JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
·
2024
·Vol. 35
·期 17
·1-12
·
IF 2.8
Liu Yang,Yang Jingdong,Wen Jiaxin,Ye Junliu,Liu Huan,Lu Liwei
Recently, rechargeable magnesium-ion batteries (MIBs) and rechargeable magnesium/lithium hybrid-ion batteries (MLHBs) have gained recognition as promising energy storage devices. However, the conventional CuS cathodes exhibit sluggish kinetics and poor cycle stability, thereby impeding the advancement and application of CuS. In this work, we have developed an economical and simple in-situ approach for synthesizing CuS@Cu foam (CSC) and evaluated its potential as a cathode material for both MIBs and MLHIBs. In both MIBs and MLHIBs, the CSC cathode demonstrates competitive performance. In MIBs, at a current density of 100 mA g −1 , the initial discharge specific capacity of the CSC is 150.94 mAh g −1 , which is higher than that of commercial CuS (3.99 mAh g −1 ). In MLHIBs, the CSC exhibits a discharge specific capacity of 502.95 mAh g −1 after 70 cycles at a current density of 100 mA g −1 , which significantly surpasses the discharge specific capacity of commercial CuS (229.52 mAh g −1 ). This performance improvement is attributed to the presence of Li + ions, which expedite the reaction kinetics, obviate the need for an activation process, and effectively facilitate the conversion reaction. In conclusion, by in-situ synthesis of CSC, the active material CuS firmly adheres to the Cu foam current collector. This approach is not only economical and simple but also significantly enhances the reactivity of the electrode material, thereby improving the electrochemical performance. This work provides valuable insights for the design, synthesis, and performance optimization of cathode materials of magnesium metal-based batteries.
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Journal of Materials Chemistry A
·
2017
·Vol. 5
·期 43
·22598-22606
·
IF 8.867
Wenju Ren,Haibiao Chen,Rongxue Qiao,Yuan Lin,Feng Pan
It is critical to monitor the state of health (SOH) of the Li-ion batteries to ensure a safe operation and to extend the service life of the batteries in electric vehicles. In this work, we demonstrated that the equivalent capacitance (Cp) and resistance (Rp) of the electrode interface derived using a first-order RC equivalent circuit under a large galvanostatic pulse (LGPM) condition can be correlated with SOH. For both the cathode and the anode, the interfacial kinetics of Li-ions were analyzed to study the electrochemical properties of active particles. The RC parameters of the equivalent circuit were correlated with the diffusion kinetics of Li-ions near the interface between the electrolyte and the active nano/micro-particles during fast charging/discharging. For fresh LiFePO4 (LFP)/Li half-cells, the values and the change of Cp and Rp were explained using the hypothesis of interparticle ion transport under a non-equilibrium condition. For graphite/Li half-cells, the buffering of Li-ions by the solid-electrolyte interphase (SEI) layer was speculated to affect Cp and Rp under a non-equilibrium condition. In commercial LFP/graphite batteries, the Cp values of unhealthy batteries were found to be higher than those of healthy batteries. In further tests, the Cp values of the half cells with the graphite anode recovered from the unhealthy batteries were found to be higher than those of the half cells with graphite from the healthy batteries. The half cells with LFP from the unhealthy batteries behaved similarly to those with LFP from the healthy batteries. With additional analysis on the microstructure, we proposed that the deterioration of the LFP/graphite batteries was mostly due to the formation of a thicker SEI on the graphite anode. The method developed in this work can be integrated in EVs at a low calculation cost. More importantly, we gained a better understanding of the interfacial kinetics of Li-ions during a non-equilibrium process.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Shimin Chen,Junnan Han,Zhihuan Li,Zijie Lin,Min Wang,Hucheng Song,Xiaodong Pi,Dongke Li,Linwei Yu,Jun Xu,Kunji Chen
Lithium-carbon dioxide (Li-CO 2 ) batteries using high ion-conductive inorganic molten salt electrolytes, as a kind of promising carbon–neutral technology, have attracted much attention due to the high safety and high energy density. However, sluggish CO 2 reduction reaction (CO 2 RR) and evolution reaction (CO 2 ER) kinetics at cathodes make these batteries losing most of their capacity and power. Here, by engineering the carbon-free three-dimensional (3D) Cr-N-Ru catalysts on silicon nanopillars (Si NP) cathodes, we report a reversible solar photothermal (SPT) molten salt Li-CO 2 battery where solar energy can be efficiently harvested (over 90 % absorption rate from 300 nm to 2500 nm), concentrated and converted to heat. Theoretical simulations support that the 3D Cr-N-Ru catalysts exhibit lower energy barrier and more effectively catalyze the CO 2 RR and CO 2 ER process compared to individual Ru or CrN catalyst. The SPT Li-CO 2 battery shows a reversible cycle lifespan of 83 cycles with lower charge potential (3.2 V) and higher energy efficiency of 72 %, corresponding to ∼ 0.9 V potential gap, than the one using conventional Ru catalysts assembled on Si NP cathode. This battery technology paves the way for developing the next-generation safe and high-energy–density energy storage batteries with carbon–neutral effect.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2022
·
IF 4.326
Helin Wang,Weiwei Wu,Qiurong Jia,Ting Liu,Fu Liu,Min Zhang,Miao Bai,Shaowen Li,Xiaoyu Tang,Bin Gan,Yue Ma
The Si anodes suffer from the repetitive buildup of the solid electrolyte interphase, electrode pulverization upon the lithiation/delithiation process, as well as the Li trapping in the alloy intermediates. Herein, a facile electrostatic self-assembly process of the Si nanosheets (SiNS) and graphite microsheets (GMs) is proposed as a viable high-capacity composite anode. Upon the appropriate interfacial tailoring, the SiNS/GMs composite not only guarantees the intimate contact mode between the sand-milled Si nanosheets and the positively charged graphite sheets but also renders the enhanced electrode conductivity and high-rate performance (886.2 mAh g–1 at current density of 5 A g–1). In addition, the prelithiated SiNS/GMs (Pre-SiNS/GMs) are fabricated by spraying stabilized lithium metal powder (SLMP) at the predetermined amounts onto the electrodes, contributing to the improved initial Coulombic efficiency (ICE) of the half cell (99%). As the Pre-SiNS/GMs anodes are assembled with the diverse commercial cathodes, the full cell models reveal the balanced cycling endurance and the high gravimetric energy/power densities.
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POLYMER
·
2026
·
IF 5.1
Chengliang Wang,Jianjiang He,Wei Zhao,Jingjiang Sun,Qingfu Wang
Solid polymer electrolytes (SPEs) synthesized via in-situ polymerization exhibit excellent interfacial compatibility; however their inherently low ionic conductivity limits their application in solid-state lithium (Li) metal batteries (LMBs). Herein, we report a type of SPE composed of succinonitrile (SN), LiTFSI, and cross-linked polymer matrix (SNCE). Within the electrolyte, Li + coordinates with ether, carbonyl, and nitrile groups; the strong SN-Li + interactions promote Li + detachment from the polymer matrix, forming continuous Li + conduction pathways. This design imparts both mechanical robustness and superior electrochemical performance to the SPEs. The cross-linked structure restricts the migration of SN, suppressing undesirable side reactions with the Li anode at the initial stage, compensating for the reduction in mechanical strength due to SN addition, and further improving electrochemical stability. The optimized SNCE-2 exhibits an ionic conductivity of 0.16 mS cm −1 at 30 °C, an electrochemical stability window (ESW) up to 5.2 V, and a Li + transference number ( t Li+ ) of 0.44. The in-situ polymerization ensures intimate electrode-electrolyte contact, and the formation of a stable solid-electrolyte interphase (SEI) on the Li anode by SNCE-2 enables Li|SNCE-2|Li symmetric cells to cycle stably for 1000 h at 0.2 mA cm −2 . The superior cycling performance of Li|SNCE-2|NCM622 and Li|SNCE-2|LFMP cells confirms the potential of SNCE-2 for high-voltage LMBs. Furthermore, the Li|SNCE-2|LFP cells demonstrates remarkable cycling durability, maintaining 86.1% of its capacity after 1000 cycles at 0.2C. Moreover, Li|SNCE-2|LFP pouch batteries also exhibit reliable safety performance. Therefore, this work provides a promising strategy for the development of SPEs for next-generation safety solid LMBs.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Zengcai Guo,Shimin Liao,Feng Li,Linlin Shi,Bihai Su,Jingbo Mu,Yanming Wang,Zhongkai Huang,Feng Xu,Chaowen Guan
The broad application of solid-state polymer electrolytes (SPEs) has been hindered by the extremely low transference number of lithium ions and ionic conductivities. This study innovatively introduces Co-doped Li 4 Ti 5 O 12 (CLTO) into poly(ethylene oxide) (PEO) matrix, CLTO not only brings a stronger interaction with TFSI − , but also weakens the Li-O bond in Li 4 Ti 5 O 12 and reduces the diffusion activation energy of Li + . Thus, CLTO introducing PEO-based polymer solid electrolytes could simultaneously promote the dissociation of Li + from LiTFSI and Li 4 Ti 5 O 12, constructing efficient dual lithium salt dissociation regions and rapid Li + conduction channels. The experimental tests and density functional theory calculations have confirmed the operational mechanisms of CLTO within the polymer matrix. As a result, the obtained SPEs exhibit a high ionic conductivity (1.09 × 10 −4 S cm −1 ) and a quite large t Li + of 0.83 at 60 °C. Moreover, the low (Highest Occupied Molecular Orbital) HOMO energy (−7.25 eV) of the CLTO-LiTFSI-PEO-10 (CLP-10) endow it can accommodate both the Li-metal anode and high-voltage cathodes. The all-solid-state LiFePO 4 ||Li and NCM811|| Li batteries offer exceptional specific capacities of 164.61 and 194.95 mAh/g at 60 °C, respectively. In addition, the pouch cell assembled with CLP-10 works stably under extreme conditions such as bending and shearing.
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Chemical Engineering Journal Advances
·
2026
·
IF 6.9
Wenbin Fan,Lizhi Jiang,Bingqing Yan,Huifang Li
Driven by surging global lithium demand, highly selective lithium separation from magnesium-rich brines is urgently required. This work systematically investigated the structure–performance relationship of four aryl-substituted phosphates (TOP, DPOP, IPPP, TPP). Moderate aryl substitution widened the coordination difference between Li + and Mg 2+ through electron-withdrawing effects, and DPOP exhibited the optimal balance of extraction capacity and selectivity. A ternary synergistic extraction system was fabricated with DPOP as the primary extractant, P204 to immobilize Fe 3+ , and eco-friendly diethyl succinate (DES) as a polar modifier. DES inhibited third-phase formation at DPOP contents of 10–50 vol.% and produced synergistic solvation via carbonyl groups. Under optimized conditions, the single-stage Li + extraction efficiency achieved ∼73%, and the Li/Mg separation factor reached 1630, nearly 80 times that of the traditional TBP–FeCl 3 system. Synergistic coordination of P204 and DES stabilized Fe 3+ in the organic phase, realizing quantitative lithium stripping with deionized water and avoiding concentrated acid and saponification. The organic phase maintained over 80% extraction efficiency after ten cycles. Slope analysis and FT-IR confirmed the extracted complex LiFeCl 4 •2DPOP•0.1DES. This work transforms DPOP into a sustainable, low-cost, closed loop industrial solution for lithium recovery from high Mg/Li brines.
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APPLIED SURFACE SCIENCE
·
2026
·
IF 6.6
Ningyu Guo,Yingqiang Zhao,Peng Zhao,Qinxing Xie
A Zn-Co bimetallic ZIF-derived N-doped porous carbon with CNT network is constructed. • Acid etching tailors hierarchical porosity and exposes catalytic metal sites. • The conductive CNT framework accelerates electron/ion transport. • Strong polysulfide immobilization and rapid redox kinetics are achieved. • High capacity and stable cycling are maintained under lean electrolyte. Efficient sulfur hosts with strong polysulfide confinement and fast redox kinetics are essential for high-performance lithium-sulfur batteries. Herein, a Zn-Co bimetallic ZIF-derived multifunctional porous carbon with in-situ grown carbon nanotubes (CNTs) is constructed via controlled carbonization followed by acid etching. The resulting ZIFCA material features a hierarchical porous architecture with Zn/N-derived polar sites, a conductive CNT network, and Co-based catalytic nanodomains coupled with defect-rich carbon interfaces. These structural characteristics synergistically enhance polysulfide adsorption and accelerate sulfur redox conversion, thereby suppressing the shuttle effect and improving reaction kinetics. As a sulfur host, ZIFCA/S delivers a reversible capacity of 1035 mAh g −1 after 200 cycles at 1.0C, and retains around 700 mAh g −1 at 5C. Notably, under lean electrolyte conditions (E/S = 5.7 μL mg −1 ), ZIFCA/S maintains a capacity of 903 mAh g −1 after 110 cycles with an areal capacity of about 2.79 mAh cm −2 . This work highlights the effectiveness of integrating conductive and catalytic functionalities in ZIF-derived carbon frameworks for advanced Li-S batteries. Download: Download high-res image (162KB) Download: Download full-size image
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IONICS
·
2026
·
IF 3.4
Zhao Yang,Zhang Wang,Jia Qingbo,Wu Can,Wang Ding,Duan Jianguo,Zhang Yingjie
P2-type cathode materials with good rate performance show significant potential for sodium-ion batteries (SIBs), but their low theoretical capacity limits further development. Here, the Na₀.₇₂Cu₀.₂₁Mn₀.₆₇Li₀.₀₆Ti₀.₀₆O₂ cathode layered material is elaborately designed, and the oxygen redox reaction of the oxygen anions gradually shifts from O²⁻ to O₂⁻ via the synergistic modulation of Li⁺ and Ti⁴⁺, especially at a higher voltage, achieving high-capacity Co/Ni-free SIBs. Notably, the NCMLT electrode delivers a capacity of 127.1 mAh·g⁻¹ after 200 cycles at the 1 C, and attains an outstanding capacity retention of 89.86%. Additionally, the metal oxide cost of the synthesized material is relatively low. Thus, this work provides a new approach to design the cathode for high-performance SIBs and offers a value for further development.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Jinghai Zhang,Kangjun Ji,Zirui Wang,Wei Shi,Zhongkai Zhao,Xiao Du,Xiaogang Hao
The rapid growth in lithium demand for battery applications has driven the need for safe and efficient extraction technologies from salt lake brines. Current methods face challenges including low recovery rates, slow adsorption kinetics, and environmental concerns from organic solvent usage. To address these limitations, the environmentally friendly electrochemically switched ion exchange (ESIX) system using a three-dimensional LiMn 2 O 4 /C/SA-c-PEO@GF electrode was developed. The electrode employs sodium alginate (SA) and polyethylene oxide (PEO) as chemically cross-linked binders on a graphite felt (GF) current collector. In the constant current-constant voltage coupling drive mode, the system achieved 97% lithium extraction efficiency with an adsorption capacity of 3.89 mg·g −1 and a Li + /Mg 2+ separation coefficient of 191, the energy consumption was 14.51 Wh·mol −1 and 485 mg·L −1 Li + solution was obtained from actual Zarkhan Salt Lake brine (Mg 2+ /Li + : ∼426.6) by one-step concentration. This study shows the LiMn 2 O 4 /C/SA-c-PEO@GF electrode with high extraction efficiency and fast adsorption rate, providing a simple and efficient method for lithium recovery from salt lake brine with high Mg 2+ /Li + ratio.
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Sustainable Energy & Fuels
·
2022
·Vol. 6
·期 9
·2207-2222
·
IF 6.813
Zhenyu Jiang,Jing Sun,Pingshan Jia,Wenlong Wang,Zhanlong Song,Xiqiang Zhao,Yanpeng Mao
With the upcoming retirement of widely employed LiFePO4 (LFP) batteries, a sustainable strategy for recycling their valuable components is urgent. In this work, spent LFP cathodes were revived through a microwave-hydrothermal relithiation process, complemented with microwave-reduced graphene oxide (MWrGO) derived from spent graphite anodes, to form a composite LFP/MWrGO cathode material. The defect–repair process, performed under optimal conditions (150 °C for 1 h), allows LFP cathodes to gain better morphology and electrochemical performance with a specific capacity of 150.5 mA h g−1 at 0.1C. The introduction of anode-revived graphene via electrostatic self-assembly helps form a hierarchical structure and conductive network for regenerated LFP, enabling fast ion and electron transfer for redox reactions. When doped with 5 wt% graphene, the regenerated LFP/MWrGO composite displays an enhanced specific capacity of 161.4 mA h g−1 and high capacity retention (i.e., 94.9% over 100 cycles) at 0.2C. Laboratory-scale economic and environmental analyses indicate that the entire regeneration process has a favorable atom economy of recovery with low energy/time/reagent consumption and greenhouse gas emission, owing to the featured microwave-material interaction. This study provides a green facile method as a reference for the regeneration of spent LFP batteries, which can be extended to other types of batteries, and promotes the sustainability of Li-ion battery downstream technology.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Sen Dang,Wei Hou,Yulin Min,Junfeng Wu,Qunjie Xu,Penghui Shi
This study aimed to further expand the scope of use of spent lithium-ion batteries (LIBs) and improve their value. We proposed a dual-function electro-oxidation strategy that can realize the highly selective recovery of Li + from spent NCM batteries and the in situ modification of delithiation materials. Under the optimum conditions, the selective recovery rate of Li + exceeded 99%. After electro-oxidation, the electrolyte can be directly heated and concentrated to obtain Li 2 CO 3 . Moreover, the large number of oxygen vacancies and metal vacancies produced by electro-oxidation, as well as the changes in structure and morphology, enabled the delithiation material to exhibit excellent catalytic performance. Within 30 min, the degradation rate of sulfamethoxazole reached 100%. This strategy can be used to recycle and reuse spent LIBs and thus achieve the goal of “turning waste into treasure”.
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