ACS Nano
·
2022
·
IF 18.027
Lanxiang Feng,Peng Yu,Xuewei Fu,Zheng-Min Zhang,Kenneth Davey,Yu Wang,Zaiping Guo,Wei Yang
Polar host materials with strong adsorption capacity of polysulfides are designed to limit the shuttle effect in sulfur cathodes. However, a critical problem is to control diffusion and deposition of lithium polysulfides during cycling, which significantly impacts cycling stability and sulfur utilization. Here, we report using a sequential adsorption-guided self-assembly to design two types of core–shell sulfur particles with opposite polysulfide adsorption gradients to explore quantitatively the regulation of polysulfide diffusion and deposition. We show that a positive core–shell design of sulfur particles (PCSD@SP), i.e., polysulfide adsorption capability decreasing from the interior to the exterior of the host, is more effective in restricting polysulfide diffusion and regulating polysulfide deposition than the negative core–shell counterpart (NCSD@SP). As a result, the PCSD@SP electrode with a sulfur loading of 7 mg cm–2 exhibits a stable areal capacity of 6 mAh cm–2 over 130 cycles at 0.2C. At intermittent discharge/charge, the PCSD@SP electrode retains excellent stability compared with the NCSD@SP. We conclude that rational design of positive core–shell active materials can be used to regulate polysulfide diffusion and deposition to boost electrochemical reaction dynamics and performance. The reported findings will be of immediate benefit to a range of researchers in the design of high-performance lithium–sulfur batteries.
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Science Advances
·
2025
·Vol. 11
·期 46
·
IF 12.5
Jin Li,Junjie Chen,Xiaosa Xu,Zhenyu Wang,Zixiao Guo,Pengzhu Lin,Jing Sun,Baoling Huang,Tianshou Zhao
Quasi–solid-state lithium metal batteries (QSSLMBs) are hindered by interfacial instability at high-voltage cathodes and uncontrolled lithium dendrite growth at the anode, limiting their cycling life and energy density. To overcome these challenges, we have developed a piperidine-based ionic liquid (IL) additive featuring a methylthiolation cationic segment that stabilizes the interphase of layered oxide cathodes and lithium anodes under fast charging and high-voltage conditions. These ILs preferentially oxidize to form a robust cathode-electrolyte interphase with LiF and sulfide species, which effectively suppresses dissolution of transition metal and enhances interfacial ion transport. Simultaneously, the IL-derived diverse inorganic species composite interphase at the anode improves mechanical strength and inhibits lithium dendrite growth. The resulting quasi–solid-state electrolyte demonstrates stable operation at a high voltage of 4.5 V, high mass loading of 21.6 mg cm −2 , high–energy density of 407 Wh kg −1 , and broad temperature range from −20° to 60°C, advancing the practical application of QSSLMBs.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Lingbing Wu,Shan Wang,Yao Niu,Zhengyao Sun,Xianghua Yao,Youlong Xu
LiNi 0.5 Mn 1.5 O 4 (LNMO) is a high-profile cathode material for lithium-ion batteries with high voltage and high specific energy. However, its practical application is severely hindered by the dissolution of Mn, primarily induced by the Jahn-Teller effect, which leads to significant capacity degradation, especially under high current densities. In this research, LiNi 0.5-7/3x Cu x Al x Mn 1.5-7/3x Ti x V x O 4 (x = 0, 0.5 %, 1 %, 3 %) was synthesized via a sol–gel method employing a multivalent ion co-doping strategy, denoted as CATV. X-ray diffraction analyses that the increase in the (311)/(400) peak ratio of CATV-1 % indicates a higher concentration of Mn 3+ , which enhances the structural disorder of the material, thereby improving its electronic conductivity. By improving the ratio of the (110) plane, which is perpendicular to the lithium-ion diffusion pathway, the lithium-ion diffusion coefficient was enhanced by three orders of magnitude. Furthermore, the Mn dissolution issue originating from the (111) plane was mitigated which shows in XRF that the Mn content deposited on the negative lithium sheet was reduced by 50 %. Specifically, it delivered specific capacity of 136.2 mAh·g −1 at 0.1C and maintained 81.74 % of its capacity after 300 cycles at 1C. Under 20C charge–discharge condition, it reached 108 mAh·g −1 , doubling that of the undoped sample. These findings provide new possibilities for the commercial application of CATV materials.
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Nature Communications
·
2022
·Vol. 13
·期 1
·1-10
·
IF 17.694
Lei Jie,Fan Xiao-Xiang,Liu Ting,Xu Pan,Hou Qing,Li Ke,Yuan Ru-Ming,Zheng Ming-Sen,Dong Quan-Feng,Chen Jia-Jia
The redox reactions occurring in the Li-S battery positive electrode conceal various and critical electrocatalytic processes, which strongly influence the performances of this electrochemical energy storage system. Here, we report the development of a single-dispersed molecular cluster catalyst composite comprising of a polyoxometalate framework ([Co 4 (PW 9 O 34 ) 2 ] 10− ) and multilayer reduced graphene oxide. Due to the interfacial charge transfer and exposure of unsaturated cobalt sites, the composite demonstrates efficient polysulfides adsorption and reduced activation energy for polysulfides conversion, thus serving as a bifunctional electrocatalyst. When tested in full Li-S coin cell configuration, the composite allows for a long-term Li-S battery cycling with a capacity fading of 0.015% per cycle after 1000 cycles at 2 C (i.e., 3.36 A g −1 ). An areal capacity of 4.55 mAh cm −2 is also achieved with a sulfur loading of 5.6 mg cm − 2 and E/S ratio of 4.5 μL mg −1 . Moreover, Li-S single-electrode pouch cells tested with the bifunctional electrocatalyst demonstrate a specific capacity of about 800 mAh g −1 at a sulfur loading of 3.6 mg cm −2 for 100 cycles at 0.2 C (i.e., 336 mA g −1 ) with E/S ratio of 5 μL mg −1 .
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Energetic Materials Frontiers
·
2025
·
IF 3.9
Jia-he Li,Feng Hao,Chang-sheng Tang,Lu-yang Wang,Yan-qiu Jiang,Yu-lin Yang,De-bin Xia,Jian Zhang,Ping Wang,Kai-feng Lin
Alloy based composite fuel has been widely studied for its higher combustion effect and energy release, compared with traditional metal fuels. The doping of organometallic salt was the key to facilitating the mass and heat transfer process in propellant combustion. In this study, the Al-Li particles were stabilized through tris(hydroxymethyl)aminomethane hydrochloride (TH) firstly, and the copper perfluorooctanoate Cu(PFO) 2 was obtained through a double displacement reaction and characterized by X-ray diffraction (XRD), fourier transform infrared spectrometer (FT-IR), Ultraviolet–visible spectroscopy (UV-vis), scanning electron microscope (SEM) and thermogravimetric analysis and differential scanning calorimeter (TG-DSC) tests. Owing to the characteristics of easy film formation, the Cu(PFO) 2 could be attached to the passivated Al-Li@TH surface through the solvent evaporation method with good hydrophobicity. The thermal oxidation and combustion characteristics were evaluated by TG-DSC and ignition test for the Al-Li@TH@Cu(PFO) 2 and propellants. The Al-Li@TH@5Cu(PFO) 2 propellant had a better burning rate of 1.21 mm·s -1 , a shorter ignition delay time of 0.67 s, a higher combustion temperature of 1411.26°C and smaller combustion residue distribution with an obvious micro-explosion effect and more stable combustion. The existence of AlF 3 also proved that the release of corrosive gases produced by Cu(PFO) 2 decomposition, which could effectively promote the rupture of Al-Li alloy shell. Besides, the activation energy of Al-Li@TH@5Cu(PFO) 2 and AP could be reduced to 139.37 kJ·mol -1 with a better catalytic effect. The combustion mechanism had also been analyzed through the combustion phenomena and residue composition. The exploration of propellant combustion could offer a promising avenue for applying Al-Li alloys in various propulsion systems.
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JOURNAL OF MEMBRANE SCIENCE
·
2024
·
IF 8.4
Na Yang,Keting Li,Yufan Hao,Longfei Zhang,Yongli Sun,Luhong Zhang,Bin Jiang
Polyethyleneimine (PEI) nanofiltration (NF) membranes hold great application prospects in lithium extraction from salt lakes due to their high positive charge properties. However, the poor permeability of the membranes caused by the dense separation layer structure severely hinders their further application. Herein, a functional end-capping strategy was employed to address this problem by adding the effective end-capping reagent, Girard's Reagent T (GRT), to the PEI aqueous phase as the co-reaction reagent. Under the dual functions of the end-capping effect and the quaternary ammonium groups of GRT, the looseness and positive charge of the membrane were simultaneously optimized. After the modification of GRT, the looser structure of the PEI/GRT NF membrane improved its pure water flux (PWF) to 115 L m −2 h −1 at 6 bar, which was around 3.7 times higher than that of the original PEI NF membrane. Meanwhile, the enhanced positive charge (from −8 to 9 mV, pH = 7) of the membrane bottom surface allowed it to maintain the high rejection rate of MgCl 2 at 97.2 %. Besides, the PEI/GRT NF membrane exhibited good Mg 2+ /Li + selectivity (S Mg 2+ /Li + = 22.7, 2000 ppm, Mg 2+ /Li + mass ratio: 20:1). Therefore, this study provides a simple and feasible strategy for the preparation of high-permeable PEI NF membranes with good Mg 2+ /Li + separation performance.
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JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2025
·Vol. 172
·期 4
·040508
·
IF 3.3
Xiaola Li,Huihong Gong,Wenjie Huang,Wenzhao Huang,Ziyang Liang,Yuqing Liu,Boyang Zhang,Shuxing Wu,Chenyu Liu,Zhan Lin,Dong Luo
Li-rich Mn-based layered oxides (LLOs) are regarded as one of the most promising next-generation cathodes for lithium-ion batteries (LIBs) due to their ultra-high capacity and low cost. However, the redox behavior of oxygen under high voltage induces severe challenges, including voltage hysteresis and voltage decay, which have become major obstacles to their commercialization. This work optimizes the oxygen redox process of O2-type LLOs by regulating the Na content in P2-type Na-based intermediates. Experimental results demonstrate that samples prepared by intermediates with optimal Na content show higher reversibility and reduction potential of oxygen redox. Meanwhile, the migration and dissolution of transition metals in the optimized samples are effectively suppressed. Therefore, the optimized samples deliver an improved voltage stability and alleviated voltage hysteresis. This work suggests that the oxygen redox process can be regulated and provides a practical solution to mitigate voltage decay and hysteresis in LLOs.
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Nature Communications
·
2022
·Vol. 13
·期 1
·1-9
·
IF 17.694
Cheng Zhu,Pan Hui,Li Fan,Duan Chun,Liu Hang,Zhong Hanyun,Sheng Chuanchao,Hou Guangjin,He Ping,Zhou Haoshen
Rechargeable Li-I 2 battery has attracted considerable attentions due to its high theoretical capacity, low cost and environment-friendliness. Dissolution of polyiodides are required to facilitate the electrochemical redox reaction of the I 2 cathode, which would lead to a harmful shuttle effect. All-solid-state Li-I 2 battery totally avoids the polyiodides shuttle in a liquid system. However, the insoluble discharge product at the conventional solid interface results in a sluggish electrochemical reaction and poor rechargeability. In this work, by adopting a well-designed hybrid electrolyte composed of a dispersion layer and a blocking layer, we successfully promote a new polyiodides chemistry and localize the polyiodides dissolution within a limited space near the cathode. Owing to this confined dissolution strategy, a rechargeable and highly reversible all-solid-state Li-I 2 battery is demonstrated and shows a long-term life of over 9000 cycles at 1C with a capacity retention of 84.1%.
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Laser & Photonics Reviews
·
2025
·
IF 10
Shenao Jiang,Chengxiang Yang,Riming Hu,Shanshan Liu,Wei Liu,Qi You,Xuan Zhou,Mu Liu,Xuchuan Jiang
Self-activated near-infrared (NIR) phosphors are promising candidates for advanced NIR light sources due to their intrinsic non-toxic composition and cost-effectiveness. However, their practical implementation is hindered by low defect concentration, which critically restricts luminescence efficiency. This study introduces a novel defect engineering strategy via interstitial lithium incorporation in BaAl 2 B 2 O 7 (BAB:Li + ), achieving simultaneous enhancement of NIR emission intensity, spectral modulation, and thermal stability. Structural characterization and density functional theory (DFT) calculations reveal that the broad 780 nm emission under 330 nm excitation originates from interstitial oxygen (O i ) defects in the BAB host. Remarkably, through this interstitial-Li induced oxygen defect engineering method, BAB:0.10Li + demonstrates an eight-fold emission intensity increase accompanied by a 72 nm blueshift, compared to the pristine BAB. Thermoluminescence (TL) analysis confirms that the improvement stems from dual key reasons: O i defects concentration and introduction of additional deep traps. The engineered deep traps endow the phosphor with excellent thermal stability, retaining 86% of initial intensity at 150 °C versus 37% for unmodified counterpart. This validates possible applications in night-vision, biological imaging and fingerprint detection. The defect engineering paradigm probably establishes a general approach for developing high-performance self-activated NIR phosphors, opening a new avenue for advanced optical materials design.
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Nature Communications
·
2025
·Vol. 16
·期 1
·10895
·
IF 15.7
Wang Wei,Wang Xinying,Yang Huanhuan,Yu Zhipeng,Zhang Weicai,Huang Haoliang,Zhao Zaowen,Zheng Xuerong,Liu Lifeng,Deng Yida,Li Yunyong
A rational design principle for selecting optimal anion dopants in transition-metal compounds to enhance sulfur redox activity is lacking in Li-S batteries. Herein, we propose an accurate p-p-s orbital electronic coupling descriptor (involving the p -orbitals of anion dopants and anions in transition-metal compounds and the s -orbitals of Li in lithium polysulfides) as a criterion for choosing anion dopants to guide the development of efficient anion-doped Li-S catalysts through machine-learning, theoretical, and experimental validation. We reveal the relationship between the electronic properties of various anion-doped WSe 2 and the thermodynamics and kinetics of sulfur redox. Our findings show that moderate p-p-s orbital electronic coupling optimizes polysulfide adsorption, facilitating Li 2 S nucleation and decomposition, thereby minimizing Gibbs free energy and maximizing catalytic efficiency for sulfur redox. A volcano relationship between the p-p-s coupling strength and catalytic activity is established. The optimal B-WSe 2 /MXene catalyst achieves a ~ 3 Ah pouch cell with 430 Wh kg −1 specific energy and good cycle life (81.3% capacity retention over 71 cycles). These findings provide a guideline for designing efficient anion-doped Li-S catalysts with moderate p-p-s coupling to enable rapid sulfur catalytic conversion in Li-S batteries.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Ximin Ling,Wutao Wei,Changwei Shan,Xuyan Qin,Mingjie Song,Zhao Liu,Liwei Mi
Mg 2+ /Li + hybrid batteries (MLHBs), which support the rapid insertion and removal of Mg 2+ /Li + bimetallic ions, are promising energy storage systems. Inspired by the Kirkendall effect, ball-in-ball bimetallic sulfides with heterostructures were prepared as cathode materials for the MLHBs. First, a nickel–cobalt precursor (NiCo-X precursor) with three-dimensional (3D) nanosheets on its surface was prepared using a solvothermal method based on the association reaction between alkoxide molecules. Subsequently, the NiCo-X precursor was vulcanized at high temperature using the potential energy difference as the driving force to successfully prepare NiS 2 @CoS 2 core–shell hollow spheres. When used as the positive electrode material for the MLHBs, the NiS 2 @CoS 2 hollow spheres exhibited excellent Mg 2+ /Li + ion storage capacity, high specific capacity, good rate performance, and stable cyclic stability owing to their tough hierarchical structure. At a current density of 500 mA g −1 , a specific capacity of 536 mAh g −1 was maintained after 200 cycles. By explaining the transformation mechanism of Mg 2+ /Li + in bimetallic sulfides, it was proven that Mg 2+ and Li + worked cooperatively. This study provides a new approach for developing MLHBs with good electrochemical properties.
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Inorganic Chemistry Frontiers
·
2024
·Vol. 11
·期 11
·3323-3333
·
IF 6.1
Shunqin Zeng,Meinan Zhao,Chen Xie,Jianhui Li,Xiaoli Ding,Liqing He,Yongtao Li,Qingan Zhang,Hai-Wen Li
Developing composite solid electrolytes (CSEs) represents a promising avenue for advancing commercial viability of all-solid-state batteries because none of the single electrolytes can meet the application requirements. However, the correlation of interfacial reconstruction among more than two composite solid electrolytes with property enhancements still remains unclear. In this study, lithium-based hydride-oxide solid electrolytes are chosen as a model to explore in situ interfacial reactions between these composites, with the goal of innovating design of electrolytes for all-solid-state batteries. Our research reveals the formation of dual core–shell-structured electrolytes with LiBO2 as the intermediate layer and LiBH4 as the outer layer embedded with LixM intermediates, resulting in the in situ reactions of LiBH4 and LixMOy (M = N, P, S) composites. These composites exhibit continuous conductive networks and demonstrate a high Li+ conductivity of ∼1.9 × 10−4 S cm−1 at 75 °C. This impressive conductivity enables stable cycling of Li–Li symmetric cells for 650 h. Moreover, the critical current density can reach about 2.3 mA cm−2, and the electrochemical window extends from −0.5 to 6 V. Notably, the reversible specific capacity attains 225.1 mA h g−1 for Li‖TiS2 batteries with an initial coulombic efficiency of 95.4%. This work provides valuable insights into the design and performance of composite solid electrolytes, offering a promising approach for the development of high-performance all-solid-state batteries.
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