ADVANCED FUNCTIONAL MATERIALS
·
2022
·Vol. 32
·期 32
·2203336
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IF 19.924
Yuzhen Hu,Linge Li,Haifeng Tu,Xiaohong Yi,Jian Wang,Jingjing Xu,Wenbin Gong,Hongzhen Lin,Xiaodong Wu,Meinan Liu
Solid-state lithium-metal batteries attract great attention due to their high energy density and superior safety. However, the sluggish Li + kinetics of solid electrolyte and poor interface compatibility between electrolyte and lithium anode lead to unsatisfied performance at room temperature, which severely limit their practical application. Herein, a Janus quasi-solid electrolyte (JSE) design is reported, which modifies the Li + solvation environment in succinonitrile (SN) plastic crystal electrolyte and creates 1D Li + transportation channels. Density functional theory calculations and Raman results reveal that Li 1.3 Al 0.3 Ti 1.7 (PO 4 ) 3 changes the Li + solvation environment from SN units to aggregated ion pairs, which accelerates the diffusion rate of Li + . As a result, JSE presents excellent ionic conductivity (0.73 mS cm −1 ) and high lithium transference number (0.72). With this efficient JSE, Li symmetric cells deliver excellent cycle stability over 600 h with a low over potential of 60 mV. LiFePO 4 |JSE|Li solid-state battery delivers an impressive performance with a specific discharge capacity of 152 mAh g −1 after 100 cycles at room temperature under 0.5 C. Moreover, the corresponding pouch cell also shows outstanding performance (140 mAh g −1 under 0.5 C) and withstands abuse tests such as bending and cutting, demonstrating its superior safety for future utilization.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2024
·
IF 8.4
Lin-Pei Guo,Zhi-Yuan Guo,Jing Wang,Pan-Pan Zhang,Zhi-Hui Huang,Zhi-Yong Ji
Monovalent selective ion-exchange membranes have been widely used for lithium extraction from brine with a high Mg/Li ratio. However, extracting Li + directly from raw brine with high Na/Li ratio remains a significant challenge. This study introduces a flexible lithium selective composite membrane by incorporating lithium-ion conductor with a quaternized polymer. The lithium-ion conductor provides pathways for lithium transmission, while the quaternized polymer effectively hinders the leakage of impurity cations. As a result, with the applied voltage of 2.0 V, the membrane achieved a high Li + /Na + separation coefficient of 35.48 with a Li + flux of 8.33 × 10 −10 mol cm −2 s −1 in the simulated Yiliping brine, which are 56.3 and 2.8 times higher than that of commercial monovalent selective cation exchange membrane (CIMS). We proposed a lithium transport mechanism involving an adsorption-dehydration-diffusion process through the membrane. Theoretical calculations indicate that the combined effects of significant adsorption energy (−0.47 eV), low dehydration energy (515 kJ mol −1 ), and low diffusion barrier (0.37 eV) leads to the high selectivity for lithium. These findings provide promising prospects for the large-scale preparation of lithium ion-selective membranes, enabling the direct lithium extraction from raw brine.
研究领域:
材料科学
·
环境工程
✓ 已验证
产品关联
DOI
高影响因子
CHINESE JOURNAL OF POLYMER SCIENCE
·
2024
·Vol. 43
·期 1
·177-187
·
IF 4.1
Wu Hao-Min,Ma Wen-Can,Cai Yi-Feng,Huang Xin,Li Jun-Heng,Kai Xi,Zhang Qiu-Hong,Jia Xu-Dong
Solid-state electrolytes are considered to be the vital part of the next-generation solid-state batteries (SSBs), due to their high safety and long operation life span. However, the two major factors that impede the expected performance of batteries are: the easy formation of lithium dendrites due to the concentration gradient of anions, and the low ionic conductivity at room temperature, which prevents reaching ideal electrochemical performance. Single-ion quasi-solid-state electrolytes (SIQSSEs) could provide higher safety and energy density, owing to absence of anion concentration gradient and solvent, as well as good lithium-ion transport ability. The porous covalent organic frameworks (COFs) are beneficial for con-structing appropriate lithium-ion transport pathway, due to the ordered 1D channel. In addition, the boroxine COFs (COF-5) offers strong ability of withdrawing anion part of lithium salt. Last but not the least, boron atom could play the role of coordinate site due to its electron deficiency. These advantages afford an opportunity to obtain a SIQSSE with high ionic conductivity and high lithium transference number (LTN) simultaneously. The COF-5 based SIQSSEs delivered a high ionic conductivity of 6.3×10 −4 S·cm −1 , with a high LTN of 0.92 and a wide electrochemical stable window (ESW) of 4.7 V at room temperature. The LiFePO 4 (LFP)/Li cells, which was assembled with COF-5 based SIQSSE, exhibited outstanding long cycle stability, high initial capacity and favorable rate performance. The results indicated COFs could be an ideal material for single-ion solid-state electrolytes in next-generation batteries.
研究领域:
材料科学
·
能源存储
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Chaoyan Zhang,Zhen Jiang,Xueying Yang,Jingyi Liu,Jianjun Song,Chuan Shi,Peng Zhang,Jinbao Zhao
Lithium-conducting fillers play crucial roles in enhancing the ionic conductivity of solid polymer electrolytes (SPEs). By providing supplementary rapid Li+ transport channels, they substantially boost the practical viability of solid-state batteries. Nevertheless, the inherent incompatibility between polymers and inorganic fillers invariably leads to phase separation, which exacerbates the transport barrier for lithium through interfaces and impedes the full utilization of these swift channels. Herein, a novel “Rotaxane chemistry” has been employed to engineer stable lithium transport pathways at the Li7La3Zr2O12(LLZO)/PEO interface. This strategy confines PEO chains within molecular semicircles on the surface of modified filler, namely LLZO@Rotaxane, which loosens chain entanglement and breaks tight coordination of (EO)n–Li. This promotes Li spontaneous diffusion to and transport through the nano-confinement space in the interface as well as through the LLZO. Consequently, the proportion of lithium transported by LLZO and interface has surged from 28.4 % to 56.0 %, endowing the PEO-LLZO@Rotaxane with an outstanding ionic conductivity of 1.90 mS cm−1 at 60 °C and Li+ transference number of 0.74. Correspondingly, the batteries fabricated with PEO-LLZO@Rotaxane also manifest excellent cyclic and rate performance. Thus, this work offers novel insights into increasing the ionic conductivity by interface engineering.
研究领域:
材料科学
·
电化学
·
能源化学
·
高分子化学
·
固态电池
✓ 已验证
产品关联
DOI
高影响因子
ADVANCED MATERIALS
·
2025
·Vol. 37
·期 20
·2418720
·
IF 26.8
Jianhui Liu,Lina Wang,Yong Cheng,Minyi Huang,Longze Zhao,Chenxi Zheng,Wangqin Li,Haowen Gao,Zhao Li,Zhenhai Wen,Guangfu Luo,Zhengliang Gong,Yong Yang,Ming-Sheng Wang
Solid-state lithium metal batteries (SSLMBs) are now under intensive research for their high energy density and excellent safety. However, the Li transport limitation in Li metal anode (LMA) leads to mass/stress accumulation, dendrite initiation and void formation at the interface, which seriously hinders the development of SSLMBs. Herein, it is demonstrated through in situ electron microscopies that a mixed ionic-electronic conducting (MIEC) 3D host can promote the Li transport in LMA by increasing the diffusion pathways along the carbonaceous framework, carbon/Li interface and Li metal surface, enabling a fast and long-distance (nearly 100 µm) diffusion of Li atoms in LMA. Consequently, the spatio-temporal sequence of Li plating/stripping can be fundamentally changed. Specifically, both deposition and dissolution can occur far away from the interface, thereby mitigating the dendrite and void issues. Impressively, the resulting cells with carbonaceous hosts can achieve excellent cyclability and the highest capacity (28.8 mAh cm −2 ) so far. This work provides valuable insight for understanding Li transport and deposition/dissolution mechanisms in MIEC host-based LMAs, and a feasible solution for tackling the interface issues without involving stack pressure in SSLMBs.
研究领域:
材料科学
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储能技术
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电化学
·
纳米科技
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）