ADVANCED MATERIALS
·
2021
·Vol. 33
·期 32
·2100921
·
IF 30.849
Pushun Lu,Lilu Liu,Shuo Wang,Jieru Xu,Jian Peng,Wenlin Yan,Qiuchen Wang,Hong Li,Liquan Chen,Fan Wu
Sulfide solid electrolytes (SEs) are recognized as one of the most promising candidates for all-solid-state batteries (ASSBs), due to their superior ionic conductivity and remarkable ductility. However, poor air stability, complex synthesis process, low yield, and high production cost obstruct the large-scale application of sulfide SEs. Herein, a one-step gas-phase synthesis method for sulfide SEs with oxide raw materials in ambient air, completely getting rid of the glovebox and thus making large-scale production possible, is reported. By adjusting substituted elements and concentrations, the ionic conductivity of Li 4- x Sn 1- x M x S 4 can reach 2.45 mS cm −1 , which represents the highest value among all reported moist-air-stable and recoverable lithium-ion sulfide SEs reported. Furthermore, ASSBs with air/water-exposed and moderate-temperature-treated Li 3.875 Sn 0.875 As 0.125 S 4 even maintains superior performances with the highest reversible capacity (188.4 mAh g −1 ) and the longest cycle life (210 cycles), which also breaks the record. Therefore, it may become one of the most critical breakthroughs during the development of sulfide ASSBs toward its practical application and commercialization.
研究领域:
材料科学
·
电化学
·
电池技术
✓ 已验证
DOI
高影响因子
Nature Communications
·
2022
·Vol. 13
·期 1
·1-9
·
IF 17.694
Cheng Zhu,Pan Hui,Li Fan,Duan Chun,Liu Hang,Zhong Hanyun,Sheng Chuanchao,Hou Guangjin,He Ping,Zhou Haoshen
Rechargeable Li-I 2 battery has attracted considerable attentions due to its high theoretical capacity, low cost and environment-friendliness. Dissolution of polyiodides are required to facilitate the electrochemical redox reaction of the I 2 cathode, which would lead to a harmful shuttle effect. All-solid-state Li-I 2 battery totally avoids the polyiodides shuttle in a liquid system. However, the insoluble discharge product at the conventional solid interface results in a sluggish electrochemical reaction and poor rechargeability. In this work, by adopting a well-designed hybrid electrolyte composed of a dispersion layer and a blocking layer, we successfully promote a new polyiodides chemistry and localize the polyiodides dissolution within a limited space near the cathode. Owing to this confined dissolution strategy, a rechargeable and highly reversible all-solid-state Li-I 2 battery is demonstrated and shows a long-term life of over 9000 cycles at 1C with a capacity retention of 84.1%.
研究领域:
材料科学
·
能源存储与转换
✓ 已验证
DOI
高影响因子
Journal of Materials Chemistry A
·
2021
·Vol. 9
·期 15
·9581-9585
·
IF 12.732
Yuemin Du,Yijie Liu,Sixie Yang,Chao Li,Zhu Cheng,Feilong Qiu,Ping He,Haoshen Zhou
The fossil fuel crisis and global warming are becoming more and more severe in this century, while the exploration of human survival on Mars is being pushed forward steadily. Hence, it is meaningful to effectively utilize CO2, the main greenhouse gas and a major component of the Martian atmosphere. Due to their high capacity and ability to capture CO2, Li–CO2 batteries have received much attention. However, there are problems that still need to be solved relating to Li–CO2 batteries, including the instability of the electrolyte and the non-negligible polarization caused by the formation and decomposition of Li2CO3. To address these issues, an all-solid-state Li–CO2 battery, which uses RuO2 nanoparticles combined with single-walled carbon nanotubes (SWCNTs) as the cathode material and a sodium super ionic conductor (NASICON)-type ceramic solid electrolyte, Li1.5Al0.5Ge1.5(PO4)3 (LAGP), has been developed and it operates over a broad temperature range. Under a pure CO2 atmosphere, this well-designed battery shows a discharge capacity of 2499 mA h g−1 and a charge capacity of 2137 mA h g−1 in the first cycle at 60 °C, and stable cycling performance over 30 cycles under a capacity limitation of 500 mA h g−1 at a current density of 50 mA g−1. This result enhances the possibility of the utilization of the Li–CO2 battery in the future.
研究领域:
材料科学
·
能源技术
·
催化化学
✓ 已验证
DOI
高影响因子
Journal of Materials Chemistry A
·
2024
·Vol. 12
·期 10
·6038-6049
·
IF 10.7
Yaqi Hu,Zongliang Zhang,Siliang Liu,Fangbo He,Yang Liu,Zhi Zhuang,Fangyang Liu
High-capacity lithium-rich sulfide cathodes with superior conductivity over S or Li2S materials are considered for all-solid-state lithium-ion batteries (ASSLBs), yet their capacity and rate performance require further improvement. In this work, lithium-rich sulfide cathodes Li2Ti1−xSixS3 with a disordered rocksalt structure and layered structure are synthesized by high-energy ball milling and high-temperature annealing, respectively. The Si doping strategy is implemented to tune the microstructure of the lithium-rich sulfide cathode and to obtain high capacity and improved ionic conductivity. The partial replacement of Ti with Si increases the cationic disorder of rocksalt and layered Li2Ti1−xSixS3, which further activates the anionic redox activity to enable a higher capacity than Li2TiS3. Moreover, the robust Si–S bonds induce distortions in the LiS6 octahedral and adjacent tetrahedral vacancies, broadening the Li+ migration channels in the Li+ percolation network and enabling rapid Li+ migration capability. The optimized rocksalt Li2Ti1−xSixS3 exhibits a higher specific capacity of 361 mA h g−1 than rocksalt Li2TiS3 (295 mA h g−1) at 0.3 C (120 mA g−1), while the layered Li2Ti1−xSixS3 has a higher capacity of 260 mA h g−1 than the layered Li2TiS3 (140 mA h g−1) at 0.3 C. An argyrodite-type sulfide solid-state electrolyte Li5.25PS4.25ClBr0.75 with high Li+ conductivity (7.64 mS cm−1) is designed to match with the rocksalt Li2Ti1−xSixS3 cathode, and the assembled ASSLB achieves a high areal capacity density of 9.79 mA h cm−2. The Si doping to tune the disordered structure provides an effective improvement approach for high-capacity rocksalt or layered sulfide cathodes and high-energy density ASSLBs.
研究领域:
材料科学
·
能源技术
✓ 已验证
DOI
高影响因子
Journal of Energy Chemistry
·
2020
·
IF 7.216
Bohao Zhang,Yulong Liu,Jia Liu,Liqun Sun,Lina Cong,Fang Fu,Alain Mauger,Christian M. Julien,Haiming Xie,Xiumei Pan
Inspired by the concept of “polymer-in-ceramic”, a composite poly(Ɛ-caprolactone) (PCL)/ceramic containing LiTFSI is prepared and investigated as a solid electrolyte for all-solid-state batteries . The composite with the optimum concentration of 45 wt% LiTFSI and 75 wt% Li 1.5 Al 0.5 Ge 1.5 (PO 4 ) 3 (LAGP, NASICON-type structure) exhibits a high ionic conductivity (σ i = 0.17 mS cm −1 ) at 30 °C, a transference number of 0.30, and is stable up to 5.0 V. The composite electrolyte is a flexible and self-standing membrane. Solid-state LiFePO 4 //Li batteries with this composite electrolyte demonstrate excellent cycling stability with high discharge capacity of 157 mA h g − 1 , high capacity retention of 96% and coulombic efficiency of 98.5% after 130 cycles at 30 °C and 0.1 C rate. These electrochemical properties are better than other PCL-based all-solid-lithium batteries, and validate the concept of “polymer-in-ceramic” by avoiding the drawback of lower conductivity in prior “polymer-in-ceramic” electrolyte at high concentration of the ceramic.
研究领域:
材料科学
·
能源存储技术
✓ 已验证
产品关联
DOI
高影响因子
Polymers
·
2020
·Vol. 12
·期 9
·1886
·
IF 3.426
Yaolong He,Shufeng Li,Sihao Zhou,Hongjiu Hu
Ensuring the material durability of an electrolyte is a prerequisite for the long-term service of all-solid-state batteries (ASSBs). Herein, to investigate the mechanical integrity of a solid polymer electrolyte (SPE) in an ASSB upon electrochemical operation, we have implemented a sequence of quasi-static uniaxial tension and stress relaxation tests on a lithium perchlorate-doped poly (vinyl alcohol) electrolyte, and then discussed the viscoelastic behavior as well as the strength of SPE film during the physical aging process. On this basis, a continuum electrochemical-mechanical model is established to evaluate the stress evolution and mechanical detriment of aging electrolytes in an ASSB at a discharge state. It is found that the measured elastic modulus, yield stress, and characteristic relaxation time boost with the prolonged aging time. Meanwhile, the shape factor for the classical time-decay equation and the tensile rupture strength are independent of the aging history. Accordingly, the momentary relaxation modulus can be predicted in terms of the time–aging time superposition principle. Furthermore, the peak tensile stress in SPE film for the full discharged ASSB will significantly increase as the aging proceeds due to the stiffening of the electrolyte composite. It may result in the structure failure of the cell system. However, this negative effect can be suppressed by the suggested method, which is given by a 2D map under different lithiation rates and relative thicknesses of the electrolyte. These findings can advance the knowledge of SPE degradation and provide insights into reliable all-solid-state electrochemical device applications.Keywords:solid polymer electrolyte;physical aging;viscoelastic;mechanical integrity;all-solid-state battery
研究领域:
材料科学
·
电化学
·
电池技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
NATURE
·
2023
·Vol. 616
·期 7955
·77-83
·
IF 64.8
Yin Yi-Chen,Yang Jing-Tian,Luo Jin-Da,Lu Gong-Xun,Huang Zhongyuan,Wang Jian-Ping,Li Pai,Li Feng,Wu Ye-Chao,Tian Te,Meng Yu-Feng,Mo Hong-Sheng,Song Yong-Hui,Yang Jun-Nan,Feng Li-Zhe,Ma Tao,Wen Wen,Gong Ke,Wang Lin-Jun,Ju Huan-Xin,Xiao Yinguo,Li Zhenyu,Tao Xinyong,Yao Hong-Bin
Inorganic superionic conductors possess high ionic conductivity and excellent thermal stability but their poor interfacial compatibility with lithium metal electrodes precludes application in all-solid-state lithium metal batteries 1 , 2 . Here we report a LaCl 3 -based lithium superionic conductor possessing excellent interfacial compatibility with lithium metal electrodes. In contrast to a Li 3 MCl 6 (M = Y, In, Sc and Ho) electrolyte lattice 3 , 4 , 5 , 6 , the UCl 3 -type LaCl 3 lattice has large, one-dimensional channels for rapid Li + conduction, interconnected by La vacancies via Ta doping and resulting in a three-dimensional Li + migration network. The optimized Li 0.388 Ta 0.238 La 0.475 Cl 3 electrolyte exhibits Li + conductivity of 3.02 mS cm −1 at 30 °C and a low activation energy of 0.197 eV. It also generates a gradient interfacial passivation layer to stabilize the Li metal electrode for long-term cycling of a Li–Li symmetric cell (1 mAh cm −2 ) for more than 5,000 h. When directly coupled with an uncoated LiNi 0.5 Co 0.2 Mn 0.3 O 2 cathode and bare Li metal anode, the Li 0.388 Ta 0.238 La 0.475 Cl 3 electrolyte enables a solid battery to run for more than 100 cycles with a cutoff voltage of 4.35 V and areal capacity of more than 1 mAh cm −2 . We also demonstrate rapid Li + conduction in lanthanide metal chlorides (LnCl 3 ; Ln = La, Ce, Nd, Sm and Gd), suggesting that the LnCl 3 solid electrolyte system could provide further developments in conductivity and utility.
研究领域:
材料科学
·
能源存储与转换
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Applied Energy Materials
·
2023
·
IF 6.4
Dongcan Zhang,Peilun Yu,Yuanbo Zhang,Xudong Zhao,Jie Yu
Substituting Li metal with silicon (Si) as the anode, owing to its high capacity, presents significant promise in polymer-based all-solid-state batteries (ASSBs) for mitigating lithium dendrite formation. However, Si anodes suffer from poor conductivity, substantial volume expansion during cycling, and unfavorable interfacial stability with solid-state electrolytes, resulting in severe capacity degradation and rendering them unsuitable for direct application. Herein, we report that vertical graphene sheets are grown on Si nanoparticles (Si@VG) by thermal chemical vapor deposition for the operation of polymer-based ASSBs. Flexible vertical graphene sheets not only form a 3D conductive network to enhance the electrical connectivity of the whole electrode but also attain a better contact with the solid polymer electrolyte for reducing the interface impedance. As the anode for ASSBs, the reversible capacity of Si@VG remains 444.9 mAh g–1 after 200 cycles at 0.5 A g–1, which exhibits significant improvement relative to Si. In addition, it can be observed from electrochemical impedance spectroscopy that the interfacial impedance between the anode and the solid polymer electrolyte significantly decreases. This study can provide valuable insights for other research endeavors aimed at addressing the interfacial challenges in ASSBs.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Materials Research and Technology-JMR&T
·
2023
·
IF 6.4
Wensheng Yang,Yue Gao,Quan Xie,Tinghong Gao,Yongchao Liang,Qian Chen,Zean Tian,Yunjun Ruan
The Ti substrate, with physicochemical stability and excellent electrical conductivity, is potential to fabricate all-solid-state batteries. However, the Titanium atoms at high-temperature synthesis makes it easy to react with active materials. Modifying the titanium surface with an inert protective layer while ensuring high electrical conductivity remains a significant challenge. Herein, a pencil was used to draw on the Ti substrate and subsequently sintering at a high temperature to obtain a graphite-coated Ti substrate (Ti-Graphite). The experimental results show that Ti-Graphite has a smoother surface and fewer defects in the graphite layer. Moreover, titanium carbide is formed at the interface of graphite and Ti substrate, which will enhance the physicochemical stability of the Ti-Graphite. To gain deep understanding of the evolution mechanism in the synthesis, molecular dynamics simulations were carried out to investigate it. The results exhibit that the voids at the C/Ti interface and stress in the model were significantly decreased after sintering and cooling treatment, proving that Ti-Graphite has a smoother surface, a more stable interface, and fewer defects at the atomic scale. Therefore, we provide a simple and facile strategy to obtain a Ti-graphite substrate with superior physicochemical stability, which reaveals excellent potential to synthesize high-performance all-solid-state batteries.
研究领域:
材料科学
·
电化学
·
计算模拟
✓ 已验证
DOI
高影响因子
Materials
·
2020
·Vol. 13
·期 7
·1719
·
IF 3.057
Qinghui Li,Chang Xu,Bing Huang,Xin Yin
NASICON-type solid electrolytes with excellent stability in moisture are promising in all-solid-state batteries and redox flow batteries. However, NASIOCN LiZr2(PO4)3(LZP), which is more stable with lithium metal than the commercial Li1.3Al0.3Ti1.7(PO4)3, exhibits a low Li-ion conductivity of 10−6S cm−1because the fast conducting rhombohedral phase only exists above 50 °C. In this paper, the high-ionic conductive rhombohedral phase is stabilized by Y3+doping at room temperature, and the hot-pressing technique is employed to further improve the density of the pellet. The dense Li1.1Y0.1Zr1.9(PO4)3pellet prepared by hot-pressing shows a high Li-ion conductivity of 9 × 10−5S cm−1, which is two orders of magnitude higher than that of LiZr2(PO4)3. The in-situ formed Li3P layer on the surface of Li1.1Y0.1Zr1.9(PO4)3after contact with the lithium metal increases the wettability of the pellet by the metallic lithium anode. Moreover, the Li1.1Y0.1Zr1.9(PO4)3pellet shows a relatively small interfacial resistance in symmetric Li/Li and all-solid-state Li-metal cells, providing these cells a small overpotential and a long cycling life.Keywords:NASICON;hot pressing;interfacial resistance;Li-ion conductivity;all-solid-state batteries
研究领域:
材料科学
·
能源存储与转换
✓ 已验证
DOI
PubMed
高影响因子
ELECTROCHEMISTRY COMMUNICATIONS
·
2022
·
IF 5.443
Yue Wu,Xiaolin Sun,Ru Li,Cheng Wang,Depeng Song,Zewen Yang,Jing Gao,Yuan Zhang,Takeo Ohsaka,Futoshi Matsumoto,Fuhua Zhao,Jianfei Wu
Sulfide solid electrolytes (SSE) are considered promising alternatives to conventional liquid electrolytes due to their high safety that is inaccessible to common liquid electrolytes and favorable ionic conductivity. Nonetheless, the poor interfacial contacts and stability between SSEs and Li anode, as well as the inhomogeneous dendrite growth severely limit their practical applications. Herein, a trinity artificial solid electrolyte interphase composed of ethyl cellulose, graphene oxide and phosphoric acid was in-situ fabricated on the surface of the Li anode. This Li anode is denoted as EGPL (ethyl-cellulose-graphene-oxide-phosphoric-acid-modified-lithium). The artificial interphase can effectively benefit the uniform deposition of lithium, promote the transport of lithium ions and improve interfacial stability. Therefore, the all-solid-state batteries incorporated with EGPL anode and LiCoO 2 cathode can maintain 94.6% of initial capacity over 100 cycles at 0.2C, and also deliver excellent rate performance. This work provides a novel approach for the interfacial modification of lithium anodes for applications in all-solid-state batteries.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
Small
·
2024
·
IF 13
Feng Sun,Zhihui Ma,Shenghai Xin,Yidi Fu,Ping Li,Jianbin Li,Qi Wan,Xuanhui Qu
Silicon (Si) anode is a promising anode material for all-solid-state lithium batteries with ultra-high theoretical specific capacity and low lithium dendrite risk. However, the inevitable vast volume expansion of Si anode during charge/discharge is recognized as a major limitation preventing its commercial application. Herein, an N, S self-doped amorphous carbon layer coated on porous micron-sized Si (p-mSi@C) is designed to construct an electron/ion conducting network while ensuring structural and interfacial stability. Uneven distribution of von mises stresses during p-mSi lithiation leads to irregular volume expansion and even fragmentation. Meanwhile, the growth of by-products at the interface between p-mSi and electrolyte contact leads to a rapid capacity decay. Compared to p-mSi anode, p-mSi@C reduces the risk of fragmentation thanks to the stress-absorbing effect of amorphous carbon, delivering excellent electrochemical performance (2679.65 mAh g −1 at 0.2 mA cm −2 with initial coulombic efficiency of 84%). More importantly, the chemical failure mechanisms of p-mSi and p-mSi@C composite anodes are revealed through structural characterization, chemical analysis, and simulation, which provides the necessary theoretical guidance for practicalization.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 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）