Improved electrochemical performance of silicon nitride film by hydrogen incorporation for lithium-ion battery anode

Huang, Xiaodong; Gan, Xueping; Zhang, F.; Huang, Qing‐An; Yang, Jianwen

doi:10.1016/j.electacta.2018.02.117

Cited by 18 publications

(15 citation statements)

References 31 publications

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“…54 These deductions are strongly supported by Si 2p and N 1s XPS spectra of cycled SiO x @NC. As shown in Figure 6c, with the occurrence of the lithiation reaction, a newly formed Li x SiN y peak appears at 99.6 eV, 55 and a similar phenomenon is also observed for the Li x SiN y peak at 399.2 eV in the N 1s spectrum (Figure 6d). 24 The formation of the high ionic conductor Li x SiN y also contributes to the Li + transport kinetics.…”

Section: Resultssupporting

confidence: 70%

Constructing a Stable Si–N-Enriched Interface Boosts Lithium Storage Kinetics in a Silicon-Based Anode

Yang

Jiang

Wang

et al. 2021

ACS Appl. Mater. Interfaces

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The stable operation of a SiO x anode largely depends on the intrinsic chemistry of the electrode/electrolyte interface; however, an unstable interface structure and undesirable parasitic reactions with the electrolyte of the SiO x anode often result in the formation of a fragile solid-electrolyte interphase (SEI) and serious capacity decay during the lithiation/delithiation process. Herein, a Si−N-enriched N-doped carbon coating is constructed on the surface of SiO x yolk−shell nanospheres (abbreviated as SiO x @NC) to optimize the SEI film. The two-dimensional covalently bound Si−N interface, on one hand, can suppress the interfacial reactivity of the SiO x anode to enable the formation of a thin SEI film with accelerated diffusion kinetics of ions and, on the other hand, acts as a Li + conductor during the delithiation process, allowing Li + to diffuse rapidly in the SiO x matrix, thereby improving the long-term cycling stability and rapid charge/discharge capability of the SiO x anode. A series of characterizations show that the interface chargetransfer barrier and the Li + diffusion energy barrier through the SEI film are the main factors that determine the interfacial electrochemical behavior and lithium storage performance. This work clarifies the relationship between the SEI characteristics and the interfacial transfer dynamics and aims to offer a more basic basis for the screening of other electrode materials.

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Section: Resultssupporting

confidence: 70%

Constructing a Stable Si–N-Enriched Interface Boosts Lithium Storage Kinetics in a Silicon-Based Anode

Yang

Jiang

Wang

et al. 2021

ACS Appl. Mater. Interfaces

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“…The principle of conversion of materials into active and inactive components during the first cycle has since been extended to other materials such as silicon oxide (SiO x ), ,− the most well-known representative within the class of conversion alloying materials at the present moment. More recently, a similar approach was used for the design and subsequent preparation of amorphous and substoichiometric silicon nitride (SiN x ) thin films. ,,− These preliminary investigations of SiN x thin film electrodes have shown rather intriguing combinations of relatively high gravimetric capacities and potentially promising cycling stability. However, with one notable exception, validation of SiN x performance as a materials in more practical particle-based composite electrodes, which could be prepared through convention slurry-based process, as well as general understanding of their functionality is lacking.…”

Section: Introductionmentioning

confidence: 99%

Stoichiometry-Controlled Reversible Lithiation Capacity in Nanostructured Silicon Nitrides Enabled by in Situ Conversion Reaction

et al. 2021

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In modern Li-based batteries, alloying anode materials have the potential to drastically improve the volumetric and specific energy storage capacity. For the past decade silicon has been viewed as a “Holy Grail” among these materials; however, severe stability issues limit its potential. Herein, we present amorphous substoichiometric silicon nitride (SiN x ) as a convertible anode material, which allows overcoming the stability challenges associated with common alloying materials. Such material can be synthesized in a form of nanoparticles with seamlessly tunable chemical composition and particle size and, therefore, be used for the preparation of anodes for Li-based batteries directly through conventional slurry processing. Such SiN x materials were found to be capable of delivering high capacity that is controlled by the initial chemical composition of the nanoparticles. They exhibit an exceptional cycling stability, largely maintaining structural integrity of the nanoparticles and the complete electrodes, thus delivering stable electrochemical performance over the course of 1000 charge/discharge cycles. Such stability is achieved through the in situ conversion reaction, which was herein unambiguously confirmed by pair distribution function analysis of cycled SiN x nanoparticles revealing that active silicon domains and a stabilizing Li2SiN2 phase are formed in situ during the initial lithiation.

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“…The cathodic process could describe the insertion of Li ions from the electrolyte that formed a broad plateau at 1.1 and 0.8 V, which indicated irreversible formation of a SEI and electrolyte decomposition (for the first cycle). 43,47,48 In the following cycles (the second to fifth), the broad peak disappeared, which indicated the stability of the SEI layer. Moreover, a Si phase transformation (crystalline to amorphous) occurred, as indicated by the peak at ∼0.21 V. 13,49 Furthermore, anodic scanning showed sharp peaks at ∼0.3 and 0.5 V related to the delithiation of Li−Si alloys, and these peaks differed as the cycles increased.…”

Section: ■ Results and Discussionmentioning

confidence: 94%

“…15 Additionally, a peak at 102.4 eV was found in Si@N-ECGB, which indicated the formation of Si 3 N 4 , which was reported to provide excellent mechanical properties (strength and toughness) and improve the cyclability with a high reversible capacity. 42,43 The XPS C 1s spectra of Si@ECGB, Si@H2-ECGB, and Si@N-ECGB are displayed in Figure S7, indicating the bonding states of CC/C−C (∼284 eV), CO (∼287 eV), and O−CO (∼289 eV). 24,44 Moreover, the functionalization and reduction process affected the existing new peak at 285 eV (C−OH) 44 for Si@H2-ECGB and 285.7 eV (C− N) 29,31 for Si@N-ECGB.…”

Section: ■ Results and Discussionmentioning

confidence: 99%

Control of Graphene Heteroatoms in a Microball Si@Graphene Composite Anode for High-Energy-Density Lithium-Ion Full Cells

Jamaluddin

Umesh

Tseng

et al. 2020

ACS Sustainable Chem. Eng.

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The use of Si and nitrogen-doped graphene to fabricate composite anodes in lithium-ion batteries (LIBs) is attracting intense attention. However, the reported strategies are limited to achieving a cost-effective, scalable, and facile approach. In particular, many reports on Si/N-graphene (N-Gra) anodes cannot achieve a high first discharge capacity while retaining a high Coulombic efficiency (CE). Herein, we report a Si@N-Gra composite with core−shelled microballs of Si NPs and electrochemically exfoliated graphene by NH 3 as a nitrogen source. We use H 2 and NH 3 to control the O and N content and to optimize the anode performance.

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Improved electrochemical performance of silicon nitride film by hydrogen incorporation for lithium-ion battery anode

Cited by 18 publications

References 31 publications

Constructing a Stable Si–N-Enriched Interface Boosts Lithium Storage Kinetics in a Silicon-Based Anode

Constructing a Stable Si–N-Enriched Interface Boosts Lithium Storage Kinetics in a Silicon-Based Anode

Stoichiometry-Controlled Reversible Lithiation Capacity in Nanostructured Silicon Nitrides Enabled by in Situ Conversion Reaction

Control of Graphene Heteroatoms in a Microball Si@Graphene Composite Anode for High-Energy-Density Lithium-Ion Full Cells

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