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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 · 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
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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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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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Journal of Materials Chemistry A · 2021 ·Vol. 9 ·期 38 ·22064-22071 · IF 12.732

Phase formation and ionic conduction in Na-doped Sr2MgSi2O7 melilite-type silicate

Wenda Zhang,Jie Feng,Fengqi Lu,Alberto J. Fernández-Carrión,Hui Fu,Xiaojun Kuang

Na-doped melilite-type silicate Sr2MgSi2O7 was reported to display high oxide ion conductivity. In this work, through multiple complementary techniques including X-ray diffraction, scanning electron microscopy, transmission electron microscopy, solid-state 29Si and 23Na nuclear magnetic resonance spectroscopy, and DFT calculations of defect formation energies, we found that it is hard to replace Sr with Na in Sr2MgSi2O7, and the Sr2−xNaxMgSi2O7−0.5x compositions formed mixed crystalline Sr2MgSi2O7 and Na-containing glassy phases. AC impedance spectroscopy measurements indicated that the ionic conduction in Sr2−xNaxMgSi2O7−0.5x could be from Na+ ions in the glassy phase, instead of the oxide ions.

研究领域: 材料科学 · 固体离子导体 · 无机非金属材料 · 能源材料 · 电化学
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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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IONICS · 2020 ·Vol. 26 ·期 9 ·4257-4265 · IF 2.394

Facile synthesis of a mixed-conductive Li2S composites for all-solid-state lithium-sulfur batteries

Jiang Huize,Han Yu,Wang Hui,Zhu Yuhao,Guo Qingpeng,Jiang Haolong,Zheng Chunman,Xie Kai

The poor interface between the active materials, solid electrolytes, and conductive additives in composite cathode materials is the key factor restricting the performance of the all-solid-state lithium-sulfur battery. Here, the composite cathode material was prepared through the method of one-step ball milling. The sulfide electrolyte Li 3 PS 4 (LPS) was formed on the surface of the active material Li 2 S while the conductive additives were incorporated, and the conductive ions and electronic network were constructed simultaneously. After adding an appropriate amount of carbon nanotubes (cnt), the composite cathode exhibited high specific capacity of 1145.2 mAh g −1 after 30 times of cycling at a current density of 0.2 mA cm −2 , and the battery with ultrahigh areal Li 2 S loading also displays high capacity of 962.6 mA g −1 . The composite cathode with high Li 2 S content (56.3%) was prepared, with excellent performance exhibited: the capacity is 741 mAh g −1 after 30 times of cycling at a current density of 0.2 mA cm −2 . Without additional sulfide electrolyte, the composite cathode materials were prepared by one-step ball milling with lithium sulfide, phosphorus pentasulfide, acetylene black, and carbon nanotubes as raw materials.

研究领域: 材料科学 · 电化学 · 能源存储 · 固态离子学 · 纳米复合材料
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Journal of Energy Chemistry · 2017 ·Vol. 27 ·期 2 ·413-418 · IF 2.594

DDQ as an effective p-type dopant for the hole-transport material X1 and its application in stable solid-state dye-sensitized solar cells

Yanyun Zhang,Xichuan Yang,Weihan Wang,Xiuna Wang,Licheng Sun

X1 (MeO-TPD) is an inexpensive and easily synthesized π -conjugated molecule that has been used as a hole-transport material (HTM) in solid-state dye-sensitized solar cells (ssDSSCs), achieving relatively high efficiency. In this paper, we characterize the physicochemical properties of 2,3-dichloro-5,6-dicyano-1,4-benzoquinone (DDQ) and show that it is a promising p-dopant in a spin-coating solution with X1 as the HTM. The doped ssDSSCs showed an increase in short-circuit current density from 5.38 mA cm –2 to 7.39 mA cm –2 , and their overall power conversion efficiency increased from 2.9% to 4.3%. Also, ssDSSCs with DDQ-doped X1 were more stable than the undoped samples, demonstrating that DDQ can act as a p-type dopant in X1 as an HTM for highly efficient, stable ssDSSCs.

研究领域: 材料科学 · 能源化学 · 光伏技术 · 纳米材料 · 半导体器件 · 表面化学 · 电化学
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ELECTROCHIMICA ACTA · 2015 · IF 4.504

Titanium Dioxide@Polyaniline Core-Shell Nanowires as High-Performance and Stable Electrodes for Flexible Solid-State Supercapacitors

Peng Zhang,Zhimeng Liu,Yuping Liu,Hongbo Fan,Yuanqi Jiao,Baiman Chen

In this work, we demonstrate a facile approach to synthesize high-performance and stable TiO 2 @PANI core-shell nanowires (NWs) as flexible electrodes for solid-state supercapacitors (SCs). The TiO 2 @PANI core-shell NWs are grown directly on highly conductive carbon cloth, which not only give efficient charge transport and accessible diffusion of the electrolyte, but also provide large surface area and active sites for redox reaction as well as good strain accommodation. Such these features enable them to deliver a large areal capacitance of 520.3   mF/cm 2 at 0.5   mA/cm 2 with outstanding rate capability. Furthermore, a flexible and stable solid-state SC device based on these TiO 2 @PANI core-shell NWs is also demonstrated. The as-fabricated solid-state SC device yields a remarkable volumetric capacitance of 898.4   mF/cm 3 , excellent flexibility and significant cycling stability with more than 97.2% retention of its capacitance after 10000 cycles. We believe that these findings may open up new opportunities to prepare high-performance PANI-based electrodes for flexible solid-state SCs.

研究领域: 材料科学 · 纳米科技 · 电化学 · 能源存储 · 功能材料 · 柔性电子学
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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
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Sustainable Energy & Fuels · 2019 ·Vol. 3 ·期 9 ·2237-2245 · IF 4.912

Nitrogen and fluorine co-doped holey graphene hydrogel as a binder-free electrode material for flexible solid-state supercapacitors

Yulin Chen,Yu Li,Fengnan Yao,Cong Peng,Chen Cao,Yiyu Feng,Wei Feng

Two-dimensional (2D) graphene-based materials are widely applied as electrodes for supercapacitors due to their vast surface area and excellent charge mobility. However, the pursuit of the theoretical capacitance of graphene has lasted besides the improvements of charge/discharge rate and cycling life. In this work, a nitrogen and fluorine co-doped holey graphene hydrogel (NF-HGH) was synthesized by using consecutive solvothermal treatments for creating vacancies on the graphene basal plane and introducing heteroatoms into the graphene framework. The NF-HGH as an electrode for supercapacitors exhibited a remarkable electrochemical performance of 345.4 F g−1 at 1 A g−1 in 6 M KOH electrolyte. In addition, the specific capacitance of the assembled all-solid-state flexible symmetric supercapacitor (SSC) was 67.3 F g−1 at 1 A g−1, with an outstanding long-term cycling stability over 10 000 cycles. The delivered maximum energy and power densities were 7.99 W h kg−1 and 10.08 kW kg−1, respectively. The abundant pyrrolic-N doped at the edge of etched vacancies and the formed semi-ionic C–F bonds around pyrrolic-N were critical for electrochemical developments, which provided a sensational method to construct carbonaceous frameworks for energy storage systems.

研究领域: 材料科学 · 电化学 · 纳米科技 · 能源存储 · 功能材料
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