Inorganic Gel-Derived Metallic Frameworks Enabling High-Performance Silicon Anodes

Abstract

Metallic matrix materials have emerged as an ideal platform to hybridize with next-generation electrode materials such as silicon for practical applications in Li-ion batteries. However, these metallic species commonly exist in the form of isolated particles, failing to provide enough free space for silicon volume changes as well as continuous charge transport pathways. Herein, three-dimensional (3D) metallic frameworks with interconnected pore channels and conductive skeletons, have been synthesized from inorganic gel precursors as buffering/conducting matrices to boost lithium storage performance of silicon anodes. As a proof-of-concept demonstration, commercial Si particles are in situ immobilized within the Sn–Ni alloy framework via a facile gel-reduction route, and the rearrangement of Si particles during cycling increases the dispersity of Si in the Sn–Ni framework as well as their synergic effects toward lithium storage. The Si@Sn–Ni all-metallic framework manifests high structural integrity, 3D Li+/e– mixed conduction pathway, and synergic effects of interfacial bonding and concurrent reaction dynamics between active Si and Sn, enabling long-term cycle life (1205 mA h g–1 after 100 cycles at 0.5 A g–1) and superior rate capability (653 mA h g–1 at 10 A g–1).

A Roadmap for 3D Metal Aerogels: Materials Design and Application Attempts

“…Another study prepared a Si-containing Sn-Ni gel by reducing a Si@Sn-Ni hybrid cyanogel (Figures 12C and 12D). 138 Uniform embedding of Si particles in the conductive Sn-Ni network enabled not only a considerably improved capacity retention and rate performance compared with naked Si particles but also a higher capacity than for a pure Sn-Ni network.…”

Core–Shell Structured C@SiO2 Hollow Spheres Decorated with Nickel Nanoparticles as Anode Materials for Lithium‐Ion Batteries

“…[16][17][18][19][20] Consequently, there is an urgent need for exploring and developing new anode materials with environmental benignity, high capacity, and low cost for the performance-enhanced LIBs.Silicon has attracted considerable attention as one of the potential anode candidates owing to the high theoretical capacity (4200 mAh g −1 ) and desired discharge voltage (<0.5 V vs Li/Li + ). [21][22][23][24] Unfortunately, the serious volume expansion of silicon (>300%) in the process of lithiation accompanied by structural fracture and pulverization limits its practical application. [25][26][27][28][29] Although massive efforts have been put in solving this issue, silicon anodes have not yet been broadly commercialized because of the costly and complex preparation.…”

Synthetic Methodologies for Si‐Containing Li‐Storage Electrode Materials

“…Wu et al designed 3D Sn–Ni alloy frameworks to in situ immobilize the commercial Si particles via the gel‐reduction route to boost lithium‐storage performance of silicon anodes. [ 302 ] Fabricating metal oxide materials (TiO 2 , [ 303 ] SnO 2 , [ 304 ] Co 3 O 4 , [ 208 ] Mn 3 O 4 , [ 305 ] Al 2 O 3 , [ 306 ] MgO, [ 307 ] ZnO, [ 308 ] etc.) protective layers has been proved to be a valid approach to produce a positive synergistic effect in integrating advantages of different nanocomponent.…”