Energy & Environmental Science
·
2023
·Vol. 17
·期 3
·1163-1174
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IF 32.5
Ganxiong Liu,Wang Wan,Quan Nie,Can Zhang,Xinlong Chen,Weihuang Lin,Xuezhe Wei,Yunhui Huang,Ju Li,Chao Wang
A persistent challenge plaguing lithium-ion batteries (LIBs) is the consumption of active lithium with the formation of SEI. This leads to an irreversible lithium loss in the initial cycle and a gradual further exhaustion of active lithium in subsequent cycles. While prelithiation has been proven effective in compensating for this loss by introducing additional active lithium into batteries, prior studies have predominantly concentrated on offsetting the initial lithium loss, often overlooking the continuous lithium consumption that occurs throughout cycling. To address this challenge, we employed a sustained in situ lithium replenishment strategy that involves the systematic release of additional lithium inventory through precise capacity control during long-term cycling. Our method utilizes a lithium replenishment separator (LRS) coated with dilithium squarate-carbon nanotube (Li2C4O4–CNT) as the lithium compensation reagent. Placing Li2C4O4 on the separator rather than within the cathode significantly reduces disruptions in conduction pathways and inhibits catalytic reactions with LiFePO4, preventing the formation of carbon residues. When implemented in the LiFePO4||graphite battery system, our approach resulted in an impressive 12.9% capacity improvement in the initial cycle and a remarkable 97.2% capacity retention over 700 cycles, surpassing the comparison group, which exhibited 80% capacity retention after 426 cycles.
研究领域:
材料科学
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电化学
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DOI
高影响因子
Nature Communications
·
2025
·Vol. 16
·期 1
·1-12
·
IF 15.7
Shao Ahu,Wang Helin,Zhang Min,Liu Jiacheng,Cheng Lu,Li Yunsong,Guo Yuxiang,Wang Zhiqiao,Jia Qiurong,Wang Xin,Tang Xiaoyu,Zhao Xiaodong,Ma Yue
Anode-free lithium batteries represent a promising avenue for high-energy-density storage, yet their practical application is hindered by lithium inventory loss from parasitic interfacial reactions, cathode degradation, and limited Li + reversibility. Herein, we propose a polyolefin separator integrated with a Li 2 S@C sacrificial layer, achieving multiscale interfacial stabilization in Ah-class anode-free pouch cells. This approach simultaneously replenishes the customized Li + inventory during the formation cycle and establishes the lithium polysulfide-containing cathode interface with high-voltage tolerance (till 4.5 V). Real-time tracking via in-situ electrochemical impedance spectroscopy and transmission-mode operando X-ray diffraction reveals accelerated Li + diffusion kinetics and stabilized phase evolution in LiNi 0.8 Co 0.1 Mn 0.1 O 2 cathode interfaced with Li 2 S@C|PE prelithiation separator. Consequently, a 1.22 Ah pouch cell with an Ag-modified Cu foil and LiNi 0.8 Co 0.1 Mn 0.1 O 2 cathode is assembled with Li 2 S@C|PE separator and exhibits gravimetric and volumetric energy densities of 450 Wh kg -1 and 1355 Wh L -1 , respectively. This prelithiation protocol demonstrates upscaling potential and generic applicability to secure the interfacial chemistries for anode free/less lithium metal batteries.
研究领域:
材料科学
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电化学
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产品关联
DOI
PubMed
高影响因子
HYDROMETALLURGY
·
2022
·
IF 4.217
Jun Li,Qinglong Luo,Mingzhe Dong,Guoliang Nie,Zhong Liu,Zhijian Wu
Powder Li/Al-layered double hydroxides (LDHs) of Li 2 Al 4 (CO 3 )(OH) 12 ·3H 2 O were hydrothermally synthesized in one pot with sodium alginate as a structure modifier and granulated by crosslinked sodium alginate. The powder and granulated Li/Al-LDHs lithium adsorbents were characterized by FT-IR spectroscopy, XRD, SEM, TEM, XPS, and porosity. The adsorption-desorption performance of the granulated Li/Al-LDHs adsorbents was evaluated. Adsorption isotherm , adsorption kinetics , adsorption thermodynamics were investigated. The effects of solution pH, temperature, and the electrolytes (NaCl, Na 2 SO 4 , MgCl 2 , and KCl) on lithium adsorption, and the dissolution of granulated Li/Al-LDHs adsorbents after cyclic adsorption-desorption were also investigated. The granulated Li/Al-LDHs adsorbed 14.5 mg/g of lithium from the brine of East Taigener Salt Lake with a lithium concentration of 1400 mg/L. The granulation of powder Li/Al-LDHs by crosslinked alginate greatly reduced the dissolution of powder Li/Al-LDHs. The granulated Li/Al-LDHs adsorbents prepared in this report are promising materials for Li + extraction from salt lake brines.
研究领域:
材料科学
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环境科学
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产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2022
·
IF 6.371
Jianghai Wei,Xuewen Zheng,Weiteng Lin,Yu Si,Kemeng Ji,Chengyang Wang,Mingming Chen
Solid polymer electrolytes (SPEs) based solid-state lithium metal batteries (SSLMBs) are widespreadly practiced as one of the main technical routes aiming for chemically essential safety with acceptable energy density . However, uncontrollable Li dendrites growth and sluggish Li + transport remain obstacles to the further development of SPEs-based SSLMBs. Herein, a porous g-C 3 N 4 (PCN) is designed and introduced into polyethylene oxide (PEO). Within the following synthesized PEO-based composite solid electrolyte (PEO/PCN/LiTFSI CSE), PCN is found to be an attractive multifunctional filler. For its porous morphology and high specific surface area, abundant Lewis basic active sites are exposed, which facilitates Li + to be uniformly distributed in PEO/PCN/LiTFSI CSE and thus more effectively mitigates the Li dendrites growth comparing to those with bulk g-C 3 N 4 filler, making PCN-involved Li symmetrical cell (Li|PEO/PCN/LiTFSI|Li) run steadily for 1400 h under the current density of 0.1 mA cm −2 at 60 °C. PCN also accelerates Li + transport in the manner of reducing PEO crystallinity and promoting LiTFSI dissociation. The Li + conductivity of PEO/PCN/LiTFSI CSE reaches 3.47 × 10 −4 S cm −1 at 60 °C. Therefore, long life span and high rate performances are together achieved in SSLMB assembled with PEO/PCN/LiTFSI CSE. This work reveals a feasible strategy to fabricate dendrite-free SSLMBs cycling within a fairly long time.
研究领域:
材料科学
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能源存储与转换
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DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2022
·
IF 14.224
Qiyue Zhang,Ersha Fan,Jiao Lin,Sisheng Sun,Xiaodong Zhang,Renjie Chen,Feng Wu,Li Li
With the large-scale application of LiFePO 4 (LFP) in energy storage and electric vehicles, the recycling of spent lithium LFP batteries has gained more attention. However, recycling spent LFP is less economically feasible owing to the poor economic value of Fe products, which causes a problem for both the efficiency and economy. This work proposes a highly economical acid-free mechanochemical approach for the efficient and selective extraction of lithium (Li) from spent LFP battery cathode materials. The selective release of 98.9 % of Li from the LFP crystal structure is achieved at a reaction time of 5 h, a rotational speed of 500 rpm, and sodium citrate (Na 3 Cit) to LFP mass ratio of 10. Meanwhile, Fe is reserved in the form of FePO 4 in the olivine structure. The use of Na 3 Cit as a co-milling agent ensures a pollution-free recovery process and efficient extraction of Li + . The chelation of Li + with organic ligands (Cit 3- ) is the key to the efficient selective recovery of Li + from the olivine LFP structure via the mechanochemical process. The economic analysis indicates that the method is feasible and ensures industrial viability. The acid-free mechanochemical (MC) process reported in this work provides a novel route to selectively recover Li from spent LFP efficiently and highly economically.
研究领域:
材料科学
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环境科学
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产品关联
DOI
PubMed
高影响因子
Journal of Materials Chemistry A
·
2021
·Vol. 9
·期 38
·21695-21702
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IF 12.732
Xiaojie Shen,Guangyu Zhao,Xianbo Yu,Huihuang Huang,Ming Wang,Naiqing Zhang
Undesirable lithium dendrite growth limits the application of lithium metal anodes in high-energy storage batteries. Here, multifunctional SnSe–C composite modified 3D scaffolds are constructed to achieve dendrite-free lithium deposition. During the initial lithiation stage, the porous SnSe–C composite converts into a Li–Sn alloy and Li2Se by lithium reduction. The lithiophilic Li–Sn alloy exhibits a low nucleation barrier and realizes homogeneous lithium nucleation. The reductive product Li2Se with a high ionic conductivity facilitates lithium ion transport, which helps realizing the homogeneous lithium ion flux and reducing concentration polarization. Benefitting from the synergistic effect of the Li–Sn alloy and Li2Se, the Li/SnSe–C anode exhibits an ultralong lifespan over 1100 h with a low overpotential of 18 mV. In full-cell configurations with LiFePO4 cathodes, the Li/SnSe–C anode demonstrates enhanced rate capability and cycle stability with a high-capacity retention of 85% over 750 cycles. This work prepares multifunctional SnSe–C composite modified 3D scaffolds to regulate lithium nucleation and transport, which offers new insights and opportunities for developing dendrite-free lithium metal battery technology.
研究领域:
材料科学
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电化学
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储能技术
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产品关联
DOI
高影响因子
Energy Storage Materials
·
2023
·
IF 20.4
Chen Wu,Jieming Hu,Hanxian Chen,Chengyi Zhang,Mingli Xu,Lin Zhuang,Xinping Ai,Jiangfeng Qian
Prussian blue analogues (PBAs) have been attracting intense attention owing to its two-electron storage capability and considerable cost advantage, especially in Na-ion and K-ion batteries. However, things are quite different when it comes to Li-ion batteries, because lithium-containing Li 4 Fe(CN) 6 precursor is not commercially available and thus the traditionally prepared Li-deficient FeFe(CN) 6 products fail to couple with commercial graphite anode for full cells. Herein, we put forward a potential matching principle to guide the chemical pre-lithiation of FeFe(CN) 6 into a Li-rich Li x FeFe(CN) 6 ( x varies from 0 to 2) cathode. The potential matching principle was convincingly confirmed by theoretical analysis and over-lithiation experiments. Perylene-Li reagent was elaborately screened to serve as both Li + and electron donor for controllable chemical lithiation reaction while preserving the host framework stable. Our work provided a general guiding principle and effective methodology for controllable synthesis of Prussian blue analogues in gradient lithiation depth, which could be served as a platform for in-depth, systematic and comprehensive research on the properties of PBAs materials.
研究领域:
材料科学
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电化学
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能源存储
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Qiyue Fan,Jie Lin,Yue Sun,Xiangting Hu,Hang Yu,Zhenda Lu
Lithium manganese oxide (LMO) ion sieves are promising for lithium extraction due to their high adsorption capacity. However, their practical application is often limited by structural degradation from manganese leakage, reduced lithium uptake, and poor Li + /Mg 2+ selectivity, especially in brines with high Mg/Li ratios. To overcome these challenges, we in-situ synthesized polyamide (PA) nanofiltration membranes on the surface of LMO using two distinct amine monomers, polyethyleneimine (PEI) and piperazine (PIP), to create novel composite adsorbents LMO@PA(PEI) and LMO@PA(PIP). Both the coated materials demonstrated improved lithium uptake capacity and cyclic stability in adsorption-desorption cycles in simulated brine. More importantly, under a challenging Li/Mg ratio of 1:50 in binary ion solutions, the separation factors (α) of HMO@PA(PEI) and HMO@PA(PIP) were 2.23 and 4.55 times higher than that of uncoated HMO, showcasing excellent Li + /Mg 2+ selectivity. These findings highlight that polyamide nanofiltration layers successfully endow LMO with enhanced capacity, selectivity, and long-term stability, presenting a promising and scalable approach for direct lithium extraction from high‑magnesium salt lakes.
研究领域:
材料科学
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分离技术
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能源材料
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环境工程
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无机化学
✓ 已验证
产品关联
DOI
高影响因子
ACTA MATERIALIA
·
2025
·
IF 9.3
An Wang,Shaozhen Huang,Zhangdi Xie,Jiahua Liao,Wenhao Li,Yuejiao Chen,Huimiao Li,Zhe Wang,Zhibin Wu,Libao Chen
A growing need for high-energy-density lithium metal batteries appeal for utilize ultrathin (≤50 μm) free-standing Li metal anodes . However, challenges such as the formation of an unstable solid electrolyte interphase and the lithium dendrites growth have led to poor cycling performance and safety concerns, limiting the commercial viability of thin lithium metal anodes. This work introduces a facile approach by designing and fabricating an ultrathin Li-In alloy anode through in-situ vacuum melting and codirectional continuous rolling. The rolled ultrathin Li-In anode achieves the induction of uniform epitaxial electrodeposition of Li(110), which is attributed to the lithiophility of the densely distributed In₃Li₁₃ alloy phase and the coherent heterogeneous relationship between textured In₃Li₁₃(311) and Li(110).The symmetrical cell assembled by 50 μm Li-In alloy anode exhibits a prolonged lifespan for 1800 h under the conditions of 1 mA cm -2 and 3 mAh cm -2 . Meanwhile, the LiFePO 4 ||Li-In (50 μm) full cell achieves sTable 450 cycles with a retention of 90.3 % at 2 C (1 C = 170 mA g -1 ). This work paves the path for the practical ultrathin Li anode for commercializing the lithium metal batteries .
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DOI
高影响因子
ACS Nano
·
2023
·
IF 17.1
Shuaishuai Yan,Fengxiang Liu,Yu Ou,Hang-Yu Zhou,Yang Lu,Wenhui Hou,Qingbin Cao,Hao Liu,Pan Zhou,Kai Liu
Solid polymer electrolytes (SPEs) are the key components for all-solid-state lithium metal batteries with high energy density and intrinsic safety. However, the low lithium ion transference number (t+) of a conventional SPE and its unstable electrolyte/electrode interface cannot guarantee long-term stable operation. Herein, asymmetric trihalogenated aromatic lithium salts, i.e., lithium (3,4,5-trifluorobenzenesulfonyl)(trifluoromethanesulfonyl)imide (LiFFF) and lithium (4-bromo-3,5-difluorobenzenesulfonyl)(trifluoromethanesulfonyl)imide (LiFBF), are synthesized for polymer electrolytes. They exhibit higher t+ values and better compatibility with Li metal than conventional lithium bis(trifluoromethanesulfonyl) imide (LiTFSI). Due to the trihalogenated aromatic anions, LiFFF- and LiFBF-based electrolytes are prone to generate an LiF- and LiBr-rich solid electrolyte interphase (SEI), therefore increasing the stability of the solid electrolyte/anode interface. Particularly, LiFBF could induce a LiF/LiBr hybrid SEI, where LiF shows a high Young’s modulus and high surface energy for homogenizing Li ion flux and LiBr exhibits an extremely low Li ion diffusion barrier in the SEI layer. As a result, the Li/Li symmetric cells could remain stable for more than 1200 h without a short circuit and the LiFePO4/Li batteries showed superb electrochemical performance over 1200 cycles at 1 C. This work provides valuable insights from the perspective of lithium salt molecular structures for high-performance all-solid-state lithium metal batteries.
研究领域:
材料科学
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电化学
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能源存储
✓ 已验证
产品关联
DOI
PubMed
高影响因子
MOLECULES
·
2024
·Vol. 29
·期 13
·2975
·
IF 4.2
Jian Liu,Jingyi Lin,Zuwei Yin,Zhen Tong,Junke Liu,Zhen Wang,Yao Zhou,Juntao Li
In conventional lithium-ion batteries (LIBs), the active lithium from the lithium-containing cathode is consumed by the formation of a solid electrolyte interface (SEI) at the anode during the first charge, resulting in irreversible capacity loss. Prelithiation additives can provide additional active lithium to effectively compensate for lithium loss. Lithium oxalate is regarded as a promising ideal cathode prelithiation agent; however, the electrochemical decomposition of lithium oxalate is challenging. In this work, a hollow and porous composite microsphere was prepared using a mixture of lithium oxalate, Ketjen Black and transition metal oxide catalyst, and the formulation was optimized. Owing to the compositional and structural merits, the decomposition voltage of lithium oxalate in the microsphere was reduced to 3.93 V; when being used as an additive, there is no noticeable side effect on the performance of the cathode material. With 4.2% of such an additive, the first discharge capacity of the LiFePO4‖graphite full cell increases from 139.1 to 151.9 mAh g−1, and the coulombic efficiency increases from 88.1% to 96.3%; it also facilitates the formation of a superior SEI, leading to enhanced cycling stability. This work provides an optimized formula for developing an efficient prelithiation agent for LIBs.
研究领域:
材料科学
·
电化学
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产品关联
DOI
PubMed
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2018
·Vol. 28
·期 13
·1706513
·
IF 13.325
Xuyan Ni,Tao Qian,Xuejun Liu,Na Xu,Jie Liu,Chenglin Yan
The “shuttle effect” that stems from the dissolution of polysulfides is the most fatal issue affecting the cycle life of lithium-sulfur (Li–S) batteries. In order to suppress the “shuttle effect,” a new strategy of using a highly lithium ion conductive lithium fluoride/graphene oxide (LiF/GO) solid electrolyte interphase (SEI) to mechanically prevent the lithium dendrite breakthrough is reported. When utilized in Li–S batteries, the LiF/GO SEI coated separator demonstrates significant feature in mitigating the polysulfide shuttling as observed by in situ UV–vis spectroscopy. Moreover, the restrained “shuttle effect” can also be confirmed by analysis of electrochemical impedance spectroscopy and characterization of lithium dendrites, which indicates that no insulating layer of solid Li 2 S 2 /Li 2 S is found on lithium anode surface. Furthermore, the LiF/GO SEI layer puts out good lithium ion conductivity as its lithium ion diffusion coefficient reaches a high value of 1.5 × 10 −7 cm 2 s −1 . These features enable a remarkable cyclic property of 0.043% of capacity decay per cycle during 400 cycles.
研究领域:
材料科学
·
电化学
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）