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Journal of Energy Chemistry · 2023 · IF 13.1

LiCoO2 sintering aid towards cathode-interface-enhanced garnet electrolytes

Xiaoye Liu,Xiangkun Kong,Wenyi Xiang,Yining Jiang,Bingqinq Xiong,Weiwei Ping,Changrong Xia,Daoming Huan,Chengwei Wang

Garnet-type Li 7 La 3 Zr 2 O 12 (LLZO) has high ionic conductivity and good compatibility with lithium metal. High-temperature processing has been proven an effective method to decrease the interface resistance of cathode|LLZO. However, its application is still hindered by the interlayer co-diffusion with the cathode and high sintering temperature (>1200 °C). In this work, a new garnet-type composite solid-state electrolyte (SSE) Li 6.54 La 2.96 Ba 0.04 Zr 1.5 Nb 0.5 O 12 -LiCoO 2 (LLBZNO-LCO) is firstly proposed to improve the chemical stability and electrochemical properties of garnet with high-temperature processing. Small doses of LCO (3%) can significantly decrease the LCO|SSE interface resistance from 121.2 to 10.1 Ω cm 2 , while the sintering temperature of garnet-type LLBZNO decreases from 1230 to 1000 °C. The all-solid-state battery based on the sintered LLBZNO-LCO SSE exhibits excellent cycling stability. Our approach achieves an enhanced LCO|SSE interface and an improved sintering activity of garnet SSE, which provides a new strategy for optimizing the comprehensive performance of garnet SSE.

CAS / MDL: 7790-69-4
研究领域: 材料科学 · 电化学
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ACS Applied Energy Materials · 2023 · IF 6.4

Rationally Designing Cathode Interphase Chemistry via Electrolyte Additives for High-Voltage Batteries

Juan Guo,Jianhui Li,Ziqiang Fan,Jingwei Qiu,Haiping Ye,Junfeng Liang,Jiaying Liang,Ronghua Zeng,Yuepeng Cai

Cathode interphase plays an important role in suppressing parasitic electrode reactions for high-voltage batteries, which highly depends on interphase chemistry. In this work, we report a rational design of cathode interphase chemistry by applying an electrolyte additive, tri-tert-butyl borate (TTBB). As demonstrated in a nickel-rich layered oxide (LiNi0.5Co0.2Mn0.3O2, NCM523)/Li/graphite pouch cell in standard electrolyte (STD, 1 M LiPF6 in the solvents of ethylene carbonate (EC)/ethyl methyl carbonate (EMC) = 3/7 (weight ratio)) without and with TTBBunder 4.5 V, the capacity retention of the cell after 550 cycles under 1C at 25 °C is enhanced from 33.5 to 87.4% and its capacity at 5C is improved from 430.3 mAh to 483.7 mAh by the introduction of TTBB. TTBB shows good performance even under harsh environments such as high temperature (45 °C), the presence of HF, and low temperature (−20 °C). Thanks to the preferential oxidation of TTBB compared with carbonate electrolyte, a thin and well-defined cathode interphase is constructed with an inner layer mainly composed of B–F species (C8H18BO2F) and an outer layer mainly composed of B–O species (C11H21BO6), which is the result of the lower binding energy of B–F species with active oxygen on the NCM523 surface (−50.2 kJ mol–1) than that of B–O species (−30.7 kJ mol–1). Additionally, these species possess high electronic insulation and excellent Li+-ion-transfer property, resulting in chemical stability and low impedance of the cathode interphase. This work emphasizes the significance of cathode interphase chemistry and provides a practical strategy for the performance improvement of various high-voltage batteries.

CAS / MDL: 114435-02-8
研究领域: 材料科学 · 电化学
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ENERGY & FUELS · 2020 · IF 3.421

Carbon-Intercalated Montmorillonite as Efficient Polysulfide Mediator for Enhancing the Performance of Lithium–Sulfur Batteries

Mao Yang,Zhenghan Li,Wei Chen,Yin Hu,Yichao Yan

The traditional separator plays a significant role in rechargeable lithium-ion batteries due to the customized features that allow ions to transfer freely with low energy barriers. However, in the lithium–sulfur battery, the commercial separator shows feeble ability for promoting the conversion of accumulated long-chain polysulfides to the short-chain polysulfides on the surface of the cathode. In this work, a carbon-intercalated montmorillonite is designed to release the imprisoned capacity of the sulfur cathode by activating the accumulated long-chain polysulfides on the surface of the cathode. Benefiting from the advantages of carbon-intercalated montmorillonite, the lithium–sulfur battery achieves a high discharge capacity of 818 mAh g–1 over 300 cycles at a current density of 1 mA cm–2 with a sulfur loading of 2.6 mg cm–2. The systematic analyses by cyclic voltammetry and AC impedance reveal that the regulation of redox environment on the cathode surface by reducing the accumulated long-chain polysulfides to short-chain sulfides is a scalable solution for constructing the actual lithium–sulfur batteries.

研究领域: 材料科学 · 电化学 · 能源存储 · 纳米复合材料 · 电池技术
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Energy & Environmental Materials · 2022 ·Vol. 6 ·期 6 ·e12477 · IF 13.443

Seamless Stitching of Redox Windows to Enable High-Voltage Resilient Solid Sodium Ion Batteries

Xiangdan Zhang,Yuanyuan Huang,Xiaoyi Hu,Ruxin Guo,Yongshang Zhang,Zhiheng Wu,Guoqin Cao,Yuran Yu,Zhuo Wang,Yonglong Shen,Guosheng Shao

While sulfide solid electrolytes such as Na 11 Sn 2 PS 12 can allow fast transport of Na + ions, their utilization in solid sodium ion batteries is rather unsuccessful since they are not electrochemically compatible to both high-voltage cathodes and sodium metal anode. In this work, we devise an effective approach toward realizing solid sodium ion batteries, using the Na 11 Sn 2 PS 12 electrolyte and slurry-coated NASICON-type Na 3 MnTi(PO 4 ) 3 @C as high-voltage cathode, highly beneficial for low processing cost and high content/loading of active cathode matter. We report that through significantly improved integrity of electrolyte-cathode interface, such solid sodium ion batteries can deliver outstanding cycling and rate performance, with a charge voltage resilience up to 4.1 V, a high cathode discharge capacity of 128.7 mAh g −1 against the Na 3 MnTi(PO 4 ) 3 @C in cathode is achieved at 0.05 C, and capacity retention ratio of 82% with a rate of 0.1 C is realized after prolonged cycling at room temperature. Besides, we demonstrate that such a solid sodium ion battery can even perform at a sub-zero Celsius temperature of −10°C, when the conventional control cell using liquid electrolyte completely fail to function. This work is to offer a dependable avenue in engineering next generation of safe solid ion batteries based on highly sustainable and much cheaper material resources.

研究领域: 材料科学 · 电化学 · 电池技术 · 能源存储
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Nano-Micro Letters · 2024 ·Vol. 16 ·期 1 ·1-18 · IF 31.6

Highly Efficient Aligned Ion-Conducting Network and Interface Chemistries for Depolarized All-Solid-State Lithium Metal Batteries

Mu Yongbiao,Yu Shixiang,Chen Yuzhu,Chu Youqi,Wu Buke,Zhang Qing,Guo Binbin,Zou Lingfeng,Zhang Ruijie,Yu Fenghua,Han Meisheng,Lin Meng,Yang Jinglei,Bai Jiaming,Zeng Lin

This study introduces an innovative 3D-printed electrolyte with vertically aligned ion transport network, which contains well-dispersed nanoscale Ta-doped Li 7 La 3 Zr 2 O 12 in a poly(ethylene glycol) diacrylate matrix. The 3DSE architecture enables efficient ion transport across the Li/electrolyte and electrolyte/cathode interfaces, which allows for increased active material mass loading and enhanced interfacial adhesion. The p-3DSE Li symmetric cell displays an impressive critical current density value of 1.92 mA cm −2 and stable operation for 2600 h at room temperature. Full cells using p-3DSE achieve notable areal capacities.

研究领域: 材料科学 · 电化学 · 电池技术 · 固态电解质
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