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ACS Applied Engineering Materials · 2024 · IF 0

Fluorine-Doped Electrolyte and Artificial SEI for Enhanced Interfacial Stability in All-Solid-State Lithium Metal Batteries

Linfeng Peng,Tianyu Lei,Cong Liao,Shuai Chen,Shijie Cheng,Jia Xie

The poor lithium metal/solid electrolyte (SE) interface compatibility presents a considerable obstacle in the progression of all-solid-state lithium metal batteries (ASSLMBs). Constructing a robust solid electrolyte interphase (SEI) offers a favorable approach to alleviating these difficulties. Herein, we propose a dual strategy involving fluorine-doped electrolyte and artificial SEI to improve the lithium metal/Li5.5PS4.5Cl1.5 (LPSC) interface stability. X-ray photoelectron spectroscopy (XPS) results unveil the formation of a LiF-rich interphase at the SE/Li metal interface, facilitated by the reaction of Li metal with an F-doped electrolyte and fluoroethylene carbonate (FEC) treatment on the Li metal surface (FEC@Li). The F-doped electrolyte Li5.5PS4.5Cl1.45F0.05 (LPSCF-0.05) maintains a high ionic conductivity of 6.37 mS cm–1 at room temperature. Consequently, the critical current density (CCD) of the Li metal symmetric cell reaches 3.52 mA cm–2. Full cells assembled with NCM622, LPSCF-0.05, and FEC@Li exhibit superior cycling and rate performances along with excellent low-temperature performance. The battery delivers a high initial discharge capacity of 172.6 mAh g–1 at 0.2C under room temperature, cycling steadily for over 100 cycles. Under a high C-rate of 2C and a low temperature of −20 °C, the batteries display high capacities of 117.7 and 139.0 mAh g–1, respectively. This study offers an effective way of constructing high-performance ASSLMBs.

研究领域: 材料科学 · 电化学 · 能源存储 · 固态离子学 · 电池技术
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Journal of Materials Chemistry A · 2025 · IF 9.5

Biodegradable starch-based hydrogel as a multifunctional SEI for ultra-stable and flexible zinc-ion batteries

Zinan Wang,Tianxu Ji,Qilin Zhang,Peng Wang,Xiaoyu Yang,Shuo Zhang,Yuhang Jin,Xiaolong Fan,Jiaxuan Zhang,Wei Duan,Ying Yue,Yang Ju,Yunpeng Liu

Constructing an artificial solid electrolyte interface (SEI) layer is an effective strategy to suppress dendrite growth and corrosion in aqueous zinc batteries (AZBs). However, 2D material-based SEI coatings are generally non-biodegradable, posing environmental risks due to their persistence in soil. This research introduces a starch/polyacrylamide (STA/PAAm) hydrogel membrane developed as a self-healing SEI layer for AZBs. The incorporation of biomass-derived starch endows the STA/PAAm hydrogel with excellent soil biodegradability, achieving complete degradation within 21 days. Meanwhile, its dual-network structure, reinforced by reversible Al3+ crosslinking, offers robust mechanical resilience, self-healing ability, and high ionic conductivity—presenting a sustainable alternative to conventional SEI materials. Theoretical calculations reveal that the hydrogel modulates Zn2+ solvation, forming a stable [Zn(H2O)4(STA)(AAm)]2+ configuration, which suppresses hydrogen evolution and promotes uniform Zn2+ deposition along the (002) plane. The STA/PAAm-coated Zn anode exhibits an extended lifespan of over 3000 h at 2 mA cm−2, significantly surpassing that of bare Zn (531 h). Paired with an AlVO-NMP cathode, the pouch-type full cell retains 87.2% capacity after 2000 cycles at 5 A g−1 and demonstrates remarkable flexibility, powering LEDs under bending and folding conditions. This work bridges high-performance energy storage with environmental sustainability, offering a green paradigm for flexible batteries.

研究领域: 材料科学 · 储能技术 · 环境可持续性 · 电化学 · 高分子科学
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Energy Storage Materials · 2021 · IF 17.789

P2-Na0.55[Mg0.25Mn0.75]O2: An SEI-free anode for long-life and high-rate Na-ion batteries

Dongxiao Wang,Shuyin Xu,Jianlin Wang,Xiaohui Rong,Feiyu Zhou,Lifen Wang,Xuedong Bai,Bingan Lu,Chengjun Zhu,Yuesheng Wang,Yong-sheng Hu

Room-temperature Na-ion batteries have attracted great interest for over a decade owing to their natural abundance and similar intercalation chemistry with Li-ion. However, due to the uncontrolled decomposition of electrolyte and formation of solid electrolyte interphase, the large majority of sodium anode materials exhibit extremely low initial Coulombic efficiency and unsatisfactory cycling stability. Here we introduce a novel layered material, P2-Na 0.547 [M g 0.25 M n 0.75 ]O 2 , as an SEI-free negative electrode. This material, delivers a reversible capacity of 126 mAh g −1 with a high initial Coulombic efficiency of 108%, and capacity retention of ∼80% after 1000 cycles at 4C rate. Pairing with Na 3 V 2 (PO 4 ) 3 cathode, excellent rate performance of ∼60% capability at 15C, and extra-high initial Coulombic efficiency of 97% are achieved, all attributed to the SEI-free feature of Na 0.547 [M g 0.25 M n 0.75 ]O 2 . These results demonstrate the practical potential of our SEI-free anode material for high-power and long-life Na-ion batteries.

研究领域: 储能 · 材料科学 · 电化学 · 电池技术
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CHEMICAL ENGINEERING JOURNAL · 2020 · IF 10.652

1,2-dimethyl-3-propylimidazolium iodide as a multiple-functional redox mediator for Li-O2 batteries: In situ generation of a “self-defensed” SEI layer on Li anode

Dan Li,Changyan Zhu,Min Zhang,Ying Wang,Ziye Kang,Yulong Liu,Jun Liu,Jia Liu,Haiming Xie

How to develop a homogeneous redox mediator (RM) towards both ORR and OER and how to prevent the shuttle effect are two main issues for Li-O 2 batteries thus far. Here, we firstly report 1,2-dimethyl-3-propylimidazolium iodide (DMPII), which serves multiple functions as a RM for discharge capacity promotion, a RM for charge potential reduction, and a Li anode protector for shuttling suppression by in situ generating a “self-defensed” SEI layer. Benefiting from these advantages, a cell with DMPII displays a stable cyclability with a low terminal charge potential of ~3.6 V till the cell death, a considerable rate performance, and a good reversibility associated with Li 2 O 2 formation and degradation. Based on the experimental and density functional theory (DFT) calculation results, a working mechanism for a cell operation is also proposed. These results represent a promising progress in the development of multiple-functional RM for Li-O 2 batteries. Moreover, we expect that this work gives an insight into the in situ protection of Li metal anode for board applications ( e.g., Li-S batteries, all-solid-state Li-ion batteries, etc. ).

研究领域: 电化学 · 材料科学
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Journal of Energy Chemistry · 2020 · IF 7.216

Enabling high-performance all-solid-state lithium batteries with high ionic conductive sulfide-based composite solid electrolyte and ex-situ artificial SEI film

Jingguang Yi,Dan Zhou,Yuhao Liang,Hong Liu,Haifang Ni,Li-Zhen Fan

All-solid-state lithium batteries (ASSLBs) employing sulfide electrolyte and lithium (Li) anode have received increasing attention due to the intrinsic safety and high energy density. However, the thick electrolyte layer and lithium dendrites formed at the electrolyte/Li anode interface hinder the realization of high-performance ASSLBs . Herein, a novel membrane consisting of Li 6 PS 5 Cl (LPSCl), poly(ethylene oxide) (PEO) and Li-salt (LiTFSI) was prepared as sulfide-based composite solid electrolyte (LPSCl-PEO3-LiTFSI) (LPSCl:PEO = 97:3 wt/wt; EO:Li = 8:1 mol/mol), which delivers high ionic conductivity (1.1 × 10 −3 S cm −1 ) and wide electrochemical window (4.9 V vs. Li + /Li) at 25 °C. In addition, an ex-situ artificial solid electrolyte interphase (SEI) film enriched with LiF and Li 3 N was designed as a protective layer on Li anode (Li(SEI)) to suppress the growth of lithium dendrites. Benefiting from the synergy of sulfide-based composite solid electrolyte and ex-situ artificial SEI, cells of S-CNTs/LPSCl-PEO3-LiTFSI/Li(SEI) and Al 2 O 3 @LiNi 0.5 Co 0.3 Mn 0.2 O 2 /LPSCl-PEO3-LiTFSI/Li(SEI) are assembled and both exhibit high initial discharge capacity of 1221.1 mAh g −1 (135.8 mAh g −1 ) and enhanced cycling   stability with 81.6% capacity retention over 200 cycles at 0.05 C (89.2% over 100 cycles at 0.1 C). This work provides a new insight into the synergy of composite solid electrolyte and artificial SEI for achieving high-performance ASSLBs .

研究领域: 材料科学 · 电化学 · 能源存储 · 固态电池 · 界面工程
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ADVANCED MATERIALS · 2025 · IF 26.8

P-Block Compounds Incorporated into SEI Enable Ultra-Stable Cell Cycling in Low-Temperature Sodium-Metal Batteries

Sike Xie,Yujie Huang,Yanjian Xie,Wei Zhang,Yijian Zhong,Zhihao Liu,Zhixin Liang,Jintao Qi,Yangyang Huang,Jian Peng,Shaoming Huang

Sodium metal anodes (SMAs) are pivotal for high-energy-density batteries but suffer from uncontrolled dendrite growth and interfacial instability caused by infinite volume expansion and a fragile solid electrolyte interphase (SEI). Herein, an innovative strategy is proposed, in which a p-block matrix is in-situ formed from NiTe 2 nanocrystals onto N-doped carbon hollow microspheres (NiTe 2 @NC) during electrochemical activation to overcome these challenges. The p-block matrix with sodiophilic Na 2 Te and conductive metallic nickel effectively reduces the nucleation barrier and establishes bi-continuous ion/electron conduction networks, guiding uniform Na plating. Critically, Na 2 Te dominates the formation of a gradient inorganic-rich SEI with high Young's modulus and low Na⁺ diffusion barrier, significantly enhancing mechanical resilience and ion transport kinetics. Consequently, the NiTe 2 @NC electrode achieves exceptional cyclability (1,000 cycles at 1.0 mA cm − 2 /1.0 mAh cm − 2 with an average Coulombic efficiency of 99.79%). When configured in full-cells with a Na 4 Fe 3 (PO 4 ) 2 P 2 O 7 cathode, it maintains the capacity retention of over 96.1% (103.9 mAh g − 1 ) after 1,200 cycles at 10.0 C. Critically, the full-cell maintains superior electrochemical resilience with high discharge-capacity and >90% retention at low-temperatures (−20 and −40 °C), demonstrating exceptional practicality for sodium metal batteries. This work establishes a new paradigm for stabilizing reactive metal anodes via in-situ-constructed multifunctional interfaces.

研究领域: 储能与转换 · 电化学 · 材料科学 · 电池技术 · 纳米材料
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Journal of Materials Chemistry A · 2022 ·Vol. 10 ·期 41 ·21905-21911 · IF 14.511

A fluorinated SEI layer induced by a fire-retardant gel polymer electrolyte boosting lateral dendrite growth

Ziyue Wen,Zhikun Zhao,Ting Zhang,Yuanshen Wang,Jinxiang Zhang,Zhaoyang Sun,Li Li,Yuejiao Li,Feng Wu,Renjie Chen

Gel polymer electrolytes (GPEs) have attracted widespread attention for Li metal batteries (LMBs) due to their excellent processability and low cost. However, they are generally flammable and incompatible with the electrode, posing serious safety hazards. Herein, a high-safe electrolyte was successfully designed and fabricated by in situ introduction of a flame-retardant phosphate-based electrolyte into a robust polymer matrix. The facile in situ polymerization method adopted in this work effectively improves the contact between the electrolyte/electrode interface. Interestingly, the controlled formation and lateral growth of Li dendrites in deposition process was regulated by the fluorinated solid-electrolyte interphase (SEI) layer, enhancing the stability and safety of LMBs. Particularly, the components and distribution of the SEI were further studied by Fourier transform infrared (FTIR), FTIR-mapping and X-ray photoelectron spectroscopy (XPS) analysis to explore the mechanism of lateral dendrite growth. As expected, the Li metal is well protected, and the Li|Li symmetric batteries were stabilized for 2100 h under changing temperature conditions. This work provides fundamental insights into a facile method for preparing GPEs with potential applicability for next-generation flexible and safe energy-storage devices.

研究领域: 材料科学 · 电化学 · 能源存储
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ADVANCED MATERIALS · 2025 · IF 26.8

In Situ Formation of LiF-Rich SEI in Quasi-Solid Electrolytes Enables Long-Life Electrochromic Devices

Chunjian Wang,Shuling Xiang,Liang Chen,Lingyan Liang,Jiangping Tu,Shengcheng Shen,Hongtao Cao,Hongliang Zhang

Electrochromic devices (ECDs) offer significant energy-saving potential for applications such as smart windows and displays by modulating optical properties in response to electrical stimuli. However, their widespread adoption is limited by challenges associated with electrolyte stability and the formation of a robust solid-electrolyte interphase (SEI). In this study, a novel quasi-solid polymer electrolyte (QSPE) based on a UV-curable matrix of poly(ethylene glycol) diacrylate (PEGDA) incorporated with poly(vinylidene fluoride-trifluoroethylene-chlorofluoroethylene) [P(VDF-TrFE-CFE), abbreviated as PVTC] is presented. The high dielectric constant of PVTC facilitates lithium-ion transport, while electrochemical cycling triggers partial dehydrofluorination, thereby promoting in situ formation of a LiF-rich SEI layer on WO 3 surface. The optimized electrolyte exhibits excellent properties, including high optical transparency (88.7%), ionic conductivity (1.76 mS cm −1 ), and mechanical robustness. When applied in ECDs, PVTC enables outstanding performance, achieving 86.29% optical retention from the 5000th to the 40 000th cycle and 98.78% charge retention after 50 000 charge–discharge cycles. Furthermore, prototype demonstrations in smart windows and electrochromic sunglasses validate the scalability and flexibility of the proposed system, highlighting a promising strategy for advancing durable, high-performance ECDs through innovative electrolyte design.

研究领域: 材料科学 · 电化学 · 能量存储 · 智能器件
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Energy Storage Materials · 2020 · IF 16.28

In-situ organic SEI layer for dendrite-free lithium metal anode

Danmiao Kang,Saydual Sardar,Rui Zhang,Hart Noam,Jingyun Chen,Linge Ma,Wenbin Liang,Chunsheng Shi,John P. Lemmon

Lithium metal (Li) is the most promising anode for high energy density secondary battery system, but the dendrite growth makes it very dangerous for commercial application. An artificial SEI layer with high ionic conductivity and low electronic conductivity has proven to be an effective way to improve the stability of Li anode. Organic layer is introduced on Li surface by in-situ spontaneous reaction between Li and carboxylic acid. The as-formed carboxylate layer can effectively limit the Li deposition under it and suppress the dendrite growth. And the uniformity of the organic layer is the key factor for achieving stable cycling performance. With a homogenous carboxylate layer of 1 ​μm, the Li electrode can sustain 1000 ​h of charge-discharge cycling at 0.5 ​mA ​cm −2 . DFT calculation demonstrates that the enhanced absorption energy by oxygen atoms in lithium carboxylate contributes to the increased lithiophilicity and decreased depositing overpotential. This research provides a way for practical application of Li metal anode .

研究领域: 材料科学 · 电化学
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Energy & Environmental Science · 2023 ·Vol. 16 ·期 3 ·1166-1175 · IF 32.5

In situ formed uniform and elastic SEI for high-performance batteries

Mingyuan Gu,Apparao M. Rao,Jiang Zhou,Bingan Lu

The solid electrolyte interphase (SEI) is one of the most important components of a battery, and plays a crucial role in the battery performance. Here, a uniform and elastic SEI was constructed by in situ electro-polymerization (ISEP-SEI) of ionic liquid electrolytes. The excellent uniformity of ISEP-SEI and its excellent contact with the substrate could passivate the electrode surface effectively. At the same time, the superior elasticity of ISEP-SEI could enable the electrode to sustain a large number of volume changes during cycling and maintain its structural integrity. Both these features are essential for building high-performance batteries. With ISEP-SEI, the potassium metal symmetric batteries stably cycled for 5000 h with only a piece of separator and no special treatment of the potassium metal surface. Moreover, a Prussian Blue (PB) cathode matched with potassium metal operated for more than 3000 cycles at 1000 mA g−1. The graphite anode, which does not cycle stably in traditional electrolytes, can be operated for more than 1000 cycles after an ISEP-SEI formed on its surface. Importantly, the flame-retardant ionic liquid guaranteed the batteries' safety. The electrochemical performance of full batteries, PB||K batteries at high temperatures, and lithium batteries with ISEP-SEI have also been explored.

研究领域: 材料科学 · 电化学 · 能源存储
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ACS Applied Materials & Interfaces · 2023 · IF 9.5

Surface Chemistry-Controlled SEI Layer on Silicon Electrodes by Regulating Electrolyte Decomposition

Long Li,Chun Fang,Gang He,Yunhui Huang

Unstable solid electrolyte interface (SEI) layers induced by significant volume changes and subsequent side reactions at the interface have prevented Si anodes from practical application in lithium-ion batteries. The interface stability plays an important role in the electrochemical performance of Si electrodes. Here, we modify the interface of a Si electrode with ion-conductive poly(ethylene glycol) diglycidyl ether (PEGDE), which controls the electrolyte decomposition route and stabilizes the SEI layer. It enables the Si electrode to achieve a capacity of more than 1800 mAh g–1 at a current density of 2 A g–1, with a capacity retention of 77.25% after 300 cycles. The PEGDE-decorated Si electrode also shows greatly improved rate capability, with specific capacity up to 777 mAh g–1 even at 20 A g–1. We demonstrate that PEGDE decoration greatly increases the Li2CO3 ratio in the SEI layer, which improves the interface stability and Li+ conductivity and hence suppresses continuous electrolyte decomposition. As a result, the structural integrity of the Si particles is maintained and capacity fading is retarded. This work reveals that surface design can effectively regulate the SEI layer composition and improve interface stability, which is a promising strategy for Si-electrode manufacture.

研究领域: 电化学 · 材料科学 · 能量存储 · 电池技术
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ELECTROCHIMICA ACTA · 2026 · IF 5.8

Fluorobenzosilane additive derived low-impedance SEI enables high-rate capacity of graphite anode

Xue Chen,Chengfeng Li,Shuai Chen,Xinzi Shi,Changyong Mo,Youhao Liao,Weishan Li

TPS containing -F/-Si bifunctional group exhibits superior film-forming capability. • A thin and uniform SEI film rich in LiF and Li x PO y F z is formed on graphite surface. • TPS-derived SEI film shows low impedance and high-temperature structural stability. • Li/graphite cell with TPS yields improved high-rate capacity and cyclic stability. As a mainstream anode material for lithium-ion batteries (LIBs), graphite suffers from undesirable interfacial reactions that damage its layered structure due to insufficient stability of solid electrolyte interphase (SEI) during prolonged lithiation/delithiation processes. To overcome the challenges associated with graphite-based LIBs, forming a stable SEI film through film-forming additives has emerged as a preferred optimization strategy. In this work, the triethoxy(pentafluorophenyl)silane (TPS) additive, enriched with -F/-Si dual functional groups, significantly enhances both the high-rate capacity and cyclic stability of graphite batteries. Addition of 1 wt% TPS boosts the rate capacity and cyclic stability of assembled batteries. Notably, the specific charge capacity of Li/graphite battery at 2 C rate increased from 81.9 mAh g⁻ 1 in baseline to 158.8 mAh g⁻ 1 , with a capacity retention of 98.7% after 250 cycles at 0.2 C, far exceeding the 61.4% of baseline system. Theoretical calculations and experimental results indicate that TPS preferentially adsorbs and reduces on graphite surface to construct a low-impedance organic/inorganic composite SEI film, suppressing electrolyte decomposition, accelerating Li + kinetics, and preserving electrode integrity. This study provides a novel approach for the precise design of interface for commercial graphite anodes by developing simple and efficient electrolyte film-forming additives, thereby offering technical and theoretical support for the sustainable application of long-life graphite-based batteries. Download: Download high-res image (241KB) Download: Download full-size image

CAS / MDL: 20083-34-5
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