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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2022 · IF 9.965

Oxygen vacancies in open-hollow microcapsule enable accelerated kinetics for stable Li-S battery

Kai Zhang,Caixia Li,Yu Zhang,Xiaoni Liu,Minghui Wang,Lei Wang

The fast development of lithium-sulfur (Li-S) batteries is catching more attention to improve cycling stability and kinetics. Herein, a hierarchical porous Ni/NiO/C microsphere (NIONC) with openings assembled by ultrathin nanosheets is introduced to solve the poor conductivity, shuttle effect, and slow electrochemical kinetics of Li-S batteries. The structure of NIONC open-hollow microcapsules combines several advantageous properties for the improvement of electrochemical performances. Primarily, a well-developed hollow structure and openings can perform as containers and doors for sulfur immobilization. Therefore, the confinement effect to sulfur species is obtained by this hollow sphere. Secondly, the nanosheets with oxygen vacancies and Ni active sites provide abundant active sites for the chemical absorption of polysulfides. Based on the open structure and oxygen vacancies of Ni/NiO, both the physical absorption and chemical immobilization of sulfur are realized, with high stability and fast kinetics. The S-injected NIONC (NIONC/S) cathode exhibits outstanding rate performance at 5 A g -1 with a high capability of 794 mAh g -1 and excellent long-cycle performance of 653 mAh g -1 after 300 cycles at 1 A g -1 . We proposed a simple and controllable route to fabricate sulfur hosts by structure and composition adjustment, which will inspire the commercial application of Li-S batteries.

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Applied Materials Today · 2022 · IF 8.663

Flexible mixed ion-electron conductor fabric for stable and dendrite-free Li-metal anodes

Yun Zhao,Jianhua Yan,Jianyong Yu,Bin Ding

Li-metal batteries are promising candidates for next generation rechargeable batteries. However, the hazards caused by the growth of Li-dendrite and enormous volume fluctuations during cycling hinder its practical applications. Here, to solve these problems, a flexible mixed ion-electron conducting fabric scaffold is constructed by uniformly incorporating Li 0.33 La 0.56 TiO 3 nanoparticles into a 3D carbon nanofiber skeleton. The mixed conductor fabric cannot only homogenize the distribution of electric filed and alleviate volume changes, but also can accelerate the migration and distribution of Li + , thus achieving uniform Li plating/stripping behavior by balanced ion/electron transport. Consequently, the obtained stable and dendrite-free Li-metal anode has a notable cycling stability and rate performance. This work provides a promising direction for the design of practical composite Li-metal anodes.

CAS / MDL: 7790-69-4
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Materials Today Energy · 2022 · IF 9.257

Li+ additive accelerated structural transformation of MoS2 cathodes for performance-enhancing rechargeable Mg2+ batteries

Bofei Li,Zhao Li,Haoyuan Chen,Xu Zhang,Shuaijin Wu,Hao Xu,Yingying Yao,Yinghui Li,Xiaolong Li,Zhigang Hu,Richard M. Laine,Jianxin Zou,Kemin Zhang

Rechargeable magnesium ion batteries (MIBs) with intercalation materials as the cathode are found to offer better performance in Li + based electrolytes. Herein, we compare the electrochemical performance of MIBs using all-phenyl complex (APC) electrolytes before and after adding Li +  additives with layered MoS 2 cathodes. We coincidentally describe the lithiation mechanism that leads to a phase transition whereby Li +  additives accelerate a MoS 2 structural transformation from 2H to 1T which accounts for the superior battery performance (150 mAh/g, around two times the capacity of that without Li + additives). In this process, MoS 2 is partly exfoliated into single-layer nanosheets during cycle as evidenced by operando electrochemical synchrotron X-ray diffraction, ex situ X-ray photoelectron spectroscopy and scanning electron microscopy analyses. Accordingly, electrochemical cells with pre-exfoliated MoS 2 nanosheets (liquid phase exfoliation) require fewer activation cycles (50 cycles, a quart of the cycles that using pristine MoS 2 ) in APC electrolyte and better rate performance. Our work thus provides new insight in designing high-performance rechargeable MIBs by optimizing the intercalation cathodes using Li + additives.

CAS / MDL: 10035-06-0 1317-33-5
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CHEMICAL ENGINEERING JOURNAL · 2022 · IF 16.744

V2O3/VN Catalysts Decorated Free-Standing Multifunctional Interlayer for High-Performance Li-S Battery

Jie Zhao,Yuyan Zhao,Wen-ce Yue,Xue Li,Ning Gao,Yu-jiao Zhang,Chao-quan Hu

The shuttle effect caused by soluble lithium polysulfides (LiPSs) hinders the practical application of lithium–sulfur batteries. The sluggish reaction kinetics of LiPSs results in rapid capacity decay. In this work, we constructed a free-standing multifunctional interlayer decorated with V 2 O 3 /VN catalysts to suppress the shuttle effect and boost the redox reaction kinetics. The introduction of VN with strong chemical adsorption improves the conductivity of V 2 O 3 , which is beneficial for the kinetics of conversion reaction. In addition, the micro/mesopores inside the structure not only facilitate ion diffusion but also buffer the volume change of the sulfur cathode during the cycling process. Benefiting from the synergistic effects, the fabricated cells exhibit a high specific capacity of 1419.5 mAh g −1 at 0.1C. The cell with V 2 O 3 /VN/C exhibits a promising cycling performance over 1000 cycles with a decay rate of 0.037% per cycle at 1C. The synergistic effects of electrocatalysts and conductive carbon material provide inspiration on the development of high-performance Li–S batteries.

CAS / MDL: 62-31-7 1314-62-1
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JOURNAL OF POWER SOURCES · 2022 · IF 9.794

Improving the stability of NASICON-type electrolyte with Li metal anode by interfacial modification

Can Huang,Zhuojie Li,Shanshan Duan,Shuhong Xie,Shuoguo Yuan,Shuen Hou,Guozhong Cao,Hongyun Jin

Sodium super-ionic conductors (NASICON)-type electrolyte Li 1.4 Al 0.4 Ti 1.6 (PO 4 ) 3 (LATP), with high ionic conductivity and low cost, is considered as one of the most attractive alternatives to liquid electrolytes . However, the poor interfacial compatibilities of LATP electrolyte in lithium batteries lead to the failure, which hinders its further development. Herein, a MoS 2 coating layer as an artificial solid electrolyte interphase (ASEI) is used for modifying the surface of LATP (MCLATP) via an economical and uncomplicated spin coating method, which not only effectively inhibits the decomposition of LATP, but also in-situ forms a conversion layer consisting of Li 2 S and Mo metal during cycling. The conversion layer can improve the interfacial charge transfer kinetics and decrease the charge transfer resistance . According to interfacial modification of MoS 2 , the symmetric cells show slight polarization, and the Li/MCLATP/LFP cells demonstrate excellent cycling performance over 300 cycles at 1 C. The enhanced batteries performance is ascribed to interfacial modification of MoS 2 as an ASEI layer, which reduces interfacial concentration polarization caused by the formed microcracks around the surface during decomposition of LATP. This work provides a promising strategy to construct the interface between Li metal and solid-state electrolytes for other unstable electrolytes beyond NASICON .

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JOURNAL OF POWER SOURCES · 2022 · IF 9.794

A multifunctional polyimide enabled high performance silicon composite anode materials for Li-Ion batteries

Xiang Li,Jianwei He,Yucong Liao,Shaoshan Zhu,Yayun Tang,Hanyang Li,Ning Lv,Yuexin Xu,Yadong Wang

Herein, a conjugate carbonyl polyimide (MF-PI) and nano-silicon composite (MF-PI/Si) is designed and synthesized through a simple one-pot method to confront rapid capacity fading and complicated electrode material preparation in silicon-based electrodes for lithium ion battery . This composite can be directly used to prepare electrode without the need of further adding of binding materials. In this composite, MF-PI acts as binder for powder electrode, active reversible lithiation material, buffering media to alleviate volume change of silicon particles, and coating shell to avoid the direct contact between silicon particles and electrolyte. These functions from MF-PI collectively assigned the MF-PI/Si composite anode material a relative high specific capacity and excellent cycling stability. The electrode prepared by this as-synthesized MF-PI/Si shows preferable electrochemical interface and surface area, further enhancing the electrode kinetics and then electrochemical performance. The improved ionic and electronic conductivity compared to other binder materials also contributes the excellent performance.

CAS / MDL: 89-32-7 3010-82-0
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Small · 2023 ·Vol. 19 ·期 46 ·2305326 · IF 13.3

Revealing the Role of Active Fillers in Li-ion Conduction of Composite Solid Electrolytes

Shida Xue,Shiming Chen,Yanda Fu,Hengyao Zhu,Yuchen Ji,Yongli Song,Feng Pan,Luyi Yang

Composite solid electrolytes (CSEs) consisting of polyethylene oxide (PEO) matrix and active inorganic fillers have shown great potential for practical applications. However, mechanisms of how different active fillers enhance ion transport in CSEs still remain inconclusive. In this work, the component dependencies of ionic conductivity of PEO-based CSEs are investigated by comparing two widely investigated active fillers: NASICON-type (LATP) and garnet-type (LLZTO). In terms of ionic conductivity, the optimum ratios are strikingly different for LLZTO (10 wt%) and LATP (50 wt%). Through experimental and computational studies, it is demonstrated that the high affinity between LATP and PEO facilitates unhindered interfacial Li + transfer so that LATP functions as a bulk-active filler to provide additional inorganic ion pathways. By contrast, Li + transfer between LLZTO and PEO is found to be sluggish. Instead, LLZTO mainly improves ionic conductivity by dissociating lithium salt, making it a surface-active filler. Through categorizing active fillers based on their Li + conductive mechanisms, this work provides new understanding and guidelines for componential design and optimization of solid composite electrolytes.

CAS / MDL: 75-05-8 90076-65-6
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JOURNAL OF ALLOYS AND COMPOUNDS · 2023 · IF 6.2

Quenching-induced construction of graphene-wrapped Fe3O4 composite as ultrahigh-performance Li-storage electrode

Shan Yin,Xin He,Xiande Zhang,Yan Hao,Kaipeng Wu,Yun Zhang

Iron oxide/graphene hybrids are outstanding electrodes with high specific capacity for secondary batteries. However, in practice there still remains challenges in alleviating the poor electrical conductivity and significant volume changes of FeO x during the lithiation/delithiation process. Herein, we describe the discovery of fabricating graphene-wrapped Fe 3 O 4 (3D-rGO/Fe 3 O 4 ) via a solution-based self-assembly process. During which, GO/Fe 3 O 4 /Na 2 SO 4 precursor was first formed by the corrosion reaction of metallic Fe in GO aqueous solution and antisolvent self-assembly, which was then quenched into water to dissolve the Na 2 SO 4 template and meanwhile enable the GO to shrink and encapsulate the Fe 3 O 4 nanoparticles spontaneously, followed by a final thermal reduction. Fe 3 O 4 nanoparticles, with a diameter of tens of nanometers, are homogeneously enwrapped into rGO framework, guaranteeing the “plane-to-plane” interconnection. The obtained 3D-rGO/Fe 3 O 4 demonstrates unprecedented Li-storage behaviors when utilized as Li-ion battery anode. Furthermore, quantitative kinetic analysis revealed that both capacitance and diffusion mechanisms account for Li-storage behavior. This contribution not only presents a ultrahigh-performance Li-storage electrode but also shows a novel methodology to design and construct other graghene-based metallic compounds for various applications.

CAS / MDL: 7757-82-6
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CHEMICAL ENGINEERING JOURNAL · 2023 · IF 15.1

Multi-perspective synergistic construction of dual-functional heterostructures for high-temperature Li-S batteries

Yiding Li,Qiang Zhang,Simin Shen,Siqi Wang,Liangliang Shi,Dequan Liu,Yujun Fu,Deyan He

Effectively limiting the shuttle effect is the key to improving the electrochemical performance of Li-S batteries. Here, the synthesis of WO 3 -WS 2 heterostructures is reported by electrospinning and in situ sulfurization strategies, combining the initial WO 3 nanoparticles with the sulfurization product WS 2 . It was found that the obtained bifunctional heterostructures enhance the electrolyte wettability, optimize intermediate regulation performance, accelerate Li + /e − diffusion, and thus exhibit excellent electrochemical characteristics in Li-S batteries. Through experiments and density functional theory (DFT) calculations, the WO 3 -WS 2 heterostructures were considered as a coupled creative solution with multiple advantages. Different from the batteries using single-component or single-configuration catalyst, the prepared Li-S batteries with the WO 3 -WS 2 heterostructures exhibited synergistic enhanced electrochemical performance and high-temperature crushing resistance. Even under severe conditions, including high sulfur loading (10.3 mg cm −2 ), lean electrolyte (5.8 μL mg −1 ), high current density (7.0 A g −1 ), extended cycling (1600 cycles), and high temperature (90 °C), the representative battery exhibited stable cycling performance.

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JOURNAL OF MEMBRANE SCIENCE · 2021 · IF 8.742

Positively-charged nanofiltration membranes constructed via gas/liquid interfacial polymerization for Mg2+/Li+ separation

Ming-Bang Wu,Hao Ye,Zhi-Yuan Zhu,Guo-Tao Chen,Lu-Lin Ma,Shi-Cheng Liu,Lin Liu,Juming Yao,Zhi-Kang Xu

Nanofiltration (NF) shows great application potentials in selectively recovering lithium (Li) from natural brine to meet the rapidly growing demands in lithium-ion batteries. However, it remains challenges in how to fabricate positively-charged NF membranes via a convenient method since conventional polyamide-based NF membranes are negatively-charged, which exhibit undesirable Mg 2+ /Li + selectivity according to the Donnan and electrostatic effects. Herein, we report a new kind of interfacial polymerization (IP) for preparing positively-charged NF membranes at the gas/liquid (GL) interface by replacing the amine solution with amine gas. Compared with the traditional liquid/liquid interfacial polymerization (LLIP), the amine monomers are always more abundant than the acyl chloride monomers during the GLIP process. Therefore, enough amino groups are desirably remained, resulting in positively-charged polyamide-based layers. In addition, the surface charges as well as the average pore sizes of the polyamide-based layers can be facilely adjusted by the reaction time due to the slow reaction kinetics in the GLIP process. The as-prepared NF membranes show a relatively high rejection for MgCl 2 of 98.5% and low rejection for LiCl of 22.6%, demonstrating their excellent Mg 2+ /Li + selectivity. Moreover, the NF membranes can also maintain the high Mg 2+ /Li + separation factors as high as 28 during a long-term operation.

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International Journal of Minerals Metallurgy and Materials · 2026 · IF 8.8

Sulfonated Li-metal–organic frameworks-enhanced wide-temperature all solid-state lithium metal batteries

She Yanjun,Si Hongxiang,Li Jiaxing,Xu Wenbin,Mamlouk Mohamed,Tian Fang,Anatolyevich Mindrov K.,Wei Tao

A sulfonic-functionalized Zr-type metal–organic framework (UiO-66-SO 3 H) was synthesized, and UiO-66-SO 3 Li was obtained via subsequent lithiation treatment. The UiO-66-SO 3 H framework was incorporated into a polymer matrix as a functional filler to obtain high-performance solid composite electrolytes (SCEs). Structural and morphological analyses, as well as various electrochemical tests, were performed. Owing to well-defined porous channels, abundant lithium-ion transport sites, and effective regulation of polymer crystallinity by SO − 3 moieties at 60°C, the optimized SCE-2 (10wt% UiO-66-SO 3 Li) exhibited a high ionic conductivity of 5.36 × 10 −4 S·cm −1 (1.86 × 10 −4 S·cm −1 at the room temperature of 25°C), along with a wide electrochemical stability window of 4.7 V and a lithium-ion transference number as high as 0.623. The Li∣SCE-2∣LiFePO 4 full cell exhibited excellent long-cycle stability at both 60°C and room temperature, as well as an excellent rate capability up to 5 C (1 C is equivalent to 170 mA·g −1 ). Moreover, SCE-2 can also be coupled with high-voltage LiNi 0.5 Co 0.1 Mn 0.3 O 2 cathodes. This study demonstrates that sulfonic-modified UiO-66-SO 3 Li can effectively regulate Li + migration, suppress lithium dendrite growth, and enhance interfacial compatibility, offering a viable approach for designing advanced solid composite electrolytes.

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Nature Communications · 2026 · IF 18.1

Studying the failure mechanism in Li-metal electrode by a reversible fluorescence analysis methodology

Liu Xiao,Zhang Peng,Guo Yunpeng,Xiong Chuncen,Fu Hongru,Liu Guilong,Sui Dong,Liu Xianming,Ma Lufang,Zhao Yong,Wen Liping

Elucidating the failure mechanisms of Li metal electrodes is critical to accelerating the development of long cycle life Li metal batteries. However, it has not yet fully been realized so far due to the challenges associated with quantitative and qualitative characterization of solid electrolyte interphase on metal at large-area scale. Herein, we establish a relationship between solid byproducts and dead Li amounts in solid electrolyte interphase on Li metal by using fluorescence imaging and fluorescence titration method. The success of this methodology depends on the finding of a highly selective molecular probe, dilithium 3-hydroxy-2-naphthoate, with reversible change in fluorescence wavelength and intensity toward Li metal. Accordingly, the continuous generation of solid byproducts is acknowledged as potential underlying reason towards dead Li accumulation, determining the failure of Li electrode. These findings provide insights into the understanding of failure mechanism of Li metal electrode and design of strategies to improve its cycle life.

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