Research Progress on Doping Modification of High-Capacity Silicon-Based Anode Materials AITranslate

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Basic Information:

DOI：10.13373/j.cnki.cjrm.XY25100011

Chinese Library Classification Number:TM912.6

Citation Information:

Silicon（Si）-based anodes are widely recognized as the most promising alternatives to conventional graphite anodes for lithium-ion batteries（LIBs）, owing to their ultrahigh theoretical specific capacity（4200 mAh·g^-1）, lowlithiation potential, abundant crustal reserves, low toxicity, and cost-effectiveness. However, their large-scale commercialization is severely hindered by two intrinsic challenges：1） drastic volume expansion（>300%）during lithiation/delithiation, which induces particle pulverization, electrode integrity degradation, and continuous rupture/reformation of the solid electrolyte interphase（SEI）films, thereby causing irreversible lithium-ion consumption； 2） extremely low intrinsic electrical conductivity（~1×10^-4 S·cm^-1）, which restricts ion/electron transport kinetics and thus degrades rate capability.To address these issues, early research efforts focused on nano-engineering of Si and the development of Si-based composites. Nanostructured Si can partially alleviate mechanical fracture by accommodating strain through size-dependent deformation mechanisms； however, it tends to agglomerate during prolonged cycling and exhibits excessive side reactions with the electrolyte, reducing the initial Coulombic efficiency（ICE）and cycling lifespan. Si/carbon（Si/C）composites design, which take advantage of the high electrical conductivity, chemical stability, and mechanical flexibility of carbon matrices, have emerged as a primary route toward commercialization. Nevertheless, challenges related to the inherently low conductivity of Si and inadequate interfacial bonding between Si and carbon remain unresolved. Against this backdrop, this review emphasized doping modification as a fundamental strategy to enhance the electrochemical performance of Si-based anodes. Starting from the lithium storage mechanism of Si—which stored lithium via an alloying/dealloying reaction to form various Li-Si alloys, with a theoretical maximum lithiation phase of Li₂₂Si₅ accommodating 4.4 Li atoms per Si atom—and its core limitations, we systematically analyzed the regulation mechanisms and functional effects of different doping approaches. These were categorized into three types：non-metallic （heteroatom） doping, metallic doping, and multi-element co-doping. Non-metallic doping（e.g., with B, P, N, or S）effectively modulated the electronic structure of Si-based materials, improved Li⁺ transport pathways, enhanced electronic conductivity, and promoted the formation of a more stable SEI layer. Metallic doping was subdivided into two categories：electrochemically inactive metals（e.g., Fe, Ti）, which enhanced electrical conduction and provided mechanical reinforcement to alleviate volume expansion, and electrochemically active metals（e.g., Mg, Ge）, which contributed additional capacity and helped accommodate volume expansion through synergistic alloying behavior. Multi-element co-doping（including non-metal/non-metal and metal/non-metal combinations）achieved synergistic optimization of multiple physicochemical properties, thus further enhancing conductivity, structural stability, and fast-charging performance. Finally, this review outlined future perspectives for doping modification technologies in Si-based anodes, including the exploration of novel co-doping systems to simultaneously address conductivity, volume expansion, and SEI stability； the optimization of doping processes for precise control over elemental distribution and concentration； and the integration of in-situ characterization techniques to deepen the understanding of the influence of doping elements on the lithium storage mechanism. This review aimed to provide fundamental theoretical insights and practical technical guidance for the development of high-energy-density and fast-charging Si-based anode materials, thereby accelerating their commercial adoption.