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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
✓ 已验证 DOI 高影响因子
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Progress in Natural Science-Materials International · 2019 ·Vol. 29 ·期 3 ·310-315 · IF 3.31

Anode material with Li-Si nano-domains in three-dimensional carbon network

Chao Hou,Ke Yang,Fawei Tang,Haibin Wang,Xuemei Liu,Xiaoyan Song

A micro-nano combined composite with Li-Si alloy nano-domains in three-dimensional carbon network was prepared as a novel electrode material. The carbon network constrained the volume contraction and promoted effectively charge transfer of the whole active material. Meanwhile, the abundant interfaces between Li-Si alloy and carbon bound by Li-C ionic bonds, not only enhanced the delithiation at interface but also ensured the structural integrity. The present composite exhibited excellent electrochemical performance. The specific capacity at the first lithiation was as high as 1133 mAh g −1 at a current density of 0.1 A g −1 , which is superior to those reported for the core-shell structured nanoparticles. The Coulombic Efficiency at the first cycle was 90.4% and kept stable at more than 99.0% after only 10 cycles. The capacity retention was nearly twice as that of the incompact mixture of Li-Si nanoparticles and carbon. The energy density of the full cell constructed by the present composite and sulfur was evaluated to be 3 times as high as that of the commercial lithium-ion batteries. This work provides a new universal strategy for developing Li-rich anode materials with high combination properties and low cost.

研究领域: 材料科学 · 电化学 · 纳米科技 · 能源存储 · 固态物理
✓ 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
✓ 已验证 DOI 高影响因子
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EcoMat · 2021 ·Vol. 3 ·期 5 ·e12134 · IF 0

Toward improved stability of nonfullerene organic solar cells: Impact of interlayer and built-in potential

Weixia Lan,Jialu Gu,Shiwei Wu,Yan Peng,Min Zhao,Yingjie Liao,Tao Xu,Bin Wei,Liming Ding,Furong Zhu

Improved efficiency and stability of the organic solar cells (OSCs) are the critical considerations for practical applications. The interface between the interlayer and bulk heterojunction has recently been shown as one of the weak links associated with the degradation in the nonfullerene acceptor (NFA)-based OSCs. It shows that the removal of the interfacial chemical reactions between the 2-(3-oxo-2,3-dihydroinden-1-ylidene)malononitrile (INCN) moieties in NFA and poly(3,4-ethylenedioxythiophene)-polystyrene sulfonate (PEDOT:PSS) hole extraction layer (HEL) is desired for enhancing the device stability. In this work, we show that the use of a bilayer MoO 3 /antimonene HEL favors the operational stability in OSCs through maintaining a high built-in potential and suppression of an undesired interfacial reaction between INCN moieties in NFA and the PEDOT structures in PEDOT:PSS. A power conversion efficiency of 16.68% is also obtained for the OSCs with a bilayer MoO 3 /antimonene HEL, prepared using a blend system of PM6:Y6, demonstrating its suitability for high-performance OSCs.

研究领域: 材料科学 · 光伏技术 · 纳米材料 · 表面化学 · 器件物理
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Journal of Materiomics · 2022 ·Vol. 9 ·期 3 ·568-576 · IF 8.589

Synergistically enabling the interface stability of lithium metal batteries with soft ionic gel and garnet-type Li6.4La3Zr1.4Ta0.6O12 ceramic filler

Qiujun Wang,Weiqi Zhu,Ya Su,Di Zhang,Zhaojin Li,Huan Wang,Huilan Sun,Bo Wang,Dan Zhou,Li-Zhen Fan

Lithium metal batteries based on solid electrolytes are considered as promising candidates with high energy density and safety. However, the weak solid-solid contact between electrolyte and electrode can easily lead to interface instability and lithium ions discontinuous migration, which seriously reduces the electrochemical performance of the battery. Herein, we construct a soft gel interfacial layer to improve the stability of the solid-solid interface between electrolyte and electrode by means of polyester-based monomers and imidazole-based ionic liquids. Based on this, garnet-type Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 (LLZTO) particles as inorganic ceramic filler were introduced in the layer to obtain composite electrolytes with high ionic conductivity (up to 1.1 × 10 −3  S/cm at 25 °C). As a result, the assembled lithium symmetric battery of Li|THCE-15%LLZTO|Li suggests excellent cycling stability with 700 h at 0.1 mA/cm 2 at 50 °C, and the lithium metal batteries of LFP|THCE-15%LLZTO|Li delivers high initial discharge capacity of 128.2 mA ·h/g with capacity retain of 75.48% after 150 cycles at 2 C. This work paves a new route to build safe and stable lithium metal batteries with synergistic introduction of composite electrolytes between electrolyte and electrode using soft gel interfacial layer and inorganic filler.

研究领域: 电化学 · 材料科学 · 能源存储 · 固体离子学 · 界面工程
✓ 已验证 DOI 高影响因子
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JOURNAL OF POWER SOURCES · 2022 · IF 9.794

Improving interfacial stability by in situ protective layer formation in 4.2V poly(ethylene oxide) based solid state lithium batteries

Wei Feng,Huirong Liu,Mingliang Zhao,Jianling Li,Feiyu Kang

The poly(ethylene oxide) based composite solid electrolyte(PEO-CSE) is an effective solution for developing high-performance solid-state lithium battery . However, the poly(ethlene oxide)(PEO) based solid-state lithium battery using 4.0 V cathode suffers from severe interfacial instability problems. In this work, we add additive lithium difluorophosphate(LiPO 2 F 2 ) into the PEO-CSE to form a stable and low resistance interphase at the cathode/electrolyte interface during charge/discharge process. The electrochemical stability window of PEO-CSE increases to ∼5.0 V. Besides, the electrochemical performance of PEO based solid-state lithium battery with LiCoO 2 as cathode is excellent. The discharge capacity of LiCoO 2 /Li cell with LiPO 2 F 2 reaches 108.5 mAh g −1 at 1.0C. In contrast, the discharge capacity that without LiPO 2 F 2 is only 60.0 mAh g −1 . Meanwhile, the PEO-CSE with LiPO 2 F 2 cell delivers stable cycle performance at 4.2 V. The capacity retention maintains 88.5% compared with 16.1%(without LiPO 2 F 2 ) after 100 cycles. Furthermore, it's still maintains 83.3% after 150 cycles. In addition, the cathode/electrolyte interface is analyzed by transmission electron microscope(TEM) and X-ray photoelectron spectroscopy(XPS). Galvanostatic intermittent titration test(GITT) is used to analyze the dynamic diffusion performance. This strategy provides a simple and effective way to improve the high voltage stability of the cathode/electrolyte interface.

研究领域: 电化学 · 材料科学 · 能源存储 · 固态电池 · 界面工程
✓ 已验证 DOI 高影响因子
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RSC Advances · 2016 ·Vol. 6 ·期 21 ·17029-17035 · IF 3.289

PbSe quantum dot films with enhanced electron mobility employed in hybrid polymer/nanocrystal solar cells

Xiaoyu Zhang,Yu Zhang,Hua Wu,Long Yan,Zhenguang Wang,Jun Zhao,William W. Yu,Andrey L. Rogach

We explore two strategies to improve the performance of hybrid solar cells fabricated using poly(3-hexylthiophene) (P3HT) and colloidal PbSe nanocrystals, which have reached a 1 sun power conversion efficiency of 2.9%. Using an atomic passivation strategy towards inorganic ligand-capped nanocrystals, the electron mobilities of PbSe quantum dot films are improved from 1.95 × 10−6 cm2 V−1 s−1 to 1.15 × 10−5 cm2 V−1 s−1. Employing ultrasmall PbSe nanocrystals allows us to adjust their bandgaps towards the type II heterojunction with P3HT, thus achieving efficient charge separation and transfer between the polymer/inorganic constituents. The device performance dropped to half after 10 days' storage, and the P3HT/PbSe interface was found to play a primary role in this efficiency degradation.

研究领域: 材料科学 · 纳米科技 · 光伏技术 · 半导体物理 · 表面与界面化学
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