Silicon has attracted huge attention in the last decade because it has a theoretical capacity ∼10 times that of graphite. However, the practical application of Si is hindered by three major challenges: large volume expansion during cycling (∼300%), low electrical conductivity, and instability of the SEI layer caused by repeated volume changes of the Si material. Significant research efforts have been devoted to addressing these challenges, and significant breakthroughs have been made particularly in the last two years (2014 and 2015). In this review, we have focused on the principles of Si material design, novel synthesis methods to achieve such structural designs, and the synthesis-structure-performance relationships to enhance the properties of Si anodes. To provide a systematic overview of the Si material design strategies, we have grouped the design strategies into several categories: (i) particle-based structures (containing nanoparticles, solid core-shell structures, hollow core-shell structures, and yolk-shell structures), (ii) porous Si designs, (iii) nanowires, nanotubes and nanofibers, (iv) Si-based composites, and (v) unusual designs. Finally, our personal perspectives on outlook are offered with an aim to stimulate further discussion and ideas on the rational design of durable and high performance Si anodes for the next generation Li-ion batteries in the near future.

The procedure for the synthesis of Li2S/C composite particles encapsulated by a nitrogen-doped carbon shell, which exhibit the highest initial discharge specific capacity ever reported in the literature.

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In this study we have investigated the electrochemical properties of hollow silicon nanospheres encapsulated with a thin carbon shell, HSi@C, as a potential candidate for lithiumion battery anodes. Hollow Si nanospheres are formed using a templating method which is followed by carbon coating via carbonization of a pyrrole precursor to form HSi@C. The synthesis conditions and the resulting structure of HSi@C have been studied in detail to obtain the target design of hollow Si nanospheres encapsulated with a carbon shell. The HSi@C obtained exhibits much better electrochemical cycle stability than both micro-and nano-size silicon anodes and deliver a stable specific capacity of 700 mA h g-1 after 100 cycles at a current density of 2 A g-1 and 800 mA h/g after 120 cycles at a current density of 1 A g-1. The superior performance of HSi@C is attributed to the synergistic combination of the nanostructured material, the enhanced conductivity, and the presence of the central void space for Si expansion with little or no change in the volume of the entire HSi@C particle. This study is the first detailed investigation of the synthesis conditions to attain the desired structure of a hollow Si core with a conductive carbon shell. This study also offers guidelines to further enhance the specific capacity of HSi@C anodes in the future.