CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Meng Yu,Xiaohui Ning
Li metal with ultra-high theoretical capacity is a promising anode for next-generation high-energy–density battery technologies. Nevertheless, the uncontrolled Li dendrite growth, continuous interfacial side reactions and irregular volume expansion bring about rapid capacity decay of Li metal anodes (LMAs). Herein, we design a bilayer host structure with an electronic conductivity gradient through a facile blade coating strategy to regulate Li deposition behavior. The electronic-insulative Si 3 N 4 top layer prevents the apical growth of Li dendrites and promotes the penetration of electrolytes into the host so as to lower electrode polarization. The carbon black/LiNO 3 mixed bottom layer creates mixed electronic-ionic conductive network to enhance the charge transfer kinetics of Li ions and lower Li nucleation barrier. Moreover, we first discover that the Si 3 N 4 protective layer avoids the cell failure resulting from the dissolution of LiNO 3 in ether electrolytes, enabling the Si 3 N 4 -C/LiNO 3 electrode to operate smoothly for over 600 cycles, delivering an average Coulombic efficiency of up to 98.65 %. Furthermore, the Si 3 N 4 -C/LiNO 3 -composited LMAs paired with 10.5 mg cm −2 LiFePO 4 cathodes achieve 200 stable cycles at a low N/P ratio of 1 under corrosive carbonate ester electrolytes, with an anode capacity utilization ratio as high as 50 %. This is the first report on the LiNO 3 -modified host materials that exhibit superior electrochemical properties in ether electrolytes, shedding a new light on the structural design of LMAs to enable high-energy–density Li metal batteries.
研究领域:
材料科学
·
电化学
·
能源存储
·
纳米材料
·
界面化学
·
电池技术
✓ 已验证
DOI
高影响因子
Journal of Energy Chemistry
·
2021
·
IF 9.676
Liansheng Li,Yuanfu Deng,Huanhuan Duan,Yunxian Qian,Guohua Chen
Solid electrolytes with desirable properties such as high ionic conductivity, wide electrochemical stable window, and suitable mechanical strength, and stable electrode–electrolyte interfaces on both cathode and anode side are essential for high-voltage all-solid-state lithium batteries (ASSLBs) to achieve excellent cycle stability. In this work, a novel strategy of using LiF and LiNO 3 as synergistic additives to boost the performance of PEO-PVDF/LLZTO-based composite solid electrolytes (CSEs) is developed, which also promotes the assembled high-voltage ASSLBs with dual-interfaces stability characteristic. Specifically, LiF as an inactive additive can increase the electrochemical stability of the CSE under high cut-off voltage, and improve the high-voltage compatibility between cathode and CSE, thus leading to a stable cathode/CSE interface. LiNO 3 as an active additive can lead to an enhanced ionic conductivity of CSE due to the increased free-mobile Li + and ensure a stable CSE/Li interface by forming stable solid electrolyte interphase (SEI) on Li anode surface. Benefiting from the improved performance of CSE and stable dual-interfaces, the assembled NCM622/9[PEO 15 -LiTFSI]-PVDF-15LLZTO-2LiF-3LiNO 3 /Li cell delivers a high rate capacity of 102.1 mAh g −1 at 1.0 C and a high capacity retention of 77.4% after 200 cycles at 0.5 C, which are much higher than those of the ASSLB assembled with additive-free CSE, with only 60.0 mAh g −1 and 52.0%, respectively. Furthermore, novel cycle test modes of resting for 5 h at different charge states after every 5 cycles are designed to investigate the high-voltage compatibility between cathode and CSE, and the results suggest that LiF additive can actually improve the high-voltage compatibility of cathode and CSE. All the obtained results confirm that the strategy of using synergistic additives in CSE is an effective way to achieve high-voltage ASSLBs with dual-interfaces stability.
研究领域:
材料科学
·
电化学
·
能源存储
·
固态电池
·
界面化学
·
高分子科学
·
无机非金属材料
✓ 已验证
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Maoxia Yang,Shaomin Li,Gen Zhang,Mengjie Huang,Jidong Duan,Yanhua Cui,Bo Yue,Hao Liu
Succinonitrile (SN)-based electrolytes have a great potential for the practical application of all-solid-state lithium-metal batteries (ASSLMBs) due to their high room-temperature ionic conductivity, broad electrochemical window, and favorable thermal stability. Nevertheless, the poor mechanical strength and low stability toward Li metal hinder the further application of SN-based electrolytes to ASSLMBs. In this work, the LiNO3-assisted SN-based electrolytes are synthesized via an in situ thermal polymerization method. With this method, the mechanical problem is negligible, and the stability of the electrolyte enhances tremendously toward Li metal due to the addition of LiNO3. The LiNO3-assisted electrolytes exhibit a high ionic conductivity of 1.4 mS cm–1 at 25 °C, a wide electrochemical window (0–4.5 V vs Li+/Li), and excellent interfacial compatibility with Li (stable for over 2000 h at a current density of 0.1 mA cm–1). The LiFePO4/Li cells with the LiNO3-assisted electrolytes present significantly enhanced rate capability and cycling performance compared to the control group. NCM622/Li batteries also exhibit good cycling and rate performances with a voltage range of 3.0 to 4.4 V. Furthermore, ex situ SEM and XPS are employed. A compact interface is observed on Li anode after cycling, and the polymerization of SN is found to be suppressed. This paper will promote the development of practical application of SN-based ASSLMBs.
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
JOURNAL OF POWER SOURCES
·
2022
·
IF 9.794
Fengwei Bai,Yan Li,Ziyu Chen,Yongchao Zhou,Chengzong Li,Tao Li
High-voltage lithium (Li)-metal batteries with cell-level energy density over 350 Wh kg −1 are promising energy storage systems . However, the aggressive interphase chemistries associated with highly reactive Li-metal anode and high-voltage cathodes impede their practical applications. Herein, we demonstrate the targeted stabilization of solid electrolyte interphase (SEI) and cathode electrolyte interphase (CEI) in high-voltage Li-metal batteries by asymmetrically sustained-releasing different additives. An asymmetric sustained-release film loaded with lithium bis-(oxalate)borate (LiBOB) and LiNO 3 on each side is investigated as a proof-of-concept. The sustained-releasing of LiBOB and LiNO 3 can maintain a localized concentration at the high-voltage cathode and Li-metal anode fronts respectively, thus forming a stable B-containing CEI and N-containing SEI. As such, issues like dendrites growth, parasitic side reactions and transition metals dissolution under high-voltage are addressed simultaneously. Based on this strategy, the 30 μm Li|LiNi 0.5 Co 0.2 Mn 0.3 O 2 (4.1 mAh cm −2 ) batteries deliver a capacity retention of 80% after 173 cycles under a cut-off voltage of 4.5 V.
研究领域:
储能系统
·
电池技术
·
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）