JOURNAL OF PHYSICS AND CHEMISTRY OF SOLIDS
·
2025
·
IF 4.9
Huan Huan,Wei Wu,Qingyi Feng,Yongliang Tang,Sean Li,Hongxiang Deng,Xia Xiang,Xiaotao Zu,Yangfang Li
Wrinkled graphene prepared by the bubbling chemical vapor deposition method was ball milled to produce active materials for lithium-ion battery anode. By controlling milling parameters, the graphene with optimum electrode performance was obtained. After 2000 cycles at a current of 2000 mA g −1 , the reversible specific capacity can be maintained at 213.04 mAh g −1 , with a retention rate of 150.61 %. It was found that two lithium storage mechanisms coexist in this graphene material, and their capacitive control plays a major role, for example, accounting for 75.87 % contribution at a voltage scan rate of 0.8 mV s −1 . To further improve the electrode performance, B and N co-doped graphene was also prepared through ball milling. The results showed that, at the current of 2000 mA g −1 , the reversible specific capacity after 2000 cycles could reach 225.59 mAh g −1 , which was 5.9 % higher than that of the undoped one.
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高影响因子
JOURNAL OF MATERIALS SCIENCE
·
2025
·
IF 3.9
Chen Zheng,Liu Peng,Cao Yu-Long,Xie Yu-Long
The manganese-based ion sieve H 1.6 Mn 1.6 O 4 shows significant advantages in lithium adsorption. Its prominent features include high adsorption capacity and low pollution characteristics of the preparation process. These combined advantages make this material important in the lithium extraction technology in salt lakes. However, problems such as high manganese dissolution loss rate, poor cyclic stability, and difficulty in powder recycling seriously restrict the industrialized application. In this paper, we propose to optimize the structure of spinel-type manganese lithium ion-sieves with a 2% Co 3+ doping strategy, which can effectively inhibit the lattice collapse triggered by Jahn–Teller aberration during the pickling cycle by replacing part of the Mn 3+ active sites with Co 3+ . After doping, the relative Mn 4+ content on the surface of the material increased from 58%–61% according to the XPS test, confirming that the introduction of Co 3+ facilitated the transition of Mn 3+ to the higher valence state Mn 4+ through the charge compensation effect. Reducing the disproportionation activity of Mn 3+ reduces the dissolution loss of Mn 2+ during the pickling process. The experimental results showed that the adsorption of doped HMCO-2 material increased from 28.8–34.9 mg/g. The adsorption capacity retention rate was 77% after five cycles, there was a high selective adsorption of Li + , and the manganese dissolving loss rate was decreased to 2.3%.
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NATURE
·
2025
·Vol. 637
·期 8047
·846-853
·
IF 48.5
Song Huimin,Münch Konrad,Liu Xu,Shen Kaier,Zhang Ruizhuo,Weintraut Timo,Yusim Yuriy,Jiang Dequan,Hong Xufeng,Meng Jiashen,Liu Yatao,He Mengxue,Li Yitao,Henkel Philip,Brezesinski Torsten,Janek Jürgen,Pang Quanquan
With promises for high specific energy, high safety and low cost, the all-solid-state lithium–sulfur battery (ASSLSB) is ideal for next-generation energy storage 1 , 2 , 3 , 4 , 5 . However, the poor rate performance and short cycle life caused by the sluggish solid–solid sulfur redox reaction (SSSRR) at the three-phase boundaries remain to be solved. Here we demonstrate a fast SSSRR enabled by lithium thioborophosphate iodide (LBPSI) glass-phase solid electrolytes (GSEs). On the basis of the reversible redox between I − and I 2 /I 3 − , the solid electrolyte (SE)—as well as serving as a superionic conductor—functions as a surficial redox mediator that facilitates the sluggish reactions at the solid–solid two-phase boundaries, thereby substantially increasing the density of active sites. Through this mechanism, the ASSLSB exhibits ultrafast charging capability, showing a high specific capacity of 1,497 mAh g −1 sulfur on charging at 2C (30 °C), while still maintaining 784 mAh g −1 sulfur at 20C. Notably, a specific capacity of 432 mAh g −1 sulfur is achieved on charging at an extreme rate of 150C at 60 °C. Furthermore, the cell demonstrates superior cycling stability over 25,000 cycles with 80.2% capacity retention at 5C (25 °C). We expect that our work on redox-mediated SSSRR will pave the way for developing advanced ASSLSBs that are high energy and safe.
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Nano Energy
·
2022
·
IF 19.069
Liping Ren,Fanpeng Kong,Xufeng Wang,Yajie Song,Xudong Li,Fang Zhang,Nan Sun,Hanwen An,Zaixing Jiang,Jiajun Wang
The limited stability and the excessive dependence on external heating sources restrict the development of polymer-based solid-state Li-O 2 batteries . Herein, we propose a multifunctional composed cathode with the photo-electro-thermal synergy to achieve a PEO-based solid-state Li-O 2 (PSS Li-O 2 ) battery operating at room temperature. The multifunctional composed cathode consists of the traditional black TiO 2 photocatalyst and carbon cloth (b-TiO 2 /CC). The b-TiO 2 /CC harvests a full spectrum of sunlight, besides the photo-generated electrons and holes enhancing reaction kinetics during discharging and charging processes, though converting solar energy into heat to achieve self-heated replace on external. The photo-electro-thermal synergy-triggered PSS Li-O 2 battery establishes a low overpotential of 0.26 V and long durability of up to 90 cycles, which is a breakthrough for PEO-based Li-O 2 batteries operating at room temperature. A flexible PSS Li-O 2 battery is constructed and exhibits superior flexibility and mechanical stability . The mechanism of the photo-electro-thermal synergy provides a new strategy for PSS Li-O 2 batteries and advances the high-efficiency utilization of solar energy in portable devices.
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Nature Communications
·
2024
·Vol. 15
·期 1
·1-9
·
IF 14.7
Chen Ze,Wang Tairan,Wu Zhuoxi,Hou Yue,Chen Ao,Wang Yanbo,Huang Zhaodong,Schmidt Oliver G.,Zhu Minshen,Fan Jun,Zhi Chunyi
The high redox potential of Zn 0/2+ leads to low voltage of Zn batteries and therefore low energy density, plaguing deployment of Zn batteries in many energy-demanding applications. Though employing high-voltage cathode like spinel LiNi 0.5 Mn 1.5 O 4 can increase the voltages of Zn batteries, Zn 2+ ions will be immobilized in LiNi 0.5 Mn 1.5 O 4 once intercalated, resulting in irreversibility. Here, we design a polymer hetero-electrolyte consisting of an anode layer with Zn 2+ ions as charge carriers and a cathode layer that blocks the Zn 2+ ion shuttle, which allows separated Zn and Li reversibility. As such, the Zn ‖ LNMO cell exhibits up to 2.4 V discharge voltage and 450 stable cycles with high reversible capacity, which are also attained in a scale-up pouch cell. The pouch cell shows a low self-discharge after resting for 28 days. The designed electrolyte paves the way to develop high-voltage Zn batteries based on reversible lithiated cathodes.
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高影响因子
Science China-Chemistry
·
2025
·
IF 9.7
Huang Wenhuan,Wang Shun,Hou Xuehan,Zhang Yanan,Zhang Xingxing,Zhao Yaoxiao,Jin Xilang,Zhang Huabin,Wang Fei,Zhang Jian
Lithium-sulfur (Li-S) battery, as a promising next-generation high-energy-density battery, suffers from lithium polysulfides (LPSs) shuttle and Li dendrites issues. Porous crystalline framework-based membranes as separator can effectively absorb and restrain LPSs but without precise structural design principal exploration and mechanism studies. Herein, bio-inspired 1D oriented lithium-ion transport channels with molecular negatively charged PO 3 (−1) have been developed in hybrid tetrazole frameworks for promoting the transmission of Li + ions. The theoretical calculations and in situ spectroscopy demonstrated the higher binding energy and inhibited diffusion of LPSs in PO 3 . The assembled PP@PO 3 Janus separator in Li-S coin cell delivered a high initial capacity of 1410.9 mAh g −1 at 0.1 C and a low attenuation rate of 0.038% per cycle over 500 cycles at 5 C. Besides, the high capacities of 862, 542 and 409 mAh g −1 based on high-sulfur-loading cathodes of 2.6, 3.8 and 5.0 mg cm −2 at 0.5 C were achieved, respectively. Moreover, the punch battery of PO 3 @PP separator with S-cathode of 1.2 mg cm −2 has been developed for demonstrating its potentials commercial application, which displays impressive capacity of 873.4 mAh g −1 with the retention of ∼78.9% over 50 cycles.
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ACS Omega
·
2025
·
IF 4.3
Zhihua Xu,Yu Wu,Yangyang Zheng,Yucheng Chen,De Li,Wenting Ji,Yong Chen
As a well-known graphite-like material in superconductivity, lithium borocarbide (LiBC) can also be utilized as an electrode material in Li-ion batteries with a high specific capacity, which is assigned to the B–B bond produced through the aqueous reaction or the initial charge process. In this work, a rod-like LiBC sample (Ti-LiBC) is synthesized with the precursors of LiH + B + graphite in a sealed Ti tube through high-temperature sintering. Compared with the normal SUS-LiBC sintered in a sealed SUS304 tube, the Ti-LiBC possesses a lot of B–B bonds and a strong EPR signal, and it delivers a higher specific capacity (ca. 500 mAh g–1 at a mean discharge and charge potentials of 0.85 and 1.89 V, respectively) with excellent rate and cycle performances. Actually, the Ti metal can react with the H2 gas to produce the TiH2 phase at a high temperature, of which the extent determines the morphology of LiBC product, and the substitution of Li metal for LiH as the precursor can also result in the rod-like structure and the high specific capacity. Therefore, a hydrogen-free atmosphere is the key to synthesizing rodlike LiBC with excellent electrochemical properties, and this strategy might be extended to other graphite-like materials.
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Joule
·
2023
·
IF 39.8
Yatao Liu,Linhan Xu,Yongquan Yu,MengXue He,Han Zhang,Yanqun Tang,Feng Xiong,Song Gao,Aijun Li,Jianhui Wang,Shenzhen Xu,Doron Aurbach,Ruqiang Zou,Quanquan Pang
The transition from dissolution-precipitation to quasi-solid-state sulfur reaction promises restricted polysulfide shuttle and lean electrolyte operation of Li-S batteries but incurs poor reaction kinetics. We here demonstrate that structural reorganization of sparingly solvating electrolytes (SSEs)—which is uniquely afforded by using low-density and low-cost aromatic anti-solvents—is vital for taming the quasi-solid-state sulfur reaction. Aromatic anti-solvents disrupt the interconnected structure of concentrated tetrahydrofuran (THF) electrolyte, uniquely creating subdomains that act to dissolve elemental sulfur, thus accelerating its consumption and re-formation while maintaining ultralow polysulfides solubility. The altered subdomains further result in robust solid electrolyte interphase (SEI) on lithium metal. As a result, the Li-S cell with a 3 mg sulfur cm −2 sulfur cathode can cycle steadily for ∼160 cycles with a lean electrolyte of 5 μL mg sulfur −1 . Our work provides new insights into fine-tuning the electrolyte microstructure through solvent innovations for developing sulfur-based batteries that are high energy, cheap, and durable.
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Materials
·
2025
·Vol. 18
·期 10
·2373
·
IF 3.2
Jing Zhu,Xiyun Yang,Yongqiang Huang,Rongzheng Yao
With the depletion of solid lithium ore, extracting lithium from salt lake brine has become a critical focus for future endeavors. A four-step method was used to synthesize high-purity H1.6Mn1.6O4for extracting Li+. Porous cubic Mn2O3was hydrothermally synthesized with carbon spheres and surfactants as templates. Then, it was converted to LiMnO2by calcining with Li2CO3. After roasting and acid pickling, H1.6Mn1.6O4was successfully synthesized. The impacts of calcination temperature, Li/Mn molar ratio and glucose addition on LiMnO2composition, loss percentage of dissolved Mn in precursor, and the adsorption characteristics of the lithium ion sieve were studied. Glucose inhibited the formation of LiMn2O4and promoted the formation of pure LiMnO2. The resulting precursor without impurities showed porous structure. After acid pickling, H1.6Mn1.6O4showed a high-adsorption performance and excellent cycle performance. After five cycles, adsorption capacity remained above 30 mg/g, and the loss percentage of dissolved Mn stabilized at about 1%. The Li+–H+exchange conformed to pseudo-second-order adsorption dynamics and the Langmuir adsorption isotherm equation, indicating that the adsorption process can be classified as monolayer chemical adsorption.
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ACS Applied Energy Materials
·
2025
·
IF 5.5
Chenxin Diao,Xianhui Jiao,Jin Xu,Hui Zhan
Lithium/carbon fluoride (Li/CFx) primary batteries have attracted wide attention because of their high energy density. However, their application in high-power devices is severely hindered by the retarded reaction kinetics caused by lithium fluoride (LiF) accumulation and difficult desolvation, which is further intensified by low temperature. In this work, an electrolyte strategy has been proposed targeting the kinetic issues. The methyl acetate (MA) low-temperature solvent weakens the Li+ coordination and facilitates the Li+ desolvation, while crown ether provides a LiF removal effect through its complexing capability. After comprehensive optimization, the benzo-12-crown-4 (B12C4)- and MA-containing electrolyte significantly enhances the rate performance as well as low-temperature output of the CFx cathode, endowing it with excellent wide-temperature adaptability. This work not only greatly improves the electrochemical property of the CFx electrode but also provides an alternative electrolyte strategy for all-climate and high-power/energy Li/CFx cells.
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JOURNAL OF MEMBRANE SCIENCE
·
2025
·
IF 9
Yushuang Lin,Nan Li,Weihao Xue,Hong Chen,Zhiruo Zhang,Zhao Dai
Achieving precise pore size tuning in nanofiltration membranes for Mg 2+ /Li + separation remains challenging due to the similar hydrated radii of the ions and the lack of real-time monitoring for dynamic adjustments. In this study, we developed a novel pH-responsive color-changing nanofiltration membrane with tunable pore sizes, enabling real-time monitoring and enhanced separation efficiency. By incorporating γ-cyclodextrin during interfacial polymerization, we achieved angstrom-level pore size tuning and reduced pH sensitivity. The color response of the membrane enables dynamic adjustments to the feed solution pH, optimizing pore radii to ∼0.41 nm, leading to a separation factor of 35.5. Molecular dynamics simulations and weight cut-off experiments confirmed that γ-cyclodextrin enhanced pore uniformity, resulting in a denser, more efficient membrane. This innovative approach offers a flexible and precise solution for Mg 2+ /Li + separation, demonstrating high permeance (15.5 L m −2 h −1 bar −1 ) and potential for applications in seawater desalination, resource recovery, and industrial ion separation.
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Nature Communications
·
2025
·Vol. 16
·期 1
·1-14
·
IF 15.7
Zou Zhijuan,Liu Pengfei,Dou Ruiyang,Liu Kaijun,Wang Yunlong,Song Lixian,Tong Liping,Yin Guolu,Kang Wenbin,Cai Wenlong,Zhang Yaping,Chen Hongbing,Song Yingze
Binders are essential for maintaining positive electrode integrity in Li||S batteries and significantly affect their performance. However, commercial linear binders often have disordered networks, poor binding efficiency, and insufficient mechanical strength. To address these challenges, three-dimensional covalent binders offer a promising solution. Traditional methods for producing cross-linked binders require additives and result in poorly controlled polymer networks due to the stochastic nature of liquid-phase polymerization. Moreover, the mechanisms by which reticulated binders stabilize the positive electrode remain unclear, requiring investigation under operando conditions. Herein, we present an approach to tailor cross-linked polyacrylamide networks using solid-state operando γ-ray irradiation chemistry, which eliminates additives and produces a pure, ordered network with remarkable binding capabilities. By integrating in situ high-resolution optical frequency domain reflectometry, multiscale synchrotron radiation characterization, and virtual simulations, this study reveals the role of binders in dynamically encaging and confining sulfur. Specifically, γ-ray-enabled polyacrylamide networks enhance battery performance through mechanical strengthening, optimized sulfur regeneration, and improved re-occupancy. Consequently, the well-designed composite positive electrode structure with only 5.0 wt% binder improves soft-packaged Li||S battery performance across various scenarios. Notably, a 1.2-Ah pouch cell achieves 410.1 Wh kg −1 specific energy with a low electrolyte/sulfur ratio of 3.0 µL mg –1 .
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