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An economical, sustainable, and industry‐acceptable process of utilizing low‐value resources to produce highly competitive silicon‐based anodes is attractive. In this study, a special anode architecture of PV nano‐Si–SiOx/graphite is developed by utilizing low‐value photovoltaic (PV) recycled silicon, which is partially converted to new hybrid PV Si–SiOx and nano‐size simultaneously and wrapped by graphite fragments. An industry‐grade ball milling techniques are exploited to assemble this special anode architecture under controlled environment conditions. The attained new PV nano‐Si–SiOx/graphite electrode‐incorporated dual binders of carboxymethyl cellulose and poly (acrylic acid) demonstrates high charge capacity and stability (600 mAh g−1 at 0.2 C after 500 cycles; 600 mAh g−1 at 1 C after 100 cycles) as well as commendable Coulombic efficiencies (87% initial and ≥ 99.5% subsequent cycles), providing new opportunities for practical application. The structural analysis reveals that the partial conversion of Si to Si–SiOx is critical to in situ generate the inert matrix of Li2O–lithium silicate, which works as a buffer in diminishing the volume variation in the electrode during initial lithiation. Our silicon anode design and subsequent assembly by environmentally friendly processes can potentially be used to produce high‐value practical silicon anodes for lithium‐ion battery technology. End‐of‐life PV silicon is upcycled into a high‐performance nano‐Si–SiOx/graphite anode via magneto ball milling. The hybrid electrode delivers 600 mAh g⁻¹, exceptional cycling stability, and high Coulombic efficiency (87% initial, ≥ 99.5% after), enabled by in situ Li₂O–lithium silicate buffering—offering a sustainable, industry‐scalable solution for next‐gen lithium‐ion batteries.

Due to its high theoretical specific capacity, a silicon anode is one of the candidates for realizing high energy density lithium-ion batteries (LIBs). However, problems related to bulk silicon (e.g., low intrinsic conductivity and massive volume expansion) limit the performance of silicon anodes. In this work, to improve the performance of silicon anodes, a vertically aligned n-type silicon nanowire array (n-SiNW) was fabricated using a well-controlled, top-down nano-machining technique by combining photolithography and inductively coupled plasma reactive ion etching (ICP-RIE) at a cryogenic temperature. The array of nanowires ~1 µm in diameter and with the aspect ratio of ~10 was successfully prepared from commercial n-type silicon wafer. The half-cell LIB with free-standing n-SiNW electrode exhibited an initial Coulombic efficiency of 91.1%, which was higher than the battery with a blank n-silicon wafer electrode (i.e., 67.5%). Upon 100 cycles of stability testing at 0.06 mA cm−2, the battery with the n-SiNW electrode retained 85.9% of its 0.50 mAh cm−2 capacity after the pre-lithiation step, whereas its counterpart, the blank n-silicon wafer electrode, only maintained 61.4% of 0.21 mAh cm−2 capacity. Furthermore, 76.7% capacity retention can be obtained at a current density of 0.2 mA cm−2, showing the potential of n-SiNW anodes for high current density applications. This work presents an alternative method for facile, high precision, and high throughput patterning on a wafer-scale to obtain a high aspect ratio n-SiNW, and its application in LIBs.

A high performance lithium anode is a key component for high energy density lithium batteries. Silicon based lithium anode materials are attractive for the lithium anode due to their high theoretical capacity. However, a severe problem is the huge volume change that occurs during cycling, resulting in a poor capacity retention. We have developed a silicon based anode that disperses silicon particles on a carbon paper made from Manila hemp. The composite silicon electrode materials showed a high initial coulombic efficiency of 83%. The initial capacity of 566 mAh g−1 based on the total weight of the electrode was retained at 491 mAh g−1 after 70 cycles at the charge and discharge rate of 100 mA g−1 and at room temperature.

Silicon (Si) is regarded as the most promising anode material for high‐energy lithium‐ion batteries (LIBs) due to its high theoretical capacity, and low working potential. However, the large volume variation during the continuous lithiation/delithiation processes easily leads to structural damage and serious side reactions. To overcome the resultant rapid specific capacity decay, the nanocrystallization and compound strategies are proposed to construct hierarchically assembled structures with different morphologies and functions, which develop novel energy storage devices at nano/micro scale. The introduction of assembly strategies in the preparation process of silicon‐based materials can integrate the advantages of both nanoscale and microstructures, which significantly enhance the comprehensive performance of the prepared silicon‐based assemblies. Unfortunately, the summary and understanding of assembly are still lacking. In this review, the understanding of assembly is deepened in terms of driving forces, methods, influencing factors and advantages. The recent research progress of silicon‐based assembled anodes and the mechanism of the functional advantages for assembled structures are reviewed from the aspects of spatial confinement, layered construction, fasciculate structure assembly, superparticles, and interconnected assembly strategies. Various feasible strategies for structural assembly and performance improvement are pointed out. Finally, the challenges and integrated improvement strategies for assembled silicon‐based anodes are summarized. This review outlines the latest progress of silicon‐based assembled anodes from the aspects of assembly strategies, emphasizing the mechanism of the functional advantages for assembled structures. These summaries further deepen the understanding of the assembly mechanism and provide the systematic theoretical basis for the construction of superior silicon‐based anodes.

Currently, lithium‐ion batteries (LIBs) are at the forefront of energy storage technologies. Silicon‐based anodes, with their high capacity and low cost, present a promising alternative to traditional graphite anodes in LIBs, offering the potential for substantial improvements in energy density. However, the significant volumetric changes that silicon‐based anodes undergo during charge and discharge cycles can lead to structural degradation. Furthermore, the formation of excessive solid‐electrolyte interphases (SEIs) during cycling impedes the efficient migration of ions and electrons. This comprehensive review focuses on the structural design and optimization of micron‐scale silicon‐based anodes from both materials and systems perspectives. Significant progress is made in the development of advanced electrolytes, binders, and conductive additives that complement micron‐scale silicon‐based anodes in both half and full‐cells. Moreover, advancements in system‐level technologies, such as pre‐lithiation techniques to mitigate irreversible Li+ loss, have enhanced the energy density and lifespan of micron‐scale silicon‐based full cells. This review concludes with a detailed classification of the underlying mechanisms, providing a comprehensive summary to guide the development of high‐energy‐density devices. It also offers strategic insights to address the challenges associated with the large‐scale deployment of silicon‐based LIBs. The significant volume change of the silicon‐based anode during cycling can lead to its structural degradation and the formation of excess solid‐electrolyte interphases. For the above problems, this review focuses on the structural design and optimization of micron‐sized silicon‐based anodes from the perspectives of materials and systems, providing a comprehensive summary to guide the development of high‐energy‐density devices.

Silicon has garnered increased attention as a potential next-generation anode for lithium-ion batteries due to its abundant availability and remarkable theoretical specific capacity. This study utilizes a life cycle assessment approach to analyze the cradle-to-gate environmental implications of a 1 kWh lithium nickel manganese cobalt oxide battery featuring a carbon-coated silicon-graphite composite anode with varying silicon content ranging from 5 to 100%. The outcomes are compared with those of a 1 kWh graphite-lithium nickel manganese cobalt oxide battery. The findings indicate that within silicon-based LIBs, batteries with higher silicon content exhibit reduced environmental impacts due to their enhanced specific capacity. At 5% silicon, the life cycle impacts are comparable to those of graphite-based LIBs, and significant reductions in impacts can be achieved by increasing the silicon content. Moreover, emissions during the manufacturing phase can be reduced by adopting renewable energy sources or an energy mix that is less reliant on fossil fuels.

HighlightsSi/C Composite and Nanostructure Engineering: Advanced Si/C composites and multidimensional nanostructures address key challenges in silicon anodes, like volume expansion and unstable SEI, enhancing LIBs performance.Artificial SEI, Prelithiation, and Binders: Focus on stable artificial SEI layers, efficient prelithiation, and cutting-edge binders to improve Coulombic efficiency and reduce capacity loss, enhancing Si anode durability and efficiency.Real-World Application and Scalability: Analysis of these strategies highlights scalability and commercial viability, transitioning Si-anode technologies to practical, high-performance LIBs applications.Silicon (Si) has emerged as a potent anode material for lithium-ion batteries (LIBs), but faces challenges like low electrical conductivity and significant volume changes during lithiation/delithiation, leading to material pulverization and capacity degradation. Recent research on nanostructured Si aims to mitigate volume expansion and enhance electrochemical performance, yet still grapples with issues like pulverization, unstable solid electrolyte interface (SEI) growth, and interparticle resistance. This review delves into innovative strategies for optimizing Si anodes’ electrochemical performance via structural engineering, focusing on the synthesis of Si/C composites, engineering multidimensional nanostructures, and applying non-carbonaceous coatings. Forming a stable SEI is vital to prevent electrolyte decomposition and enhance Li+ transport, thereby stabilizing the Si anode interface and boosting cycling Coulombic efficiency. We also examine groundbreaking advancements such as self-healing polymers and advanced prelithiation methods to improve initial Coulombic efficiency and combat capacity loss. Our review uniquely provides a detailed examination of these strategies in real-world applications, moving beyond theoretical discussions. It offers a critical analysis of these approaches in terms of performance enhancement, scalability, and commercial feasibility. In conclusion, this review presents a comprehensive view and a forward-looking perspective on designing robust, high-performance Si-based anodes the next generation of LIBs.

Silicon offers a high theoretical specific capacity for anodic lithium storage. However, its applications are hindered by the electrode instability caused by the sharp volume change, and the limited rate performance resulted from the insulating property. Herein, we introduce a facile and fast method of preparing honeycomb‐like silicon‐based anodes (MXene‐Si@C) with porous structure using MXene and carbon‐coated silicon. The dual protection from both the surface coating and as‐formed interlayered vacant spaces ameliorate the volume expansion of the silicon and thus reinforce the mechanical stability of the electrode. In addition, the highly conducting MXene and the surface carbon coating form a hierarchical and consecutive electron‐conducting network with evidently reduced resistance. With this proposed composite, a high average Coulombic efficiency of 99.73% and high capacity retention of 82.4% after 300 cycles at 1 A/g can be achieved even with an areal loading around 1.5 mg/cm2. Coupled with an NCM523 cathode, the proof‐of‐concept full cell delivers a high capacity of 164.2 mAh/g with an extremely high energy density of 574 Wh/kg (based on the mass of the electrode materials) at 0.2 C and an excellent cyclability at 0.5 C of 100 cycles with decent capacity retention (80.28%). Silicon anodes usually suffer a short lifespan due to the sharp volume change. Herein, a comprehensive and efficient method is provided to acquire a hierarchical structure with dual protection on the Si particles, which enables ultrastable long‐term cycling stability and practical feasibility in the full batteries.

Nanoporous silicon is a promising anode material for high energy density batteries due to its high cycling stability and high tap density compared to other nanostructured anode materials. However, the high cost of synthesis and low yield of nanoporous silicon limit its practical application. Here, we develop a scalable, low-cost top-down process of controlled oxidation of Mg 2 Si in the air, followed by HCl removal of MgO to generate nanoporous silicon without the use of HF. By controlling the synthesis conditions, the oxygen content, grain size and yield of the porous silicon are simultaneously optimized from commercial standpoints. In situ environmental transmission electron microscopy reveals the reaction mechanism; the Mg 2 Si microparticle reacts with O 2 to form MgO and Si, while preventing SiO 2 formation. Owing to the low oxygen content and microscale secondary structure, the nanoporous silicon delivers a higher initial reversible capacity and initial Coulombic efficiency compared to commercial Si nanoparticles (3,033 mAh/g vs. 2,418 mAh/g, 84.3% vs. 73.1%). Synthesis is highly scalable, and a yield of 90.4% is achieved for the porous Si nanostructure with the capability to make an excess of 10 g per batch. Our synthetic nanoporous silicon is promising for practical applications in next generation lithium-ion batteries.

Silicon has attracted much attention as a promising anode material for lithium-ion batteries (LIBs) due to its high theoretical capacity and rich resource abundance. However, the practical battery use of Si is challenged by its low conductivity and drastic volume variation during the Li uptake/release process. Tremendous efforts have been made on shrinking the particle size of Si into nanoscale so that the volume variation could be accommodated. However, the bare nano-Si material would still pulverize upon (de)lithiation. Moreover, it shows an excessive surface area to invite unlimited growth of solid electrolyte interface that hinders the transportation of charge carriers, and an increased interparticle resistance. As a result, the Si nanoparticles gradually lose their electrical contact during the cycling process, which accounts for poor thermodynamic stability and sluggish kinetics of the anode reaction versus Li. To address these problems and improve the Li storage performance of nano-Si anode, proper structural design should be applied on the Si anode. In this perspective, we will briefly review some strategies for improving the electrochemistry versus Li of nano-Si materials and their derivatives, and show opinions on the optimal design of nanostructured Si anode for advanced LIBs.