CHEMISTRY-A EUROPEAN JOURNAL
·
2020
·Vol. 26
·期 45
·10314-10320
·
IF 4.857
Guiqiang Cao,Zhikang Wang,Da Bi,Jing Zheng,Qingxue Lai,Yanyu Liang
Graphical Atomic cat : A single-atom Fe@NG electrocatalyst serves as the coating of separators for high-performance Li-S batteries. Atomically dispersed Fe sites on the graphene framework promote the conversion efficiency of LiPS. The Fe@NG electrocatalyst delivers an initial capacity of 1616 mA h g −1 at 0.1 C, and a reversible capacity of 546 mA h g −1 after 200 cycles at 2 C (70 % capacity retention). Lithium-sulfur batteries have been considered as potential electrochemical energy-storage devices owing to their satisfactory theoretical energy density. Nonetheless, the inferior conversion efficiency of polysulfides in essence leads to fast capacity decay during the discharge/charge cycle. In this work, it is successfully demonstrated that the conversion efficiency of lithium polysulfides is remarkably enhanced by employing a well-distributed atomic-scale Fe-based catalyst immobilized on nitrogen-doped graphene (Fe@NG) as a coating of separator in lithium-sulfur batteries. The quantitative electrocatalytic efficiency of the conversion of lithium polysulfides is determined through cyclic voltammetry. It is also proven that the Fe-N X configuration with highly catalytic activity is quite beneficial for the conversion of lithium polysulfides. In addition, the adsorption and permeation experiments distinctly indicate that the strong anchoring effect, originated from the charge redistribution of N doping into the graphene matrix, inhibits the movement of lithium polysulfides. Thanks to these advantages, if the as-prepared Fe@NG catalyst is combined with polypropylene and applied as a separator (Fe@NG/PP) in Li-S batteries, a high initial capacity (1616 mA h g −1 at 0.1 C), excellent capacity retention (93 % at 0.2 C, 70 % at 2 C), and superb rate performance (820 mA h g −1 at 2 C) are achieved.
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高影响因子
ACS Nano
·
2023
·
IF 17.1
Shuxian Zhang,Jianchao Chen,Chunyan Zhu,Qingyuan Liu,Qingyu Li,Renbo Liu,Xiaobo Jiang,Yijie Yan,Shengjian Sun,Longwei Yin,Rutao Wang
All-solid-state batteries (ASSBs) with a Li metal anode are expected to be one of the most promising energy storage systems to achieve high energy density. However, the interfacial instability between the Li metal anode and solid-state electrolyte (SSE) limits the rate capability and cycling stability of ASSBs. The main issue is the formation of voids at the Li/SSE interface during Li stripping due to the slow diffusion of Li within the bulk Li metal, then increasing internal cell resistance and inducing the formation of lithium dendrites. To address these issues, a composite Li anode (LAO) composed by Li–Ag alloy and Li2O is constructed by mixing the stoichiometric metal Li and Ag2O directly. LAO anode is capable of improving bulk Li diffusion kinetics and inhibiting the formation of interfacial voids effectively, achieving a high critical current density over 1.5 mA cm–2 and long stable cycling over 1000 h at 1 mA cm–2. The ASSBs, employing LAO as the anode, Li6PS5Cl as the SSE, and LiCoO2 as the cathode, exhibit superior rate capability and stable cycling over 4000 cycles at 5 C. Moreover, ASSBs can operate stably with a high LiCoO2 loading of 17.8 mg cm–2 for more than 100 cycles at 0.2 C.
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JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2025
·Vol. 172
·期 1
·010529
·
IF 3.3
Kemeng Song,Yuan Yuan,Hanbing Chen,Ping Lu,Ning Li,Ningyi Yuan,Fanglei Zeng
This study presents a systematic investigation of three cyclic phosphazene-based flame retardant additives, hexachlorocyclotriphosphazene (HCCP), hexafluorocyclotriphosphazene (HFPN), and ethoxy-pentafluorocyclotriphosphazene (EtPFPN), for ether-based electrolytes in lithium-sulfur batteries. Through comprehensive analysis of molecular orbital calculations, self-extinguishing time measurements, and electrochemical characterization, we reveal distinct structure-dependent flame retardancy mechanisms and their impact on battery performance. HCCP demonstrates superior flame suppression through P-Cl bond decomposition but exhibits electrochemical instability above 15 wt%. HFPN functions primarily as a co-solvent, achieving significant flame retardancy above 20 wt% while maintaining stable electrochemical performance. EtPFPN emerges as the most promising candidate, effectively integrating into the electrolyte solvation structure to provide optimal flame retardancy, though requiring higher concentrations for complete suppression. Notably, synergistic effects between LiNO3 and the flame-retardant additives enhance both safety and electrochemical stability. These findings provide critical insights for the molecular design of flame-retardant electrolytes in high-performance Li-S batteries, demonstrating the importance of balancing safety enhancement with electrochemical stability through strategic additive selection and concentration optimization.
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JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
·
2025
·Vol. 36
·期 12
·1-13
·
IF 2.8
Guo Xueyi,Cai Haiyan,Mao Gaoqiang,Jiao Wen,Yu Wanjing,Meng Kui,Tong Hui,Xu Kaihua,Zhang Kun,Zhang Yuping
Developing battery materials with high specific energy and long cycle life is a crucial core technology that needs to be broken. High-nickel and high-voltage are the development trends of cathode materials, but the structural instability seriously deteriorate electrochemical performance. Herein, to solve the above problem and obtain structurally stable high-voltage nickel-rich cathode materials, a novel high-voltage spinel-structured cladding layer was designed by wet chemistry and coated on the surface of LiNi 0.83 Co 0.11 Mn 0.06 O 2 material. LiNi 0.5 Mn 1.5 O 4 with spinel structure possesses good structural compatibility with layered cathode materials and has efficient three-dimensional Li-ion diffusion paths, which can meet the needs of Li-ion diffusion kinetics. Meanwhile, LiNi 0.5 Mn 1.5 O 4 has a high operating voltage and a very stable thermodynamic structure in the charging state which can inhibit the corrosion and interfacial side reactions of the cathode material, thus stabilizing the crystal structure. The results show that 1 wt% LiNi 0.5 Mn 1.5 O 4 -coated sample displayed the best electrochemical performance, with a discharge capacity of 203.7 mAh g −1 at 1 C, the capacity retention of 77.71% after 200 cycles, and even after 300 cycles, the capacity retention still reached 64.36%.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Xiaoqian Dai,Huitian Liu,Xu Liu,Zhaolin Liu,Yuansheng Liu,Yuhao Cao,Junyan Tao,Zhongqiang Shan
The application of silicon as anode materials for lithium-ion batteries is limited by the huge volumetric expansion and complex synthesis processes. Herein, silicon nanoparticles encapsulated in multifunctional crosslinked nano-silica/carbon hybrid matrix (Si@n-SiO 2 /C) composites are successfully synthesized via simultaneous condensation copolymerization between (3-aminopropyl)-triethoxysilane (APTES) and L-ascorbic acid (L-AA). With the introduction of nano-silica, the multifunctional nano-silica/carbon hybrid matrix can significantly maintain structural integrity during the volume change of silicon, provide a higher capacity than the traditional single carbon coating layer and enhance the conductivity of the materials. Correspondingly, the obtained Si-2@n-SiO 2 /C composites display quite outstanding cycle stability and superior structural integrity maintenance, which delivers a capacity of 800.7 mAh g −1 after 300 cycles at the current density of 1 A g −1 . Such a novel coating layer structure design and simultaneous growth of nano-silica/carbon hybrid matrix layer on silicon nanoparticles will provide a simple synthesis strategy for manufacturing high-performance Si-based anode materials.
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APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Dongyuan Lei,Jinkui Li,Mingwu Xiang,Zirui Zhao,Shixun Yang,Zhe Hu,Mingwei Yuan,Junming Guo,Yi Xia,Wei Bai
Low sulfur content and inevitable polysulfide shuttle effect have always been the critical obstacle of the practical application of high-energy–density lithium sulfur batteries. Herein, a waste passiflora edulis peel derived in-situ N -doping porous carbon (PINPC) combined with three-dimensional hollow carbon cloth interlayer (3DHCI) was designed and constructed by facile simultaneous activation/carbonization. The abundant porous structure and nitrogen heteroatom doping of the PINPC not only significantly confine the soluble polysulfides through the physical and chemical adsorption, but also the high conductivity of the 3DHCI effectively accelerate the conversion reaction of polysulfides encapsulated in the unique hollow carbon skeletons. Owing to the synergetic enhancement of the PINPC and 3DHCI, the sulfur contents of the corresponding sulfur cathode composites are easily regulated from 70 wt% to 95 wt%, whilst exhibiting excellent electrochemical performances. The PINPC/S with a sulfur content of 70 wt% and 3DHCI interlayer obtains a high initial discharge capacity of 1032 mAh·g −1 and then retains 954 mAh·g −1 at 0.2 C after 200 cycles. At 2 C, a durable cycle life with capacity retention of 86% can be achieved up to 500 cycles. Even with an ultrahigh sulfur content of 95 wt%, the relatively high initial discharge capacity of 692 mAh·g −1 and capacity retention of 96 % are also achieved at 0.2 C after 200 cycles. This work offers a potential design for high-performance lithium sulfur batteries simultaneously with a high sulfur content.
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高影响因子
CERAMICS INTERNATIONAL
·
2018
·
IF 3.057
Wei Zheng,Peigen Zhang,Li Yang,Jian Chen,Wubian Tian,Yamei Zhang,ZhengMing Sun
We report herein a fast and scalable approach to the synthesis of MO/CNT/Fe (MCI) hybrid nanostructures via microwave irradiation of MXene under ambient condition. The effect of three arcing materials, CNT, graphite (C), and carbon fiber (C f ), on the growth of carbon nanotubes on MXene-derived metal oxides were investigated. The resulted MCI nanostructures were tested as anodes in LIBs , all exhibiting better electrochemical performance than that of pristine Ti 3 C 2 . Remarkably, MCI-C f delivered reversible capacities of 430 mA h g −1 and 175 mA h g −1 at 1 A g −1 and 10 A g −1 , respectively, which is much higher than that of commercial graphite at high rates. The findings in this work open new exciting opportunities to developing hybrid electrode materials with high specific capacity for energy conversion and storage.
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高影响因子
ACS Applied Energy Materials
·
2022
·
IF 6.959
Maoxia Yang,Baiqing Zhao,Jianying Li,Shaomin Li,Gen Zhang,Shiqi Liu,Yanhua Cui,Hao Liu
Solid polymer electrolytes (SPEs) are flexible, low cost, and easily scalable for battery manufacturing. These merits make SPEs one of the most practical solid-state electrolytes. Poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP), which has good mechanical properties and good thermal stability, is considered a promising polymer for SPEs. However, PVDF-HFP is unstable due to the dehydrofluorination side reaction when PVDF-HFP-based electrolytes cycle with Li metal. This reaction leads to the deterioration of the electrolyte–electrode interface. In this work, the PVDF-HFP polymer electrolyte is modified with LiOH during the synthesis of SPEs (pre-dehydrofluorination). The modified electrolyte delivers significantly enhanced stability toward the Li metal anode. The electrochemical stable window is extended from 4.75 to 5.00 V, and the stable cycle time of the galvanostatic test of Li symmetric cells at 0.1 mA cm–2 increases from about 100 h to over 500 h. Ex situ scanning electron microscopy (SEM) and X-ray photoelectron spectroscopy (XPS) analyses indicate that the polymer degradation is suppressed after modification, and a stable interface containing more LiF and inorganic sulfur compounds forms between the electrolyte and Li metal; the interface could effectively suppress Li dendrite growth. Combining electrochemical results with ex situ SEM and XPS analysis, it is observed that the pre-dehydrofluorination is the reason for inhibiting polymer degradation and suppressing Li dendrite growth toward the Li metal anode. These findings will promote the development of safe all-solid-state Li metal batteries.
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Nature Communications
·
2023
·Vol. 14
·期 1
·1-11
·
IF 16.6
Feng Yangyang,Li Yong,Lin Jing,Wu Huyue,Zhu Lei,Zhang Xiang,Zhang Linlin,Sun Chuan-Fu,Wu Maoxiang,Wang Yaobing
Stable lithium metal negative electrodes are desirable to produce high-energy batteries. However, when practical testing conditions are applied, lithium metal is unstable during battery cycling. Here, we propose poly(2-hydroxyethyl acrylate-co-sodium benzenesulfonate) (PHS) as negative electrode protective layer. The PHS contains soft poly (2-hydroxyethyl acrylate) and poly(sodium p-styrene sulfonate), which improve electrode flexibility, connection with the Cu current collector and transport of Li ions. Transmission electron cryomicroscopy measurements reveal that PHS induces the formation of a solid electrolyte interphase with a fluorinated rigid and crystalline internal structure. Furthermore, theoretical calculations suggest that the -SO 3 - group of poly(sodium p-styrene sulfonate) promotes Li-ion motion towards interchain migration through cation-dipole interaction, thus, enabling uniform Li-ion diffusion. Electrochemical measurements of Li | |PHS-coated-Cu coin cells demonstrate an average Coulombic efficiency of 99.46% at 1 mA/cm 2 , 6 mAh/cm 2 and 25 °C. Moreover, when the PHS-coated Li metal negative electrode is paired with a high-areal-capacity LiNi 0.83 Co 0.11 Mn 0.06 O 2 -based positive electrode in multi-layer pouch cell configuration, the battery delivers an initial capacity of 6.86 Ah (corresponding to a specific energy of 489.7 Wh/kg) and, a 91.1% discharge capacity retention after 150 cycles at 2.5 mA/cm 2 , 25 °C and 172 kPa.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Chao Wu,Shuang Cao,Heng Li,Zhi Li,Gairong Chen,Xiaowei Guo,Baobao Chang,Yansong Bai,Xianyou Wang
Herein, we put forward a feasible interfacial modification strategy in virtue of Mn 3 O 4 surface coating to construct protective shell and alleviate Jahn-Teller distortion during the charge/discharge process. It has been found that the increase of the oxygen vacancy on the surface of Li 1.2 Ni 0.27 Mn 0.54 O 2 of (LRNMO) after Mn 3 O 4 protective layer modification can effectively restrain the release of oxygen and enhancing rate capability, and thus improving its comprehensive electrochemical performances. In particular, the initial coulombic efficiency of the optimized LRNMO-1 electrode is improved from 72.3% to 84.3%. The capacity retention rate is up to 95.6% at 250 mA g −1 (1C) after 200 cycles. In addition, the LRNMO-1 electrode also has a good capacity retention rate (96.4% after 100 cycles) at a high current density of 5C. Moreover, the designed LRNMO@Mn 3 O 4 cathode exhibits higher ionic conductivity and better interface stability. As a result, this work offers a practicable and valuable exploration for the development and industrialization of Co-free Li-rich Mn-based cathode materials with high energy density .
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ELECTROCHIMICA ACTA
·
2021
·
IF 6.901
Ting Liu,Li Li,Tianhao Yao,Yanni Li,Lei Zhu,Fang Li,Xiaogang Han,Yonghong Cheng,Hongkang Wang
To explore advanced anode materials with superior Li + /Na + /K + storage performances for alkaline ion batteries (AIBs), a hybrid of amorphous vanadium oxide uniformly embedded into the highly defective carbon nanofibers (denoted as VO x @CNFs) was fabricated via a facile electrospinning method followed by proper heat treatment in this work. The integrated structure synergistically combines the advantages of the amorphous VO x and the defective carbon matrices, which can not only bring abundant active sites for ion storage and multi-channels for ion diffusion, but also well accommodate the structural change induced electrode pulverization . When evaluated as anode materials for AIBs, the optimized VO x @CNFs demonstrate excellent alkaline ion storage performances with high-specific capacities, long-cycling life and high-rate capabilities, delivering a Na + storage capacity of 260 mAh g −1 at 1.0 A g −1 after 1000 cycles, a Li + storage capacity of 556 mAh g −1 at 0.5 A g −1 after 500 cycles, and a K + storage capacity of 198 mAh g −1 at 0.5 A g −1 after 400 cycles.
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Journal of Energy Chemistry
·
2025
·
IF 14.9
Zichen Zhang,Jingyi Liu,Nan Chen,Tao Jiang,Shiyu Yao,Gang Chen,Deping Wang,Fei Du
Li-rich Mn-based oxides (LRMO) are of great significance in achieving high energy density all-solid-state lithium batteries (ASSLBs), owing to their high theoretical capacity and high operation voltage. Unfortunately, their practical application is hindered by severe interface degradation due to the chemical oxidation and electrochemical decomposition of solid electrolytes (SEs), driven by high-active oxygen and electron sources from LRMO. Herein, an interfacial modification strategy is proposed to stabilize the surface lattice oxygen of LRMO and reduce electronic conduction between LRMO and SEs, synergistically. Accordingly, the byproducts from chemical oxidation (InO − ) and electrochemical decomposition (LiCl − ) are largely suppressed, leading to superior interfacial transport with the lowest resistance. Consequently, the ASSLB achieves a high reversible capacity of 227.9 mA h g −1 at 0.1 C, a cycling stability of 90.1% capacity retention after 200 cycles at 0.1 C, and a superior rate capability with a capacity of 81.7 mA h g −1 at 3.0 C. This study enriches the fundamental understanding of LRMO/SEs interfacial evolution during the electrochemical cycling and the proposed interfacial modification strategy benefits the future design of Li-rich compounds for ASSLBs.
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