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ADVANCED FUNCTIONAL MATERIALS · 2023 ·Vol. 33 ·期 36 ·2303020 · IF 19

In Situ Artificial Hybrid SEI Layer Enabled High-Performance Prelithiated SiOx Anode for Lithium-Ion Batteries

Yi Sun,Kuanxin Zhang,Run Chai,Yueda Wang,Xianhong Rui,Kang Wang,Huaxia Deng,Hongfa Xiang

Considered the promising anode material for next-generation high-energy lithium-ion batteries, SiO x has been slow to commercialize due to its low initial Coulombic efficiency (ICE) and unstable solid electrolyte interface (SEI) layer, which leads to reduced full-cell energy density, short cycling lives, and poor rate performance. Herein, a novel strategy is proposed to in situ construct an artificial hybrid SEI layer consisting of LiF and Li 3 Sb on a prelithiated SiO x anode via spontaneous chemical reaction with SbF 3 . In addition to the increasing ICE (94.5%), the preformed artificial SEI layer with long-term cycle stability and enhanced Li + transport capability enables a remarkable improvement in capacity retention and rate capability for modified SiO x . Furthermore, the full cell using Li(Ni 0.8 Co 0.1 Mn 0.1 )O 2 and a pre-treated anode exhibits high ICE (86.0%) and capacity retention (86.6%) after 100 cycles at 0.5 C. This study provides a fresh insight into how to obtain stable interface on a prelithiated SiO x anode for high energy and long lifespan lithium-ion batteries.

研究领域: 电化学 · 材料科学 · 能源存储 · 锂离子电池 · 界面化学 · 纳米材料
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CHEMICAL ENGINEERING JOURNAL · 2020 · IF 10.652

Volume expansion restriction effects of thick TiO2/C hybrid coatings on micro-sized SiOx anode materials

Fei Dou,Yuehua Weng,Guorong Chen,Liyi Shi,Hongjiang Liu,Dengsong Zhang

In this work, novel SiO x anode materials with low volume expansion and high ionic/electrical conductivity are designed by combining internal buffer space and external super thick TiO 2 /C hybrid shell of 200–400 nm. An electrochemical reaction visualizing confocal system is originally developed for characterizing electrode thickness changes, and the real-time quantitative change of electrode thickness during charging and discharging is realized. Surprisingly, the maximum thickness expansion of designed anodes with the specific capacity of 1006.2 mA h g −1 is only 37% in the first lithiation process. Subsequently, the designed anodes present stable cycle life of the capacity attenuation of 7.83% after 100 cycles compared with the capacity of 5 th cycle. It demonstrates that the designed thick TiO 2 /C hybrid coatings effectively swing the expansion stress of micro-sized SiO x to internal space. This work proves that the huge volume expansion of micro-sized SiO x particles can be controlled by reasonable design of surface hybrid coatings and bulk structure, and the long lifespan can be maintained. This strategy paves a way for the development of micro-sized SiO x anode materials with long cycle life and good process ability for high energy density lithium-ion batteries.

研究领域: 材料科学 · 能源存储技术
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ELECTROCHIMICA ACTA · 2021 · IF 6.901

A facile and scalable Fe-Cr decorating strategy to boost the lithium storage of SiOx anode

Xiaozhong Zhou,Zhaoyi Qi,Yuyuan Jiang,Pengfei Yan,Juanxia Ding,Haiyan Wang,Hongkai Lu,Dongxu Liu,Kaifa Dong,Yougen Tang,Dongfei Sun,Ziqiang Lei

SiO x is regarded as a promising anode material for the next-generation lithium-ion batteries with high energy density. However, the reduplicative volume changes during cycling cause the pulverizations of Si, leading to decreased utilization of active Si component and poor cycling performance. Herein, a facile and scalable Fe-Cr decorating strategy is reported to boost the lithium storage of SiO x anode. Our comprehensive characterizations indicate that there are strong interactions between Fe-Cr and SiO x during a facile ball milling process. After cycling, Fe-Cr nanoparticles are dispersed in the in-situ formed lithium silicates and Li 2 O matrix, which can maintain superior conductivity of lithium ion and electron for the active components through point-to-point connections. This unique structure boosts the electrochemical de-alloying process of the low-valent Li x Si (0 ≤  x  ≤ 2), and increases effective utilization of the active Si component during cycling, resulting in improvement of reversible capacity and cycling stability. This bm SiO x -FeCr electrode can deliver high reversible specific capacity (1370 m Ah g −1 at 200 mA g −1 ), good rate capability (653.8 m Ah g −1 at 2000 mA g −1 ), and superior cycling stability. This work provides a promising route for improving the utilization of active Si component and the structural stability of SiO x -based anodes.

研究领域: 材料科学 · 电化学 · 纳米材料 · 能源存储 · 电池技术 · 固态物理
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ACS Applied Materials & Interfaces · 2024 · IF 8.3

A Fast Self-Healing Binder for Highly Stable SiOx Anodes in Lithium-Ion Batteries

Manyuan Xu,Xiujuan Wei,Ziqiao Yan,Jinqiu Huang,Shuxing Wu,Kai-Hang Ye,Zhan Lin

Silicon oxide-based (SiOx-based) materials show great promise as anodes for high-energy lithium-ion batteries due to their high specific capacity. However, their practical application is hindered by the inevitable volumetric expansion during the lithiation/delithiation process. Constructing high-performance binders for SiOx-based anodes has been regarded as an efficient strategy to mitigate their volume expansion and preserve structural integrity. In this work, we propose a green water-solution PAA-LS binder composed of poly(acrylic acid) (PAA) and sodium lignosulfonate (LS) with fast self-healing properties. The designed binder can be restored due to the strong affinity between Fe3+-catechol coordination bonds, thereby effectively alleviating the volumetric strain of SiOx-based anodes. Notably, with an optimized LS content of 0.5%, the SiOx@PAA-LS electrode exhibits excellent performance, delivering a high capacity of 997.3 mAh g–1 after 450 cycles at 0.5 A g–1. Furthermore, the SiOx||NCM622 full cell also demonstrates superior cycling stability, maintaining a discharge capacity of 147.58 mAh g–1 after 100 cycles at 0.5 A g–1, with an impressive capacity retention rate of 82.72%.

研究领域: 材料科学 · 电化学 · 能源存储
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ACS Applied Energy Materials · 2023 · IF 6.4

Chemical Pre-lithiation of SiOx Anodes with a Weakly Solvating Solution of Polycyclic Aromatic Hydrocarbons for Lithium-Ion Batteries

Xin Li,Cancan Bian,Jun Zhang,Jian Hong,Rusheng Fu,Xufeng Zhou,Zhaoping Liu,Guangjie Shao

Silicon monoxide (SiOx, x ∼ 1) has emerged as a highly promising candidate for high-energy-density lithium-ion batteries due to its high specific capacity and suitable working potential. Nevertheless, the formation of a large quantity of irreversible products, such as Li2O and lithium silicates, during the initial lithiation process results in a low initial coulombic efficiency (ICE) of SiOx, which is a significant impediment to its commercial application. To overcome this limitation, two lithium aromatic complexes, namely, lithium-naphthalene-2-methyl-tetrahydrofuran (N-LAC) and lithium-biphenyl-2-methyl-tetrahydrofuran (B-LAC), with a low redox potential are used to pre-lithiate SiOx anodes. The differences in lithiation kinetics and efficacy of the two LAC solutions are identified and assessed by scrutinizing the pre-lithiation process of SiOx materials. It is revealed that both pre-lithiation agents produce solid electrolyte interphase (SEI) films on the material surface enriched with substances such as LiF, Li2CO3, and ROCO2Li, but the LiF content in the SEI of the N-LAC pre-lithiated electrode is significantly higher. Furthermore, the surface roughness of the N-LAC pre-lithiated electrode is lower, and the horizontal distribution of mechanical properties and surface potential tend to be more homogeneous, even during cycling, at approximately the same degree of lithiation. The results indicate that the N-LAC solutions not only improve the ICE of the SiOx material but also optimize the interfacial and structural stability of the SiOx electrode. When the pre-lithiated SiOx anode is paired with lithium-rich layered oxide cathode materials, the energy density and ICE are significantly improved compared to the cell using pristine SiOx anode.

CAS / MDL: 96-47-9
研究领域: 材料科学 · 电化学 · 电池技术
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