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JOURNAL OF MATERIALS CHEMISTRY · 2011 ·Vol. 21 ·期 32 ·12068-12077 · IF 5.101

Novel polyaromatic ionomers with large hydrophilic domain and long hydrophobic chain targeting at highly proton conductive and stable membranes

Dongyang Chen,Shuanjin Wang,Min Xiao,Yuezhong Meng,Allan S. Hay

A novel dihydroxyl monomer bearing 18 electron rich phenyl rings were synthesized and polymerized with other monomers bearing electron deficient phenyl rings to give dense and selective sites in macromolecules for post-sulfonation, which was successfully conducted in ClSO3H/CH2Cl2 solution at room temperature in a subsequential step. The chemical structures were confirmed by 1H NMR and FT-IR spectra. The ionic exchange capacity (IEC) was controlled to be from 0.65 to 1.21 mequiv g−1 to afford considerable proton conductivity. Distinct phase separation was observed in the resulting membranes from SAXS profiles. The SPAEK-5 with an IEC of 1.21 mequiv g−1 gave better proton conductivity than Nafion 117 at all tested temperatures under 100% relative humidity. The membranes exhibited an exceeding stability when immersing in Fenton's reagent (3 wt.% H2O2 + 2 ppm FeSO4) at 80 °C. These properties make them promising candidates for electrochemical applications.

研究领域: 材料科学 · 高分子化学 · 膜科学 · 电化学 · 能源材料
✓ 已验证 DOI 高影响因子
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Small · 2021 ·Vol. 18 ·期 5 ·2104508 · IF 13.281

A Fluoride-Ion-Conducting Solid Electrolyte with Both High Conductivity and Excellent Electrochemical Stability

Jinzhu Wang,Jipeng Hao,Chaomin Duan,Xinchao Wang,Kai Wang,Cheng Ma

Solid-state fluoride-ion batteries (FIBs) circumvent multiple formidable bottlenecks of lithium-ion batteries, but their overall performance remains inferior due to the absence of appropriate solid electrolytes. Presently the conductivity of most solid electrolytes for FIBs is too low to enable room-temperature cycling, while the few sufficiently conductive ones only allow for very low discharge voltages because of the narrow electrochemical stability window (ESW). Here, high room-temperature conductivity and a decent ESW are simultaneously achieved by designing a solid electrolyte CsPb 0.9 K 0.1 F 2.9 . Its room-temperature conductivity is 1.23 × 10 −3 S cm −1 , comparable to the most conductive system reported so far (PbSnF 4 , 5.44 × 10 −4 –1.6 × 10 −3 S cm −1 ), but the ESW is several times broader. With these appealing characteristics simultaneously achieved in the solid electrolyte, a cell with much higher voltages than other room-temperature-operable solid-state FIBs in literature is successfully constructed, and stably cycled at 25 °C for 4581 h without considerable capacity fade.

研究领域: 材料科学 · 电化学 · 固态离子学 · 能源存储 · 无机功能材料
✓ 已验证 DOI 高影响因子
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SOLID STATE IONICS · 2017 · IF 2.354

A facile strategy to improve the electrochemical stability of a lithium ion conducting Li10GeP2S12 solid electrolyte

Yan Sun,Wenning Yan,Li An,Bingbin Wu,Kaifu Zhong,Ruizhi Yang

A super solid electrolyte of Ba-substituted Li 10 GeP 2 S 12 is designed and fabricated to achieve high electrochemical stability. Among the Ba-substituted Li 10 GeP 2 S 12 solid electrolytes, the composition of Li 9.4 Ba 0.3 GeP 2 S 12 exhibits the highest ionic conductivity of 7.04   ×   10 −   4   S   cm −   1 with an activation energy of 28.27   kJ   mol −   1 at 25   °C. The electrochemical window of Li 9.4 Ba 0.3 GeP 2 S 12 is between 0 and 6   V (vs. Li), which is higher than the typical 5   V window of Li 10 GeP 2 S 12 . As compared with Li 10 GeP 2 S 12 , Li 9.4 Ba 0.3 GeP 2 S 12 demonstrates a significantly reduced polarization and a better cycle stability though its ionic conductivity is slightly lower than that of the former. The electrochemical stability of Ba-substituted Li 10 GeP 2 S 12 can be attributed to the structural stability resulting from the stable interaction between Ba 2   + and S 2   − in the structure.

研究领域: 材料科学 · 固态离子学 · 电化学 · 能源材料 · 无机固体化学
✓ 已验证 DOI 高影响因子
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MATERIALS CHEMISTRY AND PHYSICS · 2021 · IF 4.094

Deep eutectic solvent-immobilized PVDF-HFP eutectogel as solid electrolyte for safe lithium metal battery

Zhongxu Li,Shengzhao Zhang,Zhao Jiang,Dan Cai,Changdong Gu,Jiangping Tu

A novel cheap eutectogel (ETG) membrane based on the deep eutectic solvent (DES) immobilized poly (vinylidene fluoride-hexafluoro propylene) (PVDF-HFP) is proposed as a solid electrolyte for safe lithium metal batteries in this study. The composition of DES is optimized, which is prepared by mixing the N-methylacetamide (NMAC) and the lithium bis [(trifluoromethyl)sulfonyl]imid (LiTFSI) with a molar ratio of 4:1. The eutectogel is formed by incorporating 70 wt% DES into the PVDF-HFP, which is non-flammable and shows excellent mechanical properties. This ETG membrane electrolyte with a thickness about 25 μm possess a high ionic conductivity (3.05 × 10 −4  S cm −1 ) at room temperature and a wide electrochemical stability window (~5 V). The Li//ETG//LiFePO 4 full cells deliver an acceptable discharge capacity of ~133.9 mAh g −1 at 0.1C and room temperature after 100 charge-discharge cycles. The ETG membrane electrolyte can also endow the Li//ETG//LiFePO 4 pouch cell with flexibility and withstanding abuse operations, like nail penetration and cutting. We expect that the flexible and non-flammable eutectogel membrane will have implications for the use of DES based ionic liquids in the synthesis of advanced solid-state electrolytes for safer lithium batteries .

研究领域: 材料科学 · 电化学 · 能源存储 · 高分子物理 · 电池技术
✓ 已验证 DOI 高影响因子
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JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS · 2024 ·Vol. 35 ·期 2 ·140 · IF 2.8

HEC/PAM hydrogel electrolyte toward regulating the surface of zinc negative electrode for inhibited dendrite in zinc-ion batteries

Ma Di,He Hao,Huang Xinglan,Wang Jingcheng,Hu Xuebu

The inhomogeneous plating/stripping of zinc and side reactions originating from the dissolution of the cathode material in water lead to the poor stability of zinc anode, which inevitably limits the practical application of zinc-based aqueous batteries. Therefore, a novel hydrogel electrolyte made of hydroxyethyl cellulose/polyacrylamide (HEC/PAM) with a 3D network-like structure is synthesized by radical polymerization and cross-linking reinforcement. Thanks to the porous crosslinked network and massive hydrophilic groups, the electrolyte has high ion conductivity of 3.17 × 10 –2  S cm −2 and decomposition voltage of 2.6431 V. The ion conductive hydrophilic groups facilitate the interfacial compatibility of the electrode with the electrolyte and stabilize zinc plating/stripping, which suppresses the formation of zinc dendrites. Meanwhile, the hydrogel electrolyte effectively alleviates the dissolution of the positive electrode and the occurrence of side reactions, and subsequently improves the stability of the electrode. As a result, the assembled Zn–Zn symmetric cell with HEC/PAM hydrogel electrolyte is stable without short circuit and rapid increase of overvoltage at 5 mA cm −2 . The polarization voltage of the assembled Zn–Cu half-cell is 59.2 mV and initial coulomb efficiency reaches 94.3%. The assembled Zn–V 2 O 5 ·nH 2 O/CNT full cell delivers an excellent cycling stability of 186.9 mAh g −1 at 0.5 A g −1 after 500 cycles with a high-capacity retention of 92.5% (only 52.1% in aqueous system). The new idea is provided for further development of functional hydrogel electrolytes in zinc-ion batteries.

研究领域: 电化学 · 能源材料 · 功能高分子 · 电池技术 · 界面化学
✓ 已验证 DOI 高影响因子
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Nano Energy · 2020 · IF 16.602

Nano-ordered structure regulation in delithiated Si anode triggered by homogeneous and stable Li-ion diffusion at the interface

Long Li,Chun Fang,Wenfei Wei,Lei Zhang,Zhao Ye,Gang He,Yunhui Huang

The huge volume change of silicon anode during cycling results in unstable solid electrolyte interface (SEI), causing rapid performance degradation . Natural SEI layer has a heterogeneous structure, results in the inhomogeneous Li + diffusion. The repeated destruction and regeneration of SEI aggravate the inhomogeneity of Li + diffusion at the interface, leading to non-uniform alloy reaction in the Si bulk. In this work, the silicon surface is passivated by an ultrathin uniform chitosan layer with abundant lithiophilic groups. The capacity of chitosan-coated Si (Si@CS) could reach 1500 mAh g −1 at a current density of 1 A g −1 , and the capacity retention remains 91% after 400 cycles. It is demonstrated that the oxygen and nitrogen atoms in chitosan are coordinated with Li + , providing uniformly distributed Li + transfer sites, results in a homogeneous Li + flux in the surface layer. Interestingly, a nano-scale ordered atomic arrangement is observed in the delithiated Si@CS, which contributes to more stable and reversible lithiation/delithiation reaction of the Si@CS electrode. It is proposed that optimizing the reaction interface on the Si surface is able to alter the Li-ion diffusion kinetics and structure transition behavior of silicon, which can improve the structure reversibility and stability during cycling.

研究领域: 材料科学 · 电化学 · 纳米科技 · 能源存储 · 表面工程 · 锂离子电池
✓ 已验证 DOI 高影响因子
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Science China-Materials · 2021 ·Vol. 64 ·期 6 ·1378-1385 · IF 8.273

Interplay between Li3YX6 (X = Cl or Br) solid electrolytes and the Li metal anode

Fu Yuanyuan,Ma Cheng

The interplay between solid electrolytes and electrodes is of vital importance to the performance of all-solid-state Li batteries. Recently, halide superionic conductors have emerged as a new family of high-performance solid electrolytes, but their compatibility with Li metal, i.e., the anode with the highest theoretical capacity, has not been systematically studied. Here, we investigate the interaction between Li metal and two representative halide solid electrolytes: Li 3 YCl 6 and Li 3 YBr 6 . Both materials are found to form interphases with Li, similar to most solid electrolytes. However, the interphases observed here contain electronic conducting components, which are detrimental to their compatibility with Li. By elucidating this phenomenon, the present study provides guiding principles for improving the Li compatibility of halide solid electrolytes.

研究领域: 材料科学 · 电化学 · 固态离子学 · 能源存储 · 电池技术
✓ 已验证 DOI 高影响因子
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SOLID STATE IONICS · 2016 · IF 2.38

High-temperature performance of all-solid-state battery assembled with 95(0.7Li2S-0.3P2S5)-5Li3PO4 glass electrolyte

Shanshan Mo,Penghao Lu,Fei Ding,Zhibin Xu,Jiaquan Liu,Xingjiang Liu,Qiang Xu

Sulfide glasses with a high lithium-ion conductivity are promising solid electrolyte for all-solid-state lithium-ion batteries. In this study, 95(0.7Li 2 S–0.3P 2 S 5 )–5Li 3 PO 4 glass electrolyte is prepared by mixing 70Li 2 S-30P 2 S 5 (mol%) glass and Li 3 PO 4 crystal using mechanical milling technique. The effects on the structures and electrochemical properties of the obtained ternary sulfide glass were examined. The ternary sulfide glass shows a good electrochemical stability, which may exhibit a wide electrochemical window up to 10   V (vs. Li/Li + ). Furthermore, the 95(0.7Li 2 S-0.3P 2 S 5 )-5Li 3 PO 4 glass electrolyte displays an electrical conductivity of 2.513   ×   10 −   3   S   cm −   1 at 100   °C. The all-solid-state lithium-ion cell assembled with 95(0.7Li 2 S-0.3P 2 S 5 )-5Li 3 PO 4 glass electrolyte shows a favourable cyclability, which can reveal a discharge capacity of 144   mAh   g −   1 at 0.05   °C and a discharge capacity of 63.9   mAh   g −   1 at 0.1C after the 50th cycle at 100   °C, respectively.

研究领域: 材料科学 · 电化学 · 能源存储 · 固态离子学 · 锂电池技术
✓ 已验证 DOI 高影响因子
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PROGRESS IN ORGANIC COATINGS · 2022 · IF 6.206

Design and synthesis of robust superhydrophobic coating based on epoxy resin and polydimethylsiloxane interpenetrated polymer network

Shuming Liu,Shuqi Liu,Qian Wang,Zhou Zuo,Xidong Liang

Superhydrophobic surfaces, such as lotus leaves, have attracted significant attention because of their excellent performance and potential application value. However, the micro-nano hierarchy on superhydrophobic surfaces is often vulnerable and easily broken from mechanical stress or chemical corrosion, which greatly inhibits its practical application and long-term service. This study presents a low-cost and scalable superhydrophobic coating based on an interpenetrated polymer network of polydimethylsiloxane (PDMS) and epoxy resin . The composite polymer matrix exhibits mechanical robustness as derived from the epoxy resin and low surface energy as derived from the PDMS. The superhydrophobic coating is obtained by dispersing fluoroalkyl-silane-modified SiO 2 in the solution containing the composite polymer . The multi-level hierarchical structure of SiO 2 aggregations and their strong bonding with the composite polymer gives the coating outstanding mechanical durability while maintaining superhydrophobicity after multiple cycles of sandpaper abrasion, tape peeling, and water impact tests. The chemical inertness of all components ensures its chemical stability, and the surface shows super repellency to strong acids and alkaline liquids (pH = 0–14). The coating also has excellent self-cleaning properties, which has potential applications in various industrial fields.

研究领域: 材料科学 · 高分子化学 · 表面工程 · 涂层技术 · 功能材料
✓ 已验证 DOI 高影响因子
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IONICS · 2016 ·Vol. 23 ·期 10 ·2603-2611 · IF 2.119

Hybrid solid electrolytes with excellent electrochemical properties and their applications in all-solid-state cells

Chen Shaojie,Zhao Yanran,Yang Jing,Yao Lili,Xu Xiaoxiong

Three types of inorganic electrolytes [Li 10 GeP 2 S 12 (LGPS), 75Li 2 S·24P 2 S 5 ·1P 2 O 5 (LPOS), Li 1.5 Al 0.5 Ge 1.5 (PO 4 ) 3 (LAGP)] with different particle sizes and electrochemical properties are selected as active fillers incorporated into poly(ethylene oxide) (PEO) matrix to fabricate hybrid solid electrolytes. The optimum composition of each filler is found in consideration of ionic conductivity. Their electrochemical characteristics are investigated. The optimal conductivities are 1.60 × 10 −5 , 1.18 × 10 −5 , and 2.12 × 10 −5  S cm −1 at room temperature for PEO-1%LGPS, PEO-1%LPOS, and PEO-20%LAGP, respectively. The electrochemical stability windows of these hybrid solid electrolytes are all above 5 V (vs. Li + /Li). The results show that these fillers have positive effects on the ionic conductivity, lithium ion transference number, and electrochemical stability. The relationship between the type of filler and electrochemical properties has been investigated. All-solid-state cells LiFePO 4 /Li are fabricated and present fascinating electrochemical performance with high capacity retention and good cycling stability. This work provides promising electrolytes prepared by a simple method.

研究领域: 材料科学 · 电化学 · 能源存储 · 固态离子学 · 功能材料 · 锂电池技术
✓ 已验证 DOI 高影响因子
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TRANSACTIONS OF NONFERROUS METALS SOCIETY OF CHINA · 2025 ·Vol. 35 ·期 7 ·2341-2353 · IF 4.7

High-performance Li3YCl3Br3 halide solid electrolyte synthesized using wet-chemistry route for all-solid-state battery

Han-zhou LIU,Yan-chen LIU,Sheng-hao JING,Ya-qi HU,Zong-liang ZHANG,Si-liang LIU,Yang LIU,Zhi ZHUANG,Fan-qun LI,Fang-yang LIU

A dual-halide solid electrolyte, Li 3 YCl 3 Br 3 , was synthesized using a wet-chemistry route instead of the conventional mechanical ball-milling route. Li 3 YCl 3 B r3 exhibits an ion conductivity of 2.08 mS/cm and an electro- chemical stability window of 3.8 V. Additionally, an all-solid-state lithium-ion battery using Li 3 YCl 3 Br 3 and LiNi 0.83 Co 0.11 Mn 0.06 O 2 (NCM811) as the cathode material achieves a capacity retention of 93% after 200 cycles at 0.3 C and maintains a specific capacity of 115 mA·h/g during 2 C cycling. This exceptional performance is attributed to the high oxidative stability of Li 3 YCl 3 Br 3 and the in-situ formation of Y 2 O 3 inert protective layer on the NCM811 surface under high voltage. Consequently, the study demonstrates the feasibility of a simple, cost-effective wet-chemistry route for synthesizing multi-component halides, highlighting its potential for large-scale production of halide solid electrolytes for practical applications.

研究领域: 材料科学 · 电化学 · 固态离子学 · 能源存储 · 电池技术 · 无机非金属材料 · 纳米材料应用
✓ 已验证 DOI 高影响因子
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