Failure mechanisms of nano-silicon anodes upon cycling: an electrode porosity evolution model
文献信息
Etienne Radvanyi, Willy Porcher, Eric De Vito, Alexandre Montani, Sylvain Franger, Séverine Jouanneau Si Larbi
With a specific capacity of 3600 mA h g−1, silicon is a promising anode active material for Li-ion batteries (LIBs). However, because of the huge volume changes undergone by Si particles upon (de)alloying with lithium, Si electrodes suffer from rapid capacity fading. A deep understanding of the associated failure mechanisms is necessary to improve these electrochemical performances. To reach this goal, we investigate here nano-Si based electrodes by several characterization techniques. Thanks to all these techniques, many aspects, such as the behaviour of the active material or the solid electrolyte interphase (SEI) and the lithiation mechanisms, are studied upon cycling. A clear picture of the failure mechanisms of nano-Si based electrodes is provided. In particular, by combining Hg analyses, SEM observations of electrode cross-sections, and EIS measurements, we follow the evolution of the porosity within the electrode. For the first time, our results clearly show a real dynamic of the pore size distribution: the first cycles lead to the formation of a micrometric porosity which is not present initially. During the following cycles, these large pores are progressively filled up with SEI products which form continuously at the Si particle surface. Thus, from the 50th cycle, Li+ ion diffusion is dramatically hindered leading to a strongly heterogeneous lithiation of the electrode and a rapid capacity fading.
期刊推荐

Journal of the Indian Institute of Science

Main Group Chemistry

Journal of Chemical Sciences

Chinese Journal of Chemistry

Medicinal Chemistry Research

Bioorganic & Medicinal Chemistry Letters

Acta Metallurgica Sinica-English Letters

Journal of Asian Natural Products Research

Critical Reviews in Solid State and Materials Sciences

Heteroatom Chemistry
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Physical Chemistry Chemical Physics

Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.
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