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ELECTROCHIMICA ACTA · 2015 · IF 4.504

Novel graphite-carbon encased tungsten carbide nanocomposites by solid-state reaction and their ORR electrocatalytic performance in alkaline medium

K. Huang,K. Bi,J.C. Xu,C. Liang,S. Lin,W.J. Wang,T.Z. Yang,Y.X. Du,R. Zhang,H.J. Yang,D.Y. Fan,Y.G. Wang,M. Lei

Novel nanocomposites of spherical graphite-carbon encased tungsten carbide (GC-WC) are synthesized by solid state reaction with melamine and WO 3 as precursors under N 2 atmosphere. The diameters of the GC-WC composites range from 50 to 200   nm and the WC nanoparticles inside with an average size of ca. 15   nm distribute uniformly. The characterization results indicate that the GC-WC is composed of few layers of graphite carbon and WC nanoparticles with high crystallization and purity. Moreover, the electrocatalytic performance of GC-WC for the oxygen reduction reaction (ORR) in alkaline medium is further investigated by cyclic voltammetry (CV), rotating disk electrode (RDE) and chronoamperometry test with or without 3   M methanol. The results show that GC-WC has a considerable performance for ORR in the view of activity, stability and methanol tolerance, which may further used as proper supports for noble-metal based ORR catalysts in alkaline fuel cell . The synergetic interaction between the carbide nanoparticles and graphite carbon, which means that the surface graphite carbon layers are activated by WC nanoparticles for ORR and in turn protect inner WC from highly oxidizing environments has also been verified.

研究领域: 材料科学 · 纳米科技 · 电化学 · 能源材料 · 催化化学
✓ 已验证 DOI 高影响因子
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SOLID STATE IONICS · 2018 · IF 2.751

Cathode/electrolyte interface engineering via wet coating and hot pressing for all-solid-state lithium battery

Wenping Zha,Yinghui Xu,Fei Chen,Qiang Shen,Lianmeng Zhang

In this work, Li 7 La 3 Zr 2 O 12 (LLZO)-based membrane electrolyte, which has good flexibility and can be easily mass-produced, is proposed to address the intrinsic defects of ceramic electrolytes . The LLZO-based membrane electrolyte is electrochemically stable in the voltage range of 0–5.2 V vs. Li/Li + due to the good oxidative stability of LLZO. We also develop a simple and low-cost approach to fabricate the all-solid-state lithium battery (ASSLB). Wet coating and hot pressing are applied to form a continuous and homogeneous electrolyte layer on a cathode layer. Thanks to the integrated preparation process, there is no obvious interface between the cathode layer and the electrolyte layer, hence reducing the interface resistance. The Li/LiFePO 4 batteries exhibit desirable cycling performance at 60 °C, which deliver a maximum discharge specific capacity of 151.6 mAh·g −1 at 0.1C and maintain 97.8% of the capacity after 50 cycles.

研究领域: 材料科学 · 电化学 · 能源存储 · 固态离子学 · 先进电池技术
✓ 已验证 DOI 高影响因子
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Journal of Materials Chemistry A · 2018 ·Vol. 6 ·期 39 ·19231-19240 · IF 9.931

Ultrafast solid-state lithium ion conductor through alloying induced lattice softening of Li6PS5Cl

Minjie Xuan,Weidong Xiao,Hongjie Xu,Yonglong Shen,Zhenzhen Li,Shijie Zhang,Zhuo Wang,Guosheng Shao

The development of a solid electrolyte with superb Li+ conductivity is the key to enabling safe and high-performance all-solid lithium ion batteries which are free of the safety issues associated with flammable organic liquid electrolyte. Systematic experimental work has been carried out as a follow up to our recent theoretical prediction that superb ionic conductivity could be achieved through the tuning of the lattice chemistry in the cubic argyrodite Li6PS5Cl. Remarkable enhancement of the ionic conductivity has been achieved through the combined effect of excess Li and substitution of S with Te. This leads to an alloy, Li6.25PTe0.125S5.125Cl0.75, having the superb Li+ conductivity of 4.5 mS cm−1 at 25 °C, together with a low activation energy of 0.16 eV to safeguard adequate ionic conductivity at low temperature. This current work conclusively affirms the theoretical outcome that the superb ionic conductivity is attributed to weakened bonding, an enlarged unit cell, and a softened lattice, making it easier for the long-distance diffusion of Li+. In addition, this new class of solid electrolyte based on cubic chalcogenide is electrochemically compatible with the Li anode over a large potential window up to 7 V, which is highly desirable for high performance solid lithium ion batteries.

研究领域: 材料科学 · 电化学 · 能源存储 · 固体离子学 · 无机化学
✓ 已验证 DOI 高影响因子
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Nano Energy · 2016 · IF 11.553

Flexible and ion-conducting membrane electrolytes for solid-state lithium batteries: Dispersion of garnet nanoparticles in insulating polyethylene oxide

Jingxian Zhang,Ning Zhao,Miao Zhang,Yiqiu Li,Paul K. Chu,Xiangxin Guo,Zengfeng Di,Xi Wang,Hong Li

Solid-state electrolytes with high ionic conductivity , large electrochemical window, good mechanical properties , and easy processability are needed for high-energy solid-state lithium batteries . In this work, composite membranes consisting of lithium garnet (i.e. Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 , LLZTO) particles and Li-salt-free polyethylene oxides (PEOs) are produced as solid-state electrolytes. Li-ion-conducting particles in nano-scale are crucial for the enhancement of conductivity and the membranes containing ~40   nm LLZTO particles exhibit conductivities nearly two orders of magnitude larger than those with the micro-scale ones, which is attributed to the difference in specific surface area related to the percolation effect. Compared to the conventional PEO doped with lithium salt, the insulating PEO in PEO:LLZTO membrane electrolyte is conducive to the suppression of lithium dendrite growth owing to prohibition of current flow. With PEO:LLZTO membrane electrolytes in conductivity of 2.1×10 −4   S   cm −1 at 30   °C and 5.6×10 −4   S   cm −1 at 60   °C, the solid-state LiFePO 4 /PEO:LLZTO/Li and LiFe 0.15 Mn 0.85 PO 4 /PEO:LLZTO/Li cells deliver energy densities of 345   Wh   kg −1 (662   Wh   L −1 ) and 405   Wh   kg −1 (700   Wh   L −1 ) (without the package weight or volume) with good rate capability and cycling performance. This study suggests that the conjunction of nano-scale Li-ion-conducting particles and an insulating polymer provides a promising solution to produce powerful solid-state electrolytes for high-performance solid-state lithium batteries .

研究领域: 材料科学 · 电化学 · 能源存储 · 高分子科学 · 固态电池技术
✓ 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 POWER SOURCES · 2016 · IF 6.333

One-pot preparation of new copolymer electrolytes with tunable network structure for all-solid-state lithium battery

Bo Chen,Qiang Xu,Zhen Huang,Yanran Zhao,Shaojie Chen,Xiaoxiong Xu

A new class of copolymer electrolytes with tunable network structure is successfully designed and prepared via a facile one-pot reaction. The trimethylolpropane triglycidyl ether (TMPEG) is cross-linked with poly (ethylene glycol) diamine (NPEG) to create well-defined solid network polymer electrolyte (SNPE). The network structure could be tuned by changing the molar ratio of TMPEG and NPEG or the molecular weight of NPEG. The effects of molecular weight of NPEG and molar ratio of EO/Li + on the ionic conductivity are systematically investigated. The optimal electrolyte TMPEG-NPEG4K[2:1]-16:1 presents a maximum conductivity of 1.10 × 10 −4  S cm −1 under 30 °C, and an 18-fold ionic conductivity enhancement in that of PEO-based electrolyte. Furthermore, it also exhibits wide electrochemical window (0–5.4 V), excellent compatibility with metallic Li, and superior mechanical properties. The all-solid-state lithium batteries LiFePO 4 /Li are assembled with TMPEG-NPEG4K[2:1]-16:1 electrolyte, and present good cycling and rate performance under 60 °C. The initial discharge specific capacities of the batteries are 161.7 mAh g −1 at 0.2 C and 132.7 mAh g −1 at 1 C, and the capacity retention ratio can be retained at 90.6% and 90.5% after 100 cycles. This new copolymer electrolyte may become a promising candidate for applications in all-solid-state lithium battery.

研究领域: 材料科学 · 高分子化学 · 电化学 · 能源存储 · 固态离子学 · 锂离子电池
✓ 已验证 DOI 高影响因子
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JOURNAL OF POWER SOURCES · 2018 · IF 6.945

High ion conductive Sb2O5-doped β-Li3PS4 with excellent stability against Li for all-solid-state lithium batteries

Dongjiu Xie,Shaojie Chen,Zhihua Zhang,Jie Ren,Lili Yao,Linbin Wu,Xiayin Yao,Xiaoxiong Xu

The combination of high conductivity and good stability against Li is not easy to achieve for solid electrolytes , hindering the development of high energy solid-state batteries . In this study, doped electrolytes of Li 3 P 1- x Sb x S 4-2.5 x O 2.5 x are successfully prepared via the high energy ball milling and subsequent heat treatment . Plenty of techniques like XRD , Raman, SEM, EDS and TEM are utilized to characterize the crystal structures, particle sizes, and morphologies of the glass-ceramic electrolytes. Among them, the Li 3 P 0.98 Sb 0.02 S 3.95 O 0.05 ( x  = 0.02) exhibits the highest ionic conductivity (∼1.08 mS cm −1 ) at room temperature with an excellent stability against lithium. In addition, all-solid-state lithium batteries are assembled with LiCoO 2 as cathode, Li 10 GeP 2 S 12 /Li 3 P 0.98 Sb 0.02 S 3.95 O 0.05 as the bi-layer electrolyte, and lithium as anode. The constructed solid-state batteries delivers a high initial discharge capacity of 133 mAh g −1 at 0.1C in the range of 3.0–4.3 V vs. Li/Li + at room temperature, and shows a capacity retention of 78.6% after 50 cycles. Most importantly, the all-solid-state lithium batteries with the Li 10 GeP 2 S 12 /Li 3 P 0.98 Sb 0.02 S 3.95 O 0.05 electrolyte can be workable even at −10 °C. This study provides a promising electrolyte with the improved conductivity and stability against Li for the application of all-solid-state lithium batteries.

研究领域: 材料科学 · 电化学 · 固态电池 · 能源存储 · 无机非金属材料
✓ 已验证 DOI 高影响因子
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JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS · 2019 ·Vol. 31 ·期 1 ·542-547 · IF 2.195

Study on preparation of LSTP thin film electrolyte by RF magnetron sputtering and electrical properties

Zhang Xiuyun,Zhao Yunyun,Ling Qia,Zhu Guisheng,Zhou Xiujuan,Deng Jianqiu,Yan Dongliang,Liu Laijun,Xu Huarui,Yu Aibing

Amorphous Li–Si–Ti–P–O (LSTP) thin film electrolyte was successfully prepared by radio frequency magnetron sputtering using Li 1.4 Si 0.4 Ti 1.6 (PO 4 ) 3 powder targets and stainless steel sheet as substrate. The effects of sputtering power on the structure, morphology, ionic conductivity, and electronic conductivity of the LSTP thin film electrolyte were investigated. The results showed that the LSTP thin film electrolyte obtained with sputtering power kept at 160 W, displayed uniform particles compacted in arrangement, proper stoichiometric ratio to the powder target as well as sufficient Li-ion for diffusion. Hence, it held a considerable ionic conductivity of 4.12 × 10 −6 S cm −1 and a high σ ion / σ ele ratio about 8 magnitudes, indicating that it can be used as film electrolyte in all-solid-state lithium batteries.

研究领域: 材料科学 · 电化学 · 固态离子学 · 薄膜技术 · 能源材料
✓ 已验证 DOI 高影响因子
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Energy Technology · 2020 ·Vol. 8 ·期 10 ·2000606 · IF 3.404

Low-Cost Raw Materials Synthesized Na2.9375PS3.9375Cl0.0625 Solid Electrolyte

Yu Wang,Nachuan Yang,Yi Shuai,Kanghua Chen

Na 3 PS 4 -based materials, which have relatively high conductivities, make promising Na-ion solid electrolytes for realizing all-solid-state sodium batteries. Herein, Na 2.9375 PS 3.9375 Cl 0.0625 solid electrolytes’ power is prepared by a mechanical ball milling process and subsequent heat treatment process using low-cost Na, NaCl, P 2 S 5 , and S as raw materials. In addition, its electrical conductivity and electrochemical performance by compounding with polyethylene oxide–NaClO 4 are studied. The results show that Na 2.9375 PS 3.9375 Cl 0.0625 solid electrolyte heated at 550 °C with polyethylene oxide–NaClO 4 exhibits Na-ion conductivity of 8.75 × 10 −4 S cm −1 . The pragmatic and cost-effective raw materials grant the solid electrolyte with high-performance and higher practical value.

研究领域: 材料科学 · 电化学 · 能源存储 · 固体离子学 · 无机非金属材料
✓ 已验证 DOI 高影响因子
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Sustainable Energy & Fuels · 2021 ·Vol. 5 ·期 5 ·1538-1547 · IF 6.367

A facile preparation of PEO–LiClO4–fumed SiO2 composite solid-state electrolyte with improved electrochemical performance for lithium-metal batteries

Ruyan Lei,Yanping Yang,Chenjuan Yu,Yinsi Xu,Yuanzhuo Li,Jun Li

In order to improve the electrochemical performance and efficiently prepare a solid polymer electrolyte (SPE) for the lithium-metal battery (LMB), a fumed SiO2 (FS) with surface Si–OH group was used to fabricate FS-modified poly(ethylene oxide) (PEO)–LiClO4-based SPE by a facile preparation process. The influences of the FS content on the morphological properties, thermal properties, lithium salt dissociation, mechanical properties, and electrochemical properties of SPE were systematically analyzed. Results indicate that FS with the hydrophilic property was widely distributed throughout the amorphous phase of SPE, thus the crystallinity of SPE was reduced to 25.83% when the FS mass loading was 6.85 wt%. In addition, a greater dissociation degree of lithium salt was achieved after the addition of FS, and a higher ion conductivity of 3.03 × 10−4 S cm−1 and Li-ion migration number of 0.396 were recorded at 60 °C. The all-solid-state Li/SPE/Li coin cell showed excellent stable cyclability (380 h) and the LiFePO4 (LFP)/SPE/Li coin cell demonstrated good discharge specific capacity and coulomb efficiency of 96 mA h g−1 and 100.2%, respectively, after 100 cycles of galvanostatic charge–discharge operation under 0.5C at 60 °C. Thus, based on collective results, it is expected that SPE presented in this work is a promising electrolyte for next-generation high-energy all-solid-state LMB with enhanced safety.

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
✓ 已验证 DOI 高影响因子
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Energy & Environmental Materials · 2022 ·Vol. 6 ·期 3 ·e12351 · IF 13.443

Molecular Reactivity and Interface Stability Modification in In-Situ Gel Electrolyte for High Performance Quasi-Solid-State Lithium Metal Batteries

Qiyu Wang,Xiangqun Xu,Bo Hong,Maohui Bai,Jie Li,Zhian Zhang,Yanqing Lai

Quasi-solid-state lithium metal battery is a promising candidate for next generation high energy density and high safety power supply. Despite intensive efforts on electrolytes, uncontrolled interfacial reactions on lithium with electrolyte and patchy interfacial contacts still hinder its practical process. Herein, we bring in rationally designed F contained groups into polymer skeleton via in-situ gelation for the first time to establish quasi-solid-state battery. This method achieves a capacity retention of 90% after 1000 cycles at 0.5C with LiFePO 4 cathodes. The interface constructed by polymer skeleton and reaction with –CF 3 lead to the predicted solid electrolyte interface species with high stability. Furthermore, we optimize molecular reactivity and interface stability with regulating F contained end groups in the polymer. Comparisons on different structures reveal that high performance solid stable lithium metal batteries rely on chemical modification as well as stable polymer skeleton, which is more critical to construct robust and steady SEI with uniform lithium deposition. New approach with functional groups regulation proposes a more stable cycling process with a capacity retention of 94.2% at 0.5C and 87.6% at 1C after 1000 cycles with LiFePO 4 cathodes, providing new insights for the practical development of quasi-solid-state lithium metal battery.

研究领域: 电化学 · 材料科学 · 能源存储 · 界面化学 · 高分子化学
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PARTICLE & PARTICLE SYSTEMS CHARACTERIZATION · 2020 ·Vol. 37 ·期 8 ·2000164 · IF 3.099

Sub-10 nm V2O5 Crystals on Carbon Nanosheets for Advanced All-Solid-State Lithium Metal Batteries

Liwei Su,Linhui Liu,Jinpei Hei,Huan Chen,Lianbang Wang,Yuanhao Wang,Manman Ren

V 2 O 5 , as a lithium-free cathode material, has inherent defects such as sluggish kinetics and volume change and, at the same time, requires a lithium metal anode that tends to form dendrites in liquid electrolytes. Both the lithium dendrite and the flammable electrolyte solvent bring longtime safety issues. This work introduces nonflammable inorganic–organic composite solid electrolyte to inhibit the growth of the lithium dendrite and suppress the instability caused by V 2 O 5 nanometerization. However, the long-term cycling and rate performances are still insufficient even when reducing V 2 O 5 size to about 50 nm. As an improvement, sub-10 nm V 2 O 5 /C nanosheets are designed and prepared using corn stalks as precursors through simple impregnation and calcination process. The V 2 O 5 /C offers a much better electrode/electrolyte contact and interface stability than bulk V 2 O 5 and commercial V 2 O 5 in the inorganic–organic composite solid electrolyte. The discharge capacity is 228 mAh g −1 at 0.1 C after 50 cycles and ≈110 mAh g −1 at 2.0 C.

研究领域: 材料科学 · 电化学 · 纳米能源 · 固态电池 · 电极材料设计
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