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Small · 2024 · IF 13

An Elastomeric Lithium-Conducting Interlayer for High-Performance LATP-Based Lithium Metal Batteries

Zhisong Geng,Yingqi Sun,Qing Zhang,Shao-Peng Shen,Liang Zhang,Jin-Chi Zheng,Yuan Luo,Yongzheng Shi,Zhe Chen

In response to the critical challenges of interfacial impedance and volumetric changes in Li (1+x) Al x Ti (2‑x) (PO 4 ) 3 (LATP)-based lithium metal batteries, an elastomeric lithium-conducting interlayer fabricates from fluorinated hydrogenated nitrile butadiene rubber (F-HNBR) matrix is introduced herein. Owing to the vulcanization, vapor-phase fluorination, and plasticization processes, the lithium-conducting interlayer exhibits a high elasticity of 423%, exceptional fatigue resistance (10 000 compression cycles), superior ionic conductivity of 6.3 × 10 −4 S cm −1 , and favorable lithiophilicity, rendering it an ideal buffer layer. By integrating the F-HNBR interlayer, the LATP-based lithium symmetric cells demonstrate an extended cycle life of up to 1600 h at 0.1 mA cm −2 and can also endure deep charge/discharge cycles (0.5 mAh cm −2 ) for the same duration. Furthermore, the corresponding lithium metal full cells achieve 500 cycles at 0.5 C with 98.3% capacity retention and enable a high-mass-loading cathode of 11.1 mg cm −2 to operate at room temperature.

研究领域: 材料科学 · 电化学
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ACS Applied Materials & Interfaces · 2017 · IF 7.504

Separators with Biomineralized Zirconia Coatings for Enhanced Thermo- and Electro-Performance of Lithium-Ion Batteries

Jun-Ke Pi,Guang-Peng Wu,Hao-Cheng Yang,Christopher G. Arges,Zhi-Kang Xu

Porous separators are key components for lithium-ion batteries (LIBs) and they have drawn considerable attention because of their vital role in governing battery cost and performance (e.g., power density, safety, and longevity). Here, zirconia-coated separators were fabricated via a facile biomineralization process with the aim to improve the performance of commercialized polypropylene separators. The as-prepared organic–inorganic composite separators show excellent thermal stability, even at the melting temperature (160 °C) of polypropylene. This is due to the well-distributed zirconia coatings on the separator surfaces. Furthermore, the interfacial impedance of the composite separators is only 343.8 Ω, which is four times lower than the pristine polypropylene ones. The results demonstrate an attractive method to prepare organic–inorganic composite separators with outstanding properties, which makes them promising candidates for high-performance LIBs.

CAS / MDL: 9002-98-6
研究领域: 材料科学 · 能源技术
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ACS Applied Materials & Interfaces · 2021 · IF 9.229

Ultrastable Anode/Electrolyte Interface in Solid-State Lithium-Metal Batteries Using LiCux Nanowire Network Host

Qiushi Dai,Jun Zhao,Hongjun Ye,Jingzhao Chen,Yong Su,Tingting Yang,Qiunan Liu,Haiming Sun,Hui Li,Jingming Yao,Zhiying Gao,Xingjie Fu,Dingding Zhu,Jitong Yan,Mingyu Li,Hailong Qiu,Qiao Huang,Liqiang Zhang,Yongfu Tang,Xiangxin Guo,Jianyu Huang

High interfacial resistance and uncontrollable lithium (Li) dendrite are major challenges in solid-state Li-metal batteries (SSLMBs), as they lead to premature short-circuiting and failure of SSLMBs. Here, we report the synthesis of a composite anode comprising a three-dimensional LiCux nanowire network host infiltrated with Li (Li* anode) with low interfacial impedance and superior electrochemical performance. The Li* anode is fabricated by dissolving Cu foil into molten Li followed by solidification. The Li* anode exhibits good wettability with Li6.4La3Zr1.4Ta0.6O12 (LLZTO) and high mechanical strength, rendering low Li*/LLZTO interfacial impedance, homogeneous deposition of Li, and suppression of Li dendrites. Consequently, the Li* anode-based symmetric cells and full cells with LiNi0.88Co0.1Al0.02O2 (NCA), LiFePO4 (LFP), and FeF2 cathodes deliver remarkable electrochemical performance. Specifically, the Li*/LLZTO/Li* symmetrical cell achieves a remarkably long cycle lifetime of 10 000 h with 0.1 mA·cm–2; the Li*/LLZTO/NCA full cell maintains capacity retention of 73.4% after 500 cycles at 0.5C; and all-solid-state Li*/LLZTO/FeF2 full cell achieves a reversible capacity of 147 mAh·g–1 after 500 cycles at 100 mA·g–1. This work demonstrates potential design tactics for an ultrastable Li*/garnet interface to enable high-performance SSLMBs.

研究领域: 材料科学 · 电化学
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ACS Applied Energy Materials · 2024 · IF 5.4

A PVDF-HFP-Based Gel Polymer Electrolyte onto Air Cathode by UV-Curing for Lithium–Oxygen Batteries

Mingming Cui,Hong Sun,Zhichao Xue,Qiang Li,Tianyu Zhang,Qunying Kang

Using gel polymer electrolytes (GPEs) instead of liquid electrolytes is a sensible and effective strategy for safety reasons. A GPE membrane was prepared by UV-curing using poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP) as the polymer substrate material and an optimized ratio. The GPE membrane exhibited good flexibility and a higher ionic conductivity (σ = 0.63 mS cm–1). The RuO2@C/GPE/Li (abbreviated as S-GPE) battery is employed to demonstrate the electrochemical performance of GPE. The battery exhibits an Rct of 255.9 Ω, accompanied by a lack of cycle stability, with a cycle life of only 110 h. The results indicate that it is challenging to enhance the battery’s overall performance by solely improving the internal transfer performance of the electrolyte and ignoring the high interface impedance caused by the “solid–solid” contact at the electrolyte–electrode interface. Based on these findings, a straightforward one-step method is adopted to combine GPE with the air cathode by in situ photopolymerization and assemble it into RuO2@C-GPE/Li (abbreviated as I-GPE) battery used to demonstrate the electrochemical performance of the integrated GPE. The Rct value of the battery is 89.66 Ω, with a notable improvement in cycle stability. The battery’s cycle life is 940 h, which is 8.5 times that of the sandwich structure lithium–oxygen battery. The results indicate that preparing an integrated GPE by in situ photopolymerization of the electrolyte electrode is a straightforward and effective method to improve poor interfacial compatibility and can provide a theoretical basis for subsequent in-depth research.

研究领域: 材料科学 · 电化学
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JOURNAL OF POWER SOURCES · 2025 · IF 7.9

Enhancing performance in all-solid-state lithium batteries with tape cast sandwich-like flexible composite solid electrolyte membranes

Hairui Weng,Yuhao Zou,Chenyao Wang,Mingjuan Li,Luyi Sun,Xinzhi Chen

All-solid-state lithium batteries (ASSLBs) are considered to be the next generation of the most promising lithium battery technology due to their energy density, safety and stability. Nevertheless, the solid-state electrolyte (SSE), a critical element in ASSLBs, encounters notable obstacles like limited ionic conductivity and elevated interfacial impedance. A sandwich like composite solid electrolyte is proposed to address the above issues. This design features a ceramic-rich (CR) solid electrolyte membrane sandwiched between two polymer-rich (PR) solid electrolyte membranes (named PR-CR-PR). The CR membrane offers mechanical strength, preventing lithium dendrites from penetrating, while the PR membranes enhance interfacial contact with the electrodes. The PR-CR-PR electrolyte not only enhances the stability of Li metal, enabling stable cycle for over 500 h, but also extends the electrochemical window to 6.17 V. Electrochemical results show that the LiFePO 4 /PR-CR-PR/Li battery achieves a specific capacity of 161.97 mAh g −1 at 0.2 C. The battery still maintains a high discharge specific capacity of 147.72 mAh g −1 and a capacity retention rate of 91.2 % after 500 cycles. This study demonstrates a promising strategy to prepare low-cost and highly stable electrolytes using a multilayer design for further mass production of high energy density ASSLBs.

研究领域: 材料科学 · 能源技术
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ACS Applied Materials & Interfaces · 2025 · IF 8.2

Biovegan Leather Sensor: A Mycelium Functionalized Material for Electrophysiological Signal Monitoring

Rui Zhang,Siyuan Cheng,Zaifeng Pan,Fenghui Yang,Yunqing Liu,Ruifa Su,Baoli Zha,Ruijie Xie,Bing Zheng,Jiansheng Wu,Fengwei Huo

Electrode patches are becoming increasingly vital in the fields of wearable electronics and physiological health monitoring. However, the nondegradable nature and complex functionalization process of traditional dry electrodes limit their widespread use. In contrast, mycelium-based biovegan leather offers an ideal alternative for flexible electrodes, providing benefits such as biodegradability and ease of preparation. To overcome the mechanical performance and stability challenges inherent in pure mycelium, this study develops a mycelium–polypyrrole composite material (P-MCM) that demonstrates reliable mechanical and electrical properties, making it suitable for the daily monitoring of human electrophysiological signals. The P-MCM exhibits a tensile strength of 3 MPa, an elongation at break of 13%, a conductivity of 51.10 S/m, and an interface impedance of 52.6 kΩ/cm2 for the electrode–skin system at 10 Hz. The low interface impedance of P-MCM electrodes allows for the stable acquisition of electrocardiogram, electromyogram, and electroencephalogram signals with performance on par with commercial electrodes. It is expected that this work will provide valuable insights and foundational materials for the advancement of flexible electrodes.

CAS / MDL: 1401-55-4
研究领域: 材料科学 · 生物医学工程 · 可穿戴设备
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Nature Communications · 2021 ·Vol. 12 ·期 1 ·1-8 · IF 14.919

Improving the alkali metal electrode/inorganic solid electrolyte contact via room-temperature ultrasound solid welding

Wang Xinxin,Chen Jingjing,Wang Dajian,Mao Zhiyong

The combination of alkali metal electrodes and solid-state electrolytes is considered a promising strategy to develop high-energy rechargeable batteries. However, the practical applications of these two components are hindered by the large interfacial resistance and growth of detrimental alkali metal depositions (e.g., dendrites) during cycling originated by the unsatisfactory electrode/solid electrolyte contact. To tackle these issues, we propose a room temperature ultrasound solid welding strategy to improve the contact between Na metal and Na 3 Zr 2 Si 2 PO 12 (NZSP) inorganic solid electrolyte. Symmetrical Na|NZSP | Na cells assembled via ultrasonic welding show stable Na plating/stripping behavior at a current density of 0.2 mA cm −2 and a higher critical current density (i.e., 0.6 mA cm −2 ) and lower interfacial impedance than the symmetric cells assembled without the ultrasonic welding strategy. The beneficial effect of the ultrasound welding is also demonstrated in Na|NZSP | Na 3 V 2 (PO 4 ) 3 full coin cell configuration where 900 cycles at 0.1 mA cm −2 with a capacity retention of almost 90% can be achieved at room temperature.

研究领域: 材料科学 · 能源技术
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ELECTROCHIMICA ACTA · 2022 · IF 7.336

Effects of polishing treatments on the interface between garnet solid electrolyte and lithium metal

Xiaoning Ma,Youlong Xu

Garnet Li 7 La 3 Zr 2 O 12 (LLZO) is an attractive and highly promising solid electrolyte, has made a significant progress in the battery performance to achieve higher energy density and better safety. However, the poor wettability between the interface of garnet and Li metal anode leads to high interfacial impedance and the penetration of Li dendrites during cycling, which limits the practical application of garnet. Polishing treatment is a very simple and convenient physical treatment method for the surface of garnet. Here, we investigate the effects of surface treatment of Li 6.25 Al 0.2 La 3 Zr 2 O 11.85 Br 0.15 (LALZOBr 0.15 ) with different grit sizes of sandpaper on the wettability and interfacial resistance between it and Li metal. Compared to coarse and very fine sandpaper, the LALZOBr 0.15 –600 electrolyte polished with 600-grit sandpaper was significantly reduced the interfacial impedance to 20.9 Ω cm 2 , ensuring tight contact at the Li|LALZOBr 0.15 –600 interface, thereby further inhibiting the growth of Li dendrites. Moreover, benefiting from the excellent interface, Li|LALZOBr 0.15 –600|Li symmetric cell exhibited an excellent cycling stability and could be cycled at 0.3 mA cm −2 over 1300 cycles without short-circuiting. Applying it to quasi-solid-state batteries and all-solid-state batteries, which also showed great electrochemical performance. Our work demonstrates the importance of using a moderate grit sandpaper for electrolyte surface treatment.

研究领域: 材料科学 · 电化学 · 能源存储
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COMPOSITES SCIENCE AND TECHNOLOGY · 2019 · IF 6.309

Enhanced electrochemical performance of solid PEO/LiClO4 electrolytes with a 3D porous Li6.28La3Zr2Al0.24O12 network

Xuelian Fu,Yuchao Li,Chengzhu Liao,Weiping Gong,Mingyang Yang,Robert Kwok Yiu Li,Sie Chin Tjong,Zhouguang Lu

Low ionic conductivity and large interfacial impedance between the electrode and electrolyte are the main bottleneck issues of the current solid electrolytes . In this study, a novel 3D hierarchical solid electrolyte was developed to tackle the large interfacial impedance problem. A flexible polyethylene oxide/lithium chlorate (PEO/LiClO 4 ) was in-situ formed inside the 3D porous Li 6.28 La 3 Zr 2 Al 0.24 O 12 (LLZAO) network by simply using a cleanroom wiper as the template. The obtained 3D LLZAO-PEO/LiClO 4 composite solid electrolyte exhibited a high ionic conductivity of 2.25 × 10 −5  S cm −1 at 30 °C, being 30.7 times higher than that of pristine PEO/LiClO 4 electrolyte. The improved ionic conductivity was attributed to the 3D porous LLZAO structure with continuous fast ion transport pathways. In addition, the 3D LLZAO network can effectively inhibited the growth of lithium dendrite , leading to excellent stability and desirable safety during lithium stripping/plating cycling. Furthermore, the all-solid-state LiFePO 4 /Li battery system based on the obtained 3D LLZAO-PEO/LiClO 4 electrolyte showed a high initial discharge specific capacity of 143.8 mAh·g −1 and a high capacity retention of 86% after 200 cycles at 60 °C. This 3D composite solid electrolyte design is very effective in reducing the interfacial impedance and provides a solution for the further development of high-performance solid electrolyte for all-solid-state rechargeable batteries.

研究领域: 材料科学 · 电化学 · 电池技术
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2020 · IF 7.489

Construction of an ultrasensitive electrochemical sensing platform for microRNA-21 based on interface impedance spectroscopy

Tianjiao Meng,Dan Zhao,Huimin Ye,Yue Feng,Huan Wang,Yufan Zhang

A hybridization chain reaction (HCR) amplification-based electrochemical impedimetric biosensor is fabricated for the quick, sensitive, and specific detection of miRNA-21 (miR-21) via monitoring of electrode interfacial property changes in real-time. Two sequences of H1 and H2 are adopted to trigger HCR amplification. A large amount of linear DNA concatemer are formed which could change the interfacial properties of the electrode. Interfacial charge transfer resistance difference ( R ct ) is probed via electrochemical impedance spectroscopy (EIS) and Randles equivalent circuit. After amplifying via HCR, oligonucleotides with negatively charged repelling [Fe(CN) 6 ] 3−/4− ions can form a spatial blockage. HCR amplification strategy markedly enhanced the electrochemical signal with a limit of detection (LOD) down to 4.63 fM (S/N = 3). This strategy exhibited excellent selectivity for three different miRNAs: miR-199a, miR-141, and miR-155. Moreover, results show that the proposed method can be applied to miR-21 detection in the total RNA extracted from five cells. This work presents an enzyme-free and label-free EIS nucleic acid sensor for sensitively and selectively detecting miR-21, offering a promising approach in early diseases diagnosis.

研究领域: 生物化学 · 分析化学 · 生物技术 · 分子生物学
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ACS Applied Materials & Interfaces · 2023 · IF 9.5

Tuning the Covalent Coupling Degree between the Cathode and Electrolyte for Optimized Interfacial Resistance in Solid-State Lithium Batteries

Zhuohao Xie,Weicai Zhang,Yansen Zheng,Yongyin Wang,Yingliang Liu,Yeru Liang

The development of promising solid-state lithium batteries has been a challenging task mainly due to the poor interfacial contact and high interfacial resistance at the electrode/solid-state electrolyte (SSE) interface. Herein, we propose a strategy for introducing a class of covalent interactions with varying covalent coupling degrees at the cathode/SSE interface. This method significantly reduces interfacial impedances by strengthening the interactions between the cathode and SSE. By adjusting the covalent coupling degree from low to high, an optimal interfacial impedance of 33 Ω cm–2 was achieved, which is even lower than the interfacial impedance using liquid electrolytes (39 Ω cm–2). This work offers a fresh perspective on solving the interfacial contact problem in solid-state lithium batteries.

研究领域: 材料科学 · 电化学
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ACS Applied Energy Materials · 2021 · IF 6.024

Quasi-Solid-State Li–O2 Batteries Performance Enhancement Using an Integrated Composite Polymer-Based Architecture

Shidong Song,Dequan Zhang,Yanli Ruan,Limei Yu,Yongqiang Xu,Joykumar Thokchom,Donghai Mei

Heightened attention for solid-state Li–O2 batteries (SSLOBs) exists due to their improved safety, wider electrochemical window, and high energy density in addition to the solid electrolyte’s innate capability of suppressing Li dendrite penetration and shielding the Li metal anode from oxygen, CO2, and moisture in the air, in comparison with the conventional Li–O2 batteries using liquid organic electrolytes. Herein, a cathode supported quasi-SSLOB with an integrated composite polymer-based architecture (ICPA) is developed with reduced interfacial resistance, extended triple-phase boundaries (TPBs) for Li–O2 reactions, and a thin film solid-state electrolyte. The Li–O2 cell with ICPA (denoted as ICPA cell) exhibits a lower charge transfer impedance than its counterpart with the same composite polymer electrolyte (CPE) but a nonintegrated structure (termed the CPE cell). The former shows reduced interfacial impedance between electrolyte and cathode and increased TPBs. Furthermore, the ICPA cell delivers higher discharge capacity, lesser capacity decay, and significantly lower impedance rise after cycles than the CPE cell, ascribed to the continuous Li-ion transport in ICPA and the resulting more efficient discharge and charge processes. Under a limited capacity cycling protocol of 300 mAh g–1, the ICPA cell achieves excellent reversibility for 78 cycles, remarkably surpassing the CPE cell which only performs 44 cycles in addition to showing half of the after-cycle impedance compared to that for the CPE cell. Nonetheless, the same composite polymer electrolyte used for both CPE- and ICPA-based cells demonstrates excellent stability toward Li metal after long-term cycling. These findings manifest that the design and application of cathode supported SSLOB with ICPA can be a promising approach to achieve high-performance Li–O2 batteries.

研究领域: 材料科学 · 电化学 · 能源存储技术
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