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JOURNAL OF POWER SOURCES · 2018 · IF 6.945

Lithiated Nafion as polymer electrolyte for solid-state lithium sulfur batteries using carbon-sulfur composite cathode

Jing Gao,Chunshui Sun,Lei Xu,Jian Chen,Chong Wang,Decai Guo,Hao Chen

Due to flexible property and light weight, the lithiated Nafion membrane swollen with PC (PC-Li-Nafion) has been employed as both solid-state electrolyte and separator to fabricate solid-state Li-S cells. The electrochemical measurements of PC-Li-Nafion membrane show that its Li-ion transference number is 0.928, ionic conductivity of 2.1 × 10 −4  S cm −1 can be achieved at 70 °C and its electrochemical window is 0 ∼ +4.1 V vs. Li + /Li. It is observed that the Li dendrites are suppressed by using PC-Li-Nafion membrane due to its single-ion conducting property. The amounts of Li-Nafion resin binder and conductive carbon in the cathode are optimized as 40% and 10% respectively to make a balance of ionic and electronic conductivities . A thin-layer Li-Nafion resin with a thickness of around 2 μm is fabricated between the cathode and PC-Li-Nafion membrane to improve the interfacial contact and further enhance the specific capacity of the cell. When measured at 70 °C, the Li-S cell delivers a reversible specific capacity of 1072.8 mAh g −1  (S) at 0.05 C and 895 mAh g −1  (S) at 1 C. The capacity retention at 1 C is 89% after 100 cycles. These results suggest that high-performance solid-state Li-S cells can be fabricated with the Li-Nafion polymer electrolyte .

研究领域: 电化学 · 能源材料 · 固态电池 · 聚合物电解质 · 锂离子电池 · 电极界面工程 · 储能技术
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CHEMICAL ENGINEERING JOURNAL · 2024 · IF 13.3

Ternary stabilization strategies for succinonitrile-based in situ polymerized electrolyte enabling high-performance solid lithium metal batteries

Chenyu Lin,Tianqi Yang,Haiyuan Zhang,Donghuang Wang,Wenkui Zhang,Yao Wang,Yang Xia,Hui Huang,Xinhui Xia,Yongping Gan,Xinping He,Xinyong Tao,Jun Zhang

Solid-state lithium metal batteries with high energy density and safety have gained increasing attention due to their potential applications. However, the practical use of solid electrolytes is hindered by several challenges. These include poor compatibility at the electrode–electrolyte interface, low ionic conductivity at room temperature, and fast capacity degradation. To address these issues, here we propose ternary strategies by in-situ cross-linked plastic crystal electrolyte (in-situ PCE) based on succinonitrile (SN). Through the in-situ polymerization of SN with polyacrylonitrile/poly(vinylidene difluoride) (PAN/PVDF) nanofibers separator, excellent mechanical strength and compatibility at the electrode–electrolyte interface are achieved. The cross-linked structure of thermally polymerized ethoxylated trimethylolpropane triacrylate (ETPTA) immobilizes the SN molecule, preventing its contact with the lithium metal and inhibiting irreversible side reactions. Additionally, a LiF-rich passivation layer is employed to further protect the SN at the electrolyte-lithium metal interface. The dual protection from ETPTA and LiF offers excellent stability to lithium. Hence, the in-situ PCE exhibits high ionic conductivity (0.79 mS cm −1 at 30 °C) and wide electrochemical window (4.56 V, vs Li + /Li). The cells exhibit excellent cycling stability and high-rate performance. LiFePO 4 //Li cells retain 96.6 % capacity after 1000 cycles at 10C rate. This study provides valuable insights into the development of high-performance solid-state electrolytes.

研究领域: 材料科学 · 电化学 · 能源存储 · 高分子化学 · 固态离子学
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MACROMOLECULAR MATERIALS AND ENGINEERING · 2018 ·Vol. 304 ·期 1 ·1800477 · IF 2.69

Chemically Modified Polyvinyl Butyral Polymer Membrane as a Gel Electrolyte for Lithium Ion Battery Applications

Ziqiang Xu,Wenlei Li,Zhi Chen,Dongxia Wang,Tingting Feng,Hanna Potapenko,Mengqiang Wu

A novel porous membrane of chemically modified polyvinyl butyral (mPVB), with improved thermal properties and chemical stability for lithium ion battery applications, is successfully synthesized by utilizing the chain extension reaction of the OH units from PVB. The porous mPVB membranes are obtained via the tape casting and phase inversion method. The corresponding gel polymer electrolyte (GPE) is achieved by immersing the as-prepared membranes in the liquid electrolyte. The electrochemical performances of the GPE show that the mPVB membranes have the features of good uniformity, high porosity ( ≈ 90%), great thermal stability, and high mechanical strength. Moreover, the GPE exhibits good chemical stability, a wide electrochemical window, as well as high ionic conductivity ( ≈ 1.21 × 10 −3 S cm −1 ). A test of a Li/GPE/LiFePO 4 battery cell shows a capacity of 147.7 mAh g −1 and excellent cycling stability, demonstrating the great potential of the mPVB-based GPE for lithium ion battery applications.

研究领域: 材料科学 · 电化学 · 能源存储 · 高分子化学 · 电池技术
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CHEMICAL ENGINEERING JOURNAL · 2023 · IF 15.1

High-Performance transparent and flexible Zinc-Ion Solid-State batteries based on nanotube network and hydrogel electrolyte

Nan Sun,Hongjin Sun,Dongchen Tan,Qinglei Guo,Zhe Zhang,Zhiyuan Tao,Chengcheng Fang,Jingyuan Bu,Jijie Huang,Chengming Jiang

Transparent and flexible electronics research is a lively and promising domain that holds immense potential for a plethora of innovative applications in consumer electronics, healthcare, and renewable energy sectors. It would be extremely beneficial to develop internal energy sources that are transparent and do not alter the visual appearance would. In this study, we introduce the design of a transparent and flexible zinc-ion solid-state battery (TFZSB), all of whose component elements, such as the electrode, electrolyte/diaphragm, and packaging, are made of transparent and soft materials. The electrodes have been constructed with a framework of nanotube (NT) networks, while the electrolyte is built from a polyacrylamide (PAM) hydrogel material. The suggested electrode design effectively leverages the outstanding optical properties and flexibility of the NT network, while the construction assimilates the PAM hydrogel for providing electrical protection and fabricate the electrolyte, culminating in a resilient interface, which confers exceptional electrochemical stability under varying mechanical strains. With a strong visible-light spectrum transmittance of >80 % and a retention Coulombic efficiency of >92 % under large-scale strains, the TFZSB demonstrates a mass specific capacity of 122.6mAh/g. This TFZSB constitutes a breakthrough in the realm of wearable and smart electronics, and holds the potential to unlock a multitude of opportunities in the future by bridging the domains of energy storage and flexibility/transparency.

研究领域: 材料科学 · 电化学 · 能源存储 · 柔性电子学 · 纳米科技 · 高分子材料 · 生物医学工程
✓ 已验证 DOI 高影响因子
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INTERNATIONAL JOURNAL OF ENERGY RESEARCH · 2022 ·Vol. 46 ·期 12 ·17056-17067 · IF 4.672

Multicomponent doped hierarchically porous carbon derived from natural polyelectrolyte for high-performance supercapacitors

Tao Lyu,Shiying Lin,Lanlan Mo,Feijun Wang,Ziqiang Shao

Summary Natural polyelectrolyte complex has designable structure, unique advantages of composite and strong intermolecular or intramolecular force without chemical cross-linking agents, showing the advantages of good biodegradability and low toxicity. This work reports an application research of natural polyelectrolyte in energy storage device. A multi-doped hierarchically porous carbon is fabricated from polyelectrolyte of sodium lignosulfonate and chitosan and used as electrode material of supercapacitor. The material characterization reveals its large specific surface area of 1768 m 2 g −1 , pore volume of 0.94 cm 3 g −1 with optimum 3D porous structure, and high heteroatom (oxygen, nitrogen, and sulfur) concentration. Benefit from these, the electrodes it made exhibit 354 F g −1 specific capacitance at 1 A g −1 current density, outstanding rate retention of 82.9% at a testing environment of 20 A g −1 , and 97.8% capacitance retention in 3 M KOH electrolyte after 10 000 cycles. Using this material, all-solid symmetric supercapacitor devices show 30.11 Wh kg −1 energy density at 520.88 W kg −1 power density and retains 20.90 Wh kg −1 at 1.03 kW kg −1 . These remarkable electrochemical performances prove the promising porous carbon in this work as electrode material with excellent performance for supercapacitors.

研究领域: 材料科学 · 电化学 · 能源存储 · 纳米材料 · 功能材料 · 碳材料
✓ 已验证 DOI 高影响因子
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SOLID STATE IONICS · 2020 · IF 3.107

Enhancing the electrochemical performances of Li7P3S11 electrolyte through P2O5 substitution for all-solid-state lithium battery

Yayu Guo,Huilan Guan,Wenxiu Peng,Xuelei Li,Yue Ma,Dawei Song,Hongzhou Zhang,Chunliang Li,Lianqi Zhang

Li 7 P 3 S 11 (70Li 2 S·30P 2 S 5 ) sulfide is a promising electrolyte candidate for all-solid-state lithium batteries (ASSLBs) owing to its high ionic conducivity and wide electrochemical stability window. However, the sensitivity to moisture and the poor interfacial compatibility with electrodes limit the conventional application of Li 7 P 3 S 11 . Herein, we present a substitution strategy to produce a O-incorporated 70Li 2 S·(30-x)P 2 S 5 ·xP 2 O 5 (mol%) sulfide electrolyte to address above issues. The elaborately designed electrolyte is prepared via wet vibration ball milling technique with P 2 O 5 substitution content of 1, 3 and 5. As a result, the 70Li 2 S·27P 2 S 5 ·3P 2 O 5 electrolyte displays the highest ionic conductivity of 2.61× 10 −3  S cm −1 which outperforms than that of pristine Li 7 P 3 S 11 (ionic conductivity of 1.35 × 10 −3  S cm −1 ) and the assembled LiCoO 2 @LiNbO 3 /70Li 2 S·27P 2 S 5 ·3P 2 O 5 /Li-In ASSLB exhibits the superior capacity retention of 93.2% after 100 cycles at 0.5C. The reason for the developed electrochemical performance lies in the substitution of the non-bridging sulfur atom with bridging oxygen atom, from which the interaction between electrolyte and lithium ions is weakened, thereby the rapid transfer of lithium ions is facilitated. Furthermore, Raman and XRD results indicate that the adverse interfacial reactions are suppressed through P 2 O 5 substitution. This work suggests that P 2 O 5 substitution is an effective strategy for sulfide electrolyte toward high energy all-solid-state lithium batteries.

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 APPLIED POLYMER SCIENCE · 2024 ·Vol. 141 ·期 44 ·e56156 · IF 2.7

Effect of thermal pre-compressing on ionic conductivity and mechanical properties of PEO-based solid-state electrolytes

Hao Sun,Qinghua Yang,Detao Kong,Yanrui Li,Yaolong He,NengHui Zhang,Hongjiu Hu

Polyethylene oxide (PEO)-based solid polymer electrolytes are regarded as promising electrolyte materials because of their safety and flexibility. However, low ionic conductivity at ambient temperature and poor mechanical properties have been a hindrance to its development. In this work, we thermally compressed the PEO-based electrolytes and explored the ionic conductivity, mechanical performance, free volume, and thermal properties of the electrolyte under different thermal pre-compressing strains (TPC-strains). The results show that TPC-strain can significantly improve the ionic conductivity, in-plane strength, stiffness, and cell specific capacity as well as the mechanical integrity of solid polymer electrolytes within the battery environment. However, it also results in a reduction in the modulus and stiffness of the SPEs in the through-plane. In particular, applying a TPC-strain of 10%–20% to the SPEs by thermal compressing may be a suitable option, which can increase the ionic conductivity of the through-plane to a factor of 3.4 compared with the uncompressed electrolyte, and increase the in-plane strength by up to 141%, resulting in better mechanical integrity during charging/discharging processes. At the same time, the compression modulus can be maintained at 80% or higher.

研究领域: 材料科学 · 电化学 · 高分子物理 · 能源存储 · 固态离子学
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ELECTROCHIMICA ACTA · 2015 · IF 4.504

The Contradiction Between the Half-Cell and Full-Battery Evaluations on the Tungsten-Coating LiNi0.5Co0.2Mn0.3O2 Cathode

Xinhe Yang,Zicheng Zuo,Haiyan Wang,Quanbin Chen,Hui Zhang,Zhenlei Huang,Borong Wu,Henghui Zhou

A one-step synthesis method is developed to prepare the Li[Ni 0.5 Co 0.2 Mn 0.3 ]O 2 (NCM 523) cathode with uniform tungsten-coating layer for lithium-ion battery . Such modified material shows similar properties with the bare NCM 523 in terms of the primary particles, secondary structure , and specific capacity. With W coating layer , the NCM 523 gives remarkable improvement in the long-term capacity retention in the half-cell testing, which is sharply inconsistent with the result from the full-battery tests, indicating a contradiction between the half-cell and full-battery tests in some case. After further investigations, such conflict between the half-cell and full-cell tests in evaluating the W-coating strategy is attributed to the dissolution of Li 2 WO 4 layer in the electrolyte, which probably destroys the solid electrolyte interface (SEI) on the graphite anode and irreversibly consumes the active lithium ions for renovating SEI in full-cell testing. These results will benefit researchers in the area of lithium-ion batteries to fully understand the differences between the half-cell and full-cell testing, and develop the effective strategies for cathode modifications.

研究领域: 电化学 · 材料科学 · 能源存储 · 电池技术 · 表面改性 · 固态离子学
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SOLID STATE IONICS · 2019 · IF 2.886

Conformal, nanoscale γ-Al2O3 coating of garnet conductors for solid-state lithium batteries

Fan Deng,Yongmin Wu,Weiping Tang,Shufeng Song,Zhaoyin Wen,Masashi Kotobuki,Li Lu,Jianyao Yao,Ning Hu,Janina Molenda

The use of garnet-type conductors as electrolytes for safe lithium solid-state batteries is impeded by the lack of critical processing strategy to stabilize and densify the cubic lithium garnets. The synthesis and processing of dense cubic lithium garnets are typically depending on solid state reaction as a result of unintentional Al contamination from the alumina crucibles at temperatures up to 1230 °C. High Al concentration is also believed to induce the sluggish migration of lithium ions . Here, we demonstrate an ultrathin, conformal γ-Al 2 O 3 surface coating on garnet solids by a hybrid microemulsion solid-state method for accomplishing rational and controllable synthesis and processing of dense cubic garnets with low Al concentration. The γ-Al 2 O 3 coating demonstrates fast-ion conducting Al-doped Li 6.75 La 3 Zr 1.75 Ta 0.25 O 12 phase with low Al concentration (~0.17 mol per formula unit), low tetragonal-to-cubic phase transformation temperature of 500 °C, and total conductivity of ~4.4 × 10 − 4  S cm − 1 . Specifically, the desired microstructures of the sintered pellets with uniform grains are revealed. As a proof-of-concept, we demonstrate that the nanoscale γ-Al 2 O 3 modification garnet conductor Li 6.75 La 3 Zr 1.75 Ta 0.25 O 12 is available to suppress lithium dendrites in symmetric Li/γ-Al 2 O 3 coating Li 6.75 La 3 Zr 1.75 Ta 0.25 O 12 /Li cells during lithium plating/stripping at room temperature, with current densities of 0.026 to 0.5 mA cm − 2 . The Li/γ-Al 2 O 3 coating Li 6.75 La 3 Zr 1.75 Ta 0.25 O 12 /LiNi 0.5 Co 0.2 Mn 0.3 O 2 cell delivered a high initial discharge capacity of ~164.2 mAh g − 1 , more importantly, an outstanding cycling performance with a capacity retention of 90.16% after 30 cycles at 0.1C and room temperature. This new synthesis route and the utilization of nanoscale γ-Al 2 O 3 surface modification could open up new avenue to lithium garnet conductors with reliable synthesis for all-solid-state lithium batteries application.

研究领域: 材料科学 · 电化学 · 固态离子学 · 能源存储 · 纳米材料 · 电池技术
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Applied Materials Today · 2024 · IF 7.2

Flexible electrolyte-gated transistor based on InZnSnO nanowires for self-adaptive applications

Lingyan Zheng,Zhen Liu,Shuwen Xin,Qi Chen,Jinbo Ming,Liren Wu,Jiaqi Xu,Peilong Xu,Kai Liu,Ramakrishna Seeram,Fengyun Wang

A pivotal characteristic of neuromorphic systems lies in their inherent capacity for self-adaptation, facilitating environmental adaptation through the attenuation of response to repetitive stimuli. Existing electrolyte-gated synaptic transistors face challenges in simulating these self-adaptive behaviors of the brain. In this work, flexible indium zinc tin oxide (IZTO) nanowires-based synaptic transistors exhibiting self-adaptive behavior were fabricated for the first time via a facile electrospinning technique. The prepared transistors can realize typical synaptic functions by continuously modulating the conductance, including excitatory/inhibitory postsynaptic current and short/long term potentiation. These properties are well maintained even under a bending radius of 12 mm. Additionally, the neuromorphic system based on IZTO nanowires-based transistors achieves a high recognition accuracy exceeding 90 % for hand-written digits recognition. The synaptic transistor exhibits obvious self-adaptive behavior and a low energy consumption with reduction of 8.2 %. Self-adaptive neuromorphic flexible transistors can not only enhance their resemblance to biological systems, but also advance the development of wearable devices and neuromorphic calculation.

研究领域: 材料科学 · 纳米科技 · 生物电子学 · 神经形态工程 · 柔性电子器件
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JOURNAL OF NON-CRYSTALLINE SOLIDS · 2019 · IF 2.6

Enhancing ionic conductivity in Ag3PS4 via mechanical amorphization

Ang Qiao,Haizheng Tao,Yuanzheng Yue

Amorphous conductors with high ionic conductivity are a promising candidate as electrolytes in all-solid state batteries. In this work, we prepared amorphous Ag 3 PS 4 conductor via a chemo-mechanical milling process, and then characterized its structure and electrochemical properties . The results show that Ag + conductivity of the amorphous Ag 3 PS 4 was remarkably enhanced by three orders of magnitude compared to its crystalline counterpart. Furthermore, the amorphous sample exhibits lower activation energy ( E a ) for ionic conductivity as a function of temperature. Structural characterizations indicate that the tetrahedral [PS 4 ] units were retained in amorphous Ag 3 PS 4 , but the Ag + ions became more liberated than those in the crystalline state, leading to the enhanced migration of Ag + ions, thereby, the ionic conductivity in amorphous Ag 3 PS 4 is drastically increased. This work provides insight into the crucial role of the disorder in raising the ionic conductivity of amorphized chalcogenide materials containing mobile ions.

研究领域: 材料科学 · 固体化学 · 能源材料 · 电化学 · 无机非金属材料 · 固态电池 · 离子传导
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Desalination and Water Treatment · 2024 · IF 1

Surface coating of a side-chain type polyelectrolyte for endowing perm-selectivity between specific anions to an anion-exchange membrane with a small loss of membrane conductivity

Yan-zhen Shen,Xun-liang Wang,Yu-xiang Jia,Meng Wang

The endowment of perm-selectivity for specific ions will further extend the applications of heterogeneous membrane. In this work, a side-chain type weak cationic polyelectrolyte, PVDF-g-PVP, was synthesized for surface hydrophobilization of heterogeneous anion-exchange membrane (AEM) in order to impart perm-selectivity between specific anions with different Gibbs hydration energy. After microstructure observation and chemical composition analyses by SEM, AFM, EA and FTIR, the perm-selectivity between specific anions, electrical resistance, transport number, limiting current density, surface homogeneity, as well as salt permeability of the modified AEMs were investigated. Series of electrodialysis experiments in SO 4 2– /Cl – system indicated that a significant perm-selectivity was indeed achieved by the attachment of PVDF-g-PVP coating. In particular, it was worth noting that only a small loss of membrane conductivity was observed after the functionalization. This should be closely related to the micro-phase separation morphology of the coating layer which was induced by the polarity difference between the main chains and side chains of PVDF-g-PVP. Besides, the chronopotentiometric analyses indicated surface homogeneity of the heterogeneous AEM was significantly enhanced and then effectively ameliorated concentration polarization behaviors at the membrane-solution interface. Meanwhile, the perm-selectivity for co-ions was also improved and suppressed back diffusion behaviors of salt driven by concentration gradient. In brief, the modifying scheme proposed in this work can effectively improve comprehensive transport properties of conventional heterogeneous AEM.

研究领域: 膜科学与技术 · 高分子材料化学 · 分离科学 · 电化学工程 · 功能材料
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