wurtzite Si …”

Section: Resultsmentioning

confidence: 91%

“…The two reduction peaks are repeated at low scan rates, and after 20 mV s –1 , a broad peak is formed, which can refer to the extrinsic pseudocapacitance appearing in high-rate cycling. The hindrance of the second reduction peak implies that ions at high scan rates preferably are stored on the surface of the electrode due to the volume expansion of Si promoting less active surface , for ions to insert. A current increase is observed, compared with the Si/SS (Figure S2A) and MWCNT/SS (Figure S2B) electrodes, demonstrating the significant role of the Si layer in the MWCNTs, promoting reversible redox reactions and contributing to the overall capacity.…”

Section: Resultsmentioning

confidence: 99%

“…As a result, in situ CNT growth on Si anode materials reduces the risk of Si failure mechanism and may be useful in the development of more stable Si anode composites for LIBs. Furthermore, Sehlleier et al reported that functionalized MWCNTs enable excellent Si particle integration, preventing the electrode structure from deteriorating during repeated volume changes. This material’s design enhances Si-based anodes by forming a 3D porous framework in conjunction with strong electrical characteristics, which substantially increases electron and ion transport by shortening diffusion paths and increasing 3D interconnectivity .…”

Section: Introductionmentioning

confidence: 99%

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Investigation of Si-Coated Multiwalled Carbon Nanotubes as Potential Electrodes for Multivalent Metal-Ion Electrochemical Energy Storage Systems

et al. 2023

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In the present paper, we report the chemical vapor deposition of multiwall carbon nanotubes (MWCNTs) coating on stainless steel substrates and the coverage of the individual CNTs by a silicon (Si) thin layer. The study's goal is to create and evaluate electrochemically Si/MWCNT composites with varying Si loadings to act both as a mechanical support and electrical conducting path to the current collector. MWCNTs incorporated efficiently into the Si layer on their surface and aided Si's poor stability while maintaining its high-capacity values. The Si/ MWCNT composite electrodes operated in a wide potential window of 1.7 V with improved Q/V ratios (charge to voltage) and retention over cycling compared to plain MWCNTs and Si electrodes, despite the similar surface area. In addition, the composite electrodes displayed a larger integration area in cyclic voltammograms, distinct charge/discharge plateaus, and wider discharge potential, indicating a higher energy storage capacity and high relative voltammetric charge retention. In particular, the Si/ MWCNT electrodes demonstrated relative voltammetric charge retentions of 99.3% and 68% at 100 mV s −1 and stable Q/V ratios of 231 and 209 mF cm −2 at a current density of 2 mA cm −2 with retention maintained at 100% after 30 cycles in ZnSO 4 and Al 2 (SO 4 ) 3 aqueous electrolytes, respectively. Although the Q/V ratios may have distinct origins, we assumed that both electrolytes incorporate a mix of surface and bulk contributions. A combination of both ionic diffusion and pseudocapacitive behavior is displayed. Combined charge storage mechanisms are present at different electrode states, indicating the electrolyte ions' adsorption (surfacecontrolled) and insertion (diffusion-controlled) in the active sites of the composites. The results suggested that the pseudocapacitive nature combined with the reversible diffusion of ions during redox reactions worked synergistically to increase contributions to the overall Q/V ratios. The storage of ions is facilitated by the small ionic radius of Al 3+ (0.53 Å) and Zn 2+ (0.75 Å) ions. Diffusion coefficient values of Al 3+ (4.58 × 10 −11 cm 2 s −1 ) are higher than those of Zn 2+ (3.16 × 10 −11 cm 2 s −1 ) during oxidation but lower at reduction processes (6.02 × 10 −11 and 7.1 × 10 −11 cm 2 s −1 ). As a result, the Al 3+ ions are less effective while extracted with reduced reversibility than Zn 2+ ions. Agglomerations of smaller ions stored in electrodes might confine the extraction process and possibly the overall stability over intense cycling. The faradaic performance on the one side coupled with the semi-infinite diffusion and pseudocapacitive behavior could offer a promising utilization as working electrodes in Zn 2+ and Al 3+ ion hybrid energy storage systems.

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