Small
·
2023
·Vol. 19
·期 46
·2305326
·
IF 13.3
Shida Xue,Shiming Chen,Yanda Fu,Hengyao Zhu,Yuchen Ji,Yongli Song,Feng Pan,Luyi Yang
Composite solid electrolytes (CSEs) consisting of polyethylene oxide (PEO) matrix and active inorganic fillers have shown great potential for practical applications. However, mechanisms of how different active fillers enhance ion transport in CSEs still remain inconclusive. In this work, the component dependencies of ionic conductivity of PEO-based CSEs are investigated by comparing two widely investigated active fillers: NASICON-type (LATP) and garnet-type (LLZTO). In terms of ionic conductivity, the optimum ratios are strikingly different for LLZTO (10 wt%) and LATP (50 wt%). Through experimental and computational studies, it is demonstrated that the high affinity between LATP and PEO facilitates unhindered interfacial Li + transfer so that LATP functions as a bulk-active filler to provide additional inorganic ion pathways. By contrast, Li + transfer between LLZTO and PEO is found to be sluggish. Instead, LLZTO mainly improves ionic conductivity by dissociating lithium salt, making it a surface-active filler. Through categorizing active fillers based on their Li + conductive mechanisms, this work provides new understanding and guidelines for componential design and optimization of solid composite electrolytes.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF POWER SOURCES
·
2022
·
IF 9.794
Junying Yin,Xin Xu,Sen Jiang,Yue Lei,Yunfang Gao
Solid-state lithium metal batteries (SSLMBs) with high safety and high energy densities draw widespread attention in recent years. Nevertheless, the intrinsic defects of the solid-state electrolyte (SSE) such as the poor compatibility with electrodes and low ionic conductivity hamper the application of SSMLBs. Herein, we introduce rigid two-dimensional hexagonal boron nitride (BN) nanosheets and flexible One-dimensional aramid nanofibers (ANFs) as bi-nanofillers into the polyethylene oxide (PEO)-based SSEs to fabricate a composite solid-state electrolyte (CSE) ANF-PEO-BN with network structure boosting the comprehensive performance of SSMLBs. ANF and BN with special properties and structures are prone to be dispersed homogeneously in the PEO matrix to build the ANF-PEO-BN electrolyte, whose rigid and flexible network structure ensures the formation of Li dendrites inhibited. Furthermore, the dissociation of lithium bis(trifluoromethanesulphonyl)imide (LiTFSI) is promoted and more ion transport channels are provided due to the strong affinity between Lewis acid centers of ANF/BN and Li + /TFSI − . As a result, the LiFePO 4 /Li batteries deliver high-capacity retention of 86% after 500 cycles and Li/Li cells stably cycle beyond 3300 h with small overpotential of 10 mV at 0.1 mA cm −2 /0.2 mAh cm −2 .
研究领域:
材料科学
·
能源存储
✓ 已验证
DOI
高影响因子
GREEN CHEMISTRY
·
2024
·
IF 9.3
Liequan Liu,Zikang Gong,Chen Liu,Aiping Peng,Ze Zhang,Ji Yu,Jianxin Cai,Zhenyu Yang
Due to the inherent limitations of commercial liquid electrolytes, such as flammability, volatility, leakage, and their inability to effectively inhibit the growth of lithium dendrites, the lithium battery research community has shifted its attention towards advancing solid-state electrolytes. Notably, polyethylene oxide (PEO) has emerged as a respected solid-state electrolyte, but its ionic conductivity still exhibits a relatively modest level. In this study, we fabricated the Li-IL@Fe-BDC composite by integrating lithium salt-loaded ionic liquids (Li-ILs) into cost-effective and environmentally friendly Fe-based MOF frameworks (Fe-BDC). The resulting composite filler was then incorporated into a PEO matrix, yielding flexible composite polymer electrolytes (CPEs) with a “brick and mortar” hybrid structure. This unique arrangement enhances the mechanical strength of CPEs, providing dispersed sites and multi-ion transport channels. Consequently, it achieves a high conductivity of approximately 4.9 × 10−4 S cm−1, an extended electrochemical window of about 4.8 V, and a notable Li+ transference number of ∼0.6. Moreover, the composite demonstrates excellent interfacial compatibility with the Li metal and remarkable resistance against dendrite growth during plating/stripping cycles, sustaining over 800 hours at a current density of 0.2 mA cm−2. Furthermore, LiFePO4/CPEs/Li cells exhibit outstanding capacity retention, reaching as high as 95.8% after 700 cycles at 1 C. These exceptional electrochemical performances can be attributed to the distinctive characteristics of the Li-IL@Fe-BDC composite filler, which provides multiple pathways for lithium ion migration and enhances interfacial stability. Consequently, this study unveils a promising approach for achieving high Li-ion conductivity and interfacial stability in CPEs, offering valuable insights for future breakthroughs in this burgeoning field with a focus on green chemistry principles.
研究领域:
材料科学
·
绿色化学
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
Wenji Zheng,Zhen Liu,Rui Ding,Yan Dai,Xiangcun Li,Xuehua Ruan,Gaohong He
Electrospun fibers composite membrane shows an insufficient CO 2 permeability due to the impermeable polymer fibers. In this work, highly permeable poly(1-trimethylsilyl-1-propyne) (PTMSP) electrospun fiber were utilized to construct continuous and fast transport pathway with low-resistance for gas molecules in PEO matrix. The PEO/PTMSP electrospun fiber composite membrane (EFCM) was obtained by the in-situ polymerization of polyethylene glycol (PEG) into the voids of PTMSP electrospun fibers, which is demonstrated by FTIR and XPS characterizations. Furthermore, the obtained EFCM is dense and defect-free, which is confirmed by SEM images. Specifically, the PTMSP fibers and PEO matrix present good interfacial compatibility, as revealed by DSC results. In addition, PTMSP electrospun fibers perform as skeleton for EFCM to reinforce the membrane mechanical properties. The PEO/PTMSP EFCM shows CO 2 permeability of 281 Barrer and CO 2 /N 2 selectivity of 32.94. The CO 2 permeability is 280% higher than that of pure PEO membrane, which is resulted from the continuous and fast transport pathway provided by PTMSP electrospun fibers. The CO 2 /N 2 selectivity is enhanced by 4 to 6 times in comparison with pure PTMSP membrane and PTMSP c-EFM, which can be attributed to the affinity between EO groups of PEO matrix and CO 2 molecules and also the screening effect from the tortuous pathway of PTMSP fibers. This superior gas separation performance of PEO/PTMSP EFCM exceeds most reported PTMSP based membranes, especially its selectivity of CO 2 over N 2 is significantly high. Consequently, this proposed EFCM with continuous and fast transport pathway holds a competitive prospect for polymer based CO 2 capture.
研究领域:
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2022
·
IF 10.383
Xiang Ma,Mian Liu,Qingping Wu,Xiang Guan,Fei Wang,Hongmei Liu,Jun Xu
Compared with simplex ceramic or polymer solid electrolytes, composite solid electrolyte (CSE) is more promising for its better interfacial compatibility to electrode and high ionic conductivity simultaneously. Further, the interfacial compatibility within ceramic and polymer is considered to be more and more critical to the overall performance of solid-state batteries. Avoiding the agglomeration of ceramic particles at high loadings can improve the whole intrinsic characteristic and electrochemical performance of CSEs. Herein, we designed a CSE (EO@LLZTO–PEO), which consists of composite particles (EO@LLZTO) as a filler and polyethylene oxide (PEO) as polymer matrix. EO@LLZTO was prepared by chemically grafting polyethylene glycol monomethyl ether methacrylate (MPEG-MAA) on the micro-sized Li6.4La3Zr1.4Ta0.6O12 (LLZTO) particles. By introducing of polymer containing EO segments onto LLZTO, the interfacial compatibility between LLZTO and PEO matrix is highly enhanced, and the intrinsic Li+ complexation capability of MPEG-MAA is improved, even at the high loading of garnet. EO@LLZTO–PEO shows a high ionic conductivity (1.91 mS cm–1), a broad electrochemical window (∼5.2 V vs Li/Li+), and a high lithium ion transference number (0.72). The Li/EO@LLZTO–PEO/Li battery also exhibits a long cycle stability (over 1200 h of cycling). Moreover, all-solid-state batteries with LiFePO4 and LiNi0.8Co0.1Mn0.1O2 (NCM811) cathodes exhibit excellent cycling stability and rate performance. Consequently, enhancing the interfacial compatibility between organic and inorganic electrolytes is identified to be one of the crucial strategies for commercial solid-state lithium batteries.
研究领域:
材料科学
·
电化学
·
储能技术
·
纳米技术
·
高分子化学
✓ 已验证
DOI
高影响因子
Materials Chemistry Frontiers
·
2021
·Vol. 5
·期 21
·7767-7777
·
IF 6.482
Jiawei Wu,Jing Chen,Xiaodong Wang,Anan Zhou,Zhenglong Yang
For a higher safety and energy density, solid-state electrolytes with a better mechanical strength and thermal and electrochemical stability are a perfect choice. To improve the performance of PEO, using low-cost inert fillers may bring amorphous regions but limits easily appear. This paper aims to promote a network of SiO2 nanowires by applying a novel in situ crosslinking structure composed of PEA, γ-GPS and mPEG with siloxane segments as the junctions. The modified network can significantly reduce the crystallinity and glass transformation temperature, which also reduces the activation energy of ion transfer. Crosslinking can be highly influential as a comprehensive function of segment relaxation and ion complexation. The optimal sample (PEO–SNWAKP20) possesses a conductivity of 2.52 × 10−4 at 40 °C and a wide electrochemical window of 5.1 V. This unique structure also brings ideal shape stability under high temperatures, thus realizing stable cycling for 800 h at 0.1 mA cm−2. The rate and cycling performance of the LiFePO4 cell are also improved, achieving a maximum of 131.2 mAh g−1 under 0.5C with 89.3% retention after 50 cycles at 50 °C, realizing 24% improvement compared with single SNW reinforcement. By modifying the electrode, its performance can be further raised to 154 and 130.4 mAh g−1 under 0.5C and 1C, respectively, reserving 97.9% of its capacity after 100 cycles. This may inspire new strategies for synthesizing high-performance composite electrolytes.
研究领域:
材料科学
·
电化学
·
高分子科学
·
纳米技术
·
储能技术
·
化学工程
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）