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JAIST black-glasses-grafted silicon microparticles as anode material for improving battery performance

The commercial application of silicon-based electrode materials—which offer excellent energy capacity—is often hindered due to two major reasons: 1) lack of mechanical stability arising from uncontrolled volume expansion upon lithiation, the process of combining with a lithium-ion, and 2) rapid energy fading caused by the formation of unstable solid-electrode interface (SEI) formation.

Over the years scientists have developed various advanced silicon-based negative electrodes or anode materials to overcome these problems. The most prominent among them are silicon nanomaterials. However, silicon nanomaterials come with certain demerits, such as a large demand and supply gap, difficult and expensive synthesis process, and, most important, a threat of fast battery dry-up.

Now, a group of researchers from the Japan Advanced Institute of Science and Technology (JAIST) led by Prof. Noriyoshi Matsumi are proposing a solution to these issues plaguing silicon micronparticles (SiMP). In a study published in Journal of Materials Chemistry A, the team reported a holistic approach to synthesizing novel highly resilient SiMPs consisting of black glasses (silicon oxycarbide)-grafted silicon as anode material for lithium-ion batteries.

Jaist

(a and b) Schematic representation of the controlled design of black glass-grafted micron silicon particle-based resilient anode materials for LIB application. Nandan et al.


Silicon nanoparticles might provide increased effective surface area but that comes with its own drawbacks like increased consumption of electrolyte as well as poor initial coulombic efficiency after a few cycles of charging and discharging. SiMPs are the most appropriate, low-cost, and easily available alternatives, especially when combined with materials that have exceptional structural properties, such as silicon oxycarbide black glasses. Our material is not only high performing but also conducive to scale opportunities.

—Prof. Matsumi

The team designed a core-shell type material where the core was made up of SiMP coated in a layer of carbon with silicon oxycarbide black glasses grafted on as the shell layer.

The prepared materials were then used in an anodic half-cell configuration to test their ability to store lithium reversibly under different potential windows. This screening showed that the material has great lithium diffusion ability, reduced internal resistance, and overall volumetric expansion.

The new material retained 99.4% of energy capacity even after 775 cycles of charging and discharging. In addition to the superlative energy storage abilities, the material also exhibited great mechanical stability throughout the testing process.

In summary, we have explored the merit of intrinsic structural features of silicon oxycarbide black glasses (BG) for rational designing micron silicon (SiMP)-based resilient anode materials for efficient and reversible storage of Li+-ions. The facile and user-friendly nature of the proposed methodology for designing SiMP-based anodes without any sophisticated instrumentation and processing difficulties inherit the promising scalable potentials and can speed up the adoption of micron size anodes in practical LiBs.

The proposed design of thoughtful grafting using acetylene black embedded BG (ABG) on carbon-coated SiMPs (Si/C), i.e., Si/C/ABG addresses the two essential requirements of (i) structural integrity and (ii) stable solid electrolyte interphase formation by internally stabilizing the fracture-prone SiMPs and externally providing the stable electrolyte–material interface. Benefiting from superior lithium diffusion kinetics, suppressed lithiation driven volumetric expansion, reduced overall resistance, and rapid improvement in initial coulombic efficiencies, Si/C/ABG demonstrates excellent rate abilities in combination with appreciable capacity retention (99.4% post 775th cycle at 750 mA g-1) across the operational potential windows (0.010–1.2 V or 0.010–3 V) and thus advocating its ability for possible practical applications.

Importantly, the study further reveals the successful integration of Si/C/ABG as the negative electrode in full-cell when paired with commercially available lithium nickel cobalt aluminium oxide (NCA) cathode, which demonstrates appreciable rate and cyclic performances. These NCA//Si/C/ABG-based full-cells are well capable of powering portable electronic devices, too.

Overall, the proposed rational design and appealing electrochemical outcomes provided will possibly speed up the progress of stable micron silicon particle-based anode development with enduring/extended cycle life for next generation lithium-ion batteries. The present methodology can be extended to design other potent micrometre-sized electrode materials too for possible applications/adoptions in a variety of next-generation energy storage devices.

—Nandan et al.

Resources

  • Ravi Nandan, Noriyuki Takamori, Koichi Higashimine, Rajashekar Badam and Noriyoshi Matsumi (2022) “Black glasses grafted micron silicon: a resilient anode material for high-performance lithium-ion batteries” Journal of Materials Chemistry A doi: 10.1039/D2TA03068C

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