JOURNAL OF POWER SOURCES
·
2017
·
IF 6.395
Biyi Xu,Wenlong Li,Huanan Duan,Haojing Wang,Yiping Guo,Hua Li,Hezhou Liu
This paper proposes a strategy to stabilize the garnet/Li interface by introducing Li 3 PO 4 as an additive in garnet-type Li 6.5 La 3 Zr 1.5 Ta 0.5 O 12 . The Li 3 PO 4 -added Li 6.5 La 3 Zr 1.5 Ta 0.5 O 12 electrolyte exhibits a room-temperature Li-ion conductivity of 1.4 × 10 −4 S cm −1 , which is less than that of the Li 3 PO 4 -free counterparts (4.6 × 10 −4 S cm −1 ). However, the presence of Li 3 PO 4 improves the interfacial compatibility and suppresses Li-dendrite formation during Li-metal plating/stripping. The symmetric Li/garnet/Li cells with Li 3 PO 4 -added Li 6.5 La 3 Zr 1.5 Ta 0.5 O 12 have been successfully cycled at a current density of 0.1 mA cm −2 at 60 °C for 60 h; on contrast, the control cells with Li 3 PO 4 -free Li 6.5 La 3 Zr 1.5 Ta 0.5 O 12 display noisy potential with large voltage polarization and get short-circuited completely after 33-h cycling under the same operating condition. The outstanding interface stability can be attributed to the in situ reaction of the Li flux with Li 3 PO 4 to form a self-limiting and ion-conducting interphase, Li 3 P, which is confirmed experimentally.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
Battery Energy
·
2025
·Vol. 4
·期 4
·e70009
·
IF 9.9
Jun Ma,Ruilin He,Yidong Jiang,Ludan Zhang,Hongli Xu,Hongbo Zeng,Chaoyang Wang,Xiaoxiong Xu,Yonghong Deng,Jun Wang,Shang-Sen Chi
Solid-state electrolyte (SSE) is a potential way to solve the safety problems of lithium metal batteries (LMBs), and Li 6.5 La 3 Zr 1.5 Ta 0.5 O 12 (LLZTO) is one of the most extensive research SSEs due to its good air stability and wide electrochemical window. However, the residual alkali on LLZTO surface limits its application with polyvinylidene difluoride (PVDF)-contained binders, and the uncontrollable lithium dendrites growing between the grain boundaries of LLZTO particles would lead to rapid capacity fading and potential short circuit risk. Herein, by in situ coating Li 3 PO 4 (LPO) on LLZTO particles (LLZTO@LPO) evenly, the residual alkali on the LLZTO surface is neutralized and the pH value is reduced to 8.84. The modified LLZTO can be mixed with PVDF solution and shows good fluidity without a cross-linking reaction, making the subsequent ceramic coating on the separator feasible. The LLZTO@LPO coating polyethylene (PE) separator can achieve 1400 h (115% increase) stable cycling under 1 mA cm −2 current density in the Li∥Li symmetrical cell and 80% capacity retention after 260 cycles (NCM622-Li coin cell with 3 mAh cm −2 loading). Furthermore, the LLZTO SSE pellets were prepared with the LLZTO@LPO and assembled in coin cell. The critical current density (CCD) result increases from 0.7 to 1.6 mA cm −2 owing to that the LPO coating effectively inhibits the lithium dendrites formation through LLZTO grain boundaries. This work provides a strategy for fabricating the coating layer on LLZTO to improve the stability of LMBs.
研究领域:
材料科学
·
电化学
·
储能技术
·
固态电池
✓ 已验证
产品关联
DOI
高影响因子
Battery Energy
·
2025
·
IF 9.9
Jun Ma,Ruilin He,Yidong Jiang,Ludan Zhang,Hongli Xu,Hongbo Zeng,Chaoyang Wang,Xiaoxiong Xu,Yonghong Deng,Jun Wang,Shang-Sen Chi
Solid-state electrolyte (SSE) is a potential way to solve the safety problems of lithium metal batteries (LMBs), and Li 6.5 La 3 Zr 1.5 Ta 0.5 O 12 (LLZTO) is one of the most extensive research SSEs due to its good air stability and wide electrochemical window. However, the residual alkali on LLZTO surface limits its application with polyvinylidene difluoride (PVDF)-contained binders, and the uncontrollable lithium dendrites growing between the grain boundaries of LLZTO particles would lead to rapid capacity fading and potential short circuit risk. Herein, by in situ coating Li 3 PO 4 (LPO) on LLZTO particles (LLZTO@LPO) evenly, the residual alkali on the LLZTO surface is neutralized and the pH value is reduced to 8.84. The modified LLZTO can be mixed with PVDF solution and shows good fluidity without a cross-linking reaction, making the subsequent ceramic coating on the separator feasible. The LLZTO@LPO coating polyethylene (PE) separator can achieve 1400 h (115% increase) stable cycling under 1 mA cm −2 current density in the Li∥Li symmetrical cell and 80% capacity retention after 260 cycles (NCM622-Li coin cell with 3 mAh cm −2 loading). Furthermore, the LLZTO SSE pellets were prepared with the LLZTO@LPO and assembled in coin cell. The critical current density (CCD) result increases from 0.7 to 1.6 mA cm −2 owing to that the LPO coating effectively inhibits the lithium dendrites formation through LLZTO grain boundaries. This work provides a strategy for fabricating the coating layer on LLZTO to improve the stability of LMBs.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2022
·
IF 10.383
Ting-Ting Wu,Sijie Guo,Bing Li,Jin-Yang Li,Hong-Shen Zhang,Pei-Zhong Ma,Xing Zhang,Chang-Yu Shen,Xian-Hu Liu,An-Min Cao
The use of solid-state electrolytes (SSEs) instead of those liquid ones has found promising potential to achieve both high energy density and high safety for their applications in the next-generation energy storage devices. Unfortunately, SSEs also bring forth challenges related to solid-to-solid contact, making the stability of the electrode/electrolyte interface a formidable concern. Herein, using a garnet-type Li6.5La3Zr1.5Ta0.5O12 (LLZT) electrolyte as an example, we demonstrated a facile treatment based on the dip-coating technique, which is highly efficient in modifying the LLZT/Li interface by forming a MgO interlayer. Using polyvinyl pyrrolidone (PVP) as a coordination polymer, uniform and crack-free nanofilms are fabricated on the LLZT pellet with good control of the morphological parameters. We found that the MgO interlayer was highly effective to reduce the interfacial resistance to 6 Ω cm2 as compared to 1652 Ω cm2 of the unmodified interface. The assembled Li symmetrical cell was able to achieve a high critical current density of 1.2 mA cm–2 at room temperature, and it has a long cycling capability for over 4000 h. Using the commercialized materials of LiFePO4 and LiNi0.83Co0.07Mn0.1O2 as the cathode materials, the full cells based on the LLZT@MgO electrolyte showed excellent cyclability and high rate performance at 25 °C. Our study shows the feasibility of precise and controllable surface modification based on a simple liquid phase method and highlights the essential importance of interface control for the future application of high-performance solid-state batteries.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
DOI
PubMed
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2022
·Vol. 32
·期 24
·2201498
·
IF 19.924
Sijie Guo,Ting-Ting Wu,Yong-Gang Sun,Si-Dong Zhang,Bing Li,Hong-Shen Zhang,Mu-Yao Qi,Xian-Hu Liu,An-Min Cao,Li-Jun Wan
Solid-state batteries (SSBs) are promising for next-generation energy storage with advantages in both energy density and safety, but are challenged by the poor solid-to-solid contact between solid-state electrolytes (SSEs) and electrodes, particularly the lithium anode. Herein, a facile coordination-assisted deposition process is employed to build artificial Ta 2 O 5 nanofilms on SSEs, which is lithiophilic and has high stability against metallic lithium, thereby ensuring an intimate and stable interface between SSEs and lithium anode to sustain extended cycles. The feasibility is verified by using Li 6.5 La 3 Zr 1.5 Ta 0.5 O 12 (LLZT), a garnet-typed SSEs, as a model system. It is shown that a 12 nm Ta 2 O 5 nanofilm is able to significantly decrease the interfacial resistance from 1258 to 9 Ω cm 2 with a high critical current density reaching 2.0 mA cm −2 for the assembled symmetric cell, which shows an unprecedented capability to survive long-term cycling over 5200 h. This control strategy is also able to enable the use of the commercialized cathode materials of LiFePO 4 and LiNi 0.83 Co 0.07 Mn 0.1 O 2 in SSBs with both high reversible capacity and cycling capability. The study opens up a research avenue for the delicately carved interlayers through a scalable and reliable manufacturing process which can accelerate the commercialization of SSEs.
研究领域:
材料科学
·
电化学
·
能量存储
✓ 已验证
DOI
高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-9
·
IF 14.7
Zhang Nian,Ren Guoxi,Li Lili,Wang Zhi,Yu Pengfei,Li Xiaobao,Zhou Jing,Zhang Hui,Zhang Linjuan,Liu Zhi,Liu Xiaosong
Garnet-type Li 6.5 La 3 Zr 1.5 Ta 0.5 O 12 (LLZO) is considered a promising solid electrolyte, but the surface degradation in air hinders its application for all-solid-state battery. Recent studies have mainly focused on the final products of the LLZO surface reactions due to lacking of powerful in situ characterization methods. Here, we use ambient pressure X-ray spectroscopies to in situ investigate the dynamical evolution of LLZO surface in different gas environments. The newly developed ambient pressure mapping of resonant Auger spectroscopy clearly distinguishes the lithium containing species, including LiOH, Li 2 O, Li 2 CO 3 and lattice oxygen. The reaction of CO 2 with LLZO to form Li 2 CO 3 is found to be a thermodynamically favored self-limiting reaction. On the contrary, the reaction of H 2 O with LLZO lags behind that of CO 2 , but intensifies at high pressure. More interestingly, the results provide direct spectroscopic evidence for the existence of Li + /H + exchange and reveal the importance of the initial layer formed on clean electrolyte surface in determining their air stability. This work demonstrates that the newly developed in situ technologies pave a new way to investigate the oxygen evolution and surface degradation mechanism in energy materials.
研究领域:
材料科学
·
电化学
·
固态电池
·
表面化学
·
光谱学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）