MACROMOLECULES
·
2024
·
IF 5.1
Zhenzhen Yang,Jiahui Cai,Zitong Shen,Jiaqi Bian,Jiashang Chen,Yao Xu,Zecheng Fang,Congkun Du,Xing Xiang,Juan Wang,Peng Yu,Ruiyao Cui,Siwen Bi
Carbonyl-containing polymers have been considered promising candidates as hosts in solid polymer electrolytes (SPEs) due to the reasonable chelating coordination with Li+, better antioxidation for high-voltage cathodes, and higher ion transference number compared with polyether SPEs. In this work, four polyesters of poly(octamethylene succinate), poly(hexmethylene succinate) (PHS), poly(butylene succinate), and polycaprolactone were investigated. In these SPEs with different −C═O/–CH2– ratios, PHS had the highest conductivity (σ) of 1.24 × 10–4 S/cm because of the excellent ability to deionize bis(trifluoromethane)sulfonimide (LiTFSI) up to 88.3 ± 3.2% at 70 °C and the lowest activation energy of Li+ ionic conduction. The effect of Li+/–C═O ratios (r) on the ionic conductivity can be clarified into low-, middle-, and high-concentrated regions. The decrease of PHS crystallinity due to LiTFSI solvation provided ion transport paths and mainly contributed to the improvement of ionic conductivity in the middle-concentrated region, while the solvation degree dominantly facilitated ionic conduction in the high-concentrated region and at higher temperatures. By combining the DFT simulation and polymer thermal analysis, we found the transition of Li+ coordination from multichain to single-chain bindings provided more flexible segment movement. It also proved that the sequence design of active groups in a polymer chain would be a promising strategy for stable and high-performance SPEs.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Zijun Yi,Long Zhang,Fang Ding,Xuehong Ren
The Spiro-OMeTAD is one of the most widely used hole transport materials in highly efficient perovskite solar cells (PSCs), whose performance typically relies on dopants such as lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) and 4-tert-butylpyridine (TBP) to enhance conductivity and hole transport efficiency. However, these conventional dopants suffer from high volatility and hygroscopicity, severely limiting the long-term stability and commercialization potential of PSCs. To solve this problem, this work developed a novel dopant 4-isopropyl-4′-methyldiphenyl iodide tetrakis(pentafluorophenyl)borate (IMT) as a substitute for LiTFSI and TBP for synergistic doping regulation of Spiro-OMeTAD. It was revealed that IMT possessed a well-delocalized electronic structure and appropriately aligned energy levels, which effectively promoted the oxidation of Spiro-OMeTAD, thereby enhancing its electrical conductivity and hole mobility. Additionally, the incorporation of IMT improved the hydrophobicity and compactness of the Spiro-OMeTAD film, effectively mitigating moisture penetration and suppressing interfacial ion migration. The rigid and flexible PSCs based on IMT doping exhibited excellent optoelectronic performance, with the champion power conversion efficiencies reaching 24.97 % and 23.15 %, respectively, which were significantly higher than those of conventional devices using LiTFSI and TBP as dopants. More importantly, the introduction of IMT effectively improved the environmental stability of perovskite devices, enabling them to maintain high-efficiency output under high humidity, high temperature and long-term illumination conditions. This work proposes a new doping strategy for efficient, stable and LiTFSI/TBP-independent PSCs, and provides a theoretical and practical basis for the molecular design of hole transport materials.
研究领域:
光伏技术
·
材料科学
·
能源材料
·
半导体器件
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Dan Cai,Donghuang Wang,Yongjie Chen,Shengzhao Zhang,Xiuli Wang,Xinhui Xia,Jiangping Tu
Composite solid electrolytes have recently attracted widespread attention due to their acceptable lithium-ion (Li-ion) conductivity and suitable flexibility. However, isolated ceramic particles in composite electrolyte cannot provide continuous fast Li-ion transport channels. And the non-uniformity caused by particle agglomeration usually leads to a decrease in the performance of the composite electrolyte. Here, we design a “polymer in ceramic” composite electrolyte that combines three-dimensional Li 6.4 La 3 Zr 2 Al 0.2 O 12 (3D LLZAO) framework with polyethylene oxide (PEO)/LiTFSI (T-LAPL) via a template and solution method. In addition to the significantly enhanced Li-ion conductivity (2.51 × 10 −4 S cm −1 at room temperature) and the high Li-ion transference number (t Li+ = 0.53), the T-LAPL composite electrolyte also exhibits improved thermal and electrochemical stability. Both symmetrical Li/T-LAPL/Li cells and LiFePO 4 /T-LAPL/Li cells display excellent electrochemical performance. The repeated lithium stripping/plating process at 0.1 mA cm −2 can keep stable for 400 h without short circuit at room temperature. The assembled LiFePO 4 cell shows an initial discharge capacity of 165.9 mAh g −1 at 0.2C and the capacity can remain 80% after 100 cycles. This high-performance composite electrolyte reveals a promising opportunity for the next-generation lithium batteries with high energy density and high safety.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
DOI
高影响因子
POLYMER
·
2022
·
IF 4.432
Xiaoxue Wu,Tiantian Song,Zizhen Wei,Lei Shen,Hanqiu Jiang,Yubin Ke,Chunyong He,Hua Yang,Weichao Shi
Studies on phase behavior of polymer blends with lithium salts can provide a theoretical basis for developing solid polymer electrolytes in lithium-ion battery. In this paper, the liquid-liquid phase separation of PEO/PS/LiTFSI system is characterized by small angle neutron scattering (SANS) and small angle laser light scattering (SALLS). A combination of the Debye-Bueche equation and Ornstein-Zernike scattering function is employed to fit the SANS data in the homogeneous state. The thermodynamic parameters , including the forward scattering intensity I 0 , correlation length ξ , spinodal temperature T s , effective interaction parameter χ eff and cloud point boundaries, are obtained. The cloud point temperatures increase with LiTFSI concentration, especially at the low PEO fractions. We conclude that even a small amount of lithium salt enhances the liquid-liquid phase separation of PEO/PS blends significantly, and the effect of electrostatic interaction increases with temperature.
研究领域:
材料科学
·
电化学
·
聚合物科学
✓ 已验证
DOI
高影响因子
Energy Storage Materials
·
2025
·
IF 20.2
Rongrong Guo,Xiaoyun Xu,Songmei Li,Yangyang Cheng,Junwei An,Mei Yu,Jinyan Zhong,Juan Du,Shubin Yang,Bin Li
Lithium bis((trifluoromethyl)sulfonyl)azanide (LiTFSI) based electrolytes have become the preferred electrolytes for lithium metal batteries (LMBs) due to their exceptional anode stability and ionic conductivity. However, challenges including unstable cathode electrolyte interface (CEI) formation and aluminum current collector (AlCC) corrosion have hindered the application of LiTFSI-based electrolyte in high-voltage LMBs. In this work, a universal passivation strategy is proposed and achieved with additive 8-hydroxyquinoline (8-HQ) in LiTFSI based electrolyte (ED-HQ). The 8-HQ additive preferentially decomposes on the cathode surface to generate Li 3 N, inducing the formation of inorganic-rich CEI with a uniform thickness of only 10 nm. The dense and homogeneous inorganic-rich CEI enables the cycling stability of the cathode. Meanwhile, the 8-HQ additive shows strong adsorption on the AlCC surface, which promotes the formation of a composite passivation layer consisting of an Aluminum-8-hydroxyquinoline (Alq 3 ) chelate layer and an AlF 3 /LiF inorganic layer, increasing the stable operating voltage of AlCC to 4.9 V and reducing the corrosion current density to one tenth. As a result, the joint effects enable Li||LiFePO 4 cells with ED-HQ electrolyte to achieve 89.8% capacity retention after 500 cycles at an elevated cutoff voltage of 4.5 V, demonstrating a viable pathway toward stable high-voltage LMB operation.
研究领域:
电化学
·
储能
·
材料科学
·
电池技术
·
表面化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2023
·
IF 6.2
Jingxuan Cai,Tao Liu,Chuwei Liu,Guoqiang Liu
Solid electrolytes are safer alternatives to liquid electrolytes. Adding Ga to lithium lanthanum zirconium oxide (LLZO) garnet-like solid-state electrolytes effectively improves their performance. The properties of solid-state electrolytes prepared using the two mainstream methods, namely, electrospinning and sol-gel, vary and directly affect the electrochemical performance of assembled batteries. In this study, we prepared Li 6.25 Ga 0.25 La 3 Zr 2 O 12 (Ga-LLZO) nanoparticles and nanofibers using the sol-gel and electrospinning methods, respectively. The battery was also assembled with composite film consisting of the poly (vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP) polymer substrate within Ga-LLZO ceramic fillers. The electrolyte of the battery prepared by Ga-LLZO nanofibers has better conductivity. We fabricated a Li|10 wt% Ga-LLZO nanofiber/PVDF-HFP/60 wt% lithium bis(trifluoromethanesulfonyl)imide (LiTFSI)|LiFePO 4 button battery using the optimal concentration. The device demonstrated a stable cycle lasting up to 700 h, a Coulombic efficiency of 98%, a capacity retention rate of 96.5%, and an electrochemical window up to 5 V vs Li/Li + at room temperature. Over time, a suitable contact interface generated a positive feedback loop. The ionic conductivity was 1.1 × 10 −4 S·cm −1 . The newly prepared electrolyte films aid the fabrication of future solid electrolytes.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
产品关联
DOI
高影响因子
POLYMER
·
2023
·
IF 4.6
Ying Wei,Wei Chen,Xinyi Ge,Jiayi Liang,Zheng Xing,Qingguo Zhang,Zhong-Xia Wang
Ionogel electrolytes (IGEs) with chemical and thermal stability properties have attracted considerable attention for all-solid-state energy storage devices, particularly for high-performance supercapacitors (SCs). However, achieving high conductivity, flexibility, and toughness, as well as deformation and impact resistance in special cases, is challenging with the typical polymer based on ionic liquids (ILs). Here, an effective gelation strategy is proposed for the preparation of free-standing LiTFSI/[EMIM][TFSI]/PVDF-HFP ionogels (IGs) by double-additive induced physical cross-linking. The mechanical and electrochemical properties of the IGs can be synergistically optimized by the cross-linking and entanglement of LiTFSI and [EMIM][TFSI] with the PVDF-HFP network. The target IGs simultaneously exhibit excellent deformation capacity (over 50 %), high ionic conductivity (10.3 × 10 −3 S cm −1 at 25 °C), hardness (H: 728.6 kPa), and Young's modulus (E: 11.4 MPa), which can exhibit the specific capacitance of 274. 55 F g −1 , energy density of 38.13 Wh kg −1 and maximum power density of 2499.93 W kg −1 in the fabricated symmetric supercapacitor . The results will motivate us to further explore their applications for flexible electronic devices, wearable electronic skin, and flexible energy storage.
研究领域:
材料科学
·
电化学
·
高分子物理
·
能源存储
·
柔性电子学
·
纳米复合材料
✓ 已验证
DOI
高影响因子
Nature Communications
·
2026
·
IF 18.1
Dong Yangyang,Cai Dong,Ning Hongtian,Shu Meiling,Ni Haijin,Yang Shuo,Zhou Xuemei,Nie Huagui,Tu Haoran,Sun Chenghua,Han Songbai,Yang Zhi
Lithium||sulfur batteries promise high energy density but are plagued by sluggish polysulfide conversion under lean-electrolyte conditions. Here we show the formation of chiral LiPS-LiTFSI dimers, fundamentally reshaping the intrinsic chemistry of polysulfides. Building on this finding, we design biomimetic MOF catalysts (MOF-L-His-Cu) in which L-histidine-Cu centers selectively recognize the chiral dimers, accelerating sulfur redox via enzyme-like kinetics. Such MOF-L-His-Cu catalyst achieves 1.84-fold higher activity than its D-enantiomer, enabling lithium||sulfur pouch cells with specific energy of 408 Wh kg −1 (based on the mass of the whole pouch cell deducting the package) at high sulfur loading (12 mg cm −2 ) and low electrolyte/sulfur ratio (3 μL mg −1 ). Our findings suggest that chiral coordination could be a previously overlooked factor in lithium||sulfur chemistry. This insight may inform the design of selective electrocatalysts for next-generation energy storage, representing a potential step forward in the field.
✓ 已验证
DOI
PubMed
高影响因子
SOLAR ENERGY
·
2019
·
IF 4.674
Jinjun Zou,Jihuai Wu,Weihai Sun,Mingjing Zhang,Xiaobing Wang,Pengqiang Yuan,Qianjin Zhu,Jie Yin,Xuping Liu,Yuqian Yang
The performance and stability of perovskite solar cell (PSC) are inseparable from the quality of perovskite film, and the solvent engineering is being seemed as an effective strategy to enhance the properties of perovskite. Acetonitrile (ACN) is often used as a solvent to dissolve bis(trifluoromethane)sulfonimide lithium salt (LiTFSI), but ACN can corrode the perovskite film, which hinders the promotion of PSC efficiency and durability. Herein, a solvent engineering approach is implemented to search for suitable alternatives for ACN to abate the degradation of the perovskite films. The results demonstrate that isopropanol (IPA) with smaller polarity can effectively dissolve LiTFSI and slow down the degradation of the perovskite layer compared with ACN, which can result in the reduction of defects as well as the nonradiative recombination. Consequently, the devices using LiTFSI/IPA as additive achieve superior power conversion efficiencies (PCEs) with relatively less hysteresis effects and get a champion PCE of 19.43%, while the device using LiTFSI/ACN gets an inferior PCE of 17.12%.
研究领域:
材料科学
·
能源技术
✓ 已验证
产品关联
DOI
高影响因子
CERAMICS INTERNATIONAL
·
2025
·
IF 5.6
Tielin Wang,Lijie Zhai,Mengting Lv,Jiahao Ji,Tao Lin,Fang Lian,Nan Meng,Huiping Shao
With the rapid advancement of microelectronic devices, 3D printed batteries hold significant potential for development in the battery fields. In this study, the network-structured lithium iron phosphate (LFP) electrodes containing lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) were prepared by 3D gel printing (3DGP) technology and the effect of different LiTFSI content on 3D-printed LFP electrodes was investigated. With increasing the LiTFSI content from 0 to 10 wt%, the apparent viscosity of the 3D printing slurry showed a gradual increase. The printing slurry of 3 wt% LiTFSI showed an apparent viscosity of 9.43 Pa s at a shear rate of 129 s −1 with the 0.16 mm inner diameter printing needle and 0.60 MPa air pressure, and the 3 wt% LiTFSI electrode printed maintained the intact network structure and the printing lines were uniform. The LFP electrodes with LiTFSI contents of 0 wt%, 3 wt%, 6 wt% and 10 wt% showed respectively specific capacities of 147 mAh g −1 , 142 mAh g −1 , 139 mAh g −1 and 127 mAh g −1 at 0.1C. After 0.5C and 300 charge-discharge cycles, the specific capacities of the electrodes were respectively 108.6 mAh g −1 , 104.7 mAh g −1 , 101.6 mAh g −1 and 99 mAh g −1 , and the capacity retention are respectively 87 %, 85 %, 85 % and 88 %, which indicates that these electrodes are cyclically stable and provide some reference for printing composite electrodes.
研究领域:
材料科学
·
电池技术
✓ 已验证
产品关联
DOI
高影响因子
Nano Energy
·
2021
·
IF 17.881
Jiazheng Zhou,Xiao Xu,Biwen Duan,Huijue Wu,Jiangjian Shi,Yanhong Luo,Dongmei Li,Qingbo Meng
Alkali metal doping, typically Li + doping, is beneficial for CZTSSe solar cells. Herein, aiming at the low solubility of conventional LiF which is hard to directly introduce into the precursor solution , an organic lithium salt (LiTFSI, lithium bis(trifluoromethanesulfonyl)imide) has been introduced into fabricating CZTSSe solar cells for the first time. 13.2% PCE (power-conversion-efficiency) with 12.7% certified PCE has been achieved with relatively higher V OC and FF, which is the highest efficiency of lithium-doping/alloying devices so far. A comprehensive investigation on the influence of LiTFSI on the formation of precursor and selenized absorber films has been carried out. The existence forms of LiTFSI in different processes are revealed as well as the relevant mechanism. That is, during selenization, LiTFSI decomposes to LiF at early stage, then LiF combines with Se to afford the Li-Se liquid fluxing intermediate, which can facilitate the phase transition and crystal growth to give compact CZTSSe films with larger grains and less pinholes, thus leading to better surface morphology and electric properties of LiTFSI doped CZTSSe absorber films. Li + doping is thus found to enable reducing interfacial defects , improving band bending and lowering V OC deficit. This work provides an easy way to precisely modify Li + salt amount in the precursor solution and subsequent CZTSSe selenization process by using organic lithium salts for high quality CZTSSe crystals and high-performance devices.
研究领域:
材料科学
·
能源技术
✓ 已验证
DOI
高影响因子
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2020
·Vol. 167
·期 9
·090520
·
IF 3.721
Huiying Liang,Xiaoxi Zuo,Lengdan Zhang,Wenda Huang,Qiuyu Chen,Tianming Zhu,Jiansheng Liu,Junmin Nan
Developing a nonflammable electrolyte is an efficient strategy to eliminate fire hazards and improve battery safety. Electrolytes containing nonflammable phosphate solvents enhance battery safety to a certain extent, but their compatibility with electrodes remains an obstacle. Here, a nonflammable electrolyte based on carbonate solvent is designed to resolve this dilemma while guaranteeing battery performance. We demonstrate that a nonflammable electrolyte employing the popular film-forming solvent ethylene carbonate (EC) and 1,2-dimethoxyethane (DME) with 2.3 mol kg−1 lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) has excellent thermal stability owing to the unique solution molecule structure. What's more, the nonflammable electrolyte possesses excellent compatibility with both LiNi0.6Co0.2Mn0.2O2 and graphite electrode. The initial specific capacity and capacity retention rate of graphite/LiNi0.6Co0.2Mn0.2O2 punch cells employing this electrolyte are 169.3 mAh g−1 and 98.7% (after 50 cycles), respectively, which are comparable to those of cells employing traditional carbonate electrolytes. Besides, short-circuit test of the pouch cell suggests that the release of gases accompanied by decomposition of electrolyte under abuse conditions is effectively suppressed. All of these results show a promising prospect of this nonflammable electrolyte for application in high-safety Li-ion batteries.
研究领域:
材料科学
·
能源技术
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）