ADVANCED FUNCTIONAL MATERIALS
·
2023
·Vol. 34
·期 3
·2306320
·
IF 19
Zunqiu Xiao,Yutong Li,Jin Leng,Kejia Xiang,Wei Wei,Huaying Wang,Zijian Hong,Zhongtai Zhang,Shitong Wang,Zilong Tang
Oxide solid electrolytes are attractive for the implementation of solid-state Li-ion batteries. However, constrained by the large ion-transport hindrance inside the densely packed lattice, their Li-ion conductivity can hardly reach the level of liquid electrolytes. A strategy of introducing confined water into the lattice paves a new way for enhancing the Li-ion transport, which has been reported in the previous studies. To further verify the universality of this strategy and unravel the facilitation mechanism, here this work establishes an ideal model using Li-H-Cl-O quaternary compounds with a wide electrochemical stability window. As a major kind of confined water, the content and type of ─OH groups are crucial parameters affecting the Li-ion conductivity. Through a controllable dehydration technique, the hydrogen-bonded ─OH groups can be mostly removed, leaving the free ─OH groups in lattice, which is beneficial to the increase of free volume and acceleration of rotation response. The 1–2 orders of magnitude enhancement of Li-ion conductivity ensures full cells good rate and cycling performance. This work not only addresses the controversy in Li-H-Cl-O about the hydrogen effect on Li-ion transport, but also provides detailed theoretical insights for the rational design of solid electrolytes.
✓ 已验证
DOI
高影响因子
Advanced Energy Materials
·
2022
·Vol. 12
·期 48
·2201801
·
IF 29.698
Mingsheng Qin,Mengchuang Liu,Ziqi Zeng,Qiang Wu,Yuanke Wu,Han Zhang,Sheng Lei,Shijie Cheng,Jia Xie
The advancements of lithium-ion batteries indubitably call for advanced electrolytes with superior environmental adaptability and long-term stability. Propylene carbonate (PC) proves to be a competitive solvent with the high permittivity and wide-liquid range, while the application is intrinsically hindered by the poor graphite compatibility and high viscosity. Here, a PC-based electrolyte with wide-temperature range is developed by tuning the strength and topology of the Li + -PC interactions via non-solvating interactions without altering the solvation structure. Thus, the problem of graphite exfoliation caused by Li + -PC co-intercalation can be successfully mitigated. Consequently, such electrolyte shows compatibility with both graphite and high-nickel cathode, exhibiting an expanded liquid range from −90 to 90 °C. This work, breaking from the traditional EC-based formula, provides a new strategy for designing PC-enabled electrolyte featuring high performance, wide-temperature compatibility, and sustainability
✓ 已验证
DOI
高影响因子
Advanced Energy Materials
·
2023
·Vol. 13
·期 16
·2204036
·
IF 27.8
Su Wang,Qifang Sun,Qing Zhang,Chen Li,Chaoran Xu,Yue Ma,Xixi Shi,Hongzhou Zhang,Dawei Song,Lianqi Zhang
The low ionic conductivity and short service life of solid polymer electrolytes (SPEs) limit the application of ambient-temperature polymer lithium metal batteries, which is perhaps a result of the inherent restricted segment movement of the polymer at room temperature. Herein, an ambient-temperature dual-layer solid polymer electrolyte is developed and the related working mechanisms are innovatively investigated. In the strategy, poly(propylene carbonate) (PPC)/succinonitrile (SN) contacts with the cathode while polyethylene oxide (PEO)/Li 7 La 3 Zr 2 O 12 is adopted near the anode. Molecular dynamics simulations demonstrate the formation of solvated sheath-like structure [SN···Li + ], which demonstrates strong interaction with polymers (PPC···[SN···Li + ]/PEO···[SN···Li + ]). Further density functional theory calculations show that these structures, allow rapid transport of Li ions through polymer segments. These results are confirmed with Fourier transform infrared spectroscopy and nuclear magnetic resonance. Therefore, the Li-ion transport mechanism for ambient-temperature SPEs can be reasonably revealed. Remarkably, the binding energy between PPC and SN is stronger than that of PEO, which helps avoid the parasitic reaction between SN and Li. A low overpotential of 55 mV is exhibited for Li/Li symmetrical cells after 1000 h. Notably, a capacity retention of 86.3% is maintained for LiNi 0.6 Co 0.2 Mn 0.2 O 2 /Li cell at 25 °C, implying good application potential in ambient-temperature high voltage lithium metal batteries.
✓ 已验证
DOI
高影响因子
Energy Storage Materials
·
2022
·
IF 20.831
Shuixin Xia,Lingli Luo,Xun Zhang,Liangfei Shen,Junhe Yang,Wei Liu,Shiyou Zheng
The practical implementation of Li metal has been severely obstructed by the uncontrolled dendritic Li growth and poor cycling efficiency. Herein, highly lithiophilic, ultrathin (∼60 nm) and conformal bismuth-oxygen-carbon layer-modified carbon fibers (CF@BOC) first prepared from the bismuth-based MOF membrane self-assembly were rationally adopted to stabilize Li metal. Highly efficient ultrasmall (∼1.8 nm) bismuth seeds and in-situ generated Li 2 O-enriched interphase can cooperatively enable the homogeneous Li nucleation/growth and extraordinarily high Li utilization efficiency. Consequently, the modified Li metal exhibits ultrahigh rate capability (10 mA cm −2 ) and ultralong lifespan stability (6900 cycles). Impressively, the Li|LiFePO 4 full cell delivers an exceptional long-term cycling over 200 cycles under the rather harsh condition of low negative-to-positive-capacity (N/P) ratio (∼0.44) and electrolyte-to-capacity (E/C) ratio (5 g Ah −1 ). And the Li|LiCoO 2 full cell also reveals a prolonged cycling performance even at the ultralow N/P ratio (∼0.26) with a remarkable energy density of 361.3 Wh kg −1 . Furthermore, the pouch cell with a high loading cathode (3.6 mAh cm −2 ) still demonstrates prolonged cycling lifespan under the practical condition of extremely limited Li metal and lean electrolyte. This work enlightens a significant stride toward highly stable Li metal anode for practicability.
✓ 已验证
DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2025
·
IF 9
Ting Qi,Xiaona Wei,Xianfu Chen,Tiandan Lu,Dongliang Jin,Jing Zhong
Nanofiltration (NF) membranes are emerging as promising candidates for lithium extraction. However, their performance is challenged by the comparable physicochemical characteristics of Li + and Mg 2+ . In this work, a dual-reinforcement strategy is proposed to simultaneously enhance both selectivity and permeability by combining the densification of the polyamide (PA) network and the construction of Li + -selective transport channels. During the interfacial polymerization of piperazine (PIP) and trimesoyl chloride (TMC), the cross-linking density of the PA layer is increased by adding sodium dodecyl sulfate (SDS), while Li + -selective transport nanochannels are constructed by incorporating 15-crown-5 ether (CE). This synergistic modification enhances Mg 2+ rejection via intensified size exclusion and facilitates Li + permeation through ion-specific recognition. The resulting PIP/SDS/CE-PA membrane exhibits a high cross-linking degree of 91.26 %, a reduced pore size of 0.70 nm, and a narrow pore size distribution (σ = 1.22). Molecular dynamics simulations confirm the preferential complexation of CE with Li + , and that Li + exhibits faster and more favourable translocation in the PIP/SDS/CE-PA membranes, thereby facilitating its selective transport. Experimentally, the membrane achieves a high MgCl 2 rejection of 97.1 % and a low LiCl rejection of 56.7 %, yielding an exceptional Li + /Mg 2+ selectivity of 30 in a MgCl 2 /LiCl binary system, while maintaining a water permeance of 5 L m −2 h −1 bar −1 . These findings demonstrate the strong potential of the PIP/SDS/CE-PA membrane for the direct treatment of high Mg 2+ /Li + ratio salt-lake brines and offer a versatile strategy for designing next-generation NF membranes for selective ion separations.
✓ 已验证
产品关联
DOI
高影响因子
Materials Today Chemistry
·
2025
·
IF 6.7
Yuan Wang,DouDou Zhang,Hao song,Xiuxia Yang,Zhichao Liu,Yuankang Wang,Jie Yu,Xu Tian
X-ray scintillators are crucial for medical, industrial, and security imaging systems. However, achieving dual-mode of real-time and delayed imaging within a single matrix still faces challenges. Herein, LiGa 5 O 8 : Tb 3+ was successfully synthesized by the high-temperature solid-phase method. By controlling the atmosphere and optimizing the Li + /Ga 3+ ratio, the trap structure of LiGa 5 O 8 : Tb 3+ spinel phosphors is effectively adjusted, which achieved excellent dual-mode imaging. The air-synthesized Li 1.6 Ga 5 O 8 :4 %Tb 3+ exhibits intense X-ray excited persistent luminescence (X-PersL, 595 nm), while the sample of LiGa 5 O 8 :Tb 3+ reduced in H 2 /N 2 shows enhanced radioluminescence (RL) without X-PersL. This precise manipulation of anti-occupancy defects controls the charge trapping/detrapping dynamics, enabling switchable RL (real-time imaging) and X-PersL (delayed imaging) modes through the single Tb 3+ ions emission. The result resolves the incompatibility between prompt and persistent X-ray responses in conventional scintillators. The defect-regulation method establishes a universal strategy for developing scintillators compatible with complex operational demands, advancing high-performance X-ray imaging technologies.
✓ 已验证
产品关联
DOI
高影响因子
Energy & Environmental Science
·
2024
·Vol. 17
·期 11
·3807-3818
·
IF 32.4
Shenyang Xu,Zhefeng Chen,Wenguang Zhao,Wenju Ren,Chenxin Hou,Jiajie Liu,Wu Wang,Chong Yin,Xinghua Tan,Xiaobing Lou,Xiangming Yao,Zhihai Gao,Hao Liu,Lu Wang,Zuwei Yin,Bao Qiu,Bingwen Hu,Tianyi Li,Cheng Dong,Feng Pan,Mingjian Zhang
As commercial cathodes with the highest practical capacity, the structural nature of Li-rich Mn-based (LMR) cathodes, composite or solid solution, is still under debate. Due to the extreme structural similarity of two layered-phase components, namely, the monoclinic phase (C2/m) and rhombohedral phase (Rm), no single tool can resolve this concern alone. Herein, we combined multiple advanced techniques to comprehensively study the structural changes during synthesis of LMR cathodes from different aspects such as the elemental distribution, local structure, long-range structure, and short-range structure, revealing a clear process from the formation of two phases to the gradual phase fusion and eventually to a nearly solid solution. Particularly, X-ray pair distribution function (PDF) analysis combined with theoretical simulations reveals for the first time that the transition metal (TM)–TM distance increases with the progress of the phase fusion, which makes the short-range structural change in TM–TM atomic pairs an effective parameter for judging the extent of phase fusion. Eventually, excellent electrochemical performance was achieved by balancing capacity and cycling stability through adjusting the phase fusion to a medium extent in lithium and sodium two layered-phase components. This study establishes an approach to investigate the structural evolution in the complicated multiple-phase system and provides valuable insights into the design and optimization of cathodes by tuning the phase fusion extent.
✓ 已验证
DOI
高影响因子
DESALINATION
·
2025
·
IF 9.8
Shuwei Jia,Jun Wei,Xinyu Ma,Zhi Wang
High-efficiency lithium extraction from salt lakes is pivotal to meet escalating lithium demand driven by energy storage and electric vehicle industries. In this study, the small-molecule aminoacetonitrile (AAN) was introduced as an aqueous-phase co -monomer to modulate the interfacial polymerization process between polyethyleneimine (PEI) and trimesoyl chloride (TMC). Specifically, the primary amine in AAN molecules reacted with acyl chloride moieties in TMC, occupying reaction sites and thereby preserving a larger fraction of unreacted primary amine groups on the PEI chains within the separation layer, which significantly enhanced the membrane's surface positive charge. Simultaneously, the nitrile groups of AAN preferentially coordinated with Li + ions to effectively counteract the repulsive effect of the strongly positively charged membrane surface on Li + . This “charge-coordination” synergistic mechanism enabled precise control over the separation process. When treating mixed salt solution with a Mg 2+ /Li + mass ratio of 100, the optimized membrane achieved a separation factor of 74.7, along with enhanced MgCl 2 rejection of 99.3 % compared to virgin membrane's 93.9 %, and reduced LiCl rejection from 56.3 % to 49.3 %. Notably, upon treatment of simulated salt lake brine, the membrane manifested a pronounced Li + enrichment effect, with a LiCl rejection rate of −8.8 % while retaining a high MgCl 2 rejection capacity. This study employed a simple preparation process with industrialization potential, providing a guiding strategy for constructing high-selectivity membranes for Mg 2+ /Li + separation.
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Yuhang Shan,Hang Yang,Libo Li,Yangmingyue Zhao,Shubo Fan,Suo Li
Lithium-sulfur batteries that utilize polymer electrolytes can significantly reduce polysulfide shuttling, offer high safety, and represent a promising energy storage solution. However, constructing efficient ion transport pathways at the electrode/electrolyte interface and within the cathode of solid-state lithium-sulfur batteries remains challenging. In this study, we proposed a polymer electrolyte made from a poly (vinylidene fluoride co-hexafluoropropylene) (PVDF-HFP) matrix with neodymium trioxide (Nd 2 O 3 ) nanorods as fillers. This polymer electrolyte slurry was incorporated into the cathode to establish a lithium-ion pathway between the electrode and the electrolyte. The potential difference between Nd 2 O 3 and the carbon layer generates an internal electric field, facilitating the formation of a smooth lithium-ion transport channel in a solid-state environment. We visualized these lithium-ion transport channels across the cathode interface using Molecular Dynamics (MD) simulations in an electric field. Simultaneously, the abundant oxygen vacancies in Nd 2 O 3 can interact with carbon groups in N,N-Dimethylformamide (DMF), promoting the formation of [Li(DMF) x ] + complexes. This interaction effectively reduces the radicalized DMF and enhances lithium-ion (Li + ) conduction. As a result, the solid-state lithium-sulfur battery demonstrated excellent cycling performance at room temperature, achieving a specific capacity of 940.8 mAh g −1 at a rate of 0.1C. This work contributes valuable insights for developing solid-state lithium-sulfur batteries with improved compatibility at electrode/electrolyte interfaces.
✓ 已验证
产品关联
DOI
高影响因子
Nano Energy
·
2021
·
IF 17.881
Dewang Li,Xiuyao Lang,Yong Guo,Yiqiao Wang,Yanyin Wang,Hucheng Shi,Shichao Wu,Weichao Wang,Quan-Hong Yang
Li-O 2 batteries are one of the most promising next generation batteries due to their high energy density . However, they suffer from high charge overpotentials and severe side reactions. Here we report a bifunctional CeVO 4 catalyst that not only lowers the charge potential by a photo-assisted mechanism, more importantly, promotes the efficient conversion of highly reactive oxidative intermediates to Li 2 O 2 , thus avoiding the oxidative decomposition of the electrolyte/cathode during discharge. Benefiting from its efficient electrocatalysis and the improved charging ability, 1.6x higher discharge capacity up to 6.14 mAh cm -2 , low charge potential of 3.48 V and stable cycling performance are simultaneously achieved. Theoretical calculation and in-situ Raman spectra confirm the superior adsorptive and conversion ability of superoxide species by electrochemical reduction and chemical disproportionation reactions on the CeVO 4 catalyst. These results indicate an effective strategy to break through the reported limitations of photo-assisted cathodes that are of a low electrocatalysis ability and limited discharge capacity. The significance of retaining a high energy density in photo-assisted Li-O 2 batteries is highlighted.
✓ 已验证
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2024
·
IF 7.1
Tingyan Ren,Keyi Lin,Man Zhao,Bozhang Lai,Jujun Ruan
Selective extraction of Li from spent lithium-ion batteries (LIBs) is currently a hot topic. However, current research techniques focus on selectively extracting Li from cathode materials, and there are problems with high energy consumption, complex processes, and high difficulty in technical application. And Li in the anode material was ignored. Therefore, this study proposes a technique for selectively extracting Li from anode materials using aqueous solutions. The experimental results show that there is 4.15% Li in the anode material carbon black powder. Under acidic, alkaline, and pure water conditions, the extraction rate of Li from anode materials is greater than 90.00%. Acidic and alkaline conditions can leach heavy metals such as Ni/Co/Mn/Cu, requiring secondary treatment of wastewater, while the concentration of heavy metals leached from water can be directly discharged. When ultrasonic leaching is used for 5–10 min, the leaching rate is greater than 90.00%. When shaking leaching is used for 30–60 min, the leaching rate is greater than 90.00%. When standing leaching is used for 60–120 min, the leaching rate is greater than 90.00%. In the actual production process, suitable enhanced leaching methods can be selected according to different needs. This article may be the first study to propose the selective extraction of Li from anode materials using aqueous solutions.
✓ 已验证
DOI
高影响因子
RSC Advances
·
2025
·Vol. 15
·期 16
·12528-12537
·
IF 4.6
Junbo Wang,Jie Jiang,Jing Wang,Shouyuan Hu,Jiahao Hu,Yalong Li,Zhiyu Tao,Chengju Wu,Pei Li,Liang Chen
Nanofiltration has emerged as an effective technique for the selective separation of mono- and divalent ions, such as Mg2+/Li+ mixtures, and plays a crucial role in lithium extraction from salt lakes. In this study, a graphene oxide (GO) membrane with positively charged channels was prepared by crosslinking arginine (Arg) onto GO nanosheets, followed by vacuum filtration to form the membrane, and then thermal reduction (Arg-rGO). The Arg-rGO membrane exhibits high performance in the ion separation of a typical brine with a Mg2+/Li+ mass ratio of 20. The separation factor (SLi/Mg) reached up to 45.6—two times the highest separation factor reported—while maintaining an advanced water permeance of 21.3 L m−2 h−1 bar−1. Furthermore, the Mg2+/Li+ mass ratio was reduced from 20 to 0.2 after two-stage crossflow filtration with high flux under high pressure. The observed separation performance can be attributed to the synergistic effect of electrostatic repulsion and size-exclusion. These findings confirmed efficient separation of Mg2+/Li+ using GO membranes, demonstrating potential for practical application in lithium extraction from salt lakes.
✓ 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）