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Inorganic Chemistry Frontiers · 2025 · IF 6.4

Crosslinked ion-conducting hybrid coating layers for robust artificial solid-electrolyte interphase towards high-performance silicon anodes

Yuhui Weng,Xingyu Sun,Siying Li,Zhuoying Wu,Ziwei Chen,Yongqun Ma,Zefan Zheng,Feng Lin,Ming Zhang,Kejun Zhang,Min Ling,Keli Yang,Chengdu Liang,Jun Chen

High-capacity silicon (Si)-based anodes have been recognized as particularly promising candidates for high-energy-density lithium-ion batteries (LIBs). Rational design and tailoring of an artificial interface for Si anodes can effectively mitigate volume expansion, suppress detrimental side reactions, and enhance lithium-ion (Li+) diffusion kinetics—three critical factors widely acknowledged as fundamental prerequisites for enabling long-term cycling stability and fast-charging capabilities. Therefore, we introduced an organic/inorganic composite interface design strategy combining high elasticity and ion-conductive properties. Lithium metasilicate (LMS) not only functions as an effective protective layer and Li+ conductor but also inhibits lithium hexafluorophosphate (LiPF6) hydrolysis to suppress the generation of corrosive hydrofluoric acid (HF). When integrated with carboxyl-rich polyacrylic acid (PAA), the nanocomposite coating layer demonstrates high elasticity to accommodate volume expansion, establishes continuous Li+ diffusion pathways, and promotes the formation of a robust lithium fluoride (LiF)-rich artificial solid-electrolyte interphase (SEI). Consequently, the as-developed Si@PL-10 electrode demonstrates significantly enhanced cycling performance (2297 mAh g−1 after 200 cycles at 1 A g−1) and high-rate capability (1854 mAh g−1 at 6 A g−1). This work provides valuable insights for designing scalable multifunctional coatings for high-performance Si anodes.

CAS / MDL: 9004-32-4
研究领域: 储能技术 · 材料科学 · 电化学 · 纳米技术 · 电池技术
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY · 2019 · IF 3.218

Multi-functional carbon integrated rGO-Fe3O4@C composites as porous building blocks to construct anode with high cell capacity and high areal capacity for lithium ion batteries

Zhi-Chao Xiao,Yan Li,Cheng-Lu Liang,Yang Liu,Rui-Ying Bao,Ming-Bo Yang,Wei Yang

For lithium ion batteries (LIBs), a high cell capacity, which requires both a high capacity and a high loading mass of active materials, is crucial for practical application. However, how to fabricate efficient anodes with high cell capacity and high areal capacity remains a challenge. To solve this issue, we design a structure of porous building block composed of multi-functional carbon integrated rGO-Fe 3 O 4 @C composites. The carbon shell of Fe 3 O 4 @C derived from polydopamine (PDA) acts as an artificial solid electrolyte interface (SEI) film to avoid the excessive SEI formation, within which there are sufficient lithium ion diffusion pathways derived from the spaces between Fe 3 O 4 nanocrystals. The carbon derived from the in-situ polymerized polyacrylamide and rGO act as a glue to integrate the as-obtained Fe 3 O 4 @C composites to form the porous building blocks. Due to the compact stacking of building blocks, the composite electrode achieves a high active material loading mass of 5.94   mg (5.25   mg   cm −2 ), while maintains a satisfying capacity (685   mAh   g −1 after the 100th cycle at 0.5   A   g −1 ) and good rate performance (440   mAh   g −1 at 3   C). Therefore, a high cell capacity (4.02   mAh) and a high areal capacity (3.6   mAh   cm −2 ) at 2.62   mA   cm −2 in a single CR2032 coin cell are achieved.

CAS / MDL: 62-31-7 77-86-1
研究领域: 材料科学 · 电化学 · 能源存储
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Functional Materials Letters · 2024 · IF 1.2

The study of electrochemical stabilization mechanism of Pt, GC, SS304, Ti and Cu as current collectors for aqueous lithium-ion batteries by electrochemical approaches

Shenwei Zhang,Dongrui Chen,Wenmin Guo,Xiaoming Wang,Zhibin Ding,Xiaofu Tang,Junxia Zhang,Haijiang Wu,Diping Zeng,Hongqing Wei,Wenjun Wang,Yi Ma,Jinhua Zhou,Zaijun Su

This paper employs electrochemical methods (linear sweep voltammetry (LSV) and electrochemical impedance spectroscopy (EIS)) to investigate the electrochemical behavior of platinum, glassy carbon, 304 stainless steel, titanium, and copper in 21 and 1 M LiTFSI electrolytes. The LSV results indicate that the electrochemical stability window of the materials varies with the electrolyte concentration, and the stability window is wider in the high-concentration system. Through Tafel polarization curves and EIS analysis, the overpotential of the charge exchange process differs due to the type of material and the concentration of the electrolyte, mainly attributed to the influence of the proportion of free water, electrolyte viscosity, and SEI film formation on electrode process kinetics. After comparative analysis, glassy carbon exhibits a higher overpotential than other materials at both the cathode and anode, effectively suppressing water decomposition. These findings provide theoretical support for the development of high-performance aqueous lithium-ion battery current collector materials.

研究领域: 电化学 · 储能 · 材料科学 · 电池技术
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ChemElectroChem · 2022 ·Vol. 9 ·期 24 ·e202200957 · IF 4.782

A Quasi-Solid Electrolyte by In Situ Polymerization of Selective Solvent for Lithium-Metal Batteries

Jin Wang,Chengzhou Tao,Jiaming Cao,Xiaoxia Jiao,Lina Wang,Tianxi Liu

Graphical A viable quasi-solid electrolyte by an in situ polymerization process of polyethylene glycol methyl ether acrylate for Li-metal batteries is demonstrated, and the LiF-rich solid electrolyte interphase is simultaneously constructed to suppress the growth of lithium dendrites. Lithium (Li) metal is a competitive anode material for rechargeable high energy density batteries due to its high specific capacity and low reduction potential. However, great challenges remain in addressing uncontrollable Li dendrite growth and unstable interface. Herein, we report a quasi-solid electrolyte enabled by in situ polymerization of polyethylene glycol methyl ether acrylate. Meanwhile, a LiF-enriched solid electrolyte interphase (SEI) is built on Li-metal surface by function of the fluoroethylene carbonate additive. The SEI with a good mechanical stability prompts the dense and uniform Li deposition behavior. The in situ polymerized gel polymer electrolyte exhibits an ionic conductivity of 1.71×10 −4 S cm −1 at 30 °C, and a considerable oxidative stability up to 4.5 V (vs. Li/Li + ). The Li||Li symmetric cells delivers a long-term cycle life over 1400 h and a low voltage hysteresis at 0.5 mA cm −2 , 1 mAh cm −2 . To be paired with a LiFePO 4 positive electrode, the cell shows a high discharge capacity of 135.6 mAh g −1 and capacity retention of 92.7 % after 300 cycles. This work provides a reference for the practical development of quasi-solid electrolyte for lithium-metal battery.

研究领域: 材料科学 · 电化学 · 储能技术 · 高分子化学 · 纳米技术
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ACS Applied Nano Materials · 2024 · IF 5.3

Carbon-Coated Si Nanosheets as Anode Materials for High-Performance Lithium-Ion Batteries

Guoqiang Qin,Zhitong Jia,Songyuan Sun,Huigui Wu,Kaihan Hu,Dongmei Liu,Yiqun Gao,Jingbo Chen

Silicon (Si) and Si-based compounds have been considered by many researchers as one of the anode materials for the next-generation lithium-ion batteries (LIBs) due to their extraordinarily large theoretical capacity, moderate operating voltage, and abundant resources. However, silicon’s poor conductivity and significant volume changes during charge and discharge, compared to conventional carbon materials, severely restrict its widespread use in LIBs. In this study, a two-dimensional (2D) mesoporous Si nanosheet/carbon (pSi@C) composite is designed using cetrimonium bromide–disodium edetate dihydrate (CTAB–EDTA) as a template via a sol–gel method, magnesium thermal reduction method, and thermal decomposition method. The vertical diffusion distance of Li+ is significantly reduced by the 2D Si nanosheets. Additionally, the carbon coating on the Si surface provides a protective layer to limit the volume expansion of Si and form a stable solid electrolyte interface (SEI). This enhances the structural integrity and cycle stability of the pSi@C anode material during Li+ insertion and extraction. At a current density of 1 A g–1, the reversible capacity of the pSi@C composite after 150 cycles is 2236 mAh g–1, with a capacity retention rate of 71.5%. The electrode’s capacity is 467.8 mAh g–1 after 500 cycles at a current density of 5 A g–1. Therefore, this unique template and technology can be used to design 2D anode composites with excellent properties, thereby providing an effective strategy for commercial application of LIBs.

研究领域: 材料科学 · 电化学 · 纳米技术 · 能量存储
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JOURNAL OF MEMBRANE SCIENCE · 2025 · IF 9

Aromatic polyurea ion-solvating membranes for stabilized quasi-solid-state lithium metal batteries

Hao Wang,Shuangyan Kang,Aiting Liu,Zixin Lv,Junhao Xin,Feng Wang,Qinghai Chen,Junfen Li,Hongying Tang,Nanwen Li

In Solid lithium metal batteries (LMBs), polymer electrolytes have been extensively studied due to their intrinsic safety and high energy density. However, commonly used polymer matrix such as polyethylene oxide (PEO), polyacrylonitrile (PAN), and polyvinylidene fluoride (PVDF) cannot solve the problem of lithium dendrites and low ionic conductivity, resulting in short battery life and low-capacity retention. Here, a series of aromatic polyurea ion-solvating membranes (ISMs) with rigid and flexible structures is designed and prepared. With incorporation of LiTFSI, these ISMs exhibit high ionic conductivity (1.81 × 10 -3 S cm -1 ), good electrochemical stability (5.1 V vs Li + /Li), and excellent mechanical strength (39 MPa). The formed inorganic/organic solid electrolyte interphase (SEI) layer enriched with LiF, Li 3 N, and Li-N-C in the batteries leads to a uniform lithium deposition. As expected, the Li|Li symmetrical cells show a stable galvanostatic Li plating/stripping cycling performance with a low overpotential of 900 h at 0.1 mA cm −2 . Most importantly, the LFP|ISM|Li coin cells still have a high capacity of 142.9 mAh g -1 after 650 cycles at 0.5 C, with a capacity retention rate of 91%.

研究领域: 材料科学 · 电化学 · 储能技术 · 高分子科学 · 锂离子电池
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ADVANCED FUNCTIONAL MATERIALS · 2025 · IF 19

Thermally Stable, Ion-Regulating Aramid Nanofiber-Polyacrylamide Modified Separator Enabling Safe and High-Performance Lithium Metal Batteries

Tianyang Yu,Xue Pang,Teng Zhao,Ke Wang,Wangming Tang,Anqi Zhao,Chenxi Xu,Nan Chen,Li Li,Feng Wu,Renjie Chen

Lithium metal batteries (LMBs) face critical challenges such as unstable solid electrolyte interphase (SEI), dendritic lithium growth, and transition metal dissolution from high-nickel cathodes, which compromise cycling stability and safety. To address these issues, a multifunctional composite separator is developed by constructing an aramid nanofiber (ANF)-polyacrylamide (PAM) hybrid layers on PP separators. The ANF-PAM@PP separator exhibits exceptional thermal stability, mechanical robustness, and uniform pore structure, enabling homogeneous Li-ion flux distribution and suppressed dendrite initiation. The PAM is rich in amide groups and effectively chelates dissolved transition metal ions via coordination bonding, reducing SEI degradation and electrolyte decomposition. Density functional theory (DFT) calculations confirm strong metal ion adsorption on ANF-PAM due to high binding energies. Li||Li symmetric cells with the modified separator achieve stable cycling for >1000 h at 2 mA cm −2 , while Li||NCM811 cells retain 81.8% capacity after 150 cycles at 3C. This work provides a scalable strategy for designing high-performance separators to enable durable and safe LMBs.

CAS / MDL: 25014-41-9
研究领域: 材料科学 · 电化学 · 储能 · 电池技术
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SusMat · 2024 · IF 18.7

Designing weakly and strongly solvating polymer electrolytes: Systematically boosting high-voltage lithium metal batteries

Tianyi Wang,Yimeng Zhang,Xueyan Huang,Peifeng Su,Min Xiao,Shuanjin Wang,Sheng Huang,Dongmei Han,Yuezhong Meng

Practical high-voltage lithium metal batteries hold promise for high energy density applications, but face stability challenges in electrolytes for both 4 V-class cathodes and lithium anode. To address this, we delve into the positive impacts of two crucial moieties in electrolyte chemistry: fluorine atom (-F) and cyano group (-CN) on the electrochemical performance of polyether electrolytes and lithium metal batteries. Cyano-bearing polyether electrolytes possess strong solvation, accelerating Li + desolvation with minimal SEI impact. Fluorinated polyether electrolytes possess weak solvation, and stabilize the lithium anode via preferential decomposition of F-segment, exhibiting nearly 6000-h stable cycling of lithium symmetric cell. Furthermore, the electron-withdrawing properties of -F and -CN groups significantly bolster the high-voltage tolerance of copolymer electrolyte, extending its operational range up to 5 V. This advancement enables the development of 4 V-class lithium metal batteries compatible with various cathodes, including 4.45 V LiCoO 2 , 4.5 V LiNi 0.8 Co 0.1 Mn 0.1 O 2 , and 4.2 V LiNi 0.5 Co 0.2 Mn 0.3 O 2 . These findings provide insights into design principles centered around polymer components for high-performance polymer electrolytes.

研究领域: 材料科学 · 电化学 · 电池技术 · 聚合物化学
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ACS Nano · 2022 · IF 18.027

Tailoring Electrolyte Solvation for LiF-Rich Solid Electrolyte Interphase toward a Stable Li Anode

Haifeng Tu,Linge Li,Zhicheng Wang,Jian Wang,Hongzhen Lin,Mingchao Wang,Cheng Yan,Meinan Liu

A solid electrolyte interphase (SEI) with robust mechanical property and high ionic conductivity is imperative for high-performance lithium metal batteries since it can efficiently impede the growth of notorious lithium dendrites. However, it is difficult to form such a SEI directly from an electrolyte. In this work, a crowding dilutant modified ionic liquid electrolyte (M-ILE) has been developed for this purpose. Simulations and experiments indicate that the 1,2-difluorobenzene (1,2-dfBen) dilutant not only creates a crowded electrolyte environment to promote the interaction of Li+–FSI–, leading to abundant aggregate ion pairs (AGGs), but also participates in the reduction to construct a robust and high ionic-conductive SEI. With this M-ILE, Li/LiFePO4 cells achieve a capacity retention of 96% over 250 cycles with 9.5 mg cm–2 mass loading, and Li/LiNi0.5Co0.2Mn0.3O2 cells also deliver a discharge capacity of 132 mAh g–1 with a high retention of 88% after 100 cycles. Therefore, the use of a crowding diluent is considered to be an efficient way to construct an advanced SEI for a Li anode.

研究领域: 电化学 · 储能技术 · 材料科学 · 锂离子电池
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CHEMICAL ENGINEERING JOURNAL · 2024 · IF 13.3

Revolutionizing aqueous Zn-ion batteries: Precision control of H2O activity and Zn deposition through ammonium oxalate additive

Wenhao Ding,Guolang Zhou,Xiangjie Guo,Cheng Liu,Tianshi Wang,Yongsheng Fu,Jingzhou Yin,Lili Zhang,Edison Huixiang Ang

The natural reactivity of Zn metal in aqueous environments leads to surface deterioration and uncontrolled dendrite growth, posing challenges in the advancement of Zn-ion batteries. In this research, we introduce an environmentally friendly and cost-effective electrolyte additive, ammonium oxalate (AO), to significantly extend the cycle life of Zn-ion batteries with minimal usage. Oxalate ions within AO actively participate in the solvation of hydrated Zn ions and attach to the Zn anode surface prior to H 2 O molecules, creating a robust solid-electrolyte interface (SEI) layer. This SEI layer serves a dual purpose: it inhibits further reactions with H 2 O and restricts the two-dimensional movement of Zn ions, promoting the preferential growth of the (0   0   2) crystal plane. Consequently, Zn||Zn cells exhibit an impressive lifespan surpassing 1800 h (at 1 mA cm −2 , 1 mAh cm −2 ), and Zn||Cu cells experience a tenfold increase in cycling life. Moreover, Zn||MnO 2 full cells, incorporating this low-cost and highly efficient inorganic additive, maintain an outstanding 80.84 % capacity retention after 1200 cycles at 1 A g −1 . This breakthrough with AO offers a promising avenue for the practical implementation of Zn-ion batteries, emphasizing their cost-effectiveness and environmental sustainability.

CAS / MDL: 7446-20-0
研究领域: 材料科学 · 电化学 · 能源存储
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JOURNAL OF POWER SOURCES · 2022 · IF 9.794

Targeted stabilization of solid electrolyte interphase and cathode electrolyte interphase in high-voltage lithium-metal batteries by an asymmetric sustained-release strategy

Fengwei Bai,Yan Li,Ziyu Chen,Yongchao Zhou,Chengzong Li,Tao Li

High-voltage lithium (Li)-metal batteries with cell-level energy density over 350 Wh kg −1 are promising energy storage systems . However, the aggressive interphase chemistries associated with highly reactive Li-metal anode and high-voltage cathodes impede their practical applications. Herein, we demonstrate the targeted stabilization of solid electrolyte interphase (SEI) and cathode electrolyte interphase (CEI) in high-voltage Li-metal batteries by asymmetrically sustained-releasing different additives. An asymmetric sustained-release film loaded with lithium bis-(oxalate)borate (LiBOB) and LiNO 3 on each side is investigated as a proof-of-concept. The sustained-releasing of LiBOB and LiNO 3 can maintain a localized concentration at the high-voltage cathode and Li-metal anode fronts respectively, thus forming a stable B-containing CEI and N-containing SEI. As such, issues like dendrites growth, parasitic side reactions and transition metals dissolution under high-voltage are addressed simultaneously. Based on this strategy, the 30 μm Li|LiNi 0.5 Co 0.2 Mn 0.3 O 2 (4.1 mAh cm −2 ) batteries deliver a capacity retention of 80% after 173 cycles under a cut-off voltage of 4.5 V.

研究领域: 储能系统 · 电池技术 · 材料科学 · 电化学
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Advanced Energy Materials · 2023 ·Vol. 13 ·期 34 ·2301509 · IF 27.8

Enhancing the Whole Migration Kinetics of Na+ in the Anode Side for Advanced Ultralow Temperature Sodium-Ion Hybrid Capacitor

Jiafeng Ruan,Sainan Luo,Shaofei Wang,Jiaming Hu,Fang Fang,Fei Wang,Min Chen,Shiyou Zheng,Dalin Sun,Yun Song

Boosting the ultralow temperature (below −30 °C) performance of Na-ion hybrid capacitors (SIHCs), which integrate the high energy density of batteries with the high output power and long life of supercapacitors, is critical for the application of advanced electronics in extreme environments. However, their low-temperature performance, especially fast charging capability, is hindered by difficult desolvation and slow pass solid electrolyte interphase (SEI) together with sluggish diffusion within the electrode. Herein, a “single-solute–single-solvent” electrolyte is developed and a through-hole hollow carbon sphere (TH-HCS) is constructed, and it is demonstrated through theoretical calculations and experimental investigations that the weakly solvated structure and high ionic conductivity facilitate the Na + transportation at low temperatures, the highly fluorinated SEI facilitates the Na + migration, and the through-hole hollow structure alleviates the volume expansion during sodiation, thus ensuring fast kinetics and structural stability. As expected, TH-HCS using this electrolyte exhibits a high specific capacity of 87.5 mAh g −1 after 11 000 cycles at 1.0 A g −1 and −40 °C. Coupled with activated carbon, the assembled SIHC displays an energy density of 106.1 and 52.0 Wh kg −1 at 25 and −40 °C, respectively, far exceeding the performance of commercial energy storage systems at low temperature.

研究领域: 储能技术 · 电化学 · 材料科学 · 电池技术 · 低温能源器件
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