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CHEMICAL ENGINEERING JOURNAL · 2025 · IF 13.2

LiAl-LDHs additives in carbonate electrolytes for realizing dendrite-free lithium deposition in Li metal batteries

Baolei Li,Qingsong Cai,Jianmin Zhang,Kai Zhang,Zongmin Zheng

The lithium metal batteries (LMBs) using Li metal as the anode are becoming one of the representatives of next-generation high-energy–density batteries. However, uneven deposition and stripping of Li usually cause capacity loss during cycling. To address these issues, NO 3 − intercalated LiAl layered double hydroxides (LiAl-LDHs) nanosheets were used as novel solid additives for conventional carbonate electrolytes. The abundant Li + transport pathways brought by LiAl-LDHs and the interlayer NO 3 − in LiAl-LDHs are beneficial to the uniform concentration distribution of Li + and high-quality solid electrolyte interface (SEI), thereby achieving stable deposition/stripping of Li. The assembled Li||Li symmetric cell was cycled stably for 500 h at a current density of 0.5 mA cm −2 . The Li||LFP(LiFePO 4 ) full cell had a capacity retention of 90 % after 800 cycles at 1C. Even at a high operating temperature of 50 °C, the Li||Li symmetric cells and Li||LFP full cells can still obtain steady charging-discharging performances.

CAS / MDL: 15365-14-7
研究领域: 材料科学 · 电化学
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CHEMICAL ENGINEERING JOURNAL · 2022 · IF 16.744

Weak coulomb interaction between anions and Na+ during solvation enabling desirable solid electrolyte interphase and superior kinetics for HC-based sodium ion batteries

Xin Hou,Tianyu Li,Yanling Qiu,Mingqin Jiang,Qiong Zheng,Xianfeng Li

Electrolyte plays an important role in conducting sodium ions and carrying out chemical/electrochemical reactions. However, the impact mechanism of microscopic solvation structure remains vague but is significant for the electrolyte design. Here we reveal that the inner relationship between solvation structure and electrochemical reaction is manifested intuitively by manipulating the anions in the solvated shell, which determines Na storage kinetics and SEI evolution process. The result elucidates the weak coulomb interaction between PF 6 − and Na + could promote Na + transport number in bulk liquid and Na storage kinetics. And it could induce PF 6 − to reduce preferentially and facilitate additive to enter solvation structure, thereby forming a thin&compact&protective SEI with layered morphology. The excellent SEI would protect anode effectively, inhibiting decomposition of solvents and improving battery performances. As expected, 5 Ah Na 3 V 2 (PO 4 ) 3 -hard carbon pouch-type batteries with well-matched PF 6 − -based electrolyte display a high specific energy of 129 Wh kg −1 , a superior rate capability with capacity retention of 90 % at 5 C and cycling stability with retention of 86.82 % at 1 C after 700 cycles.

CAS / MDL: 21324-39-0
研究领域: 材料科学 · 电化学
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ELECTROCHIMICA ACTA · 2015 · IF 4.504

In-situ carbon coating to enhance the rate capability of the Li4Ti5O12 anode material and suppress the electrolyte reduction decomposition on the electrode

Xing Li,Jun Xu,Pengxiao Huang,Wei Yang,Zhiqiang Wang,Mingshan Wang,Yun Huang,Ying Zhou,Meizhen Qu,Zuolong Yu,Yuanhua Lin

The in-situ carbon coated LTO composite (LTO/C-PR) is synthesized via a wet chemical method from the phenolic resin coated TiO 2 (TiO 2 /PR) and Li 2 CO 3 . The results indicate that the coated carbon layer pyrolyzing from phenolic resin exhibits higher degree of graphitization than that of pyrolyzing from glucose. The LTO/C-PR composite shows better rate capability and cyclic performance than the LTO/C-G composite using glucose as pyrolytic carbon source. Furthermore, it is found that the higher graphitization of carbon layer can more efficiently suppress the interfacial reactions between the LTO and the electrolyte at the cut-off voltages of 1–3   V. Moreover, the higher graphitization of carbon layer is also favorable to impede the deeper reduction decomposition of the electrolyte below 1.0   V by forming a more successive and thinner SEI film on the LTO electrode. These results indicate that coating the LTO with higher graphitization of carbon layer should be more preferable to solve both the rate capability and the gas generation behavior of the LTO anode material.

CAS / MDL: 13463-67-7
研究领域: 材料科学 · 电化学
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ENERGY & FUELS · 2022 · IF 4.654

A Lithium-Ion Battery Cathode with Enhanced Wettability toward an Electrolyte Fabricated by a Fast Light Curing of Photoactive Slurry

Bingying Zhu,Tianle Zheng,Jianwei Xiong,Xiaotang Shi,Ya-Jun Cheng,Yonggao Xia

In an Li-ion battery, the ability of the electrolyte to wet the electrode is related to the capacity and high rate discharge performance of the battery. Poor wettability can lead to low capacity utilization of the electrode, increased resistance, and even safety problems. Currently, the primary manufacturing process of the electrode is based on the slurry technology; however, the electrode prepared using this method is difficult to be wetted by the electrolyte. In this study, ethylene carbonate/dimethyl carbonate (EC/DMC) (3:7 by volume) has been used as the electrolyte solvent instead of NMP, and the electrode is prepared by photopolymerization. This method contributes to the wetting and ion transport of the electrode. The LFP|LiPF6-3EC/7DMC|Li semicell was cycled for 100 cycles at a surface current of 0.5 mA cm–2, with a capacity retention of 90%. This new electrode construction technology provides a new idea for the process design of lithium-ion batteries.

研究领域: 材料科学 · 能源技术
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ACS Applied Materials & Interfaces · 2023 · IF 9.5

Multifunctional Electrolyte Additive Enables Highly Reversible Anodes and Enhanced Stable Cathodes for Aqueous Zinc-Ion Batteries

Xianjin Gong,Huiting Yang,Jie Wang,Guichang Wang,Jinlei Tian

Aqueous zinc-ion batteries (AZIBs) are charming devices for large-scale power grid energy storage because of their characteristics of environment friendliness, low cost, high abundance, and safe operation. However, the inferior reversibility of the anode and the loss of cathode capacity always hinder the application of AZIBs. Herein, we propose a simple multifunctional electrolyte additive, diethylenetriamine (DETA), which can inhibit the formation of zinc dendrites and the occurrence of side reactions on the anode, reconstruct the solvated structure and uniform ion flux in the electrolyte, restrain the dissolution of active materials, and induce the crystal transformation on the cathode concurrently. Molecular dynamics Simulation and density functional theory both verified the extraordinary efficacy of DETA. With the assistance of DETA, the Zn anode gained a life of up to 2000 h, and the cathode with commercial V2O5 retained a capacity of 125.2 mA h g–1 at the 1000th discharge process. From the perspective of practical application, this work can open up the application prospect of AZIBs in large-scale energy storage and provide reference for the subsequent works. The findings will greatly promote the application of AZIBs in large-scale energy storage and provide more inspiration for future research.

CAS / MDL: 872-50-4
研究领域: 材料科学 · 电化学
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ACS Nano · 2025 · IF 16

Intermolecular Interaction Adjustment for LiNO3 Solubility Promotion toward High-Performance Li||NCM811 Batteries

Chong Xu,Shuang Liu,Sai Che,Guang Ma,Gong Cheng,Dongyuan Zhang,Junjie Fu,Ye Wang,Jiahao Yang,Yuci Tian,Yongpeng Cui,Weihua Chen,Yongfeng Li

Incorporating lithium nitrate (LiNO3) as a film-forming additive into carbonate-based electrolytes presents a promising strategy to enhance the stability of high-energy-density Li||NCM811 batteries. However, the small size of Li+ and the high donor number (DN) of NO3– hinder the dissociation of LiNO3, and its limited solubility (<800 ppm) in carbonate-based electrolytes poses significant challenges for practical application. To address this issue, we propose a “Small-Sized Carrier” strategy that enhances the solubility of LiNO3 in carbonate solvents by modulating the intermolecular interactions within the solvent system. This approach employs vinylene carbonate (VC), a small molecule with moderate polarity, to enhance the dissolution of LiNO3 without compromising the compatibility of the electrolyte with the lithium metal anode. The introduction of the “Small-Sized Carrier” additive system simultaneously enhances the stability of the electrode–electrolyte interfaces and optimizes the solvation structure of the electrolyte. As a result, the electrolyte developed through this strategy demonstrates outstanding electrochemical performance, with Li||NCM811 batteries achieving a capacity retention of 83.8% after 600 cycles. This work provides an insightful approach to designing advanced electrolytes tailored to high-energy-density lithium metal batteries (LMBs).

CAS / MDL: 27860-83-9 7790-69-4
研究领域: 电化学 · 储能材料 · 电池技术 · 材料科学 · 化学工程
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PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA · 2024 ·Vol. 121 ·期 17 ·e2311075121 · IF 9.4

Unveil the origin of voltage oscillation for sodium-ion batteries operating at −40 °C

Lanfang Que,Fuda Yu,Jihuai Wu,Zhang Lan,Yutong Feng,Ruizheng Zhao,Zhihao Sun,Zhuo Yang,Hao Luo,Dongliang Chao

Voltage oscillation at subzero in sodium-ion batteries (SIBs) has been a common but overlooked scenario, almost yet to be understood. For example, the phenomenon seriously deteriorates the performance of Na3V2(PO4)3 (NVP) cathode in PC (propylene carbonate)/EC (ethylene carbonate)-based electrolyte at −20 °C. Here, the correlation between voltage oscillation, structural evolution, and electrolytes has been revealed based on theoretical calculations, in-/ex-situ techniques, and cross-experiments. It is found that the local phase transition of the Na3V2(PO4)3 (NVP) cathode in PC/EC-based electrolyte at −20 °C should be responsible for the oscillatory phenomenon. Furthermore, the low exchange current density originating from the high desolvation energy barrier in NVP-PC/EC system also aggravates the local phase transformation, resulting in severe voltage oscillation. By introducing the diglyme solvent with lower Na-solvent binding energy, the voltage oscillation of the NVP can be eliminated effectively at subzero. As a result, the high capacity retentions of 98.3% at −20 °C and 75.3% at −40 °C are achieved. The finding provides insight into the abnormal SIBs degradation and brings the voltage oscillation behavior of rechargeable batteries into the limelight.

研究领域: 材料科学 · 电化学
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ELECTROCHIMICA ACTA · 2020 · IF 6.215

The function of Mn2+ additive in aqueous electrolyte for Zn/δ-MnO2 battery

Ce Qiu,Xiaohui Zhu,Liang Xue,Mingzhu Ni,Yang Zhao,Bo Liu,Hui Xia

Adding Mn 2+ in aqueous electrolyte is a well adopted approach to improve cycle performance for Zn/MnO 2 batteries. The function of Mn 2+ additive in aqueous electrolyte, however, is not well understood, which could affect revealing the real performance of the MnO 2 cathode itself. In this work, a battery system with Zn anode and birnessite MnO 2 cathode is constructed and systematically investigated by using MnSO 4 additive in the electrolyte with different concentrations. The function of Mn 2+ in the electrolyte, the structural evolution of the electrode, the reaction mechanism, and the cause for capacity fading are comprehensively investigated in this system. It is found that Mn 2+ can be continuously electro-oxidized at the cathode and form ε-MnO 2 when the charge voltage is above 1.7 V during cycling, leading to successive capacity increase up to hundreds of cycles. The capacity increase, however, stops after certain cycle numbers, and is followed by fast capacity fading, which is correlated to the competition between ε-MnO 2 formation and phase transition from birnessite to spinel ZnMn 2 O 4 . It is suggested that addition of Mn 2+ in the electrolyte cannot stabilize the MnO 2 cathode and the improved cycle performance is achieved at the expense of consuming the Mn 2+ in the electrolyte.

研究领域: 电化学 · 材料科学
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INTERNATIONAL JOURNAL OF ENERGY RESEARCH · 2019 ·Vol. 43 ·期 14 ·8049-8056 · IF 3.343

A sandwich-structured separator based on in situ coated polyaniline on polypropylene membrane for improving the electrolyte wettability in lithium-ion batteries

ZhenDong Hao,CongRong Wu,QianQian Zhang,JingBing Liu,Hao Wang

Summary Designing separators with excellent electrolyte wettability is of great significance to improve the electrochemical behavior of lithium-ion batteries (LIBs). Herein, we develop a sandwich-structured separator by facile in situ polymerization of polyaniline (PANI) on the both sides of polypropylene (PP) separator. The introduction of PANI coating improves the electrolyte wettability of the PP separators. Consequently, the cells equipped with this sandwich-structured separator demonstrate superior electrochemical performance including initial capacity, rate performance, and cyclic stability compared with the PP separator. This work may provide a facile approach for separator modification to improve the performance of LIBs.

研究领域: 材料科学 · 电化学
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JOURNAL OF POWER SOURCES · 2024 · IF 8.1

Full gradient compensation of LiNO3 in the suspension electrolyte for lithium metal batteries

Jun Wei,Zhijie Guo,Fei Wang,Xianyi Zhao,Sihan Chen,Xinyao Zhang,Xinyao Wang,Ye Liang,Xiaobing Wang

Uncontrolled side reactions between lithium metal and organic electrolytes seriously deteriorates the stability of corresponding battery due to the non-uniform Li + deposition. Using lithium nitrate (LiNO 3 ) as an additive can adjust the components in solid-electrolyte-interphase (SEI) for optimizing of lithium metal interface . However, the low solubility and rapid consumption of LiNO 3 in ester-based electrolytes limit its further application. Herein, a kind of suspension electrolyte containing micron-sized LiNO 3 particles is reported to realize a full gradient compensation against the consumption of NO 3 − . Benefiting from the uniformly dispersion of LiNO 3 particles, a SEI layer containing even-distributed Li 3 N and LiN x O y with high content is constructed that promotes the rapid and uniform plating of Li + . Consequently, the Li/Cu batteries present a polarization of only 15–20 mV, and exhibit a consistent performance for 230 cycles with the CE of 98.1%, which is 4 times than that of conventional carbonate electrolytes. In addition, the cycling life of the assembled Li/NCM811 batteries can be extended to 260 cycles with a high capacity retention of 82.4 %.

CAS / MDL: 7439-93-2
研究领域: 材料科学 · 电化学
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JOURNAL OF THE ELECTROCHEMICAL SOCIETY · 2017 ·Vol. 164 ·期 7 ·A1559 · IF 3.259

A Flame Retardant Ionic Conductor Additive for Safety-Reinforced Liquid Electrolyte of Lithium Batteries

Qingfu Wang,Pingping Liu,Shizhen Li,Xiao Wang,Fangzhou Li,Jun Ma,Jingchao Chai,Jianjun Zhang,Gaojie Xu,Zhaoge Huang,Guanglei Cui

An ionic conducting ethyl phosphate-polyethylene glycol based copolymer (abbreviated as EPCP) as a promising flame retardant additive is presented in this study. The flammability tests demonstrate that the liquid electrolyte with 15 wt% EPCP (abbreviated as EPCP15-LE) is totally nonflammable. More importantly, benefitted from the ionic transport capability of EPCP, the ionic conductivity of EPCP15-LE at room temperature is comparable with the liquid electrolyte (shorted as LE). Moreover, the resultant electrolyte possessed wide electrochemical window (4.3 V), which can be matched with relatively high voltage cathode materials. In addition, the cell using EPCP15-LE exhibits superior cycle performance and excellent rate capability. In a word, this flame retardant ionic conductor is a promising additive for safety-reinforced lithium battery.

研究领域: 材料科学 · 能源技术
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Scientific Reports · 2019 ·Vol. 9 ·期 1 ·1-16 · IF 4.011

S-containing and Si-containing compounds as highly effective electrolyte additives for SiOx -based anodes/NCM 811 cathodes in lithium ion cells

An Fuqiang,Zhao Hongliang,Zhou Weinan,Ma Yonghong,Li Ping

Recently, high-energy density cells containing nickel-rich cathodes and silicon-based anodes have become a practical solution for increasing the driving range of electric vehicles. However, their long-term durability and storage performance is comparatively poor because of the unstable cathode-electrolyte-interphase (CEI) of the high-reactivity cathode and the continuous solid-electrolyte-interphase (SEI) growth. In this work, we study several electrolyte systems consisting of various additives, such as S-containing (1,3,2-dioxathiolane 2,2-dioxide (DTD), DTD + prop-1-ene-1,3-sultone (PES), methylene methanedisulfonate (MMDS)) and Si-containing (tris(trimethylsilyl) phosphate (TTSP) and tris(trimethylsilyl) borate (TMSB)) compounds, in comparison to the baseline electrolyte (BL = 1.0 M LiPF 6  + 3:5:2 w-w:w EC: EMC: DEC + 0.5 wt% lithium difluoro(oxalato)borate (LiDFOB) + 2 wt% lithium bis(fluorosulfonyl)imide (LiFSI) + 2 wt% fluoroethylene carbonate (FEC) + 1 wt% 1,3-propane sultone (PS)). Generally, electrolytes with Si-containing additives, particularly BL + 0.5% TTSP, show a lower impedance increase in the full cell, better beginning-of-life (BOL) performance, less reversible capacity loss through long-term cycles and better storage at elevated temperatures than do electrolytes with S-containing additives. On the contrary, electrolytes with S-containing additives exhibit the advantage of low SEI impedance but yield a worse performance in the full cell than do those with Si-containing additives. The difference between two types of additives is attributed to the distinct function of the electrodes, which is characterized by cyclic voltammetry (CV), electrochemical impedance spectroscopy (EIS) and X-ray photoelectron spectroscopy (XPS), which was performed on full cells and half cells with fresh and harvested electrodes.

研究领域: 材料科学 · 电化学 · 能源存储
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