JOURNAL OF ALLOYS AND COMPOUNDS
·
2024
·
IF 5.8
Xueye Zhuang,Shiman He,Long Hu,Qian Shi,Hui Wang,Renzong Hu
LiBH 4 has been considered as a promising solid electrolyte for lithium-ion batteries. However, the low ionic conductivity at room temperature has been the biggest challenge of LiBH 4 solid-state electrolyte (SSE) toward practical solid-state batteries. In this work, a ternary electrolyte is designed and prepared by milling LiBH 4 with LiNH 2 and interfacially decorated with g-C 3 N 4 . It is revealed that the soft dispersed phase of two-dimensional g-C 3 N 4 can build an effective transportation network in the composite electrolyte, thereby decreasing the interfacial impedance and reducing the energy barrier for lithium ion diffusion. The optimized SSE, LiBH 4 -2LiNH 2 -g-C 3 N 4 -10 % (LBN-CN-10 %), exhibits an ionic conductivity of 1.5×10 −3 S cm −1 , five orders of magnitude higher than that of the LiBH 4 electrolyte at 30 °C. The LiIn symmetric cell with LBN-CN-10 % electrolyte delivers a low polarization of ∼89 mV over 10,000 h. When assembling with Li 4 Ti 5 O 12 cathode, the all-solid-state battery exhibits excellent cycling over 1000 cycles at 30 ℃, achieving a breakthrough in the lifetime of solid-state batteries with LiBH 4 -based electrolyte. Moreover, the all-solid-state battery with LiNi 0.8 Co 0.1 Mn 0.1 O 2 cathode also delivers a discharge plateau at 3.0 V, revealing the high voltage withstanding of LBN-CN-10 % electrolyte. This work provides new options for the development and practical application of room-temperature hydride all-solid-state batteries.
研究领域:
材料科学
·
能源存储技术
✓ 已验证
DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2025
·
IF 19
Haochang Zhang,Pengcheng Yu,Ziang Cui,Hailun Jin,Wen Tang,Chunlei Zhao,Jiuwei Lei,Shuaika Liang,Zhepu Shi,Jianhui Wang,Ying Li,Fiaz Hussain,Jinlong Zhu,Wei Xia
Lithium-metal-halide (Li-M-X) solid-state electrolytes (SSEs) offer significant potential for high-energy-density all-solid-state batteries (ASSBs) due to their high ionic conductivity, deformability, and compatibility with cathodes. However, to prevent direct reactions between halide SSEs and reductive anodes, sulfide SSEs are commonly used as interlayers in ASSBs. Yet, the chemical and electrochemical incompatibilities between halides and sulfides pose a new challenge. Here, a dual-anion strategy is proposed and demonstrated to address this issue by introducing O 2− anions into the halide framework. These findings reveal that high-concentration oxygen incorporation in Zr-based halide SSEs can be achieved without compromising ion conductivity, while simultaneously reducing interfacial reaction energy with Li 6 PS 5 Cl sulfide SSEs. This results in the formation of a dense, low-resistance Li 3 PO 4 -enriched interfacial layer, which contributes to superior electrochemical performance in full cells. ASSBs utilizing this electrolyte pair and a high-loading LiCoO 2 cathode (19.3 mg cm −2 ) achieve an impressive areal capacity of 2.8 mAh cm −2 and stable cycling performance exceeding 400 cycles. The O/Cl dual-anion strategy is also applicable to other halide SSEs paired with representative sulfide SSEs, including Li 6 PS 5 Cl, Li 10 GeP 2 S 12 , Li 3 PS 4 , Li 7 P 3 S 11, and Li 6.7 SiSb 0.5 S 5 I. This work provides valuable insights and strategies to improve the compatibility between halide and sulfide SSEs, advancing the development of ASSBs.
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
ELECTROCHEMISTRY COMMUNICATIONS
·
2023
·
IF 5.4
Zhenggang Jia,Xuexi Zhang,Mingfang Qian,Yingmin Jin,Yueping Xiong
Considering the high ion conductivity and good machining properties of lithium thiophosphate (LPS), it has attracted increasing attention as a solid electrolyte for all-solid-state batteries. Chemical and thermal stability can be significantly enhanced by increasing lithium content. However, in past reports, the lithium content of LPS is commonly less than 40 %. LPS with high lithium content (Li > 40 at%) shows low ion conductivity and high grain boundary resistance. In the present work, LPS with 47.2 at% lithium was prepared by cryomilling and solid-state reaction, avoiding crystallization and adhesion in the ball milling process. By improving the ball milling process, the ion conductivity (1.36 mS/cm) and ion activation energy (10.80 kJ/mol) were optimized by 106.1 % and 41.5 %, respectively. The resulting all-solid-state battery showed a high capacity retention of 104 % after 100 cycles.
研究领域:
材料科学
·
电化学
·
固态离子学
·
能源材料
·
电池技术
✓ 已验证
DOI
高影响因子
SOLID STATE IONICS
·
2025
·
IF 3.3
Shihao Fu,Pingmei Li,Shiyu Yu,Yang Hu,Yibo Liu,Daming Chen,Yaqing Wei,Yuanxun Li,Yong Chen
The garnet-type Li 7 La 3 Zr 2 O 12 (LLZO) has garnered significant attention due to its superior thermal stability and broad electrochemical window. However, LLZO exhibits instability at room temperature and readily transforms from a cubic phase ( c -LLZO) to a tetragonal phase ( t -LLZO), resulting in issues such as low ionic conductivity. Herein, the effect of Ga doping on LLZO is investigated. Combined with SEM, activation energy, ionic conductivity and XRD refinement, the results demonstrate that Li 7-3x Ga x La 3 Zr 2 O 12 exhibits better properties when x = 0.25. Solid-state nuclear magnetic resonance (SSNMR) showed that Ga0.25-LLZO was favorable for promoting Li + transport. Moreover, Li| [email protected] |Li symmetric cells exhibit lower interfacial specific impedance (IASR) and higher critical current density (CCD) than both Li|Ag@Ga0-LLZO|Li and Li| [email protected] |Li and was stabilized at 0.15 mA/cm 2 for 1300 h of stable cycling. In addition, the all-solid-state battery Li| [email protected] |LFP was cycled at 0.2C for 100 cycles with 82 % capacity retention, demonstrating its promising application in lithium batteries.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
Batteries-Basel
·
2023
·Vol. 9
·期 5
·257
·
IF 4
Xinjie Yu,Pengbo Zhai,Ning Zhao,Xiangxin Guo
Solid polymer electrolytes (SPEs) are seen as the key component in the development of solid-state lithium batteries (SSLBs) by virtue of their good processability and flexibility. However, poor mechanical strength, low room-temperature lithium-ion (Li-ion) conductivity and unsatisfactory interfacial compatibility with electrodes limit their practical application. In this work, a composite electrolyte consisting of polyvinylidene fluoride and polyvinylidene carbonate with a Li6.4La3Zr1.4Ta0.6O12(LLZTO) active filler (PFPC: LLZTO-SPE) is reported to achieve excellent ionic conductivity (4.25 × 10−4S cm−1at 30 °C), a wide electrochemical window (>4.6 V), a high Li-ion transference number (tLi+= 0.49) and good interfacial compatibility with the electrode. Incorporating LLZTO as an active filler not only increases the ionic conductivity of the electrolyte, but also homogenizes Li-ion flux and stabilizes the electrode/electrolyte interface, thereby preventing lithium dendrites from piercing the electrolyte. As a result, Li/Li symmetrical cells using PFPC: LLZTO-SPEs deliver more than 800 h of cyclability at 0.1 mA cm−2and a high critical current density (CCD) of 2.6 mA cm−2. The assembled Li/PFPC: LLZTO/LFP SSLBs achieve 87% capacity retention after 150 cycles at 0.2 C and 89% capacity retention for 100 cycles at 0.5 C. This work inspires new insights into designing high-performance SPEs.Keywords:LLZTO;in-situ polymerization;solid polymer electrolytes;solid-state lithium batteries
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
Membranes
·
2023
·Vol. 13
·期 2
·216
·
IF 4.2
Shishuo Liang,Dong Yang,Jianhua Hu,Shusen Kang,Xue Zhang,Yanchen Fan
With the rapid development of energy storage and electric vehicles, thiophosphate-based all-solid-state batteries (ASSBs) are considered the most promising power source. In order to commercialize ASSBs, the interfacial problem between high-voltage cathode active materials and thiophosphate-based solid-state electrolytes needs to be solved in a simple, effective way. Surface coatings are considered the most promising approach to solving the interfacial problem because surface coatings could prevent direct physical contact between cathode active materials and thiophosphate-based solid-state electrolytes. In this work, Li7La3Zr2O12(LLZO) and LiNbO3(LNO) coatings for LiCoO2(LCO) were fabricated by in-situ interfacial growth of two high-Li+conductive oxide electrolytes on the LCO surface and tested for thiophosphate-based ASSBs. The coatings were obtained from a two-step traditional sol–gel coatings process, the inner coatings were LNO, and the surface coatings were LLZO. Electrochemical evaluations confirmed that the two-layer coatings are beneficial for ASSBs. ASSBs containing LLZO-co-LNO coatings LiCoO2(LLZO&LNO@LCO) significantly improved long-term cycling performance and discharge capacity compared with those assembled from uncoated LCO. LLZO&LNO@LCO||Li6PS5Cl (LPSC)||Li-In delivered discharge capacities of 138.8 mAh/g, 101.8 mAh/g, 60.2 mAh/g, and 40.2 mAh/g at 0.05 C, 0.1 C, 0.2 C, and 0.5 C under room temperature, respectively, and better capacity retentions of 98% after 300 cycles at 0.05 C. The results highlighted promising low-cost and scalable cathode material coatings for ASSBs.Keywords:solid-state batteries;LiCoO2;sulfide solid-state electrolyte;LiNbO3-coating;LLZO-coating
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
PubMed
高影响因子
ADVANCED MATERIALS
·
2024
·Vol. 36
·期 39
·2407128
·
IF 27.4
Jinhui Zhu,Jiayao Luo,Jingyan Li,Senhe Huang,Haozhe Geng,Zhenying Chen,Linan Jia,Yongzhu Fu,Xi Zhang,Xiaodong Zhuang
Compared to lithium (Li) anode, the alloy/Li-alloy anodes show more compatible with sulfide solid electrolytes (SSEs), and are promising candidates for practical SSE-based all-solid-state Li batteries (ASSLBs). In this work, a porous Li–Al alloy (LiAl-p) anode is crafted using a straightforward mechanical pressing method. Various characterizations confirm the porous nature of such anode, as well as rich oxygen species on its surface. To the best knowledge, such LiAl-p anode demonstrates the best room temperature cell performance in comparison with reported Li and alloy/Li-alloy anodes in SSE-based ASSLBs. For example, the LiAl-p symmetric cells deliver a record critical current density of 6.0 mA cm −2 and an ultralong cycling of 5000 h; the LiAl-p|LiNi 0.8 Co 0.1 Mn 0.1 O 2 full cells achieve a high areal capacity of 11.9 mAh cm −2 and excellent durability of 1800 cycles. Further in situ and ex situ experiments reveal that the porous structure can accommodate volume changes of LiAl-p and ensure its integrity during cycling; and moreover, a robust Li inorganics-rich solid electrolyte interphase can be formed originated from the reaction between SSE and surface oxygen species of LiAl-p. This study offers inspiration for designing high-performance alloy anodes by focusing on designing special architecture to alleviate volume change and constructing stable interphase.
研究领域:
材料科学
·
电化学
·
储能技术
·
纳米技术
✓ 已验证
DOI
高影响因子
Small
·
2024
·Vol. 20
·期 35
·2310547
·
IF 13
Pengfei Zhai,Shuangquan Qu,Niaz Ahmad,Ze Hua,Ruiwen Shao,Wen Yang
The interfacial instability between PEO-based solid electrolyte (SPE) and high-voltage cathode materials inhibits the longevity of high-energy-density all-solid-state polymer lithium metal batteries (ASSPLBs). Herein, for the first time it is demonstrated, that contact loss caused by gas generation from interfacial side reactions between the high-voltage cathode and solid polymer electrolyte (SPE) can also arise in ASSPLBs. To alleviate the interfacial side reactions, a LiNb 0.6 Ti 0.5 O 3 (LNTO) layer is well coated on LiNi 0.83 Co 0.07 Mn 0.1 O 2 (NCM83), denoted as (CNCM83). The LNTO layer with low electronic conductivity reduces the decomposition drive force of SPE. Furthermore, Ti and Nb in the LNTO layer spontaneously migrate inside the NCM83 surface to form a strong Ti/Nb─O bond, stalling oxygen evolution in high-voltage cathodes. The interfacial degradation phenomena, including SPE decomposition, detrimental phase transition and intragranular cracks of NCM83, and void formation between cathode and SPE, are effectively mitigated by the LNTO layer. Therefore, the growth rate of interfacial resistance (R CEI ) decreases from 37.6 Ω h −0.5 for bare NCM83 to 2.4 Ω h −0.5 for CNCM83 at 4.2 V. Moreover, 4.2 V PEO-based ASSPLBs achieve impressive cyclability with high capacity retention of 135 mAh g −1 (75%) even after 300 cycles at 0.5 C.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
Energy Storage Materials
·
2022
·
IF 20.831
Hongpeng Zheng,Guoyao Li,Jiqiong Liu,Shaoping Wu,Xingmin Zhang,Yongmin Wu,Hong Zhu,Xiao Huang,Hezhou Liu,Huanan Duan
Lithium-stuffed garnets , one of the most promising solid electrolytes for all-solid-state lithium batteries (ASSLBs), are typically vulnerable to water or moisture. In this work, Li 6.5 La 3 Zr 1.5 Ta 0.5 O 12 (LLZT) with ionic conductivity of 7.36 × 10 −4 S cm −1 at room temperature and ultrahigh moisture stability is designed and synthesized by a solvent-free route with no excess lithium source. After storing in ambient atmosphere for four months, the LLZT maintains an ionic conductivity of 6.41 × 10 −4 S cm −1 . With optimized lithium contents, the LLZT is stored in an atmosphere rich in H 2 O and CO 2 at 65°C for 24 hours and the ionic conductivity only decreases by 6.9% to 6.6 × 10 −4 S cm −1 . Even undergone water-immersion, the LLZT pellet shows good electrochemical stability, which allows an interfacial resistance of 14.6 Ω cm 2 with Li and stable cycling performance of Li|LLZT|LFP cell, exhibiting a high capacity retention of 93% after 100 cycles. Several important features including high relative density, few grain boundaries, water-stable secondary phase of La 2 Zr 2 O 7 , and the Li + -deficient garnet lattice are combined to contribute to the moisture stability as suggested by morphology and surface chemistry analysis and first-principles calculations. This study provides valuable insights into synthesizing fast and moisture-stable lithium garnets in a time-efficient way, which is vital for developing garnet-based ASSLBs.
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
Nature Communications
·
2025
·Vol. 16
·期 1
·1-9
·
IF 15.7
Hong Bolong,Gao Lei,Li Changping,Lai Genming,Zhu Jinlong,Huang Dubin,Zuo Yunxing,Yin Wen,Sun Mengyu,Zhao Shusen,Zheng Jiaxin,Han Songbai,Zou Ruqiang
A pressing need for enhancing lithium-ion battery (LIB) performance exists, particularly in ensuring reliable operation under extreme cold conditions. All-solid-state batteries (ASSBs) offer a promising solution to the challenges posed by conventional LIBs with liquid electrolytes in low-temperature environments. In this study, leveraging the benefits of amorphous solid-state electrolytes (SSEs) x Li 3 N-TaCl 5 (1 ≤ 3 x ≤ 2), we develop ASSBs capable of functioning effectively under extreme cold conditions. The designed ASSBs, employing LiCoO 2 positive electrode with a mass loading of 4.46 mg cm ‒2 and a Li-In negative electrode, demonstrate initial discharge capacities of 183.19, 164.8 and 143.78 mAh g ‒1 under 18 mA g ‒1 at ‒10, ‒30, and ‒40 °C, respectively, and exhibit a final discharge capacity of 137.6 mAh g ‒1 at 18 mA g ‒1 and ‒30 °C in the 100th cycle. Moreover, the ASSBs demonstrate an initial discharge capacity of 51.94 mAh g ‒1 at 18 mA g ‒1 and ‒60 °C with cycling over 200 h.
研究领域:
材料科学
·
能源技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED PHYSICS A-MATERIALS SCIENCE & PROCESSING
·
2021
·Vol. 128
·期 1
·1-12
·
IF 2.584
Liang Xinghua,Li Suo,Yang Guanhua,Wu Xi,Huang Dongxue,Ning Yujue,Luo JianGuo,Fang Zhijie
All-solid-state lithium batteries are considered to be the most promising electrochemical energy storage equipment due to their high safety, high energy density, and simple structure. However, the preparation of solid electrolytes with high lithium-ion conductivity and superior electrode–electrolyte interface contact is the development needs. In this study, the electronic structures of garnet-type Li 7 La 3 Zr 2 O 12 (LLZO) and Sb-doped LLZO electrolytes were investigated using the first-principles method based on density functional theory (DFT). Theoretical calculations have confirmed that elemental doping facilitates the migration of lithium ions in solid-state electrolytes at the micro-atomic level. Based on the theoretical calculations and analysis results, Li 6.7 La 3 Zr 1.7 Sb 0.3 O 12 (LLZSbO) with high ionic conductivity was synthesized by the conventional solid-state method. To reduce the interfacial impedance between electrolyte and electrode, the composite solid electrolytes (CSEs) containing LLZSbO active fillers were prepared by the solution casting method. The prepared CSEs exhibits a high ionic conductivity of 0.97 × 10 –4 S cm −1 at 30 °C and a stable electrochemical window of 5.3 V as well as the lithium-ion transference number up to 0.37. The all-solid-state battery using the CSEs prepared with 20 wt% LLZSbO has excellent rate performance and cycle stability. The initial discharge specific capacity can reach 148.4 mAh g −1 when the rate is 0.1 C. The capacity can cover 138.8 mAh g −1 after 100 cycles at 0.2 C with a capacity retention rate of 97.5%.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
NATURE
·
2025
·Vol. 637
·期 8047
·846-853
·
IF 48.5
Song Huimin,Münch Konrad,Liu Xu,Shen Kaier,Zhang Ruizhuo,Weintraut Timo,Yusim Yuriy,Jiang Dequan,Hong Xufeng,Meng Jiashen,Liu Yatao,He Mengxue,Li Yitao,Henkel Philip,Brezesinski Torsten,Janek Jürgen,Pang Quanquan
With promises for high specific energy, high safety and low cost, the all-solid-state lithium–sulfur battery (ASSLSB) is ideal for next-generation energy storage 1 , 2 , 3 , 4 , 5 . However, the poor rate performance and short cycle life caused by the sluggish solid–solid sulfur redox reaction (SSSRR) at the three-phase boundaries remain to be solved. Here we demonstrate a fast SSSRR enabled by lithium thioborophosphate iodide (LBPSI) glass-phase solid electrolytes (GSEs). On the basis of the reversible redox between I − and I 2 /I 3 − , the solid electrolyte (SE)—as well as serving as a superionic conductor—functions as a surficial redox mediator that facilitates the sluggish reactions at the solid–solid two-phase boundaries, thereby substantially increasing the density of active sites. Through this mechanism, the ASSLSB exhibits ultrafast charging capability, showing a high specific capacity of 1,497 mAh g −1 sulfur on charging at 2C (30 °C), while still maintaining 784 mAh g −1 sulfur at 20C. Notably, a specific capacity of 432 mAh g −1 sulfur is achieved on charging at an extreme rate of 150C at 60 °C. Furthermore, the cell demonstrates superior cycling stability over 25,000 cycles with 80.2% capacity retention at 5C (25 °C). We expect that our work on redox-mediated SSSRR will pave the way for developing advanced ASSLSBs that are high energy and safe.
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）