Journal of Energy Chemistry
·
2022
·
IF 13.599
Xi Wang,Yong Wang,Yiyu Wu,Yunmiao Fan,Yang Tian
Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 (LLZTO) solid garnet-type electrolyte has been widely reported due to its outstanding safety and electrochemical stability. However, the inherent rigidity and brittleness of LLZTO lead to poor contact with anode/cathode and the operation failure of full cells. Herein, the dual-interlayers are constructed as the fast interfacial ion-migration channel by using Ti 3 C 2 T x (MXene, T x is –O, –OH, –F) with trace ionic liquid (IL), which promote the intimate contact between LLZTO and anode/cathode and suppress Li-dendrites growth. Notably, IL can wet the cathode to promote intimate interface contact and be decomposed into some inorganic compounds (such as Li 3 N, LiF, and Li 2 S x ), resulting in reduced interfacial resistance and fast Li-ion transportation. Consequently, in the prepared Li-symmetric cell, the interfacial resistance on the anode side plunges to 33.1 Ω cm −2 , and stably maintains over 1000 h without short circuit at 0.05 mA cm −2 . The full cell of Li|LiFePO 4 delivers a high initial capacity of 158.52 mA h g −1 and outstanding retention of 90.18% after 100 cycles at 60 °C and 0.2 C. Our work provides an efficient strategy to design dual-interlayers between LLZTO and anode/cathode for the interfacial modification to enhance the performance of solid garnet batteries.
研究领域:
材料科学
·
电化学
·
固态电池
·
界面工程
·
能源材料
✓ 已验证
DOI
高影响因子
JOURNAL OF POWER SOURCES
·
2018
·
IF 6.945
Jing Gao,Chunshui Sun,Lei Xu,Jian Chen,Chong Wang,Decai Guo,Hao Chen
Due to flexible property and light weight, the lithiated Nafion membrane swollen with PC (PC-Li-Nafion) has been employed as both solid-state electrolyte and separator to fabricate solid-state Li-S cells. The electrochemical measurements of PC-Li-Nafion membrane show that its Li-ion transference number is 0.928, ionic conductivity of 2.1 × 10 −4 S cm −1 can be achieved at 70 °C and its electrochemical window is 0 ∼ +4.1 V vs. Li + /Li. It is observed that the Li dendrites are suppressed by using PC-Li-Nafion membrane due to its single-ion conducting property. The amounts of Li-Nafion resin binder and conductive carbon in the cathode are optimized as 40% and 10% respectively to make a balance of ionic and electronic conductivities . A thin-layer Li-Nafion resin with a thickness of around 2 μm is fabricated between the cathode and PC-Li-Nafion membrane to improve the interfacial contact and further enhance the specific capacity of the cell. When measured at 70 °C, the Li-S cell delivers a reversible specific capacity of 1072.8 mAh g −1 (S) at 0.05 C and 895 mAh g −1 (S) at 1 C. The capacity retention at 1 C is 89% after 100 cycles. These results suggest that high-performance solid-state Li-S cells can be fabricated with the Li-Nafion polymer electrolyte .
研究领域:
电化学
·
能源材料
·
固态电池
·
聚合物电解质
·
锂离子电池
·
电极界面工程
·
储能技术
✓ 已验证
DOI
高影响因子
SOLID STATE IONICS
·
2019
·
IF 2.886
Fan Deng,Yongmin Wu,Weiping Tang,Shufeng Song,Zhaoyin Wen,Masashi Kotobuki,Li Lu,Jianyao Yao,Ning Hu,Janina Molenda
The use of garnet-type conductors as electrolytes for safe lithium solid-state batteries is impeded by the lack of critical processing strategy to stabilize and densify the cubic lithium garnets. The synthesis and processing of dense cubic lithium garnets are typically depending on solid state reaction as a result of unintentional Al contamination from the alumina crucibles at temperatures up to 1230 °C. High Al concentration is also believed to induce the sluggish migration of lithium ions . Here, we demonstrate an ultrathin, conformal γ-Al 2 O 3 surface coating on garnet solids by a hybrid microemulsion solid-state method for accomplishing rational and controllable synthesis and processing of dense cubic garnets with low Al concentration. The γ-Al 2 O 3 coating demonstrates fast-ion conducting Al-doped Li 6.75 La 3 Zr 1.75 Ta 0.25 O 12 phase with low Al concentration (~0.17 mol per formula unit), low tetragonal-to-cubic phase transformation temperature of 500 °C, and total conductivity of ~4.4 × 10 − 4 S cm − 1 . Specifically, the desired microstructures of the sintered pellets with uniform grains are revealed. As a proof-of-concept, we demonstrate that the nanoscale γ-Al 2 O 3 modification garnet conductor Li 6.75 La 3 Zr 1.75 Ta 0.25 O 12 is available to suppress lithium dendrites in symmetric Li/γ-Al 2 O 3 coating Li 6.75 La 3 Zr 1.75 Ta 0.25 O 12 /Li cells during lithium plating/stripping at room temperature, with current densities of 0.026 to 0.5 mA cm − 2 . The Li/γ-Al 2 O 3 coating Li 6.75 La 3 Zr 1.75 Ta 0.25 O 12 /LiNi 0.5 Co 0.2 Mn 0.3 O 2 cell delivered a high initial discharge capacity of ~164.2 mAh g − 1 , more importantly, an outstanding cycling performance with a capacity retention of 90.16% after 30 cycles at 0.1C and room temperature. This new synthesis route and the utilization of nanoscale γ-Al 2 O 3 surface modification could open up new avenue to lithium garnet conductors with reliable synthesis for all-solid-state lithium batteries application.
研究领域:
材料科学
·
电化学
·
固态离子学
·
能源存储
·
纳米材料
·
电池技术
✓ 已验证
DOI
高影响因子
Journal of Energy Chemistry
·
2020
·
IF 7.216
Jingguang Yi,Dan Zhou,Yuhao Liang,Hong Liu,Haifang Ni,Li-Zhen Fan
All-solid-state lithium batteries (ASSLBs) employing sulfide electrolyte and lithium (Li) anode have received increasing attention due to the intrinsic safety and high energy density. However, the thick electrolyte layer and lithium dendrites formed at the electrolyte/Li anode interface hinder the realization of high-performance ASSLBs . Herein, a novel membrane consisting of Li 6 PS 5 Cl (LPSCl), poly(ethylene oxide) (PEO) and Li-salt (LiTFSI) was prepared as sulfide-based composite solid electrolyte (LPSCl-PEO3-LiTFSI) (LPSCl:PEO = 97:3 wt/wt; EO:Li = 8:1 mol/mol), which delivers high ionic conductivity (1.1 × 10 −3 S cm −1 ) and wide electrochemical window (4.9 V vs. Li + /Li) at 25 °C. In addition, an ex-situ artificial solid electrolyte interphase (SEI) film enriched with LiF and Li 3 N was designed as a protective layer on Li anode (Li(SEI)) to suppress the growth of lithium dendrites. Benefiting from the synergy of sulfide-based composite solid electrolyte and ex-situ artificial SEI, cells of S-CNTs/LPSCl-PEO3-LiTFSI/Li(SEI) and Al 2 O 3 @LiNi 0.5 Co 0.3 Mn 0.2 O 2 /LPSCl-PEO3-LiTFSI/Li(SEI) are assembled and both exhibit high initial discharge capacity of 1221.1 mAh g −1 (135.8 mAh g −1 ) and enhanced cycling stability with 81.6% capacity retention over 200 cycles at 0.05 C (89.2% over 100 cycles at 0.1 C). This work provides a new insight into the synergy of composite solid electrolyte and artificial SEI for achieving high-performance ASSLBs .
研究领域:
材料科学
·
电化学
·
能源存储
·
固态电池
·
界面工程
✓ 已验证
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2023
·
IF 6.2
Yanhua Zhang,Yuhang Mei,Xinglong Gao,Yumei Xiao,Zijun Tang,Xing Xiang,Jiadong Deng
The lithium dendrite problem of Li 7 La 3 Zr 1.4 Ta 0.6 O 12 (LLZTO) solid electrolyte restricts the practical application and development of all-solid-state lithium batteries (ASSLBs). Herein, a LiPON interlayer with Li + conductive and electron non-conductive dynamic properties is constructed at the Li/LLZTO interface. Results show that the electronic conductivity of solid electrolyte after LiPON modification decreased by nearly three orders of magnitude, indicating that it has good ability to hinder electron conduction . The interlayer enhances the wettability between the Li metal anode and LLZTO, resulting in a decrease of battery resistance from 3400 Ω to 700 Ω. The critical current density of the ASSLBs increase from 0.1 mA cm −2 to 1.2 mA cm −2 at room temperature, and the battery cycle number increase from 31 h to over 1000 h. XPS deep etching results show that the LiPON/LLZTO interface has good electrochemical stability. The Kelvin probe force microscope displays a sharp increase in potential within the LiPON interlayer, indicating its successful hindrance of electron conduction to the solid electrolyte. The effective inhibition of lithium dendrites growth is due to LiPON can promote the Li + transmission from LLZTO solid electrolyte to Li anode, and also hinder the electron conduction to LLZTO to form lithium dendrites.
研究领域:
材料科学
·
电化学
·
能源存储
·
固态电池
·
界面工程
✓ 已验证
DOI
高影响因子
Nano Energy
·
2016
·
IF 11.553
Jingxian Zhang,Ning Zhao,Miao Zhang,Yiqiu Li,Paul K. Chu,Xiangxin Guo,Zengfeng Di,Xi Wang,Hong Li
Solid-state electrolytes with high ionic conductivity , large electrochemical window, good mechanical properties , and easy processability are needed for high-energy solid-state lithium batteries . In this work, composite membranes consisting of lithium garnet (i.e. Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 , LLZTO) particles and Li-salt-free polyethylene oxides (PEOs) are produced as solid-state electrolytes. Li-ion-conducting particles in nano-scale are crucial for the enhancement of conductivity and the membranes containing ~40 nm LLZTO particles exhibit conductivities nearly two orders of magnitude larger than those with the micro-scale ones, which is attributed to the difference in specific surface area related to the percolation effect. Compared to the conventional PEO doped with lithium salt, the insulating PEO in PEO:LLZTO membrane electrolyte is conducive to the suppression of lithium dendrite growth owing to prohibition of current flow. With PEO:LLZTO membrane electrolytes in conductivity of 2.1×10 −4 S cm −1 at 30 °C and 5.6×10 −4 S cm −1 at 60 °C, the solid-state LiFePO 4 /PEO:LLZTO/Li and LiFe 0.15 Mn 0.85 PO 4 /PEO:LLZTO/Li cells deliver energy densities of 345 Wh kg −1 (662 Wh L −1 ) and 405 Wh kg −1 (700 Wh L −1 ) (without the package weight or volume) with good rate capability and cycling performance. This study suggests that the conjunction of nano-scale Li-ion-conducting particles and an insulating polymer provides a promising solution to produce powerful solid-state electrolytes for high-performance solid-state lithium batteries .
研究领域:
材料科学
·
电化学
·
能源存储
·
高分子科学
·
固态电池技术
✓ 已验证
DOI
高影响因子
Small
·
2018
·Vol. 14
·期 31
·1801420
·
IF 9.598
Kuirong Deng,Jiaxiang Qin,Shuanjin Wang,Shan Ren,Dongmei Han,Min Xiao,Yuezhong Meng
A novel single-ion conducting polymer electrolyte (SIPE) membrane with high lithium-ion transference number, good mechanical strength, and excellent ionic conductivity is designed and synthesized by facile coupling of lithium bis(allylmalonato) borate (LiBAMB), pentaerythritol tetrakis (2-mercaptoacetate) (PETMP) and 3,6-dioxa-1,8-octanedithiol (DODT) in an electrospun poly(vinylidienefluoride) (PVDF) supporting membrane via a one-step photoinitiated in situ thiol–ene click reaction. The structure-optimized LiBAMB-PETMP-DODT (LPD)@PVDF SIPE shows an outstanding ionic conductivity of 1.32 × 10 −3 S cm −1 at 25 °C, together with a high lithium-ion transference number of 0.92 and wide electrochemical window up to 6.0 V. The SIPE exhibits high tensile strength of 7.2 MPa and elongation at break of 269%. Due to these superior performances, the SIPE can suppress lithium dendrite growth, which is confirmed by galvanostatic Li plating/stripping cycling test and analysis of morphology of Li metal electrode surface after cycling test. Li|LPD@PVDF|Li symmetric cell maintains an extremely stable and low overpotential without short circuiting over the 1050 h cycle. The Li|LPD@PVDF|LiFePO 4 cell shows excellent rate capacity and outstanding cycle performance compared to cells based on a conventional liquid electrolyte (LE) with Celgard separator. The facile approach of the SIPE provides an effective and promising electrolyte for safe, long-life, and high-rate lithium metal batteries.
研究领域:
材料科学
·
电化学
·
能源存储
·
高分子化学
·
电池技术
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
XinLong Zhang,HaiYan Zhang,Yuan Geng,ZhangQin Shi,Sheng Zhu,QunJie Xu,YuLin Min
Lithium–sulfur (Li–S) batteries are considered as very promising energy storage systems due to their higher theoretical performance and lower active material cost. However, the notorious shuttle effect and lithium dendrite growth have severely restricted the industrial production of Li–S batteries. In this study, we used polyethylene oxide (PEO) as the matrix and added multifunctional nanofillers (nano In 2 O 3 ) to effectively inhibit the shuttle effect caused by the dissolution of lithium polysulphides (LiPSs) in Li–S batteries. As a multifunctional filler, nano-In 2 O 3 not only improves the ionic conductivity of the PEO electrolyte, but also forms a Li–In alloy layer in situ at the polymer/anode interface, which can cause the rapid diffusion of lithium ions and prevent the side reactions between lithium metal anode and the electrolyte. Achieving the effect of stabilizing the lithium metal anode and suppressing the shuttle effect. Multiple problems in the system are solved by introducing a single component with multiple functions. The symmetrical lithium battery based on the PEO/LiTFSI/In 2 O 3 solid polymer electrolyte (PEO/LiTFSI/In 2 O 3 SPE) has higher cycle stability (over 1200 h) because it is more stable to the lithium metal anode. The Li–S full battery also exhibits excellent electrochemical performance. After 500 cycles at 1C, its capacity can be maintained at 570 mAh g −1 , the capacity decay rate is 0.038%. The coulombic efficiency (CE) during the cycle is also close 100%.
研究领域:
电化学
·
能源材料
·
固态离子学
·
电池技术
·
纳米复合材料
✓ 已验证
DOI
高影响因子
JOURNAL OF POWER SOURCES
·
2022
·
IF 9.794
Yuanyuan Li,Jun Cheng,Jianwei Li,Zhen Zeng,Yixuan Guo,Hongqiang Zhang,Hongbin Liu,Xiao Xu,Yiwei Rao,Deping Li,Lijie Ci
Sulfide solid state electrolytes capture much attention owing to their high conductivity and decent mechanical property. Nevertheless, the moisture instability and poor interfacial compatibility against lithium metal anode remain challenging and hinder the practical application. Herein, we report a novel indium (In) doping strategy based on the hard-soft-acid-base theory to tackle these issues. Optimized Li 7 P 2.9 S 10.9 In 0.1 electrolyte exhibits a high ionic conductivity of 4.1 × 10 −3 S cm −1 and achieves an enhanced interfacial compatibility. Importantly, as In partially replaces the phosphorus (P), the amount of released hydrogen sulfide can be significantly decreased and the air stability is improved. The all-solid-state battery assembled with the Li 7 P 2.9 S 10.9 In 0.1 electrolyte demonstrates a high discharge capacity and a good cycling stability under a high current density of 1.0 C. This work provides a practical and effective method to design sulfide-based solid-state electrolyte with high ionic conductivity and enhanced air stability for all-solid-state battery applications.
研究领域:
材料科学
·
电化学
·
能源存储
·
固态离子学
·
电池技术
✓ 已验证
DOI
高影响因子
ELECTROCHIMICA ACTA
·
2020
·
IF 6.215
Shi Wang,Qingyuan Li,Minglei Bai,Jixin He,Chongyang Liu,Zengxi Li,Xiangfeng Liu,Wen-yong Lai,Liaoyun Zhang
Lithium-ion batteries (LIBs) using solid-state electrolytes (SSEs) can improve safety and energy density comparable with the liquid electrolytes (LE)-based counterparts. Especially, employing garnet-type SSEs to prepare solid-state LIBs are promising to achieve high-energy cells. However, the unbending and brittle issues of the inorganic SSE films are not suitable to fabricate flexible and stretchable energy storage devices. Here, We find that introducing specific polymer (30 wt%) into Li 6.75 La 3 Zr 1.75 Ta 0.25 O 12 (LLZTO) can strongly increase the strength of the composite polymer-in-inorganic electrolyte (CIE) film. Both in-situ and ex-situ characterizations demonstrate that CIE delivers an excellent ability to suppress the growth of Li dendrites due to the close packing of LLZTO and effective filled grain boundaries and voids inside the CIE film by the polymer. The CIE inherits impressive electrochemical performance from LLZTO. As a result, the assembled LiFePO 4 (LFP)/CIE/Li cell delivers better cell performance than LFP/LE-separator/Li cell at ambient temperature (AT). The assembled high-voltage cathode (Li 1.2 Mn 0.6 Ni 0.2 O 2 , 4.8 V)/CIE/Li cell also displays an excellent cell performance at AT. The present study offers new insights into exploring of flexible polymer-in-ceramic electrolytes for high-voltage LIBs with improved safety and energy density .
研究领域:
材料科学
·
电化学
·
能源存储
·
固态电池
·
纳米复合材料
·
界面工程
✓ 已验证
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
·
IF 8.128
Xin-yu Hu,Mao-xiang Jing,Hua Yang,Quan-yao Liu,Fei Chen,Wei-yong Yuan,Le Kang,Dong-hong Li,Xiang-qian Shen
Poor room-temperature ionic conductivity and lithium dendrite formation are the main issues of solid electrolytes. In this work, rod-shaped alumina incorporation and graphite coating were simultaneously applied to poly (propylene carbonate) (PPC)-based polymer solid electrolytes (Wang et al., 2018). The obtained alumina modified solid electrolyte membrane (Al-SE) achieves a high ionic conductivity of 3.48 × 10 −4 S/cm at room temperature with a wide electrochemical window of 4.6 V. The assembled NCM622/Al-SE/Li solid-state battery exhibits initial discharge capacities of 198.2 mAh/g and 177.5 mAh/g at the current density of 0.1 C and 0.5 C, with the remaining capacities of 165.8 mAh/g and 161.3 mAh/g after 100 cycles respectively. The rod-shaped structure of Al 2 O 3 provides fast transport channels for lithium ions and its Lewis acidity promotes the dissociation of lithium salts and release of free lithium ions. The lithiophilic Al 2 O 3 and Graphite form intimate contact with metallic Li and create fast Li + conductive layers of Li-Al-O layer and LiC 6 layer, thus facilitating the uniform deposition of Li and inhibiting Li dendrite formation during long-term cycling. This kind of composite Al-SE is expected to provide a promising alternative for practical application in solid electrolytes.
研究领域:
材料科学
·
电化学
·
能源存储
·
固态离子学
·
纳米复合材料
·
锂金属电池
✓ 已验证
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2023
·
IF 6.2
Chengyu Mo,Yutao Yang,Zhenyu Wang,Yanpeng Lv,Rongzheng Tian,Zixiang Zhao,Hongzhou Zhang,Chunliang Li,Lianqi Zhang,Yongan Yang,Dawei Song
Sulfide solid electrolytes have attracted wide attention due to their high ionic conductivity . Li 6 PS 5 Cl is one of the most promising electrolytes for all-solid-state lithium batteries with high-energy-density. It is reported that the disordered arrangement of Cl - in the aragonite structure has a significant effect on the conductivity of Li 6 PS 5 Cl. In this work, the disorder of anion sites is modestly regulated by adjusting the ratio of S and Cl in Li 6−x PS 5−x Cl 1+x electrolyte. In addition, to verify the commonality of this strategy, Li 5.6 PS 4.6 Cl 1.4 is prepared using self-made Li 2 S, and similar results are obtained. On this basis, the density of Li 5.6 PS 4.6 Cl 1.4 electrolyte sheet is improved by hot-pressing, which can successfully inhibit the growth of lithium dendrites . As expected, the ionic conductivity of the sulfide electrolyte and the electrochemical performance of the ASSLBs are greatly improved. A highest ionic conductivity of 8.2 × 10 −3 S cm −1 of Li 5.6 PS 4.6 Cl 1.4 is obtained at room temperature. A high capacity retention of 99.99 % is maintained for NCM811 @Li 2 O//Li 5.6 PS 4.6 Cl 1.4 //Li-In system after 400 cycles at 1 C with ultra-high cathode loading of 35.6 mg cm −2 . Besides, the cost of sulfide electrolytes can be reduced as the decreased usage of Li 2 S. This work proposes a novel synthesis method of low-cost and high-performance Li 6−x PS 5−x Cl 1+x electrolytes.
研究领域:
材料科学
·
电化学
·
能源存储
·
固态离子学
·
电池技术
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）