Frontiers in Chemistry
·
2019
·
IF 3.782
Yu Juan,Gao Na,Peng Jiaxin,Ma Nani,Liu Xiaoyan,Shen Chao,Xie Keyu,Fang Zhao
Nowadays, lithium (Li) metal batteries arouse widespread concerns due to its ultrahigh specific capacity (3,860 mAh g−1). However, the growth of Li dendrites has always limited their industrial development. In this paper, the use of concentrated electrolyte with lithium difluoro(oxalate)borate (LiODFB) salt in 1, 2-dimethoxyethane (DME) enables the good cycling of a Li metal anode at high Coulombic efficiency (up to 98.1%) without dendrite growth. Furthermore, a Li/Li cell can be cycled at 1 mA cm−2 for over 3,000 h. Besides, compared to conventional LiPF6-carbonate electrolyte, Li/LiFePO4 cells with 4 M LiODFB-DME exhibit superior electrochemical performances, especially at high temperature (65°C). These outstanding performances can be certified to the increased availability of Li+ concentration and the merits of LiODFB salt. We believe that the concentrated LiODFB electrolyte is help to enable practical applications for Li metal anode in rechargeable batteries.
研究领域:
材料科学
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电化学
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产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Hao Xu,Dong Zhu,Wen Zhu,Fengzhan Sun,Jianxin Zou,Richard M. Laine,Wenjiang Ding
Rechargeable magnesium sulfur batteries (MSBs) assembled with earth-abundant and safe Mg anodes less prone to form dendrites on surface and sulfur-containing cathodes offer considerable potential for high energy densities. Nevertheless, suitable sulfur host materials and electrolytes are at present key factors that retard commercial introduction. Here, we explore preparation of Ti 3 C 2 @CoO composites as sulfur hosts with high concentration electrolytes consisting of Mg(TFSI) 2 and AlCl 3 in diglyme as new types of MSBs. Density functional theory (DFT) simulations indicate that CoO adsorbs magnesium polysulfides more strongly than Ti 3 C 2 while Ti 3 C 2 is more conductive to Mg 2+ diffusion and transfer than CoO. Coincidentally, use of 1 M electrolyte restrains dissolution of magnesium polysulfides in electrolytes during battery cycling. The experiments indicate that combining Ti 3 C 2 @CoO sulfur hosts and 1 M Mg(TFSI) 2 /AlCl 3 /diglyme electrolyte provides viable MSBs, maintaining discharge capacities of 540 mAh g −1 after 70 cycles at 100 mA g −1 . Mechanistic studies indicate that these MSBs work via a S/MgS x ( x = 2–8) redox process although oxidation of polysulfide to sulfur is not efficient in initial cycling. The systems studied here may offer valuable insights and inspiration in the design of appropriate electrolytes and sulfur-host materials for MSBs.
研究领域:
材料科学
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电化学
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DOI
高影响因子
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
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2021
·Vol. 168
·期 12
·120548
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IF 4.316
Mingwei Shi,Zailei Zhang,Man Zhao,Xianmao Lu,Zhong Lin Wang
For supercapacitors, high self-discharge rate is an inevitable issue that causes fast decay of cell voltage and loss of stored energy. Designing supercapacitors with suppressed self-discharge for long-term energy storage has been a challenge. In this work, we demonstrate that substantially reduced self-discharge rate can be achieved by using highly concentrated electrolytes. Specifically, when supercapacitors with 14 M LiCl electrolyte are charged to 0.80 V, the open circuit voltage (OCV) drops to 0.65 V in 24 h. In stark contrast, when the electrolyte concentration is reduced to 1 M, the OCV drops from 0.80 to 0.65 V within only 0.3 h, which was 80 times faster than that with 14 M LiCl. Decreased OCV decay rate at high electrolyte concentration is also confirmed for supercapacitors with different electrolytes (e.g., LiNO3) or at higher charging voltages (1.60 V). The slow self-discharge in highly concentrated electrolyte can be largely attributed to impeded electron transfer between the electrodes and electrolyte due to the formation of hydration clusters and reduced amount of free water molecules, thereby faradaic reactions that cause fast self-discharge are reduced. Our study not only supports the newly revised model about the formation of electric double layer with the inclusion of electron transfer, but also points a direction for substantially reducing the self-discharge rate of supercapacitors.
研究领域:
材料科学
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电化学
✓ 已验证
DOI
高影响因子
Materials Today Energy
·
2022
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IF 9.257
ZhiLong Han,Han Zhang,Qiang Wu,ShuPing Li,Wei Zhong,RenJie He,ShiJie Cheng,Jia Xie
Silicon-sulfur (Si-S) full cells show significant potential in energy storage due to their high theoretical energy density compared to commercial lithium-ion batteries. Nevertheless, a majority of electrolytes reported for Si-S full cells still cannot meet the requirements of stable long-duration cycling. Herein, we report a high-areal-capacity Si-S full cell consisted with prelithiated SiO, thick Li 2 S-Se 0.05 S 0.95 @pPAN electrode and a trifluorobenzene (F 3 B) modified and diluted high-concentration electrolytes. This novel electrolyte can effectively mitigate the volume expansion of the prelithiated SiO anode and enhance the utilization of active S in the cathode, showing excellent compatibility with electrodes. The assembled Si-S full cell using modified electrolyte displays remarkable cyclability over 100 cycles at 0.1C, exhibiting higher capacity retention (54.0% vs . 17.5%) than the pristine electrolyte without F 3 B. More importantly, a full cell with a thick sulfur cathode (16 mg/cm 2 ) exhibits a superior initial areal capacity of 8.34 mAh/cm 2 and high-capacity retention of 52% after 80 cycles, even at a lean electrolyte condition (2 μL/mg). This work provides guidance for the achievement of high-performance Si-S full cells under lean electrolytes.
研究领域:
材料科学
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电化学
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能源存储
✓ 已验证
DOI
高影响因子
Journal of Materials Chemistry A
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2021
·Vol. 9
·期 39
·22347-22352
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IF 12.732
Shunqiang Chen,Qingshun Nian,Lei Zheng,Bing-Qing Xiong,Zihong Wang,Yanbin Shen,Xiaodi Ren
High concentration electrolyte (HCE) provides a great opportunity for the development of long-life aqueous zinc (Zn) metal batteries because it can eliminate Zn dendrites and promotes higher Zn coulombic efficiencies (CEs) than conventional aqueous electrolytes. However, its application is limited by high cost, high viscosity, poor wettability and ionic conductivity. In this work, a localized high concentration electrolyte (LHCE) with 1,4-dioxane as the diluent and the hydrogen-bond modulator is reported for aqueous Zn metal batteries to overcome these limitations. More importantly, compared to the HCE, the unique solvation structure in the LHCE greatly boosts the anion chemistries to induce fluorinated interphases on the Zn anode and the V2O5 cathode. As a result, the LHCE not only achieves higher rate capabilities for Zn metal anodes and Zn‖V2O5 batteries, but also enables the Zn CE to quickly reach an average of 99.7% without the formation of dendrites (compared to <99% for the corresponding HCE). This approach can also be used in other aqueous battery systems to adjust the electrolyte physical properties and control the interphase formation process for practical applications.
研究领域:
电化学
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材料科学
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能源存储
✓ 已验证
产品关联
DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
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2020
·Vol. 31
·期 1
·2005991
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IF 16.836
Zhipeng Jiang,Ziqi Zeng,Xinmiao Liang,Li Yang,Wei Hu,Ce Zhang,Zhilong Han,Jiwen Feng,Jia Xie
Highly concentrated electrolytes (HCEs) significantly improve the stability of lithium metal anodes, but applications are often impeded by their limitation of density, viscosity, and cost. Here, fluorobenzene (FB), an economical hydrocarbon with low density and low viscosity, is demonstrated as a bifunctional cosolvent to obtain a novel FB diluted highly concentrated electrolyte (FB-DHCE). First, the addition of FB suppresses the decomposition of dimethoxyethane (DME) on the Li metal by strengthening the interactions of DME and FSI − around Li + . Second, FB efficiently elevates the content of LiF in the solid electrolyte interphase (SEI) based on its electrochemical reduction reaction. The unique solvation and interfacial chemistry of FB-DHCE enable dendrite-free deposition of lithium with high Coulombic efficiency (up to 99.3%) and prolong cycling life (over 500 cycles at 1 mA cm −2 ). The performance of FB-DHCE is further demonstrated in full cells under practical conditions, including ambient to low temperature (–20 °C), high areal capacity (7.6 mAh cm −2 ), high current density (3 mA cm −2 ), limited excess Li (20 µm Li), and lean electrolyte (3 g Ah −1 ). Employing FB as a cosolvent not only opens a novel pathway to stabilize Li metal anodes, but also could greatly advance the development of Li metal batteries.
研究领域:
材料科学
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电化学
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能源存储
✓ 已验证
DOI
高影响因子
Energy Storage Materials
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2021
·
IF 17.789
Zhipeng Jiang,Ziqi Zeng,Wei Hu,Zhilong Han,Shijie Cheng,Jia Xie
Lithium-sulfur (Li-S) battery, with their inherent advantages of high-energy density, low-cost, and eco-friendliness, shows promise as next-generation energy storage system . However, the practical Li-S batteries are far from achieving high-energy density and stable operation, because of the irreversible loss of active materials in both Li anode and S cathode. Herein, a modified diluted high concentration electrolyte (MDHCE) was designed for the practical Li-S batteries, which achieves a high energy density of 325 Wh kg –1 and stable cycling. Such an electrolyte enables a hybrid interface with high stability and fast Li-ion transport, thus improving the reversibility of Li anode and ameliorative kinetics of S cathode. The practicability of the MDHCE is further demonstrated in a 0.4 Ah Li-S pouch cell, which presents no obvious capacity fading with a steady Coulombic efficiency of 99.6%. This work not only provides guidance for electrolyte design, but also shines new lights towards practical high energy density Li-S batteries.
研究领域:
能源材料
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电化学
✓ 已验证
DOI
高影响因子
Battery Energy
·
2025
·
IF 9.9
Guojie Li,Yanwei Zhao,Bin Guo,Junlong Zhang,Jingmiao Jia,Aoxuan Wang,Chuntai Liu
Aluminum-based aqueous batteries are considered one of the most promising candidates for the upcoming generation energy storage systems owing to their high mass and volume-specific capacity, high stability, and abundant reserves of Al. But the side reactions of self-corrosion and passive film severely impede the advancement of aluminum batteries. Besides, the ideal matched electrolyte system and cathode working mechanism still need to be explored. Herein, a high specific energy aqueous aluminum–manganese battery is constructed by interfacial modified aluminum anode, high concentration electrolyte and layered manganese dioxide cathode. At the anode, in addition to boosting the wettability of the interface between the electrolyte and aluminum electrode, the altered surface of aluminum anode can also retard side reactions. At the same time, high concentration electrolyte (5 mol L −1 Al(OTF) 3 ) with a broad electrochemical window allows the battery system to attain a specific capacity of 452 mAh g −1 at 50 mA g −1 and an energy density of 542 Wh kg −1 , with greatly increased cycle stability. At the cathode, the mechanism investigation reveals that δ-MnO 2 is reduced to soluble Mn 2+ during the first cycle discharge, whereas Al x Mn (1− x ) O 2 generates during the charging process, acting as a highly reversible active material in the succeeding cycle. This comprehensive study paves the way for the development of aluminum-based energy storage devices.
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
高影响因子
ACS Nano
·
2023
·
IF 17.1
Yongchuan Liu,Yuansheng Lin,Zhanlin Yang,Changxin Lin,Xiangxin Zhang,Sujing Chen,Guolin Hu,Baisheng Sa,Yuanqiang Chen,Yining Zhang
For lithium metal batteries (LMBs), the elevated operating temperature results in severe capacity fading and safety issues due to unstable electrode–electrolyte interphases and electrolyte solvation structures. Therefore, it is crucial to construct advanced electrolytes capable of tolerating harsh environments to ensure stable LMBs. Here, we proposed a stable localized high-concentration electrolyte (LHCE) by introducing the highly solvating power solvent diethylene glycol dimethyl ether (DGDME). Computational and experimental evidence discloses that the original DGDME-LHCE shows favorable features for high-temperature LMBs, including high Li+-binding stability, electro-oxidation resistance, thermal stability, and nonflammability. The tailored solvated sheath structure achieves the preferred decomposition of anions, inducing the stable (cathode and Li anode)/interphases simultaneously, which enables a homogeneous Li plating–stripping behavior on the anode side and a high-voltage tolerance on the cathode side. For the Li||Li cells coupled with DGDME-LHCE, they showcase outstanding reversibility (a long lifespan of exceeding 1900 h). We demonstrate exceptional cyclic stability (∼95.59%, 250 cycles), high Coulombic efficiency (>99.88%), and impressive high-voltage (4.5 V) and high-temperature (60 °C) performances in Li||NCM523 cells using DGDME-LHCE. Our advances shed light on an encouraging ether electrolyte tactic for the Li-metal batteries confronted with stringent high-temperature challenges.
研究领域:
材料科学
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电化学
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能源存储
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Nanoscale
·
2024
·
IF 5.8
Jiuqing Wang,Hai Xu,Ruanye Zhang,Gengzhi Sun,Hui Dou,Xiaogang Zhang
Aqueous Zn ion-based fiber-shaped batteries (AZFBs) with the merits of high flexibility and safety have received much attention for powering wearable electronic devices. However, the relatively low specific capacity provided by cathode materials limits their practical application. Herein, we first propose a simple strategy for fabricating high-capacity Zn-iodine fiber-shaped batteries with a high concentration electrolyte and a reduced graphene oxide fiber (GF) cathode. It was found that oxygen functional groups in the graphene sheet demonstrate strong interaction with polyiodides but hinder electron conductivity; thus, the optimal balance between the specific capacity and coulombic efficiency of the GF electrode can be a function of the surface properties at different hydrothermal temperatures. Besides, the regulated high concentration electrolyte effectively suppresses the diffusion of polyiodides, which is attributed to the constrained freedom of water. More importantly, a four-electron redox mechanism was experimentally revealed through in situ Raman spectra. As a result, this fiber-shaped battery delivers a superior high reversible capacity of 390 mA h cm−3 at 1 A cm−3, an excellent rate performance of 125.7 mA h cm−3 at a high current density of 8 A cm−3 and outstanding cycling life with 82% capacitance retention after 2500 cycles.
研究领域:
材料科学
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能源存储
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纳米技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
·
2019
·
IF 3.218
Dongxue Luo,Ping Lei,Yunxuan Huang,Guorong Tian,Xingde Xiang
Rechargeable aqueous sodium-ion batteries (SIBs) are urgently pursued as a low-cost candidate for grid-scale storage of intermittent renewable energies. NASICON-type NaTi 2 (PO 4 ) 3 holds great promises as anode material for aqueous SIBs owing to the high theoretical capacity and low redox potential , but being severely challenged by poor cycling performance and low reaction kinetics. Herein, graphene-integrated NaTi 2 (PO 4 ) 3 /C composite is prepared with a facile sol-gel approach as anode material for aqueous SIBs. Electrochemical properties of the material in high-concentration aqueous electrolyte (6 M NaClO 4 ) are systematically investigated by using cycling voltammetry , galvanostatic technique and electrochemical impedance spectroscopy . It is found that it shows an improved charge/discharge performance with a high practical capacity of 104.6 mAh g −1 at 100 mA g −1 , excellent high-rate capability with a reversible capacity of 88.0 mAh g −1 at 2000 mA g −1 , and good cycling stability with 92% capacity retention after 100 cycles. The improved electrochemical performance is attributed to the synergetic contribution of carbon-blending nanostructure and high-concentration electrolyte, which largely enhances structural stability and reaction kinetics of the material. In addition, the redox mechanism is discussed based on experimental results from cyclic voltammetry and X-ray diffraction technique.
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
高影响因子
ACS Nano
·
2025
·
IF 16
Xin Hu,Wen Sun,Anbin Zhou,Ziyue Wen,Huirong Wang,Zhengqiang Hu,Tianyang Xue,Yongxin Huang,Li Li,Feng Wu,Renjie Chen
The electrochemical properties of anions as carriers in graphite-based dual-ion batteries (GDIBs) play an important role in achieving long cycling stability and high-rate performance. However, anion behavior in the electrolyte was neglected in previous studies. To balance high voltage and fast conduction, the anion behavior after introducing diluent in a highly concentrated electrolyte|high concentrated electrolyte (HCE) to form locally highly concentrated electrolyte|locally high concentrated electrolyte (LHCE) in GDIBs was deeply investigated. In contrast to the highly aggregated coordinated ion pairs in the HCE, more free anions can be attained in the LHCE without significant reunion. These free anions can rapidly migrate to the electrode surface under the electric field drive and then intercalate between graphite layers with a lower energy barrier. Meanwhile, an inorganic-rich interfacial layer with rapid ion conduction and a thinner thickness can be formed to prevent further decomposition of anions and stabilize the structure of the cathode. As a consequence, the dual-graphite DIBs achieved a superior capacity of 98.3% after 1000 cycles at a high rate of 200 mA g–1 in LHCE, and the corresponding pouch cells exhibited a stable cycling process. This work advances the understanding of anion chemistry, enabling the regulation of the anion status to enhance the electrochemical performance of GDIBs.
研究领域:
电化学
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子