Silicon‐Based Anodes for Lithium‐Ion Batteries: From Fundamentals to Practical Applications

Abstract

Silicon has been intensively studied as an anode material for lithium-ion batteries (LIB) because of its exceptionally high specific capacity. However, silicon-based anode materials usually suffer from large volume change during the charge and discharge process, leading to subsequent pulverization of silicon, loss of electric contact, and continuous side reactions. These transformations cause poor cycle life and hinder the wide commercialization of silicon for LIBs. The lithiation and delithiation behaviors, and the interphase reaction mechanisms, are progressively studied and understood. Various nanostructured silicon anodes are reported to exhibit both superior specific capacity and cycle life compared to commercial carbon-based anodes. However, some practical issues with nanostructured silicon cannot be ignored, and must be addressed if it is to be widely used in commercial LIBs. This Review outlines major impactful work on silicon-based anodes, and the most recent research directions in this field, specifically, the engineering of silicon architectures, the construction of silicon-based composites, and other performance-enhancement studies including electrolytes and binders. The burgeoning research efforts in the development of practical silicon electrodes, and full-cell silicon-based LIBs are specially stressed, which are key to the successful commercialization of silicon anodes, and large-scale deployment of next-generation high energy density LIBs.

Re‐Engineering Poly(Acrylic Acid) Binder toward Optimized Electrochemical Performance for Silicon Lithium‐Ion Batteries: Branching Architecture Leads to Balanced Properties of Polymeric Binders

“…Finding high‐energy anode materials suitable for lithium‐ion batteries (LIBs) is a crucial pursuit due to the huge demand for high‐energy batteries for consumer electronics and electric vehicles . Silicon (Si), which can form an alloy with lithium (Li), stands out as one of the most promising anode materials because of its high theoretical specific capacity (3570 mAh g −1 when alloyed into Li 4.4 Si), earth abundance, and mature processing techniques . However, Si nanoparticles (SiNPs) experience drastic volume changes (up to 300%) during the lithiation/delithiation process, which results in particle pulverization, electrode delamination, unstable electrode/electrolyte interface, and eventually drastic capacity fade .…”

“…[1][2][3] Silicon (Si), which can form an alloy with lithium (Li), stands out as one of the most promising anode materials because of its high theoretical specific capacity (3570 mAh g −1 when alloyed into Li 4.4 Si), earth abundance, and mature processing techniques. [4,5] However, Si nanoparticles (SiNPs) experience drastic volume changes (up to 300%) during the lithiation/delithiation process, which results in particle pulverization, electrode delamination, unstable electrode/electrolyte interface, and eventually drastic capacity fade. [6,7] As a component that works directly with active particles, a binder plays the critical role in affecting the electrochemical performance of Si-based electrodes as it not only holds the integrity of the electrode matrix but also affects the ion conductivity.…”

Assembly of Si@Void@Graphene Anodes for Lithium‐Ion Batteries: In Situ Enveloping of Nickel‐Coated Silicon Particles with Graphene

“…The performance of lithium‐ion batteries is largely rested on electrode materials . Silicon has great application potential and market prospects as it possesses the highest ever‐known theoretical specific capacity (4200 mAh g −1 ), which is more than 10 times that of graphite anode (372 mAh g −1 ) . And, compared with other anodes, it also has a lower operating potential (0.4 V vs Li / Li + ) .…”

Catalytic Growth of Graphitic Carbon‐Coated Silicon as High‐Performance Anodes for Lithium Storage

“…To further increase the cycling life and rate capacity, constructing silicon/carbon composites are widely used . Carbon materials have become potential negative electrode materials due to their small volume change, good cycle stability, and electrical conductivity, which make them good components to combine with silicon anode . Among various carbon materials, porous carbon has been considered an ideal candidate for reserving a space to accommodate the volume variation and beneficial to electrolyte infiltration for Li + transfer .…”