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CHINESE JOURNAL OF CHEMICAL ENGINEERING · 2020 · IF 2.627

A design of Nafion-coated bilayered quasi-solid electrolyte for lithium-O2 batteries with high performance

Yingfei Hou,Lin Jiang,Yaoyao Zhang,Zhiwen Qin,Chi Jiang,Ming Wang

Lithium-air (also known as lithium-oxygen) batteries have attracted considerable global attention in recent years due to their extremely high energy density (11,140 W·h·kg −1 ). The electrolyte is a key element in lithium-air batteries and the traditional organic electrolyte has great safety risk due to leakage. On the contrary, the polymer electrolyte has the advantages of high safety, high stability and easy processing comparing with the organic liquid electrolytes. In this paper, a new idea was proposed to coat the Nafion membrane on a layer of polymer for blocking the oxidation reduction electric (RM) and Li based on the selective permeability on lithium ion of the Nafion membrane. Self-made thickness-controllable Nafion membrane, polyvinylidene fluoride-hexafluoropropylene copolymer (PVDF-HFP) and 2,2,6,6-tetramethylpiperidinooxy (TEMPO) were used to prepare a quasi solid polymer electrolyte (NSPE). Electrochemical workstation and LAND battery testing system were used to perform a galvanostatic charge/discharge test on Li-O 2 . The ionic conductivity of NSPE was 4.3 × 10 −4 S·cm −1 at room temperature and the discharge platform was 2.6 V and the charging voltage was 3.7 V after 50 cycles with the cut-off capacity of 500 mA·h·g −1 .

研究领域: 材料科学 · 电化学
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JOURNAL OF POWER SOURCES · 2024 · IF 8.1

Multistage channel PVDF-HFP pregnant ZIF-8@SiO2 quasi-solid electrolyte for lithium-metal batteries

Hu Wang,Jiangchao Chen,Pengfei Pang,Yiran Bai,Zhiqiang Zheng,Tao Huang,Kunpeng Jiang,Yunyun Zhao,Guisheng Zhu,Huarui Xu

The development of lithium-metal batteries (LMBs) with high energy density and safety is considered a top priority for the next generation of rechargeable batteries. However, the mitigation of the inevitable reaction between lithium and the liquid electrolyte (LE), as well as the subsequent formation of Li dendrites, poses a crucial challenge that needs to be addressed. Upgrading traditional LEs serves as a pivotal strategy in achieving this objective. Here, we report a ZIF-8@SiO 2 /PVDF-HFP (ZSPH) quasi-solid electrolyte (QSE) with ultra-multistage pore crosslinked network structure. The interconnected micro-stage pore structure in a honeycomb-like morphology of polyvinylidene fluoride-co-hexafluoropropylene (PVDF-HFP) and the rich multistage pore structure of nanoscale SiO 2 “armored” zeolite imidazolium ester backbone-8 (ZIF-8@SiO 2 ) collectively establish a multi-stage ion transport channel. This unique structure facilitates appreciable ionic conductivity (2.21 × 10 −3  S cm −1 at 30 °C) and provides a wide and stable electrochemical window (approximately 5.0 V). The Li/ZSPH9-LiPF 6 /Li quasi-solid-state cell demonstrates an impressive longevity of over 1800 h at a current density of 0.2 mA cm −2 . The high compatibility of the interface between electrode and ZSPH QSE and effective inhibition of Li dendrites growth create synergistic effects, which make it possible to realize high energy density and safe LMBs.

研究领域: 材料科学 · 电化学
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APPLIED SURFACE SCIENCE · 2025 · IF 6.9

LiDFOB-Regulated interfacial chemistry enables high-coulombic-efficiency elastomeric electrolytes for lithium metal batteries

Yali Liu,Fanglongwen Xu,Chen Wang,Xiaofei Cao,Jiarui Cheng,Zilong Zeng,Hao Yao,Youlong Xu

The application of lithium-metal batteries (LMBs) has been hindered by dendritic deposition, low coulomb efficiency (CE) and significant volume changes during repeated plating/stripping process. Herein, we developed an elastomeric quasi-solid electrolyte (QSE) through in-situ polymerization method with a tailored composition. The incorporation of difluoro(oxalato)borate (LiDFOB) facilitated the generation of a uniform lithium deposition morphology and significantly enhanced the CE of LMB. Remarkably, the Li/Cu cell exhibited a high CE of 98.33 % compared to the battery without LiDFOB (97.09 %). Moreover, the Li/Li symmetric cell demonstrated long-term cycling stability about 600 h at 0.3 mA cm −2 for 0.3 mAh cm −2 . The Li/LiFePO 4 (LFP) cell displayed an initial discharge capacity of 144.2 mAh g −1 at 1 C, with a capacity retention of 98.54 % after 400 cycles. Additionally, the average CE over 400 cycles was improved to 99.93 %. Density functional theory (DFT) calculations revealed that Slab-DFOB − -Li + has a lower binding energy, enabling LiDFOB to preferentially absorb and react on the lithium metal surface, thereby facilitating smooth and dendrite-free lithium deposition. The incorporation of functional LiDFOB into elastomeric QSE effectively enhances the electrochemical performance of LMBs. The compatible modification strategy provides a new perspective for improving the performance of elastomeric electrolytes.

研究领域: 材料科学 · 电化学
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ADVANCED MATERIALS · 2024 ·Vol. 36 ·期 27 ·2402401 · IF 27.4

In Situ Polymerization Facilitating Practical High-Safety Quasi-Solid-State Batteries

Xinyu Rui,Rui Hua,Dongsheng Ren,Feng Qiu,Yu Wu,Yue Qiu,Yuqiong Mao,Yi Guo,Gaolong Zhu,Xiang Liu,Yike Gao,Chang Zhao,Xuning Feng,Languang Lu,Minggao Ouyang

Quasi-solid-state batteries (QSSBs) are gaining widespread attention as a promising solution to improve battery safety performance. However, the safety improvement and the underlying mechanisms of QSSBs remain elusive. Herein, a novel strategy combining high-safety ethylene carbonate-free liquid electrolyte and in situ polymerization technique is proposed to prepare practical QSSBs. The Ah-level QSSBs with LiNi 0.83 Co 0.11 Mn 0.06 O 2 cathode and graphite–silicon anode demonstrate significantly improved safety features without sacrificing electrochemical performance. As evidenced by accelerating rate calorimetry tests, the QSSBs exhibit increased self-heating temperature and onset temperature ( T 2 ), and decreased temperature rise rate during thermal runaway (TR). The T 2 has a maximum increase of 48.4 °C compared to the conventional liquid batteries. Moreover, the QSSBs do not undergo TR until 180 °C (even 200 °C) during the hot-box tests, presenting significant improvement compared to the liquid batteries that run into TR at 130 °C. Systematic investigations show that the in situ formed polymer skeleton effectively mitigates the exothermic reactions between lithium salts and lithiated anode, retards the oxygen release from cathode, and inhibits crosstalk reactions between cathode and anode at elevated temperatures. The findings offer an innovative solution for practical high-safety QSSBs and open up a new sight for building safer high-energy-density batteries.

研究领域: 材料科学 · 能源技术
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MACROMOLECULAR RAPID COMMUNICATIONS · 2022 ·Vol. 44 ·期 3 ·2200685 · IF 5.006

Highly Stretchable, Self-Healing, and Low Temperature Resistant Double Network Hydrogel Ionic Conductor as Flexible Sensor and Quasi-Solid Electrolyte

Xudong Ma,Xieraili Maimaitiyiming

With the rapid development of flexible energy storage and wearable strain sensing, conductive hydrogels are attracting attention as electrolyte materials for flexible strain sensors and flexible supercapacitors due to their excellent flexibility and wetting properties. In this work, antifreezing hydrogels with high stretchability, adhesion, and conductivity are designed and prepared by introducing phosphoric acid solutions into polyacrylamide and chitosan systems. The multifunctional hydrogel samples prepared by this method can be used as both quasi-solid electrolytes and wearable strain sensors. The hydrogel-based supercapacitor shows a charge/discharge efficiency of 99.67% and a capacitance retention of 98.85% after 10 000 cycles charge/discharge tests at −30 °C. The tiny characteristic heartbeat wave forms are detected by the hydrogel as a flexible strain sensor. It is foreseeable that PCP multifunctional hydrogel can be a promising flexible material for a new generation of flexible sensors and flexible energy storage devices in a certain range of temperatures.

CAS / MDL: 9002-84-0
研究领域: 材料科学 · 能源存储 · 生物医学工程
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Journal of Energy Chemistry · 2022 · IF 13.599

A cerium-doped NASICON chemically coupled poly(vinylidene fluoride-hexafluoropropylene)-based polymer electrolyte for high-rate and high-voltage quasi-solid-state lithium metal batteries

Tao Huang,Wei Xiong,Xue Ye,Zhencheng Huang,Yuqing Feng,Jianneng Liang,Shenghua Ye,Jishou Piao,Xinzhong Wang,Yongliang Li,Xiangzhong Ren,Chao Chen,Shaoluan Huang,Xiaoping Ouyang,Qianling Zhang,Jianhong Liu

The isolated inorganic particles within composite polymer electrolytes (CPEs) are not correlated to the Li + transfer network, resulting in the polymer dominating the low ionic conductivity of CPEs. Therefore, we developed novel quasi-solid-state CPEs of a Ce-doped Na super ion conductors (NASICON) Na 1.3+ x Al 0.3 Ce x Ti 1.7− x (PO 4 ) 3 (NCATP) chemically coupled poly(vinylidene fluoride-hexafluoropropylene) (PVDF-HFP)/Li-bis(trifluoromethanes-ulfonyl)imide (LiTFSI) matrix. A strong interaction between Ce 3+ from NCATP and TFSI − anion from the polymer matrix contributes to the fast Li + transportation at the interface. The PVDF-HFP/NCATP CPEs exhibit an ionic conductivity of 2.16 × 0 −3 S cm −1 and a Li + transference number of 0.88. A symmetric Li/Li cell with NCATP-integrated CPEs at 0.1 mA cm −2 presents outstanding cycling stability over 2000 h at 25 °C. The quasi-solid-state Li metal batteries of Li/CPEs/LiFePO 4 at 2 C after 400 cycles and Li/CPEs/LiCoO 2 at 0.2 C after 120 cycles deliver capacities of 100 and 152 mAh g −1 at 25 °C, respectively.

研究领域: 材料科学 · 电化学 · 能源存储
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Matter · 2024 · IF 17.3

Physical ionogels with only 2 wt % gelators as efficient quasi-solid-state electrolytes for lithium batteries

Xueao Jiang,Zhaoen Liu,Weijian Liu,Da Yu,Jun Zhang,Xiwen Wang,Yan Zhang,Shiguo Zhang

Ionic liquid (IL)-based gel electrolytes (ionogels) show great potential as quasi-solid-state electrolytes (QSSEs) for lithium-ion batteries (LIBs). However, conventional ionogels face challenges involving complex gelation processes, high gelator content (usually greater than 20 wt %), lower conductivity than neat ILs, and low Li + transference numbers. Here, we create novel lithium salt-containing supramolecular ionogels (SIGs) as efficient QSSEs for LIBs through a simple and environmentally friendly approach. By using a low-molecular-weight gelator, specifically 12-hydroxyoctadecanoic acid, lithium-containing IL electrolytes can be solidified at a gelator concentration of only 2 wt %. The resulting physical ionogels exhibit remarkable characteristics, including high ionic conductivity similar to neat ILs and improved electrochemical stability. In addition, these SIGs demonstrate a distinctive thermally reversible gel-to-sol transition, a quality not attainable in other QSSEs. This feature promotes better electrode/electrolyte contact, enabling excellent battery performance using LiFePO 4 , LiNi 0.8 Co 0.1 Mn 0.1 O 2 , and LiCoO 2 cathodes, along with Li metal and Li 4 Ti 5 O 12 anodes.

CAS / MDL: 538-74-9 9005-38-3
研究领域: 材料科学 · 能源技术
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Small · 2025 · IF 12.1

3D Silsesquioxane Cage-Based Covalent Organic Frameworks Enabling Efficient Ion Transport in Quasi-Solid-State Lithium Metal Batteries

Yuxin Xue,Qiong Lin,Xiangfeng Sun,Dongxia Li,Yulin Fu,Zhiqi Li,Yuanhao Shi,Chongxian Luo,Xuefeng Gui,Kai Xu

The resurgence of lithium metal batteries (LMBs) necessitates advancements in electrolyte engineering to regulate ion transport and manipulate interfacial characteristics. Noteworthy strategies encompass the development of high-efficiency lithium-ion conductors for quasi-solid-state composite electrolytes. In this context, two crystalline 3D COFs are presented that are thoughtfully designed by selecting decasilsesquioxane (T 10 ) cage building blocks and linear linkers to open up efficient ion-conducting pathways. The cage silsesquioxane-knotted COFs (CSQ-COFs) feature densely interconnected pore channels and a multimodal pore size distribution, which gives them the potential to function as ionic conductors. In addition, the dissociation of electrolyte salts by the silsesquioxane framework, along with the strong adsorption of anions, synergistically enhances ion transport. The coin cell assembled with CSQ-COF displays an ionic conductivity of 0.727 mS cm −1 at 80 °C, an E a of 0.12 eV, and t Li+ of 0.83. Therefore, Li symmetrical cell demonstrates excellent Li plating/stripping behaviors for 600 h under 0.5 mA cm −2 . The Li/LiFePO 4 cell containing the CSQ-COF solid-state electrolyte delivers an initial discharge capacity of ≈159.6 mAh g −1 at a rate of 0.5 C at room temperature with excellent capacity retention after 150 cycles. This work provides a novel insight on the development of 3D COF ionic conductors.

研究领域: 材料科学 · 电化学
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JOURNAL OF POWER SOURCES · 2022 · IF 9.794

Anticorrosion of hydrophobic membrane on aluminum electrode for alkaline quasi solid Al-air batteries

Songmao Zhang,Yichun Wang,Yawen Li,Manhui Wei,Keliang Wang

Primary quasi-solid Al-air batteries with hydrogel have attracted increasing research attention owing to their high energy density , ionic conductivity , good handling and safety. However, a severe corrosion at open-circuit potential destroy the lifespan and performance of discharge. Suppressing the corrosion of Al anode at standby is of great importance. Here, we present a coating hydrophobic membrane on Al surface to restrain open-circuit corrosion, where the hydrophobic property of the protective membrane is analyzed by contact angle test , changing from 22.48 to 149.48°. The results of electrochemical polarization measurement demonstrate that the corrosion inhibition efficiency of the hydrophobic membrane are 81.6%. Also, the discharge performance of assemble quasi solid Al-air batteries are revealed, and compared with pure Al electrode, the lifetime and special capacity of coated Al electrode is enhanced, expressing special capacity of 1126 mA h g −1 at 10 mA cm −2 and a power density of 36.3 mW cm −2 . Meanwhile, the lifespan of coated Al electrode is approximately prolonged by 34% at interval discharge mode . This work demonstrates a hydrophobic membrane on Al-electrode opens up a prospect of a corrosion inhibition for Al-air batteries.

研究领域: 材料科学 · 电化学
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Sustainable Energy & Fuels · 2023 ·Vol. 7 ·期 4 ·986-995 · IF 5.6

In situ UV-cured composite electrolytes for highly efficient quasi-solid-state lithium ion batteries with wide temperature range applications

Pengcheng Zhou,Yuxian Liu,Jian Chen,Shouqiang Lu,Huiyang Li

The replacement of flammable electrolytes with non-flammable electrolytes is the ultimate solution for addressing the safety concerns related to lithium-ion batteries. In this context, inorganic/polymer composite electrolytes (IPCEs) offer the advantages of high flexibility, stability, ionic conductivity, and interfacial compatibility and therefore have received growing research attention. Herein, a novel IPCE based on a Norland optical adhesive (NOA81) and a Li-rich fast ion conductor Li10.7Al0.24La3Zr2O12 for quasi-solid-state lithium-ion batteries was designed and synthesized via solvent-free in situ ultraviolet (UV) curing. In this system, polyethylene oxide and poly(vinylidene fluoride-co-hexafluoropropylene) were used to modify the polymers, and sebaconitrile was used as a plasticizer. Screen printing was also employed during the manufacturing process. The composite electrolyte displayed a lithium-ion conductivity of 1.3 × 10−4 S cm−1 at 25 °C and sustained good stability up to 5.43 V (vs. Li+/Li). Lithium-ion batteries fabricated using the composite electrolyte, a LiNi1/3Mn1/3Co1/3O2 (NMC111) cathode, and a Li4Ti5O12 (LTO) anode achieved a specific capacity of 128 mA h g−1 and exhibited an 80% capacity retention after 154 cycles at 0.2C under testing at 25 °C. In addition, this battery exhibited an extremely high coulombic efficiency (>99.5%) over its entire cycle life. The NMC111 loading in the cathode reached 11.7 mg cm−2, which is comparable to those of commercialized electrodes. Significantly, the battery retained excellent electrochemical performances over a wide temperature range from 25 to 100 °C and achieved the highest specific capacity of 143 mA h g−1 at 45 °C.

CAS / MDL: 90076-65-6 9011-17-0
研究领域: 材料科学 · 能源存储技术
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Surfaces and Interfaces · 2023 · IF 6.2

Ultra-long cycle life flexible quasi-solid-state alkaline zinc batteries enabled by PEDOT:PSS encapsulated Ni3S2 nanorods

Xinying Guo,Lian Wu,Longbin Li,Jingfei Zhang,Chen Wu,Liwen Wang,Yizhong chen,Wei Zeng

Alkaline nickel-zinc (Ni-Zn) batteries are considered as one of the most promising rechargeable battery systems. However, the poor cycling stability of the Ni cathode limit their service life. Herein, a conductive polymer (PEDOT:PSS) encapsulated Ni 3 S 2 hollow nanorod structure via facile immersion is proposed. PEDOT:PSS coating layer can not only provide adhesion for Ni 3 S 2 nanorods to prevent Ni 3 S 2 from falling off the substrate during cycling, but also facilitate electron transfer via the complete conductive pathway. The hollow nanorods structure of Ni 3 S 2 is beneficial to mitigate the volume change and accelerate the rapid transport of ions. Besides, a gel electrolyte with double network porous structure in our battery system is well designed. The ionic association of sodium alginate on Zn 2+ can effectively reduce the activity of bound water molecules in the solvation sheath of Zn 2+ , inhibit the side reaction and dendrite generation through the ion-confinement effect, to achieve uniform deposition of zinc ions . As a consequence, the as-designed quasi-solid-state flexible Ni-Zn battery demonstrates a high specific capacity of 1.06 mAh cm −2 (276.04 mAh g −1 ) at 8 mA cm −2 and an ultra-long cycle stability over 10,000 cycles with a capacity retention of 88.96% at 30 mA cm −2 .

研究领域: 材料科学 · 电化学 · 能源存储
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Nature Communications · 2025 ·Vol. 16 ·期 1 ·1-12 · IF 15.7

Ion bridging enables high-voltage polyether electrolytes for quasi-solid-state batteries

Hou Tianyi,Wang Donghai,Jiang Bowen,Liu Yi,Kong Jia,He Yanbing,Huang Yunhui,Xu Henghui

Polyether electrolytes have been widely recognized for their favorable compatibility with lithium-metal, yet they are hampered by intrinsically low oxidation thresholds, limiting their potential for realizing high-energy Li-metal batteries. Here, we report a general approach involving the bridge joints between non-lithium metal ions and ethereal oxygen, which significantly enhances the oxidation stability of various polyether electrolyte systems. To demonstrate the feasibility of the ion-bridging strategy, a Zn 2+ ion-bridged polyether electrolyte (Zn-IBPE) with an extending electrochemical stability window of over 5 V is prepared, which enables good cyclability in 4.5 V Li||LiCoO 2 batteries. Ampere-hour-level quasi-solid-state batteries of SiO-graphite||LiNi 0.8 Mn 0.1 Co 0.1 O 2 (10 Ah, N/P ratio of 1.12, 303 Wh kg −1 at 0.1 C based on the total weight of the pouch cells) and 60 μm-Li||LiNi 0.9 Mn 0.05 Co 0.05 O 2 (18 Ah, N/P ratio of 2.5, 452 Wh kg −1 at 0.33 C based on the total weight of the pouch cells) pouch cells with Zn-IBPE present elevated electrochemical performance, benefiting from adequate interfacial stability. Nail penetration tests evidence high battery safety enabled by Zn-IBPE in 4 Ah graphite||LiNi 0.8 Mn 0.1 Co 0.1 O 2 pouch cells without combustion or smoke. This work offers a pathway for designing high-voltage polymer electrolytes and a general solution for achieving high-performance quasi-solid-state batteries.

CAS / MDL: 33454-82-9
研究领域: 材料科学 · 电化学 · 能源存储
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