Journal of Materials Chemistry A
·
2024
·
IF 10.7
Minghui Li,Cai Chen,Hongze Luo,Qingshuai Xu,Keyou Yan,Yongcai Qiu,Guangmin Zhou
Li metal anodes are considered among the most ideal candidates for next generation batteries owing to their lowest electrochemical potential and high theoretical capacity. However, the highly reactive Li metal is subject to continuous side reactions with conventional carbonate electrolytes. The resulting unsatisfying solid electrolyte interface (SEI) induces severe Li dendritic growth. Therefore, there is an urgent need to effectively control the components of SEI to solve the electrolyte/anode interface electrochemical instability. Herein, LiDFP and LiNO3 are introduced into the electrolyte to modulate the composition of the SEI. Owing to the lower lowest unoccupied molecular orbital (LUMO) energy levels of LiDFP and LiNO3 relative to those of the solvents, LiDFP and LiNO3 have preferential reducibility and thus generate a stable SEI containing LiF and Li3N, which has swift ion migration kinetics and homogeneous Li deposition behaviors. As a result, our electrolyte modified by additives enables the anode to achieve an excellent coulombic efficiency of 98% and exhibits an ultra-long cycling life of over 700 h in symmetrical cells. Li metal full cells paired with the LFP or NCM811 cathode also have excellent long cycling performance. This work demonstrates that additive-modified electrolytes are a viable and simple strategy for the evolution of Li metal batteries.
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 Applied Materials & Interfaces
·
2022
·
IF 10.383
Hanxiao Zhou,Huimin Shang,Tianhui Li,Wenjing Liu,Zhihao Guo,Yuxuan Guo,Jingjing Gao,Meizhen Qu,Huan Zhang,Gongchang Peng
Lithium anodes have attracted much attention because of their high energy density, but the existence of lithium dendrites tremendously limits their practical application. Herein, it is creatively proposed to employ N,O-bis(trimethylsilyl)trifluoroacetamide (BSTFA) as an electrolyte additive to stabilize the solid electrolyte interface. BSTFA is reduced on the lithium anode surface prior to other components to form a passivation layer composed of LiF, Li3N, and SiOx, which not only significantly prevents the continuous consumption of the electrolyte and reduces side reactions but also effectively promotes the uniform deposition of lithium ions with fast Li+ transmission, thereby solving the problem of lithium dendrites. Electrochemical results indicate that BSTFA can obviously reduce polarization in a Li||Li battery at a current density of 1 mA cm–2. Besides, an excellent cycling performance (107 mA h g–1) and Coulombic efficiency (99%) can be obtained for a Li||LiNi0.6Co0.2Mn0.2O2 (NCM622) battery with 0.5 wt % BSTFA at 2 C after 200 cycles, even at a high NCM622 loading of 6 mg cm–2.
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Energy Technology
·
2024
·Vol. 12
·期 8
·2400433
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IF 3.6
Xueqi Yu,Cheng Yang,Chang Liu,Yanfeng Gao,Yu Liu
Hard carbon (HC) is the most promising anode material for sodium-ion batteries (SIBs). The main obstacle to HC's application is its incompatibility with the phosphate flame-retardant additive, a common SIB additive. This incompatibility arises from the unstable solid electrolyte interphase (SEI) caused by phosphate molecule decomposition. For the first time, in this work, a new type of highly adaptive flame-retardant electrolyte is proposed. The electrolyte ensures the stability of the electrode/electrolyte interface by the introduction of pioneering long-chain nitrile as the SEI-forming additive and solvated structural regulator. Long-chain nitriles decompose before phosphate and form a stable SEI containing N element, which prevents the phosphate from inserting into the HC's layers and reduces its sodium-storage capacity. As a proof of concept, the HC anode demonstrates a higher initial Coulombic efficiency of 80.78% in the as-designed highly adaptive flame-retardant electrolyte, which is about 1.8 times than that before regulation. It can cycle stably for 1250 cycles at 3 C with a capacity retention of 60%. Moreover, the electrolyte has good flame retardancy and can extinguish naturally within 1 s. In this work, an innovative method is provided for developing high-safety SIBs based on HC anodes.
研究领域:
材料科学
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能源技术
✓ 已验证
产品关联
DOI
高影响因子
NATURE
·
2025
·Vol. 637
·期 8045
·339-346
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IF 48.5
Xu Qingshuai,Li Tan,Ju Zhijin,Chen Guangxu,Ye Daiqi,Waterhouse Geoffrey I. N.,Lu Yingying,Lai Xuejun,Zhou Guangmin,Guo Lin,Yan Keyou,Tao Xinyong,Li Hong,Qiu Yongcai
Lithium (Li) metal batteries (LMBs) are promising for high-energy-density rechargeable batteries 1 , 2 , 3 . However, Li dendrites formed by the reaction between highly active Li and non-aqueous electrolytes lead to safety concerns and rapid capacity decay 4 , 5 , 6 , 7 . Developing a reliable solid–electrolyte interphase is critical for realizing high-rate and long-life LMBs, but remains technically challenging 4 , 8 . Here we demonstrate that adding excess m -Li 2 ZrF 6 (monoclinic) nanoparticles to a commercial LiPF 6 -containing carbonate electrolyte of LMBs facilitates the release of abundant ZrF 6 2 – ions into the electrolyte driven by the applied voltage, converting to t -Li 2 ZrF 6 (trigonal) and creating a stable solid–electrolyte interphase in situ with high Li-ion conductivity. Computational and cryogenic transmission electron microscopy studies revealed that the in situ formation of the t -Li 2 ZrF 6 -rich solid–electrolyte interphase markedly enhanced Li-ion transfer and suppressed the growth of Li dendrites. As a result, LMBs assembled with LiFePO 4 cathodes (areal loading, 1.8/2.2 mAh cm −2 ), three-dimensional Li–carbon anodes (50-µm-thick Li) and Li 2 ZrF 6 -based electrolyte displayed greatly improved cycling stability with high capacity retention (>80.0%) after 3,000 cycles (1C/2C rate). This achievement represents leading performance and, thus, delivers a reliable Li 2 ZrF 6 -based electrolyte for durable LMBs under practical high-rate conditions.
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2024
·Vol. 34
·期 46
·2407867
·
IF 18.5
Mingyuan Gu,Hongwei Fu,Apparao M. Rao,Jiang Zhou,Yue lin,Shuangchun Wen,Ling Fan,Bingan Lu
Solid electrolyte interphase (SEI) plays a crucial role in a battery. This study leverages the assistance of weak interactions to construct a uniform and elastic SEI for potassium batteries. The caffeic acid phenethyl ester (CAPE) is introduced into the electrolyte, and the weak interactions between CAPE and anodes enable CAPE to contact electrons preferentially during cycling. The unsaturated carbon═carbon double bonds in CAPE molecules receive electrons and undergo polymerization reactions on the anode surface, forming a uniform and elastic SEI. Such SEI exhibits good uniformity and excellent mechanical elasticity, enabling the SEI to adapt well to the huge volume changes of the anode to maintain structural stability during cycling. As a result, the graphite anode exhibits over 1500 stable cycles at a current density of 100 mA g −1 . The potassium metal full battery based on a Prussian blue (PB) cathode cycles over 5700 times at a current density of 1000 mA g −1 . In addition, the pouch potassium-ion full battery based on a graphite anode and a PB cathode also shows excellent electrochemical performance, which operates stably for over 600 cycles without significant attenuation in capacity at a current density of 200 mA g −1 , showing potential practical value.
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 Omega
·
2023
·
IF 4.1
Hao-wen Jiang,Yu Qin,Yi-ming Nie,Zhi-fang Su,Yun-fei Long,Yanxuan Wen,Jing Su
The strategy of material modification for improving the stability of silicon electrodes is laborious and costly, while the conventional binders cannot withstand the repeated massive volume variability of silicon-based materials. Hence, there is a demand to settle the silicon-based materials’ problems with green and straightforward solutions. This paper presents a high-performance silicon anode with a binder obtained by in situ thermal cross-linking of citric acid (CA) and β-cyclodextrin (β-CD) during the electrode preparation process. The Si electrode with a binder synthesized by the one-pot method shows excellent cycling performance. It maintains a specific capacity of 1696 mAh·g–1 after 200 cycles at a high current of 0.5 C. Furthermore, the carbonylation of β-CD to carbonyl-β-CD (c-β-CD) introduced better water solubility, and the c-β-CD can generate multidimensional connections with CA and Si, which significantly enhances the specific capacity to 1941 mAh·g–1 at 0.5 C. The results demonstrate that the prepared integrated electrode facilitates the formation of a stable and controllable solid electrolyte interface layer of Si and accommodates Si’s repeated giant volume variations.
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
ACS Sustainable Chemistry & Engineering
·
2024
·
IF 7.1
Zining Man,Hao Tian,Xingbao Zhu,Zhe Lü
One experiment in this study utilized the plasticizer succinonitrile and lithium salt LiTFSI to directly create an ionic liquid electrolyte, with an artificial solid electrolyte interface layer generated using fluoroethylene carbonate. The typical electrolyte exhibited an ionic conductivity of 10–3 S cm–1 at room temperature and an electrochemical window of up to 5.3 V based on electrochemical impedance spectroscopy and linear sweep voltammetry tests. This electrolyte system effectively addresses the issues of decomposition and deterioration of traditional organic electrolytes in Li–O2 batteries at high voltages (over 4.5 V), as well as the problem of direct oxidation of the anode caused by oxygen shuttling, thereby greatly improving the lifespan of Li–O2 batteries. Additionally, the electrolyte’s low volatility and flame retardancy allowed for reliable operation of the battery in an air atmosphere. A Li–O2 battery assembled with the novel electrolyte was capable of cycling in a pure oxygen atmosphere for more than 1000 cycles at a capacity density of 200 mA h g–1 and over 150 cycles at 500 mA h g–1. Even when connected to ambient air without an additional oxygen selective membrane (OSM), the battery can still cycle continuously for more than 350 and 150 cycles at these two kinds of capacity density.
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
Journal of Energy Chemistry
·
2021
·
IF 9.676
Xiao-Ru Chen,Chong Yan,Jun-Fan Ding,Hong-Jie Peng,Qiang Zhang
Lithium (Li) metal attributes to the promising anode but endures the low Columbic efficiency (CE) and safety issues from the inactive Li accumulation. The metallic Li which is isolated from the lithium anode (named dead Li 0 ) consists the major component of the inactive Li. We systematically and meticulously investigated the formation and evaluation of dead Li 0 during stripping process from electron transfer, the oxidation of Li 0 to Li + and the diffusion of Li + through solid electrolyte interphase (SEI). The above-mentioned processes were regulated by adjusting the contact sites of electron channels , the dynamic rate of conversion from Li 0 to Li + , and the structure as well as components of SEI. The design principles for achieving less dead Li 0 and higher CE are proposed as a proof of concept in lithium metal batteries . This new insight sheds a comprehensive light on dead Li 0 formation and guides the next-generation safe batteries for future application.
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
·
2022
·
IF 18.027
Gongxun Lu,Jianwei Nai,Huadong Yuan,Juncheng Wang,Jianhui Zheng,Zhijin Ju,Chengbin Jin,Yao Wang,Tiefeng Liu,Yujing Liu,Xinyong Tao
The lithium metal anode (LMA) is regarded as one of the most promising candidates for high-energy Li-ion batteries. However, the naturally formed solid electrolyte interface (SEI) is unsatisfied, which would cause continuous dendrite growth and thus prevent the practical application of the LMA. Herein, a stable electrolytic carbon-based hybrid (ECH) artificial SEI is constructed on the LMA via the in-situ electrodeposition of an electrolyte sovlent at ultrahigh voltage. This nanostructured carbon strengthened SEI exhibits much improved ionic conductivity and mechanical strength, which enables uniform Li+ diffusion, stabilizes the interface between the electrolyte and lithium metal, and inhibits Li dendrite breeding and Li pulverization. With the protection of this ECH layer, the symmetrical cells show stable long-term cycling performance over 500 h with an ultrahigh plating capacity of 5 mAh cm–2 at the current density of 5 mA cm–2. A full cell assembled with a Li[Ni0.8Co0.1Mn0.1]O2 or LiFePO4 cathode exhibits a long-term cycling life and excellent capacity retention.
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Materials Chemistry A
·
2023
·Vol. 11
·期 11
·5636-5644
·
IF 11.9
Shi Zhou,Yiting Zhu,Haoran Hu,Chenghan Li,Jie Jiang,Jianyu Huang,Biao Zhang
LiF, which is considered as a key component of the solid electrolyte interface (SEI), can promote the uniform deposition of lithium. However, excessive LiF will limit the transport of lithium ions (Li+) in the SEI, resulting in low coulombic efficiency and lithium dendrite growth. Regulating the LiF concentration in the SEI is challenging but critical to the development of solid-state lithium metal batteries (SSLMBs). Herein, we synthesized porous organic polymers (POPs) that can be flexibly modified at the molecular level. These modified POPs (denoted as POPs-X-FP, X = 2, 3, 4) are added into a PEO electrolyte as fillers to form composite solid electrolytes (denoted as CSE-X-FP, X = 2, 3, 4, respectively). CSE-X-FP have different catalytic decomposition capabilities of TFSI− anions in the electrolyte due to the different fluorine atom substitution positions on the benzene ring of the POPs. Consequently, the LiF concentration in the SEI can be optimized by tuning the fluorine atom substitution positions on the benzene rings of the POPs to boost the performance of PEO based ASSLMBs. Using the LiF optimized SEI, the LiFePO4(LFP)//CSE-4-FP//Li full cell delivered a long cycle life of 1200 cycles with an initial capacity of 160.7 mA h g−1 at 0.5C. This study provides a new strategy to regulate the LiF content in the SEI layer to boost the performance of SSLMBs.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
Energy Storage Materials
·
2023
·
IF 20.4
Chunfeng Chen,Jinlong Chen,Shuangshuang Tan,Xueting Huang,Yaoyao Du,Bo Shang,Baihua Qu,Guangsheng Huang,Xiaoyuan Zhou,Jingfeng Wang,Lingjie Li,Fusheng Pan
Rechargeable magnesium batteries (RMBs) are considered a highly promising energy storage system . However, the lack of low-cost and highly effective electrolytes severely hinders the development of RMBs. Herein, a tris(2,2,2-trifluoroethyl) borate (B(Otfe) 3 ) co-solvent is introduced into the magnesium-aluminum-chloride complex electrolyte. The electrophilic B(Otfe) 3 as an electron pair acceptor can react with the passivation layer to avoid the electrolytic conditioning process. The B(Otfe) 3 -modified solvation structure with low desolvation energy increases the concentration of active cation, effectively improving the ionic conductivity and area current density. Meanwhile, the B(Otfe) 3 -modified solvation ions with lower LUMO energy induce the formation of the B-F/B-O-containing and MgF 2 -containing solid electrolyte interphase (SEI), reducing the interfacial transfer impedance. The prepared B(Otfe) 3 /MgCl 2 /AlCl 3 (BMA) electrolyte exhibits excellent electrochemical performance with low overpotential (∼122 mV), high average coulombic efficiency (CE) (∼98.2%) and long-term cycling stability (1000 h). Moreover, the BMA electrolyte shows good compatibility with Mo 6 S 8 and CuS cathodes. The Mg|CuS full cell keeps a high specific capacity of 231 mAh g −1 after 80 cycles at 56 mA g −1 , and the Mg|Mo 6 S 8 cell operates 1000 cycles with an average CE of nearly 100%. This work provides an effective way to simultaneously improve the electrolyte solvation sheath and SEI structure for stable magnesium batteries.
研究领域:
材料科学
·
能源存储
✓ 已验证
产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Zhencheng Huang,Tao Huang,Xue Ye,Xingyu Feng,Xiuyuan Yang,Jianneng Liang,Shenghua Ye,Yongliang Li,Xiangzhong Ren,Wei Xiong,Xiaoping Ouyang,Qianling Zhang,Jianhong Liu
Lithium metal is a promising anode material due to its high theoretical capacity and low redox potential. However, lithium metal anode suffers from lithium dendrite, which reduces the cycle stability and reversibility of lithium metal batteries (LMBs). In order to solve this issue, we designed an in-situ polymerization method of organic–inorganic composite materials (methyl methacrylate (MMA)/MXene) to prepare artificial solid-electrolyte interphase (SEI). The as-prepared LMBs exhibit good interfacial contact and high electrochemical performance owing to the charge redistribution effect of MXene layer for decreasing the nucleation energy barrier and on the lithium metal anode. The specific capacity can sustain 106.6 mAh/g even after 1000 h cycles at 1C, and the capacity retention is 80.1 % with LiFePO 4 (LFP) as a cathode material. Therefore, we believe this simple and inexpensive method can effectively restrain the growth of lithium dendrites and improve the cyclic stability and reversibility of the LMBs.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）