ELECTROCHEMISTRY
·
2020
·Vol. 88
·期 1
·8-13
·
IF 1.099
Kun WANG,Dongying JU,Guiying XU,Beibei HAN,Yongfei WANG,Jian ZHANG,Maorong CHAI,Shaobei CHEN,Weimin ZHOU
The carbon black (CB) is modified successfully by the two-step modifications such as organo-chlorination and organo-sulfuration using the chemical reagents of thionyl chloride and ethanethiol continuously. The organosulfur groups of –C–SR and –COSR forming on the CB surface play the main role to improve the electrochemical performances, which is verified by electrochemical studies. For instance, after carrying out the charge-discharge 100 times, the organosulfur modified CB (MCB) shows the Li+ ion storage capacity at 392 mAh/g, which is higher than CB showing at 176 mAh/g. Furthermore, the improvement storage capacity is attributed to the enhanced capacitive effects which are verified by the detailed measurements of cyclic voltammetry (CV). These results are able to provide effective way to enhance the storage capacity of general carbon materials such as CB, graphite, graphene oxide (GO) and so on.
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International Journal of Minerals Metallurgy and Materials
·
2026
·
IF 8.8
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
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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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Wenguang Wang,Chao Wang,Yanqiu Zhang,Hanyang Xu,Lu Shao
Advanced monovalent cation exchange membranes (MCEMs) have been applied to extract key monovalent cations (Li + or Na + ) from nature, but it is challenging to design high-performance MCEMs with low membrane area resistance and specific charge properties. Herein, a positively-charged Fe 3+ -bridged pyrogallic/polyethyleneimine membrane (Fe 3+ -bridged PY/PEIM) for efficient Li + /Mg 2+ separation is fabricated through a covalent bond and coordination bond (CB/COB) competitive reaction. Various physicochemical characterizations elucidate that the formation of COBs reduces the reaction sites of PY and PEI molecules for Michael-addition and Schiff-base reactions, which reduces the thickness of the selective layers to reduce the membrane area resistance from 6.58 to 4.83 Ω·cm 2 . A highly positively-charged selective layer caused by unreacted NH 2 groups and Fe 3+ makes the optimal Fe 3+ -bridged PY/PEIM exhibit a superior separation performance (perm-selectivity (Li + /Mg 2+ ) of 45.57 with a Li + flux of 4.61 × 10 −8 mol·cm −2 ·s −1 ). Moreover, the optimal Fe 3+ -bridged PY/PEIM also has excellent separation performance (high Li + flux and perm-selectivity) and operational stability when treating three simulated solutions with different Mg/Li mass ratios and salinities. The new strategy for constructing a thin, defect-free and positively-charged selective layer through a CB/COB competitive reaction can provide new insights for designing high-performance MCEMs towards environmental remediation and energy harvesting.
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ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Chenkun Li,Yao Xiao,Xiaosong Zhang,Hongwei Cheng,Ya-Jun Cheng,Yonggao Xia
The irreversible capacity loss of lithium-ion batteries during initial cycling directly leads to a decrease in energy density, and promising lithium cathode replenishment can significantly alleviate this problem. In response to the problems of complex preparation, instability in air, and unfavorable residue of the conventional cathode lithium replenishment materials, a Li2CO3/carbon nanocomposite is prepared and utilized as the lithium replenishment material. With high-speed ball-milling, a nanocomposite with a tight embedment structured Li2CO3/Ketjen Black (KB) composite composed of nanosized Li2CO3 and KB is synthesized. The decomposition potential of Li2CO3 is effectively decreased to 3.8 V, and the amount of the active lithium ion being released is significantly increased, corresponding to a specific capacity of 645.2 mAh·g–1 during the initial charging cycle. It has been introduced into the full-cells composed of the NCM523 cathode and graphite anode, resulting in a capacity increase of 44 mAh·g–1 in the initial cycle and a 26.4% improvement in capacity retention over 100 cycles. The working mechanism of the Li2CO3/KB nanocomposite as the lithium replenishment agent has been discussed. The outcome of the work provides a practically feasible route to realize lithium-ion battery technology with improved energy density and cycling life.
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PubMed
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Advanced Materials Interfaces
·
2022
·Vol. 9
·期 13
·2101955
·
IF 6.389
Anping Tang,Ziqin Liang,Hezhang Chen,Guorong Xu,Haishen Song
A new type of cathodic active material for lithium-ion batteries based on a composite of Li 3 PO 4 and V 2 O 3 is proposed in this work. Although the V 2 O 3 component is almost inactive in the voltage range of 2–4.5 V versus Li + /Li, the mixture of the two components can deliver a larger reversible specific capacity of ≈190 mA h g −1 in the voltage range of 2–4.5 V at a current density of 15 mA g −1 . X-ray photoelectron spectroscopy data and cyclic voltammetry data suggest that the vanadium ions are probably oxidized and reduced repetitively upon cycling and that the V 3+ ions are partially oxidized to V 4+ and even V 5+ ions during charging to 4.5 V. This distinctive lithium-ion uptake and release phenomenon, in which Li 3 PO 4 functions as a lithium source of surface conversion reaction, will introduce a new path for designing unique cathodic active materials for lithium-ion batteries.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2023
·
IF 6.2
Wenhui Zhu,Ali Reza Kamali
Thermal oxidation in air of molybdenum disulfide (MoS 2 ) into layer structured molybdenum trioxide (α-MoO 3 ) is investigated using a combination of thermal analysis, electron microscopy , Raman, X-ray diffraction and photoelectron spectroscopy . The phase evolutions occurred during the thermal process is characterized by the surface oxidation of MoS 2 , followed by the bulk oxidation to form α-MoO 3 and the formation of Mo 17 O 47 at higher temperatures. The single-phase MoO 3 formed at optimum temperature condition is found to possess crystalline defects and considerably greater values of Li-ion storage cycling and rate performances in comparison with samples prepared at alternative temperatures and also the initial MoS 2 . This sample (P-MoO 3 -820) exhibits a charge capacity of 628 mA h g −1 after 250 cycles (100 mA g −1 ) with a Li + diffusion coefficient of 2.3 × 10 -13 cm 2 s −1 , substantially greater than that of initial MoS 2 (8.1 × 10 −16 cm 2 s −1 ). The electrochemical performance of P-MoO 3 -820 in full-cell configuration against a commercial LiFePO 4 cathode is evaluated and a specific capacity of 100 mAh g −1 after 500 cycles is recorded. This article, for the first time, discusses the thermal oxidation in air of MoS 2 as a simple and relatively clean approach to fabricate defective crystalline MoO 3 with enhanced Li-ion storage kinetics.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2023
·
IF 6.2
Bing Xue,Xiangkun Wu
The high energy density cathode material , nickel-rich layered oxide LiNi 0.8 Co 0.1 Mn 0.1 O 2 (LNCM), has been extensively researched for its potential applications. Nevertheless, its structural instability, weak conductivity and unsafe properties greatly impede its further development. To address these issues, the method of surface coating by graphene and element doping by Mg atom for LNCM is proposed, and its structural and electrochemical properties , as well as the promoting mechanism are comprehensively studied. Such as, the structural and morphological features are investigated by X– ray diffraction (XRD), Raman spectroscopy , thermogravimetric analysis (TGA), scanning electron microscopy (SEM) coupled with energy dispersive X – ray spectroscopy (EDX) and transmission electron microscopy (TEM). Characterization techniques depict the composites’ dimension, modified construction and components. Electrochemical performances are studied using cyclic voltammetry , electrochemical impedance spectroscopy , and galvanostatic charge – discharge test. The typical redox peaks of Ni 2+ /Ni 4+ and Co 3+ /Co 4+ are well-defined for LNCM@rGM, and its improved electrochemical performance compared to LNCM are demonstrated. Specifically, LNCM@rGM exhibits a higher capacity retention of 58%, maintaining a capacity of 123.3 mAh g −1 after the 200th cycle, from an initial value of 211.0 mAh g −1 . Additionally, LNCM@rGM shows a higher rate capability of 80.2 mAh g −1 at 5 C, as well as improved Li + diffusion and higher exchange current density. The findings indicate that the composite structure consisting of graphene coating and element doping shows improved electrochemical performance when exposed to an optimal heating temperature, resulting in enhanced structural stability, elevated ionic/electronic conductivity, and synergistic effects on the materials.
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Small
·
2023
·Vol. 19
·期 46
·2305326
·
IF 13.3
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.
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Inorganics
·
2023
·Vol. 11
·期 6
·257
·
IF 2.9
Rui Yan,Fangchao Liu,Zhengwen Fu
Li-SeS2batteries balance the opposing and complimentary qualities of Li-S and Li-Se batteries by having a high specific capacity and high electrical conductivity. However, there is still a lack of knowledge regarding the electrochemical characteristics of Li-SeS2all-solid-state batteries (ASSB). Herein, transmission electron microscopy (TEM) is used to reveal the electrochemistry of a Li-SeS2battery. It is discovered that, without the Polyethylene glycol (PEG), amorphous SeS2in Li-SeS2ASSB change into crystalline selenium and a small amount of sulfur. The continuous loss of sulfur from the active material may be related to the failure of the cell at 15 cycles and the severe instability of the Coulombic efficiency. It was found that the PEG coating selenium disulfide graphene composite (PEG@rGO-SeS2) cathode maintained a specific capacity of 258 mAh g−1and a stable Coulombic efficiency of about 97% after 50 cycles. TEM analysis shows that the charging product remains as a granular amorphous selenium disulfide with a constant Se/S ratio during cycling. The PEG-protected selenium disulfide can effectively limit the loss of elemental sulfur and regulate the reaction mechanism of the Li-SeS2batteries.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
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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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Xinjian Li,Yanhui Su,Yong Ma,Le Wei,Ying He,Yuting Gu,Shiwei Mei,Qiaoqiao Mu,ChengYuan Peng,Yang Peng,Zhao Deng
Photo-assisted charge/discharge has witnessed marked success in Li-O 2 batteries (LOBs) to overcome the sluggish kinetics of triphasic reactions at the cathode, but challenges remain to develop high-efficiency but low-cost photocathode catalysts. Herein, a photoactive electron mediator is applied, for the first time, as bifunctional photocathode catalyst in solar-assisted LOBs. The facilely synthesized tris(2,2-bipyridine) cobalt(II) complex (Co-bpy) manifests good electrocatalytic activity in dark and high photoactivity under illumination, concertedly affording an superior charge/discharge voltage gap of 0.12 V and round-trip efficiency of 97%. Moreover, a significantly enhanced charge/discharge reversibility was attained under illumination and attributed to the light-induced amorphization of Li 2 O 2 that further extends the cycle life. A two-circuit model is proposed to rationalize the better reduction of charge/discharge polarization at lower operating current density. This work not only extends the family of photocathode catalysts to small-molecule complexes, but also offers new insights into the mechanism of photoenergy storage in LOBs.
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