NEW JOURNAL OF CHEMISTRY
·
2025
·Vol. 49
·期 27
·11985-11995
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IF 2.5
Yu Chen,Ziteng Yang,Yanlong Wang,Guojian Zhao,Taoran Wang,Minghui Feng,Mengxi Zhao,Xihou Wang,Dexin Dong
Lithium iron phosphate (LFP)-based lithium-ion batteries (LIBs) are widely used in various fields due to their advantages such as low cost, long service life, and high energy density. The widespread use of LFP-based LIBs leads to the generation of large quantities of spent LFP cathode materials, which contribute to environmental pollution and resource waste. Therefore, it is necessary to develop a new strategy to recycle spent LFP cathode materials from LIBs. Here, we use non-toxic, low-cost and naturally available vegetable-/fruit-derived solvents (VFSs) to efficiently and mildly recover LFP cathodes from LIBs. The highest leaching efficiency of Li and Fe from LFP using VFSs is 98.8% and 99.8%, respectively. The superhigh leaching efficiency of Li and Fe achieved by VFSs is comparable to that obtained using other green solvents, including ionic liquids, deep eutectic solvents, and low-melting mixture solvents; however, VFSs in this work are greener, cheaper and even could be edible. In addition, a high precipitation efficiency of Li (83.4%) and Fe (98.5%) could be achieved at room temperature after screening 69 kinds of antisolvents.
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产品关联
DOI
高影响因子
Polymer Chemistry
·
2024
·
IF 4.1
Haomin Wu,Wencan Ma,Xin Huang,Yifeng Cai,Junheng Li,Qiaobo Liao,Kai Xi,Qiuhong Zhang,Xudong Jia
Single-ion quasi-solid-state electrolytes (SIQSSEs) attract increasingly attention recently, due to their ability in suppressing the growth of lithium dendrite and offering higher safety. However, the low ionic conductivity is still the major bottleneck for preventing the practical application. Covalent organic frameworks (COFs) are considered as potential candidates for quasi-solid-state electrolytes (QSSEs) due to their high porosity and ordered structures. Herein, we demonstrate a series of crystalline covalent organic frameworks with sulfonimide groups as a new class of single-ion electrolytes. Owing to the directional lithium transport pathway and adequate binding site for lithium-ions, these COF-based electrolytes deliver good ionic conductivity (4.3×10-4 S cm-1) at 298 K, with high lithium transference number (LTN, ~0.90) and a low activation energy (0.24 eV). We also find both strong electron-withdrawing substituent and delocalized substituent could promote lithium-ion transportation. Furthermore, the Li||LiFePO4 (LFP) cells based on the sulfonimide-functionalized covalent organic framework (SF-COF) electrolytes deliver outstanding rate performance with long cycle life (99% capacity retention after 100 cycles at 0.2 C). Our work demonstrates that crystalline covalent organic frameworks show great potential for application as building blocks of solid electrolytes in lithium metal batteries.
研究领域:
材料科学
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电化学
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能量存储
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Kejin Jiao,Shujie Liu,Yanyan Ma,Shuo Chen,Liying Wei,Jianhua Yan
Lithium (Li) metal battery is a promising next generation energy storage system due to its high energy density , but what hinders its commercialization is the safety hazard of Li-anode, especially under high current densities. Here, we report a dual strategy of using electronic conductive black TiO 2−x nanofiber films to construct composite Li-metal anodes with stable 3D networks and applying an in-situ polymerized ionic conductive gel-electrolyte to construct efficient quasi-solid-state Li-batteries (QSSLBs). The 3D nanofibrous Li-anode shows a stable and small nucleation barrier and can run stably (>1600 h) at a high current density of 10 mA/cm 2 . When matching with high-loading cathodes of LiFePO 4 , the QSSLBs exhibit excellent long-term cycling stability (>500 cycles) and high-rate capability (>1 C). In addition, the in-situ polymerization strategy can be incorporated with the commercial lamination manufacturing to produce 63-Ah pouch cells of LiFePO 4 ||graphite, which deliver a high initial Coloumbic efficiency, a large energy density at 0.3 C, excellent rate capability from 0.25 to 2 C, and long-term cycling performance at 0.3 and 1 C, showing potential commercial prospects.
研究领域:
能源存储
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材料科学
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电化学
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电池技术
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DOI
高影响因子
ACS Applied Energy Materials
·
2020
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IF 4.473
Zihao Chen,Baichuan Han,Yuansheng Shi,Senhao Wang,Zhizhen Zhang,Xia Lu,Dapeng Cao
In this work, a hierarchical PVDF-HFP gel polymer electrolyte (GPE) membrane is prepared intentionally and placed between the solid electrolyte and the electrodes. The fabricated LiFePO4/GPE/LAGP/GPE/Li hybrid solid-state cell displays superior rate performance and capacity retention. After 300 cycles at 0.5 C, negligible degradation can be observed, and the specific capacity remains as high as 145.6 mA h/g at room temperature. The excellent battery performance is ascribed to the significantly improved interfacial stability of the sandwich-like hybrid electrolyte and the remarkably enhanced charge transfer kinetics across the interface due to the flexibility of GPE.
研究领域:
材料科学
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电化学
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电池技术
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DOI
高影响因子
Journal of Materials Chemistry A
·
2022
·Vol. 11
·期 4
·1966-1977
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IF 14.511
Zhiheng Ren,Jixiao Li,Minghui Cai,Ruonan Yin,Jianneng Liang,Qianling Zhang,Chuanxin He,Xiantao Jiang,Xiangzhong Ren
Polymer electrolytes (PEs) synthesized from an in situ polymerization strategy are considered as promising candidates to improve interfacial compatibility. However, most in situ formed PEs still suffer from problems such as low lithium-ion transference number (tLi+) and insufficient ionic conductivity at room temperature (RT). Herein, a series of copolymer electrolytes (CPEs) consisting of 1,3-dioxolane (DOL) and 1,3,5-trioxane (TXE) monomers are synthesized. Due to the additive of succinonitrile (SN), and the promoted dissociation of lithium salt, the obtained polymer electrolyte (SN-CPE) exhibits an excellent ionic conductivity (4.06 × 10−4 S cm−1) and a high lithium-ion transference number (tLi+ = 0.881) at RT, as well as a high voltage oxidation window of 5.1 V. Thanks to the in situ formed intimate contacted electrode/electrolyte interface, the symmetric Li/Li cell can achieve long-term cycling stability over 1500 h without a short circuit. A LiF-rich organic–inorganic composite layer is formed on both the solid electrolyte interphase (SEI) and cathode electrolyte interphase (CEI) as demonstrated by XPS, TEM, and SEM analyses. Thereafter, the LiFePO4/Li cell has a high capacity retention of 84.1% after 900 cycles at RT, and it can still work effectively at high temperatures (e.g. 80 °C). Furthermore, SN-CPE exhibits excellent electrochemical performance and safety in the LiCoO2/Li cell and LiFePO4/graphite pouch cell, which again supports the promising application of SN-CPE.
研究领域:
材料科学
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电化学
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能源存储
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电池技术
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DOI
高影响因子
Nature Communications
·
2023
·Vol. 14
·期 1
·1-11
·
IF 16.6
Huang Shaozhen,Wu Zhibin,Johannessen Bernt,Long Kecheng,Qing Piao,He Pan,Ji Xiaobo,Wei Weifeng,Chen Yuejiao,Chen Libao
A practical high-specific-energy Li metal battery requires thin (≤20 μm) and free-standing Li metal anodes, but the low melting point and strong diffusion creep of lithium metal impede their scalable processing towards thin-thickness and free-standing architecture. In this paper, thin (5 to 50 μm) and free-standing lithium strips were achieved by mechanical rolling, which is determined by the in situ tribochemical reaction between lithium and zinc dialkyldithiophosphate (ZDDP). A friction-induced organic/inorganic hybrid interface (~450 nm) was formed on Li with an ultra-high hardness (0.84 GPa) and Young’s modulus (25.90 GPa), which not only enables the scalable process mechanics of thin lithium strips but also facilitates dendrite-free lithium metal anodes by inhibiting dendrite growth. The rolled lithium anode exhibits a prolonged cycle lifespan and high-rate cycle stability (in excess of more than 1700 cycles even at 18.0 mA cm −2 and 1.5 mA cm −2 at 25 °C). Meanwhile, the LiFePO 4 (with single-sided load 10 mg/cm 2 ) ||Li@ZDDP full cell can last over 350 cycles with a high-capacity retention of 82% after the formation cycles at 5 C (1 C = 170 mA/g) and 25 °C. This work provides a scalable approach concerning tribology design for producing practical thin free-standing lithium metal anodes.
研究领域:
材料科学
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电化学
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电池技术
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DOI
PubMed
高影响因子
JOURNAL OF POWER SOURCES
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2024
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IF 8.1
Zixuan Li,Dequan Bao,Wei Zhao,Wenxuan Xu,Yingheng Huang,Xiyong Chen,Hao Zhang,Xuhui Sun
Gel polymer electrolytes (GPEs) have emerged as a highly promising alternative to conventional liquid electrolytes for stable lithium-metal batteries (LIBs). However, their inherent poor mechanical properties and limited interfacial compatibility with lithium metal usually lead to unexpected growth of lithium dendrites , hindering commercial viability. Herein, an asymmetric polymer electrolyte with h-BN (HGPE) as protective layer was fabricated via a facile one-step coating strategy. Compared to pure GPE, the asymmetric polymer electrolytes exhibit significantly enhanced mechanical strength from 4.4 MPa to 7.4 MPa, effectively suppressing lithium dendrite growth. Furthermore, the HGPE improves interfacial compatibility with the anodes by preventing direct contact between GPE and lithium metals. The addition of h-BN also enhances the lithium-ion transfer number (t Li+ ), reaching 0.87 compared to 0.53 for pure GPE, attributed to the hindrance of anion movement by the protective layer. Consequently, the Li symmetric battery assembled with HGPE demonstrate exceptional long-term stability, maintaining performance over 1600 h at 0.1 mA cm −2 . Furthermore, the assembled Li|LiFePO 4 battery can deliver a high-capacity retention rate of 93.8 % after 500 cycles at room temperature, showcasing the promising potential of asymmetric polymer electrolytes for high-performance LMBs.
研究领域:
材料科学
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电化学
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能源存储
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2022
·
IF 16.744
Dexuan Pei,Ziying Liu,Rui Ma,Shuo Huang,Shuen Hou,Min Liu,Guozhong Cao,Hongyun Jin
Composite polymer electrolytes (CPEs) have shown extraordinary promise for use in all-solid-state lithium metal batteries (LMBs) because of their tunable merits in ionic conductivity and mechanical flexibility. Their practical application is however hindered by the poor interface stability and the uncontrollable Li dendrite formation. Addressing these two issues, we report an in-situ formed Li-Al-O interface layer between CPEs and Li metal anode by introducing Al 2 O 3 nanoparticles in CPEs. X-ray photoelectron spectroscopy results indicated that the CPE-Al 2 O 3 could slowly release Al atoms which react with Li metal to form the current Li-Al-O interface layer. We highlight that the Li-Al-O interface layer can stabilize lithium deposition/stripping over 1400 h in lithium symmetric batteries, and afford an impressive cycle life of 300 cycles in LiFePO 4 -Li batteries with almost no capacity loss. The present findings demonstrate that in-situ constructing a slow-release Li-Al-O interface layer is an easy and effective approach to stabilize the solid electrolyte interface and suppress the Li dendrites growth. Furthermore, the obtained batteries show excellent cycling stability, indicating the strategy with in-situ formed CPEs shed light on improving the processability of fabrication of high-performance electrolytes.
研究领域:
材料科学
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电化学
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能源存储
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DOI
高影响因子
TRANSACTIONS OF NONFERROUS METALS SOCIETY OF CHINA
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2024
·
IF 4.7
Liu-bin SONG,Tian-yuan LONG,Min-zhi XIAO,Min LIU,Ting-ting ZHAO,Yin-jie KUANG,Lin JIANG,Zhong-liang XIAO
A composite solid electrolyte comprising a Cu−Al bimetallic metal-organic framework (CAB), lithium salt (LiTFSI) and polyethylene oxide (PEO) was fabricated through molecular grafting to enhance the ionic conductivity of the PEO-based electrolytes. Experimental and molecular dynamics simulation results indicated that the electrolyte with 10 wt.% CAB (PL-CAB-10%) exhibits high ionic conductivity (8.42×10 −4 S/cm at 60 °C), high Li + transference number (0.46), wide electrochemical window (4.91 V), good thermal stability, and outstanding mechanical properties. Furthermore, PL-CAB-10% exhibits excellent cycle stability in both Li−Li symmetric battery and Li/PL-CAB- 10%/LiFePO 4 asymmetric battery setups. These enhanced performances are primarily attributable to the introduction of the versatile CAB. The abundant metal sites in CAB can react with TFSI − and PEO through Lewis acid–base interactions, promoting LiTFSI dissociation and improving ionic conductivity. Additionally, regular pores in CAB provide uniformly distributed sites for cation plating during cycling.
研究领域:
材料科学
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电化学
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电池技术
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聚合物科学
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DOI
高影响因子
Inorganic Chemistry Frontiers
·
2024
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IF 6.1
Yongquan Zhang,Hongchang Gao,Jingshun Wang,Qingguo Chi,Tiandong Zhang,Changhai Zhang,Yu Feng,Yue Zhang,Dianxue Cao,Kai Zhu
All-solid-state lithium metal batteries (ASSLMBs) are considered the most competitive next-generation energy storage batteries due to their high energy density and high safety. Polyethylene oxide (PEO) is an ideal solid-state electrolyte due to its high chain flexibility, high dielectric constant, and strong dissociation ability towards lithium salts. However, the application of PEO is severely hindered by drawbacks such as low ion conductivity at room temperature and low electrochemical window. In this work, we constructed a Li1.25Al0.25Zr1.75(PO4)3 (LAZP)/PEO composite solid-state electrolyte (CSSE) with improved ion conductivity, enlarged electrochemical window, and stable charge–discharge cycle performance. The CSSE leads to an obvious LiF layer and Li2CO3 formation at the interface of lithium metal. Meanwhile, the addition of LAZP reduces the side reaction between PEO and the lithium metal significantly and suppresses the deterioration of ion conductivity. In addition, we modified LiFePO4 (M-LFP), the cathode sheet of the ASSLMBs, by adding an appropriate proportion of multi-walled carbon nanotubes (MWCNTs), PEO and lithium bis(trifluoromethane sulfonimide) (LiTFSI) to improve the ionic and electronic conductivity inside the cathode of the ASSLMBs. The Li/CSSE/M-LFP full cell exhibits a specific discharge capacity of 152 mA h g−1 at 60 °C and 2 C rate and a capacity retention rate of 93.5% after 200 cycles at 1 C. This work demonstrates an effective strategy for increasing the specific capacity, rate ability and long-cycle performance of ASSLMBs.
研究领域:
材料科学
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电化学
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能源存储
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DOI
高影响因子
ELECTROCHIMICA ACTA
·
2020
·
IF 6.215
Wenyan Shang,Chaoqun Niu,Guangping Chen,Yubing Chen,Jie Du
Lithium metal shows great promise as an anode material for high-performance next-generation batteries due to its low redox potential , low weight, and high specific capacity. However, the uncontrolled growth of lithium dendrites during charge–discharge cycling limits the practical application of lithium metal anodes . In this work, an anion-inhibited solid framework polymer electrolyte (SFPE) was prepared through the polymerization of vinyl polyhedral oligomeric silsesquioxane (VPOSS) and diallyl dicarbonate (DDC) as a means to suppress lithium dendrite formation. The structure of the electrolyte was found to reduce the electric field at the anode surface by restricting the free movement of the anions (TFSI − ) of the lithium salt , which facilitated the orderly, uniform, and safe deposition of lithium ions on the anode. The SFPE presented a high lithium ion transference number (0.63), a wide window of electrochemical stability (5.6 V versus Li + /Li), and high ionic conductivity (0.31 mS cm −1 ) at 25 °C. A LiFePO 4 /Li cell containing the SFPE achieved a specific discharge capacity of 165 mAh g −1 and a capacity retention of 91.3% after 200 cycles at 0.1 C (1 C = 180 mAh g −1 ) and 25 °C, and the lithium anode surface remained smooth after 600 h of constant-current charge–discharge cycling. Based on these results, this SFPE is an excellent candidate for use in high-performance lithium metal batteries .
研究领域:
材料科学
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电化学
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电池技术
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Pingping Chen,Qinghui Zeng,Qingyuan Li,Ruihua Zhao,Zhenfeng Li,Xin Wen,Wen Wen,Yu Liu,Anqi Chen,Zengxi Li,Xiangfeng Liu,Liaoyun Zhang
Solid-state polymer electrolytes (SPEs) have gained considerable attention in the application of all-solid-state lithium batteries (ASSLBs), but the low ionic conductivity at room temperature and inferior interfacial compatibility largely drag the practical development of SPEs. Herein, a ketone-containing poly(allyl acetoacetate) (PAAA) based polymer electrolyte is designed and prepared for the first time. The structure of ester and ketone groups provides PAAA polymers with not only strong dissociation of lithium salts but also weak coordination interactions with Li + ions. Thus the prepared PAAA polymer electrolytes show excellent ion conductive behavior with ionic conductivity as high as 1.1 × 10 -4 S cm −1 at 30 °C. Moreover, the PAAA polymer electrolytes still maintain superior viscoelasticity without compromising mechanical integrity. When assembling cells, the reduction-tolerant poly(ethylene oxide) (PEO) polymer electrolytes are employed as interlayers between the PAAA SPEs and lithium electrodes in order to improve interfacial stability. As a result, the hierarchical polymer electrolytes possess wide electrochemical window above 4.8 V, thus matching well with LiFePO 4 or Li 1.2 Ni 0.2 Mn 0.6 O 2 high-voltage cathode. The hierarchical structure does not affect interfacial contact, and the Li/PEO-PAAA-PEO/Li cells show low interfacial resistance and stable striping/plating behavior for at least 500 h at 0.2 mA cm −2 and 60 °C. This study enriches carbonyl-based polymer electrolytes by allying ketone with ester groups, and provides guidance for designing novel high-performance polymer electrolytes for practical application.
研究领域:
材料科学
·
电化学
·
电池技术
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DOI
高影响因子
危险品化学品经营许可证（带存储）