Journal of Energy Storage
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2026
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IF 10.7
Meng Yu,Qianqian Liu,Zhixun Lei,Panpan Wang,Ruirui Wang,Miao Cheng,Jing Hu,Wei Lu,Bo Liu,Wanfei Li
The high energy density and inherent safety feature of solid-state lithium metal batteries (SSLMBs) have drawn considerable interest. Nevertheless, the widespread deployment of SSLMBs remains constrained by insufficient ionic conductivity. Herein, we report a high-performance Li-salt-loaded cellulose nanocrystal-reinforced PVDF-HFP solid-state electrolyte (Li-CPSE) through a sustainable freeze-casting, salt-loading, and in situ photopolymerization strategy. This design enables vertically aligned ion-transport pathways, integrates internal Li + reservoirs with stabilized interfacial chemistry, and constructs a mechanically robust rigid-flexible 3D framework. Owing to these synergistic advantages, Li-CPSE exhibits fast Li + transport (1.06 mS cm −1 at 30 °C), a reduced activation barrier (0.18 e V ), and a broad electrochemical window reaching 5.0 V. Meanwhile, SSLMBs based on Li-CPSE exhibit long-term cycling durability, retaining 98.2% of the original capacity over 500 cycles in Li/LiFePO 4 cells. Flexible pouch cell further demonstrated excellent mechanical resilience and cycling stability, retaining 92.2% capacity over 70 cycles with an average coulombic efficiency of 99.9%, while continuously powering LEDs under bending and cutting. Additionally, bipolar stacking of two pouch cells delivers 6.78 V , sufficient to power commercial 5.3 V devices. The work highlights a scalable and sustainable strategy for advancing high-performance polymer electrolytes toward practical SSLMB applications.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2026
·
IF 12.5
Qiujun Wang,Wei Zhang,Gaofeng An,Zhaojin Li,Huilan Sun,Qujiang Sun,Di Zhang,Ranran Li,Fei Yuan,Bo Wang
PEGDME and Li 3 OCl synergistically reduce the crystallinity of PVDF and create additional Li + transport pathways. • The modified PVDF electrolyte exhibits an ionic conductivity of 8.65 × 10 −4 S cm −1 and a Li + transference number of 0.55 at 25 °C. • The assembled LFP cell maintains 80.2% capacity after 500 cycles at 0.5C and 25 °C Owing to superior flexibility and processability, polymer electrolytes have received considerable research attention. Poly(vinylidene fluoride) (PVDF) is a promising electrolyte candidate with high dielectric constant and tunable chain structure, Nevertheless, in lithium metal batteries (LMBs), its high crystallinity results in insufficient Li-ion conductivity, while its inherent porous structure tends to induce uneven Li deposition, thereby causing poor electrolyte-electrode interfacial stability. Herein, a novel PVDF-based composite solid electrolyte is developed by introducing the plasticizer poly(ethylene glycol) dimethyl ether (PEGDME) and Li-rich anti-perovskite Li 3 OCl as fillers. Li 3 OCl can complex with PVDF and induce deprotonation, offering an extra Li + transport pathway, while the synergistic effect between PEGDME and Li 3 OCl effectively reduces PVDF crystallinity and promotes chain mobility. This synergistic design suppresses polymer crystallization, introduces additional Li + conduction channels, and prevents Li dendrites, leading to markedly improved Li + transference number and ionic conductivity, along with a stabilized electrolyte–electrode interface. At 0.5C and 25 °C, the Li | PVDF-LiTFSI-PEGDME-1%Li 3 OCl | LiFePO 4 cell exhibits a capacity retention of 80. 2% after 500 cycles. This research provides an innovative strategy for constructing solid electrolytes with favorable interfacial compatibility and superior ionic conductivity for high-performance LMBs. This study used a solution casting method to prepare a composite polymer solid electrolyte with polyvinylidene fluoride (PVDF) as the polymer, polyethylene glycol dimethyl ether (PEGDME) as the small molecule plasticizer, and lithium rich perovskite resistant Li 3 OCl as the inorganic filler. PEGDME and Li 3 OCl inhibited the crystallization of PVDF, opening up additional channels for Li + transport and significantly improving the efficiency of Li + transport. Meanwhile, the introduction of Li 3 OCl effectively suppressed the growth of lithium dendrites and improved the electrode electrolyte interface problem. After 500 cycles at 0.5C and 25 °C, the capacity retention rate of the assembled LiFePO 4 (LFP) battery reached 80.2%. Download: Download high-res image (182KB) Download: Download full-size image
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Journal of Energy Storage
·
2026
·
IF 10.7
Huihui Gan,Jia Dong,Siqi Ying,Dexian Zhou,Jiao Zhang,Daiwei Li,Jing Wang,Binghua Zhou,Shizheng Zheng,Changyuan Hu
Li-rich Mn-based oxide (LRMO) represents a promising cathode for next-generation lithium-ion batteries due to its superior energy density. However, its widespread commercialization is hampered by severe capacity fade, voltage decay, and inferior rate performance. Herein, modification of LRMO with Li 3 PO 4 (LPO) is achieved by a novel one-step strategy that seamlessly integrates freeze-drying with subsequent calcination in air. Crucially, this LPO significantly enhances lithium-ion diffusion kinetics without altering the bulk crystal structure. The optimized cathode with a 3 wt% LPO delivers superior cycling stability, with a remarkable capacity retention of 67.8% after 600 cycles at 1C and 25 °C, significantly outperforming the blank cathode (54.9%). It also exhibits outstanding rate capability (102.9 mAh g −1 at 10C) and long-term cyclability (58.0% capacity retention after 1000 cycles at 3C). Furthermore, the practical applicability is further demonstrated under a 1.5C/0.5C protocol and in a full cell with a Si@C anode. This work provides a scalable synthesis route, advancing the development of practical high-energy LRMO cathodes.
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ADVANCED MATERIALS
·
2026
·
IF 29.1
Xingwu Zhai,Yuchun Liu,Tianchen Wei,Leyi Su,Jing Zhang,Liang Wu,Yuxin Xiao,Tianqi Liu,Xinyun Wang,Cong Han,Zhaodi Fan,Min Zhou
The practical implementation of Li─CO 2 batteries is constrained by the challenging decomposition of Li 2 CO 3 . While cleaving C─O bonds is predominantly focused on, Li─O cleavage is the initial and rate-limiting step. The Li─O bond strength is a key descriptor for this process, which involves increasing the population of its antibonding orbital. The HOMO of Li 2 CO 3 is composed of O p -orbitals that couple with d -orbitals of transition metals. Herein, over-coordination of metal sites modulates the electronic distribution in metal d -orbitals and promotes O p -orbital polarization, converting symmetric metal pairs into asymmetric pairs. This resulting localized dipole moment induces an asymmetric interfacial polarized electron density distribution and targeted bond polarization. The dipole at asymmetric sites polarizes O p -orbitals and promotes electron transfer into the Li─O antibonding orbital. Using WB as proof-of-concept, this asymmetry electronic polarization increases the population of Li─O antibonding orbitals and weakens their interaction. This results in a markedly low decomposition energy barrier of 0.53 eV for Li 2 CO 3 and an ultralow charge voltage of 2.99 V. The battery also exhibits stable operation for 500 h at 120°C with high energy efficiency (74.43%). This work highlights local dipole engineering and establishes electronic asymmetry-mediated activation for efficient Li─CO 2 batteries.
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高影响因子
ENERGY
·
2026
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IF 10.1
Yuchen Zhang,Yuanchao Zhang,Jiawei Wu,Wei Li,Jie Wu,Junjie Yang,Song Li,Weixiong Wu
MOF-based composite phase change materials (CPCM) have been developed as promising solutions for the thermal management of lithium-ion batteries to maintain suitable temperatures. Nevertheless, the discrepancy in the thermal management performance of various MOFs-based and MOFs-derived carbon-based CPCMs awaits investigation. In this work, CPCMs were synthesized by combining polyethylene glycol, polyvinylpyrrolidone, and expanded graphite with three large production metal-organic frameworks, including ZIF-8, Al-fumarate, MIL-101(Cr), whose pore size gradually increased, and their derived carbons. All the CPCMs exhibited excellent shape stability, high thermal stability, and enhanced thermal conductivity, while MIL-101(Cr) exhibited overstrong nanoconfinement effects, leading to the decrease of enthalpy during the phase transition. However, after carbonization, CPCM-MIL-101(Cr)-C achieved the highest melting enthalpy of 99.0 J g −1 and a higher proportion of ordered carbon domains that enhanced thermal properties. Battery tests under different discharge rates and long-term discharge-charge cycles showed that the CPCMs effectively reduced the peak temperatures of the battery surface even at 5C discharge rate. Economic analysis of such large-production MOFs revealed that CPCM-ZIF-8 was the most cost-effective at moderate discharge rates, while CPCM-MIL-101(Cr)-C was better under extreme conditions of 5C. This study provides a comprehensive evaluation of MOF-based and MOF-derived carbon-based CPCMs for Li-ion battery thermal management, highlighting their practical potential in the battery thermal management field.
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY
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2026
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IF 4.6
Chenghao Wei,Chenglei Wang,Mengyi Wang,Junfeng Chen,Weijie Liu
Developing high-performance non-noble metal electrocatalysts is critical for efficient oxygen evolution reaction (OER) in water electrolysis. High-entropy oxides (HEOs) have attracted extensive attention owing to their multi-element synergy and structural stability, but their practical applications are limited by high interfacial resistance and insufficient intrinsic activity. In this work, Li-doped FeCoNiMnZn HEOs were synthesized via a sol-gel combustion method and loaded onto bare nickel foam (NF) and ONF. The effects of Li doping and substrate modification on crystal structure, electronic state, and OER performance were systematically investigated. Results show that 7.5% Li doping optimizes the electronic structure and modulates oxygen vacancy defects, while the ONF substrate greatly reduces interfacial charge-transfer resistance. The optimal ONF-7.5% catalyst exhibits a low overpotential of 240 mV at 10 mA·cm −2 , a small Tafel slope of 54.84 mV·dec −1 , and excellent long-term stability for 100 h. This work provides a feasible strategy of combining Li doping and substrate interfacial engineering to boost OER performance of HEOs.
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ACS Sensors
·
2026
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IF 10.9
Zhefu Mu,Xianjie Xu,Jiaxin Sun,Guo Chen,Zijun Huang,Xinkai Qi,Hongwei Liu,Yanhong Wei,Jialiang Zhou,Peng Wang,Xiuquan Gu,Sheng Huang
Monitoring internal electrolyte decomposition byproducts is pivotal for the early warning of thermal runaway in lithium-ion batteries yet remains a formidable challenge due to the harsh chemical environment. Herein, we engineer a robust electrochemical sensor based on a CsPbBr3/Al2O3@EVA heterojunction architecture to achieve real-time, in situ tracking of lithium methoxide (CH3OLi) evolution. Through interface engineering, the synthesized quantum dot−Al2O3 composite (8.7at%Al) achieves exceptional stability in reducing electrolytes, attributed to the synergistic dual-passivation of Br−Al interfacial bonding and EVA encapsulation. The sensor exhibits superior sensitivity (0.3 at 10% CH3OLi) and rapid kinetics (response/recovery: 8.98 s/56.11 s), driven by the promoted molecular diffusion in mesoporous Al2O3 and polarized adsorption within the Pb+2−Br− framework. Density functional theory (DFT) calculations further corroborate this mechanism, revealing a strong Li+ binding energy of −1.54 eV at Al−O−Br active sites. Furthermore, by integrating the sensor signals with an XGBoost machine learning algorithm (accuracy >99%), we demonstrate a smart monitoring system capable of accurately predicting battery voltage variations and identifying potential safety hazards. This work establishes a new paradigm merging interface-stabilized materials with intelligent algorithms, transforming battery safety management from passive protection to active early warning.
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Nature Communications
·
2026
·
IF 18.1
Zheng Nengzhan,Zhu Yanfei,Ji Haocheng,Wang Junxiong,Wu Zhuozhao,Ji Guanjun,Shi Ruyu,Li Bo,Zhou Guangmin
Direct recycling of spent lithium-ion batteries is an essential approach to address challenges related to energy security and resource sustainability. However, previous direct recycling methods could only restore spent electrode materials to their original state, limiting their ability to meet rapidly advancing performance benchmarks. Herein, we present a promising upcycling strategy that reconstructs degraded ternary layered positive electrode materials into Li-rich oxides, thereby achieving with substantial capacity advantages. Microstructure characterizations and theoretical calculations demonstrate that intrinsic vacancy defects in the degraded materials provide energetically favorable atomic-scale diffusion pathways for exogenous lithium-ions, mediating the conversion of the layered R-3m structure into the C2/m phase and the formation of Li 2 TMO 3 -type domains. With activated anion redox reactions, it attains a specific capacity increase from 100 to over 274 mAh g −1 at 0.1 C and maintains 92.5% capacity retention over 300 cycles at 0.5 C. The strategy has been scaled to kilogram-level production, achieving a specific energy of 377 Wh kg −1 in a 14 Ah-level pouch cell. This result validates the upcycling approach, bridging laboratory research and industrial manufacturing of high-energy-density batteries via sustainable recycling.
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ACS Applied Materials & Interfaces
·
2026
·Vol. 18
·期 34
·46260-46269
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IF 7.8
Chen Wen-Ze,Zhai Xiaoyi,Ma Xiao-Qing,Zhang Jin,Zhang Guo-Qin,Tong Yuan-Bo,Cao Dong-Qiang,Gao Xu-Sheng,Luo Hong-Bin,Zhu Chenjie,Ren Xiao-Ming
Covalent organic frameworks (COFs) have garnered increasing attention as versatile platforms for Li + conduction in lithium-based batteries; however, achieving high ionic conductivity in COF-based electrolytes remains a formidable challenge. Herein, we demonstrate a robust cationic vinylene-linked COF (COF-Br) as an efficient host for constructing high-performance composite electrolytes and highlight its great potential for practical application in lithium-metal batteries. The composite electrolyte, named as IL@COF-Br, was prepared by incorporating an ionic-liquid electrolyte (Li-IL) within the well-defined nanochannels of COF-Br. The cationic framework enhances dielectric screening, thereby promoting lithium-salt dissociation, while strong electrostatic interactions between the framework and anions effectively suppress anion mobility, leading to preferential Li + transport. As a result, IL@COF-Br delivers a high ionic conductivity exceeding 10 −3 S cm −1 , a large Li + transference number (0.79), and a wide electrochemical stability window (5.42 V). In addition, the composite electrolyte exhibits excellent interfacial compatibility with lithium metal and effectively mitigates dendrite formation during repeated cycling. When integrated into lithium-metal batteries, IL@COF-Br enables the batteries to achieve outstanding electrochemical performance, including good rate capability, a high specific capacity of 137.6 mAh g −1 at 0.5 C, and remarkable cycling stability, with a capacity retention of 90.4% and a Coulombic efficiency of 99.5% after 300 charge–discharge cycles. This study provides an effective strategy for leveraging cationic COF architectures to develop advanced quasi-solid-state electrolytes for next-generation lithium-metal batteries.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2026
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IF 9.6
Min Cheng,Xu Zhou,Zixuan Chen,Junhao Chen,Fangyi Zha,Yuhang Liang,Yuanhui Zheng
Extending the lifetime of lithium metal batteries requires electrolyte strategies that coordinate Li + solvation with interfacial chemistry. Here, we introduce hydrogen-bond-mediated cross-sheath molecular association as a design principle for an ether-based localized high-concentration electrolyte. Spectroscopic analyses, noncovalent-interaction calculations and ab initio molecular dynamics simulations indicate that 1,1,2,2-tetrafluoroethyl-2,2,3,3-tetrafluoropropyl ether (TTE) and fluoroethylene carbonate (FEC) reside predominantly in the outer solvation environment, whereas 1,2-diethoxyethane (DEE) remains an important inner-shell solvent. The pre-associated FEC–TTE motif exhibits a stronger overall association with DEE than isolated TTE, providing a plausible molecular bridge between the outer and primary solvation environments. This cross-sheath association contributes to weaker average Li + –DEE coordination and increased participation of bis(fluorosulfonyl)imide (FSI − ) and isosorbide dinitrate (ISDN), yielding a compact, anion-enriched local solvation structure. At the electrode interface, the reconstructed solvation environment cooperates with the reduction chemistry of FEC, FSI − and ISDN to suppress excessive solvent decomposition and promote a homogeneous LiN x O y /LiF-rich solid electrolyte interphase. Consequently, Li||Li symmetric cells sustain stable plating/stripping for approximately 1354 h at 1 mA cm −2 and 1 mAh cm −2 , while high-loading Li||LiFePO 4 cells cycle for approximately 1188 cycles at 1 C. Unlike conventional approaches focused primarily on direct regulation of the first Li + solvation shell, this work demonstrates that engineering molecular associations across solvation environments offers an effective route to couple solvation redistribution with interfacial film formation. Download: Download high-res image (232KB) Download: Download full-size image Hydrogen-bond-mediated cross-sheath associations promote anion-enriched Li⁺ solvation and couple solvation redistribution with interfacial reduction chemistry, facilitating the formation of a LiN x O y /LiF-rich SEI and uniform lithium deposition.
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Nanomaterials
·
2025
·Vol. 15
·期 13
·1010
·
IF 4.3
Qiya Liu,Min Zhang,Xinsheng Yang,Tixian Zeng,Minghu Pan
Topological insulators (TIs) can be widely applied in the fields of ultrafast optical and spintronic devices owing to the existence of topologically protected gapless Dirac surface states. However, the study of ultrafast dynamics of carriers in TIs remains elusive. In this work, the carrier dynamics of Li-doped Bi2−xSe3single crystals were investigated by femtosecond (fs) transient optical spectroscopy (ΔR/R(t) signals). The temperature dependence for the relaxation rates of the electron–electron interaction and electron–phonon coupling is consistent with the results of electrical transport, which indicates the carrier dynamics of TI is highly related with carrier concentrations. We find that the carrier type and concentration of Bi2Se3can be tuned by Li doping, leading to a metal-insulation transition at low temperatures (T ≤ 55 K), indicating that electron–electron interactions are dominant at low temperature. For T > 55 K, electron–phonon coupling in the bulk carriers becomes the main electric transport mechanism.
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NEW JOURNAL OF CHEMISTRY
·
2025
·
IF 2.5
Rong Li,ZhiHui Hao,Xiangwei Zhao,Huilin Zhou,Zhimin He,Qin Dong,Wei Hong,Xinglong Gou
Metal sulfides, such as SnS2, have been extensively studied as separator modifiers in lithium–sulfur batteries (LSBs) owing to their dual functionality in chemically anchoring lithium polysulfides (LiPSs) and catalytically facilitating redox reactions. Nevertheless, poor electrical conductivity and limited catalytic efficiency restrict their practical implementation for LiPS transformation kinetics. To address these issues, we prepared Mo-doped SnS2 (Mo–SnS2) nanosheets with sulfur vacancies through a rapid one-pot formamide-assisted method. The incorporation of Mo heteroatoms not only improves conductivity but also induces favorable sulfur vacancies, synergistically promoting both adsorption and electrocatalytic conversion of LiPSs. The Li–S cell with a Mo–SnS2 nanosheet-modified separator delivers a remarkable initial capacity of 1007.5 mAh g−1 at 1C, maintains 799.5 mAh g−1 after 600 cycles with a low fading ratio of 0.034% per cycle, and demonstrates a favorable rate performance of 591.9 mAh g−1 at 5C. This defect engineering strategy through heteroatom doping offers a promising approach to concurrently mitigate the polysulfide shuttle effect and enhance the reaction kinetics in sulfur-based energy storage systems.
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