硅基负极预锂化技术的研究进展、关键挑战与发展趋势

doi:10.6023/A26050153

化学学报 ›› 2026, Vol. 84 ›› Issue (10): 1664-1678.DOI: 10.6023/A26050153 上一篇下一篇

综述

硅基负极预锂化技术的研究进展、关键挑战与发展趋势

王也, 周俊杰, 许崇^*(), 李永峰^*()

中国石油大学(北京) 重质油全国重点实验室北京 102249

投稿日期:2026-05-09 发布日期:2026-08-07

作者简介:

王也, 中国石油大学(北京)材料科学与工程学院博士研究生, 已发表SCI论文15篇, 申请国家发明专利2项, 曾获得国家奖学金等荣誉, 研究方向为高性能硅基负极材料、单壁碳纳米管开发等, 并参与相关材料体系的中试开发工作, 熟悉从实验室基础研究到工程化放大的关键流程.

周俊杰, 男, 中国石油大学(北京) 材料科学与工程学院材料科学与工程专业本科生. 主要从事锂离子电池硅基负极材料、碳包覆与界面工程、锂离子电池粘结剂等方面的研究.

许崇,中国石油大学(北京)副教授，校青年拔尖人才. 从事锂电池电解液设计及电极材料设计研究, 主持国家自然科学基金、校青年拔尖人才项目等; 累计已发表论文50余篇, 其中以第一作者/通讯作者在Energy Environ. Sci.、ACS Nano、Nano Lett.、Energy Storage Mater. (3篇)、Small、Chem. Eng. J. (5篇)、J. of Colloid and Interf. Sci. (5篇)等期刊发表SCI论文30余篇; 授权专利4项, 申请专利10项.

李永峰, 教授, 博士生导师, 材料科学与工程学院院长. 首批海外高层次人才入选者, “国家优秀青年基金”获得者. 北京市昌平区政协委员, 中国颗粒学会第六、七届理事会理事, 中国复合材料学会矿物复合材料专业委员会副主任, 第七届石墨及石墨材料产业专业委员会理事等.

基金资助:
国家自然科学基金(22238012); 国家自然科学基金(22408398); 中国石油大学(北京)科学基金(2462025BJRC006); 中国石油大学(北京)科学基金(2462026PTJS011); 中国石油大学(北京)科学基金(SKLHOP20260109); 中国石油大学(北京)科学基金(ZLDXYC2026003)

Research Progress, Key Challenges, and Future Perspectives of Prelithiation Technologies for Silicon-Based Anodes

Ye Wang, Junjie Zhou, Chong Xu^*(), Yongfeng Li^*()

State Key Laboratory of Heavy Oil Processing, College of Materials Science and Engineering, China University of Petroleum, Beijing 102249, China

Received:2026-05-09 Published:2026-08-07
Contact: *E-mail: chongxu@cup.edu.cn; yfli@cup.edu.cn
Supported by:
National Natural Science Foundation of China(22238012); National Natural Science Foundation of China(22408398); Science Foundation of China University of Petroleum, Beijing(2462025BJRC006); Science Foundation of China University of Petroleum, Beijing(2462026PTJS011); Science Foundation of China University of Petroleum, Beijing(SKLHOP20260109); Science Foundation of China University of Petroleum, Beijing(ZLDXYC2026003)

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摘要/Abstract

硅基负极具有高理论比容量, 是提升锂离子电池能量密度的重要候选材料, 但其首次不可逆锂损失、固态电解质界面(SEI)持续形成和体积效应会显著降低首次库仑效率并削弱循环稳定性. 预锂化可在电极制备、装配或化成阶段引入额外活性锂, 用于补偿首圈锂消耗并改善全电池可利用锂库存. 全文按照作用位置与锂源引入路径, 将硅基负极预锂化技术归纳为负极侧预锂化、正极侧预锂化以及电芯级预锂化与界面调控策略三类; 其中, 负极侧预锂化进一步分为直接接触预锂化、负极补锂添加剂和化学预锂化, 直接接触预锂化又可按照接触/回路构型细分为内部短路、外部短路和复合层预锂化. 重点比较了不同技术在补锂效率、均匀性、界面调控、空气稳定性、安全性、工艺复杂度和产业适配性方面的差异. 最后, 围绕精准补锂、界面稳定、补锂剂环境耐受性、连续化制造和材料-工艺-设备协同设计等关键问题, 总结了硅基负极预锂化技术的发展趋势.

关键词: 硅基负极, 预锂化技术, 直接接触预锂化, 负极补锂添加剂, 化学预锂化, 正极侧预锂化, 界面调控

Silicon-based anodes are promising candidates for high-energy-density lithium-ion batteries, but their initial irreversible lithium loss, continuous solid electrolyte interphase (SEI) formation, and volume variation reduce the initial Coulombic efficiency and undermine cycling stability. Prelithiation introduces additional active lithium before electrode fabrication, cell assembly, or formation to compensate first-cycle lithium consumption and improve the usable lithium inventory of full cells. This review classifies prelithiation technologies for silicon-based anodes according to the compensation location and lithium-source introduction pathway, including anode-side prelithiation, cathode-side lithium compensation, and separator/cell-level integrated strategies. Within anode-side prelithiation, direct-contact routes are subdivided into internal short-circuit, external short-circuit, and composite-interlayer prelithiation, and are discussed together with anode-additive and chemical prelithiation; cathode-side lithium compensation and separator/cell-level integrated strategies are compared in terms of compensation efficiency, uniformity, interfacial regulation, air stability, safety, processing complexity, and manufacturing compatibility. Key challenges and future directions are discussed with emphasis on precise lithium compensation, interface stabilization, environmental tolerance of prelithiation reagents, continuous manufacturing, and coordinated materials-process-equipment design.

Key words: silicon-based anodes, prelithiation technology, direct-contact prelithiation, anode prelithiation additives, chemical prelithiation, cathode-side prelithiation, interfacial engineering

引用此文

王也, 周俊杰, 许崇, 李永峰. 硅基负极预锂化技术的研究进展、关键挑战与发展趋势[J]. 化学学报, 2026, 84(10): 1664-1678.

Ye Wang, Junjie Zhou, Chong Xu, Yongfeng Li. Research Progress, Key Challenges, and Future Perspectives of Prelithiation Technologies for Silicon-Based Anodes[J]. Acta Chimica Sinica, 2026, 84(10): 1664-1678.

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图/表 11

图1. 锂离子电池预锂化效果

Figure 1. Schematic of the effect of prelithiation in LIBs

图2. 综述示意图

Figure 2. Schematic diagram for this review

图3. 直接接触预锂化代表性策略: (a)锂网集成原位预锂化[14]; (b) c-SiOx电极电短接/电化学可控预锂化及卷对卷工艺[15]; (c) SiO/Gr复合负极与锂铜复合带的激光图案化[16]; (d) Si薄膜的固态化学/电化学腐蚀预锂化(SCC/SEC)[17]; (e)超薄锂箔直接接触预锂化示意[18]; (f)高/低Li+浓度介质对电极预锂化行为的影响[19]; (g)单面预锂化石墨电极的制备流程[20]

Figure 3. Representative direct-contact prelithiation strategies: (a) in situ prelithiation by directly integrating lithium mesh[14]; (b) electrical short-circuit/electrochemically controlled prelithiation of c-SiOₓ electrodes and the roll-to-roll process[15]; (c) laser-patterned SiO/Gr composite anode coupled with Li-Cu composite tape[16]; (d) solid-state chemical/electrochemical corrosion prelithiation (SCC/SEC) of Si thin films[17]; (e) direct-contact prelithiation using ultrathin lithium foil[18]; (f) effect of high- and low-Li+ concentration media on electrode prelithiation behavior[19]; (g) fabrication process of single-side prelithiated graphite electrodes[20]

图4. 负极补锂添加剂代表性策略: (a) A-LixSi表面钝化负极补锂试剂的制备[28]; (b)脱氢驱动的无锂金属预锂化相变示意图[29]; (c) LESG锂预储和制造工艺示意图[30]

Figure 4. Representative anode-side prelithiation additive strategies: (a) preparation of surface-passivated A-LiₓSi anode prelithiation reagent[28]; (b) schematic illustration of the dehydrogenation-driven phase transformation for Li-metal-free prelithiation[29]; (c) schematic illustration of the lithium pre-storage and fabrication process of LESG[30]

图5. 化学预锂化代表性策略: (a)使用Li-芳烃(4,4'-二甲基联苯)对Si/SiOx预锂化前后的锂化/脱锂模型[33]; (b)使用有机锂化合物(Li-9,9-二甲基-9H-芴四氢呋喃)对SiO基负极进行预锂化流程图[34]; (c) SLMP-SiOx/C和LiBp-SiOx/C的合成过程和内应力的示意图[35]; (d)化学预锂化的常见过程[36]

Figure 5. Representative examples of chemical prelithiation: (a) lithiation/delithiation behavior of Si/SiOx before and after prelithiation with Li-arene (4,4'-dimethylbiphenyl)[33]; (b) flowchart of the Prelithiation process for SiO anodes using an organolithium compound (Li-9,9-dimethyl-9H-fluorenyl tetrahydrofuran complex)[34]; (c) schematic illustration of the synthesis process and internal stresses for SLMP-SiOx/C and LiBp-SiOx/C[35]; (d) the common process involved in chemical prelithiation[36]

图6. 化学预锂化的典型界面工程策略: (a)稳定μSiO的化学预锂化和界面工程示意图[38]; (b)化学预锂化及原位富无机界面构建示意图[39]; (c) ZNP-SiOx负极的SEI结构示意图[40]; (d) Si@LiF-x的合成示意图[41]; (e)合成锂补偿和碳涂层的Li-SiO@C样品工作流程[42]; (f) LiF/Li-SiO/C预锂化过程示意图[43]

Figure 6. Representative interfacial engineering strategies in chemical prelithiation: (a) schematic diagram of chemical prelithiation and interphase engineering for stabilizing μSiO[38]; (b) schematic diagram of chemical prelithiation and in situ inorganic-rich interphase pre-construction[39]; (c) schematic illustration of the SEI structure on the ZNP-SiOx anode[40]; (d) schematic synthesis of Si@LiF-x[41]; (e) experimental workflow for synthesizing the lithium-compensated and carbon-coated Li-SiO@C sample[42]; (f) schematic diagram of the LiF/Li-SiO/C prelithiation process[43]

图7. 正极侧补锂剂代表性策略: (a)基于在Li2NiO2表面进行LiTaO3包覆的工艺示意图[44]; (b)裸NCM811和LFO涂层NCM811的无锂阳极ASSB示意图[45]; (c)高能球磨制备CLO预锂化剂的示意图[46]; (d) N-Li2CO3的合成及正极侧补锂示意图[47]

Figure 7. Representative cathode-side lithium-compensation strategies: (a) schematic illustration of the process based on LiTaO3 coating on the surface of Li2NiO2[44]; (b) schematic illustration of anode-free ASSBs using bare NCM811 and LFO-coated NCM811[45]; (c) schematic illustration of the preparation of the CLO prelithiation agent by high-energy ball milling[46]; (d) schematic illustration of the synthesis of N-Li2CO3 and cathode-side lithium compensation[47]

图8. 正极侧补锂剂代表性策略: (a)高能球磨制备Co-Li2CO3@LCO预锂化试剂的示意图[50]; (b) Li2C2O4@Co3O4-QDs/CNTs的合成示意图[51]; (c) Li2S-LiI的合成示意图[52]; (d) LBO的示意图[53]

Figure 8. Representative lithium-salt-based cathode-side lithium-compensation strategies: (a) schematic illustration of the preparation of the Co-Li2CO3@LCO prelithiation reagent by high-energy ball milling[50]; (b) schematic illustration of the synthesis of Li2C2O4@Co3O4-QDs/CNTs[51]; (c) schematic illustration of the synthesis of Li2S-LiI[52]; (d) schematic illustration of LBO[53]

类别	代表体系与稳定性	主要问题与改性策略
富锂过渡金属氧化物	Li₂NiO₂、Li₆CoO₄; 空气/湿气稳定性较差	易释氧、开裂和界面副反应; 可采用LiTaO₃包覆、元素调控和表面钝化^[44,46]
Li₅FeO₄及衍生物	Li₅FeO₄、Mn掺杂LFO、LFO涂层; 稳定性中等	电子/离子传输与残余相影响界面; 可采用Mn掺杂、功能涂层和界面保护耦合^[45,49]
碳酸盐型补锂剂	Li₂CO₃、Co-Li₂CO₃; 空气稳定性较好	活化电位高、导电性差; 可通过富晶界纳米化、Co掺杂和晶格缺陷活化^[47,50]
草酸盐型补锂剂	Li₂C₂O₄; 空气稳定性较好, 固体残余少	分解电位偏高、动力学迟缓; 可采用Co₃O₄量子点催化和CNT导电网络^[51]
硫化物/硼酸盐体系	Li₂S-LiI、LBO; 体系差异大, LBO空气暴露8 d后仍保留约70%容量	关注离子输运、固态界面和壳层稳定; LiI复合或Li₂CO₃/无定形碳壳层可改善稳定性^[52-53]

表1. 代表性正极侧补锂剂的空气稳定性与改性策略比较

Table 1. Comparison of the air stability and modification strategies of representative cathode-side prelithiation additives.

图9. 电芯级预锂化与界面调控代表性策略: (a) FSP工业制造示意图[54]; (b) LixPAA 粘结剂的合成方案与化学结构[55]; (c)脱锂过程中SiO和SiO@Fe电极中电子转移的界面和接触性质图示[56]; (d)预锂化PL-SiNP/LIG复合负极的制备[57]

Figure 9. Representative cell-level prelithiation and interfacial regulation strategies: (a) industrial manufacture of FSP[54]; (b) synthesis route and chemical structure of the LiₓPAA binder[55]; (c) interfacial/contact characteristics of electron transfer in SiO and SiO@Fe electrodes during delithiation[56]; (d) preparation of prelithiated PL-SiNP/LIG composite anodes[57]

预锂化方式		电极材料	量化性能				参考文献
预锂化方式		电极材料	容量	ICE/%	循环寿命	容量保持率/%	参考文献
直接接触	超薄锂箔	Si	—	191.64%	910	74.00%	[18]
	外部短路	SiO	1369.3 mAh•g^－1	94.9%	100	74.3%	[15]
	SEC复合层	Si	—	94.13%	135	86.70%	[17]
负极添加剂	SLMP	Si	1500~2500 mAh•g^－1	≈100%	50	93%	[31]
	LiH	SiO	1203 mAh•g^－1	90.5%	300	38.5%	[29]
	LESG	Si	620 mAh•g^－1	116%	413	≈89%	[30]
化学预锂化	Li-DMBP/HFPN	SiO	1064.1 mAh•g^－1	99.57%	350	90.67%	[38]
	Bp-Li/2-MeTHF	SiO	≈800 mAh•g^－1	91.0%	500	92.2%	[42]
	反应器＋NF₃	SiO	1476 mAh•g^－1	93.2%	200	96.1%	[43]
正极添加剂	LiTaO₃@Li₂NiO₂	SiO	194.4 mAh•g^－1	78.2%	200	84.5%	[44]
	Co-Li₂O/CLO	SiO	197.2 mAh•g^－1	61.0%	1000	92%	[46]
	Li₂S-LiI	Si	194.0 mAh•g^－1	72.1%	100	87.4%	[52]
其他	Fe纳米团簇	SiO	1950.8 mAh•g^－1	87.2%	275	66.7%	[56]
	Li_xPAA粘结剂	SiO	141 mAh•g^－1	≈70%	100	77.3%	[55]
	激光集成	Si	>1700 mAh•g^－1	>97%	2000	>98%	[57]

表2. 代表性预锂化方法的量化性能比较a

Table 2. Quantitative performance comparison of representative prelithiation methods

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硅基负极预锂化技术的研究进展、关键挑战与发展趋势

Research Progress, Key Challenges, and Future Perspectives of Prelithiation Technologies for Silicon-Based Anodes

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