iScience
·
2025
·
IF 4.1
Kai Chen,Jia−Yi Du,Haoran Zhang,Yingqi Fan,Dong−Yue Yang,Jin Wang,Kai Li,Gang Huang
Lithium (Li)−CO 2 batteries, capable of converting CO 2 to Li 2 CO 3 /C while delivering significant energy, have attracted extensive research interest. However, their feasibility remains controversial and underexplored. To address this, a rigorous testing system combining ECC−Air battery models and differential electrochemical mass spectrometry (DEMS) was developed to ensure a pure gas environment. Findings reveal that even minute O 2 permeation (0.5%) from air can elevate the discharge plateau, misleadingly transforming Li−CO 2 into Li−O 2 /CO 2 batteries. Under strict testing, true Li−CO 2 battery performance falls short of reported successes. Experimental and theoretical confirmation shows the 4Li + 3CO 2 → 2Li 2 CO 3 + C reaction proceeds at a lower discharge plateau (<2.0 V), a voltage window traditionally overlooked. This work underscores the need for rigorous testing to enhance scientific reliability in Li−CO 2 battery research so that this field can develop sustainably.
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DOI
PubMed
高影响因子
CERAMICS INTERNATIONAL
·
2017
·
IF 2.986
Junhao Zhang,Tingting Yu,Jiale Chen,Huili Liu,Dongqin Su,Zehua Tang,Jinfeng Xie,Lei Chen,Aihua Yuan,Qinghong Kong
Germanium-based materials possess promising potential as novel anode materials for high performance lithium-ion batteries (LIBs). However, the considerably huge volume change causes rapid capacity fade during the charge-discharge process. A simple strategy was devised to prepare porous GeO 2 nanoparticles via thermal decomposition of (Hbipy) 2 [Ge(C 2 O 4 ) 3 ]·2H 2 O in air atmosphere. As an anode material for LIBs, it shows superior electrochemical performance in comparison with commercial GeO 2 microparticles . The initial discharge capacity of porous GeO 2 nanoparticles is high to 2578.8 mA h/g, and it still retained 581.9 mA h/g after 100 cycles. Even at 2 A/g, a reversible discharge capacity of 184.2 mA h/g is yet obtained. The superior lithium storage performances should be chalked up to the positive synergism of nanoscale, porous structure and low crystalline nature, which effectively retard the huge volume change of GeO 2 and are beneficial for fast diffusion of lithium ions during cycling.
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高影响因子
Nanomaterials
·
2021
·Vol. 11
·期 6
·1429
·
IF 5.076
Qiang Pang,Xiangyu Yu,Shijing Zhang,Wei He,Siyu Yang,Yao Fu,Ying Tian,Mingming Xing,Xixian Luo
Aqueous zinc-ion batteries (AZIBs) are promising candidates for large-scale energy storage because of their low cost and high safety. However, their practical applications are impeded by low energy density and short service life. Here, an aqueous Zn2+/Li+hybrid-ion battery is fabricated using the LiV3O8nanorods as the cathode, metallic Zn as the anode, and 3 M Zn(OTf)2+ 0.5 M LiOTf aqueous solution as the electrolyte. Compared with the batteries using pure 3 M Zn(OTf)2electrolyte, the cycle performance of the hybrid-ion battery is significantly improved. After 4000 cycles at 5 A g1, the remaining capacity is 163.9 mA h g−1with impressive capacity retention of 87.0%. Ex-situ XRD, ex-situ XPS, and SEM tests demonstrate that the hybrid electrolyte can inhibit the formation of the irreversible Zn3(OH)2V2O7·2H2O by-product and restrict Zn dendrite growth during cycling, thereby improving the cycle performance of the batteries.
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高影响因子
Journal of Materials Chemistry A
·
2024
·
IF 10.7
Zhedong Liu,Cuihua Zeng,Jingchao Zhang,Jiawei Luo,Zhaoxin Guo,Zekun Li,Rui Liu,Wei-Di Liu,Jia Ding,Yanan Chen,Wenbin Hu
Li-rich cathode materials are one of the most potential candidates for next-generation Li-ion batteries. However, they suffer from severe capacity degradation because of cracks and the continuous structural transformation during cycling. Defect engineering can effectively tune the electronic and crystal structure of nanomaterials and improve the electrochemical performance of cathode materials. Up to now, it is challenging to introduce dense defects into the materials synthesized by conventional tube furnace calcination due to the thermodynamic and kinetic equilibrium. In this work, a non-equilibrium high temperature shock (HTS) strategy with ultra-fast cooling, accompanied by the processes of rapid heating and cooling, is reported to introduce the twin boundaries (TBs) into the Li1.2Ni0.13Co0.13Mn0.54O2. The rock-salt phase along the TBs acts as a rigid framework that mitigates the inherent phase transformation of Li-rich layered-oxide materials during cycling. Benefiting from the unique structure, Li1.2Ni0.13Co0.13Mn0.54O2 prepared by HTS method exhibits a superior reversible capacity of 278 mAh g-1 at 0.1 C, a high initial Coulombic efficiency of 81%, and capacity retention of 89.4% after 100 cycles at 0.5 C. This work exerts profound implications on understanding defect engineering for modulating structure and electrochemical performance of materials.
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高影响因子
Energy Storage Materials
·
2025
·
IF 20.2
Yiping Liu,Yuxin Huang,Qiang Zhang,Rouyan Guo,Guangqi Zhang,Jie Dong,Liancheng Zhao,Liming Gao
Ideal solid electrolyte interphase (SEI) is required for non-dendrite lithium (Li) deposition of lithium metal batteries (LMBs). However, the spontaneously-formed SEI is non-homogenous in the composition and structure and thus cause oriented distribution of Li + flux, which leads to the detrimental formation of lithium dendrites and poor cyclability of batteries. Here we propose a vertical & lateral ion-flux modulated ion-conductive SEI for high-voltage Li-metal batteries. A fluorinated MCM-41 (FMCM-41) modified LiPF 6 electrolyte is designed to construct the SEI film, which consists of homogenously distributed LiF and Li x SiO y , to regulate Li + transport paths in the lateral and the vertical direction, respectively, achieving uniform lithium plating. With the FMCM-41 modified electrolyte, the prepared Li||Li cell presents a long-term stability over 1000 h, and the Li||NCM622 full cell exhibits outstanding cycling performance with a high specific capacity of 169.9 mAh g -1 and a high-capacity retention of 93.3 % over 100 cycles at 0.5 C. This lateral-vertical concept provides a promising strategy for designing a desired SEI with uniform Li + transport paths to achieve ultra-long and high-rates lithium metal batteries.
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高影响因子
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.
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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
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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.
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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.
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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.
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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.
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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.
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