CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Yan Meng,Yuanheng Wang,Qingjiang Liu,Xingyu Chen,Enhui Wang,Weihua Chen,Hongji Pan,Jinghao Zhao,Xin Li,Jia-Yan Liang
Local high concentration electrolytes (LHCEs) have great potential for sodium-ion batteries (SIBs) owing to their anion-enriched solvation structures that facilitate the formation of inorganic-rich solid electrolyte interphases (SEIs). However, insufficient solvent-cation interactions in solvation structure inherently lead to limited ion migration kinetics and compromised electrolyte thermodynamics. Here, we report a novel LHCE design employing methyl 2,2,2-trifluoroethyl ester (FEMC) as a functional diluent. The dipole-dipole interaction between FEMC and ethylene carbonate (EC) induces the electrons polarization of fluorine atoms toward carbonyl group in FEMC, thereby strengthening the coordination ability of FEMC. The solvation structure, maintaining more anion participation, with enhanced FEMC diluent coordination significantly improves ion migration kinetics and derives a stable inorganic-rich (NaF/Na x PO y ) SEI, effectively mitigating cell interfacial concentration polarization. This reconfigured LHCE enables hard carbon (HC) anode to deliver a remarkable specific capacity of 287.00 mAh g −1 with 80.1 % capacity retention over 1000 cycles under 0.1 A g −1 and achieve extraordinary cycling stability over a wide temperature range. This work provides a new insight into designing electrolyte solvation structure via intermolecular dipole-dipole interactions.
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Journal of Energy Chemistry
·
2026
·
IF 15.6
Kun Shi,Chenyin Peng,Xueling Cheng,Tingting Xu,Zeheng Yang,Weixin Zhang
A long-standing trade-off between fire safety and electrochemical performance in lithium-ion batteries arises from aggressive parasitic reactions between highly reactive flame retardants and electrodes. Herein, a phosphorus-fixed gel polymer electrolyte is constructed by covalently integrating 9,10-dihydro-9-oxa-10-phosphaphenanthrene 10-oxide (DOPO) into a vinylene carbonate-pentaerythritol tetraacrylate copolymer network through phosphorus-hydrogen addition. Covalent fixation confines DOPO within the gel matrix, delivering intrinsic flame retardancy while circumventing detrimental phosphorus-related side reactions. The abundant polar O=P–-O moieties in DOPO not only promote lithium salt dissociation and provide additional coordination sites to facilitate rapid Li + transport, but also actively reshape the Li + solvation environment. Specifically, the DOPO-incorporated polymer tethers solvent molecules and restricts their entry into the primary coordination sheath, shifting the solvation equilibrium toward an anion‑dominated configuration. This solvation reconfiguration fosters LiF‑rich robust interphases on both electrodes, ensuring stable lithium deposition and exceptional oxidative stability. As a result, the as -prepared electrolyte achieves outstanding compatibility exceeding 3500 h against lithium anode, significantly enhanced cycling stability in LiFePO 4 , high-voltage LiNi 0.8 Co 0.1 Mn 0.1 O 2 and LiNi 0.9 Co 0.05 Mn 0.05 O 2 -based full cells, as well as remarkable tolerance to flame, physical damage, and high-temperature operation. This work establishes a new paradigm for high-safety lithium-ion batteries, where phosphorus-based solvation engineering secures durable electrode interfaces under demanding conditions. The safety-performance trade-off in lithium-ion batteries is overcome by covalently fixing phosphorus-containing flame retardants into a gel polymer electrolyte, which reshapes Li + solvation to form durable LiF-rich interphases for uniform Li deposition and high-voltage stability. Download: Download high-res image (117KB) Download: Download full-size image
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2026
·Vol. 65
·期 31
·16523-16533
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IF 3.9
Tian Xin,Liu Wen,Peng Wenchao,Li Chunli,Liu Jiapeng
The green chemical dimethyl carbonate has become indispensable
in multiple industries and is commonly produced by transesterification.
Heterogeneous catalysts have received considerable research attention
owing to their recyclability and environmental benefits. This work
reports a series of Na-doped C 3 N 4 catalysts
with adjustable acid−base sites. The synergistic effect between
acid−base sites significantly enhances methanol adsorption
and dissociation, thereby promoting dimethyl carbonate formation.
Theoretical calculations reveal charge redistribution in 0.15Na-CN,
and the calculated adsorption energy and bond dissociation energy
confirm that the synergistic effect accounts for enhanced methanol
activation. In situ characterization confirms the adsorption and activation
of reactants on the catalyst surfaces. The 0.15Na-CN catalyst achieves
a dimethyl carbonate yield of 89.94% and a selectivity of 99.56% at
80 ° C after 4 h of reaction, with a turnover frequency of 37.37
h −1 . Moreover, 0.15Na-CN demonstrates excellent
catalytic stability. This work provides an approach for the synergistic
catalytic synthesis of dimethyl carbonate.
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Nanomaterials
·
2026
·Vol. 16
·期 15
·969
·
IF 4.8
Junaid Aslam,Muhammad Arif Khan,Weiwei Sun,Chao Yang
Germanium (Ge) is a promising high-capacity anode material for lithium-ion batteries; however, its practical application remains limited by substantial volume variation, unstable interfacial reactions, and rapid capacity degradation during repeated lithiation/delithiation. In this work, a binder-free Ge/C/MXene@NF hybrid electrode was developed through a sequential fabrication process, where Ge nanoparticles were immobilized within a PVP-derived carbon matrix supported on a three-dimensional nickel-foam scaffold and subsequently integrated with a Ti3C2TxMXene conductive network to construct a hierarchical Ge/C/MXene hybrid architecture. The nickel foam provides a continuous current-collecting framework and mechanical support, while the MXene network improves electrical connectivity, electrolyte accessibility, and interfacial charge-transfer kinetics. Structural and compositional analyses further indicate the presence of PVP-derived carbon and a possible minor NiGe interfacial phase formed during annealing. Comparison with Ge@NF and the individual component electrodes provides insight into the respective contributions of MXene, Ge, and the PVP-derived carbon framework to the electrochemical behaviour of the composite electrode. Using the total deposited active-material mass as the normalisation basis, the MXene@Ge@NF electrode retains a reversible specific capacity of 789.8 mAh g−1after 100 cycles at an effective current density of 76.2 mA g−1. The observed electrochemical behaviour originates from the integrated contributions of Ge nanoparticles, the PVP-derived carbon matrix, the conductive Ti3C2TxMXene network, the three-dimensional nickel-foam scaffold, and possible Ni–Ge interfacial interactions. Rather than representing a Ge-dominated electrode, this architecture demonstrates the advantages of integrating multiple functional components within a binder-free Ge/C/MXene hybrid architecture.
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Nano-Micro Letters
·
2026
·Vol. 18
·期 1
·245
·
IF 38.5
Wang Peng,Wang Jian,Bai Longwei,Li Na,Zhou Chuancong,Chen Mingyang,Zhang Jialiang,Xing Zhenyue,Zhao Zaowen,Zhang Wei,Shi Xiaodong
An effective and facile injection strategy based on iodine redox chemistry is proposed to restore lost lithium component in spent LiFePO 4 battery.
In-situ spectroscopic characterization is conducted to unveil the underlying redox mechanism of iodine-mediated lithium reactivation, elucidating its impact on both the cathode and anode.
Regenerated LiFePO 4 cells exhibit ~ 7% capacity recovery, fast charge transfer behavior, and extended cycle life beyond 300 cycles at 1C, outperforming conventional direct recycling methods while maintaining superior cyclic stability.
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Nature Communications
·
2026
·
IF 18.1
Hong Xufeng,Wang Xizhe,Harris Stephen J.,Zhao Hongbo,Meng Jiashen,Jia Qingshan,Zhao Qianchuan,Xu Kang,Pang Quanquan,Jiang Benben
Designing electrolyte materials for high-energy lithium metal batteries requires navigating vast, discrete chemical spaces, where intricate interphasial and electrolyte chemistries render component interactions largely unclear. Traditional trial-and-error methods struggle with discontinuous electrolyte-performance relationships and inefficient adaptation to new molecular candidates, hindering discovery. Here, we propose a two-stage deep active learning framework with knowledge transfer for rapid electrolyte design. In stage one, deep active learning with deep kernel learning selects informative experiments and models discontinuous relationships between formulation and performance, improving sample efficiency and reducing experimental cost. In stage two, target statistic coding quantifies what was learned and transfers it to new design settings, such as expanded formulation spaces and newly introduced components, using only a small number of additional measurements. Using this framework, we found electrolytes that increase the average lifetime of lithium metal symmetric cells by threefold after three learning iterations, and we rapidly identified improved formulations for Li 0 | |LiNi 0.8 Co 0.1 Mn 0.1 O 2 full cells in expanded chemical spaces. This work provides an experiment-driven, sample-efficient route to explore complex electrolyte formulation spaces and quantify inter-component correlations, as well as a realistic, high-cost, small-data benchmark for probabilistic surrogate modeling and sequential decision-making in discrete chemical spaces.
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CHEMICAL ENGINEERING SCIENCE
·
2026
·
IF 5.1
LiJun Tang,Xue Liang,Xiaodong Zhu,Jian Gao
The rise of Na-storage devices has imposed more stringent demands on storage electrode materials with large capacity, long service life, and fast rate capability. However, the application of electrode material is still hampered by its poor electrical conductivity and severe volume expansion. Herein, the reduced graphene oxide-based composite aerogel (rGO gel) is fabricated by implementing a self-shrinking strategy and leveraging the columnar support effect of one-dimensional nano-gaskets (T-Nb 2 O 5 and CNT). Benefiting from the synergistic effect of nano-gaskets and pore structure design, the composite electrode enhances the mechanical strength while buffering the volume change of the active materials. The well-connected conductive network not only promotes the diffusion of Na + but also provides abundant accessible active sites. Therefore, a half-cell assembled using rGO/T-Nb 2 O 5 as working electrode achieves maximum specific capacity of 546.5 mAh g −1 at 0.1 A g −1 . Moreover, the constructed 3D rGO/T-Nb 2 O 5 //rGO/CNT sodium-ion hybrid supercapacitor delivers a mass specific capacitance of 96.5F g −1 at the current density of 2.0 A g −1 . In addition, the high mass energy density of 66.2 Wh kg −1 and power density of 2225 W kg −1 are demonstrated. This work provides a novel structural design strategy for advancing high-performance Na-storage devices.
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DESALINATION
·
2026
·
IF 9.9
Qiang Xian,Xingrui Tang,Shibing Zuo,Di Wu,Lei Xie,Hao Li,Jun Wen
Adsorbents with same grafting ratio but varied chain densities were obtained. • Different grafting densities yield distinct conformations and uptake abilities. • High-density, short-chain materials show better salt tolerance; • High-density adsorbent reaches 9.6 mg/g in seawater-twice that of low-density one. Polymers with distinct chain conformations exhibit pronounced performance differences across various applications, and the grafting density as a critical parameter that governs both chain conformation and the overall performance of polymeric materials. However, existing seawater uranium extraction materials rely exclusively on grafting ratio as the sole criterion for functionalization, but neglecting the critical role of grafting density, resulting in insufficiently extended chain conformations and limited accessibility of adsorption sites, which ultimately constrains uranium extraction efficiency. Herein, a series of materials with identical degrees of functionalization but varying grafting densities and chain lengths of the polymers were obtained, and their uranium adsorption behavior were systematically investigated. In aqueous systems, the adsorption capacities of these adsorbents are comparable. However, in saline environments (including simulated, U-spiked and natural seawater) the adsorbent with high grafting density and short chains architecture exhibits the highest uranium adsorption performances. To gain deeper insight into the underlying mechanisms, the conformational behaviors of polymer chains were monitored by Quartz Crystal Microbalance with Dissipation (QCM-D). The results reveal that high grafting density and short chains display a significantly stronger anti-polyelectrolyte effect compared to that low grafting density and long chains. Consequently, the high grafting density and short of polymer chain adsorbent demonstrates superior resistance to salt-shrinkage and achieves higher uranium extraction capacity (9.6 mg/g) in natural seawater, substantially outperforming the low grafting density long chain (4.9 mg/g). This study provides critical design principles for developing polymeric adsorbents tailored for high-salinity environment applications, such as uranium extraction from seawater.
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ACS Applied Polymer Materials
·
2026
·
IF 5.2
Luo Yanpeng,Cheng Jinyuan,Fang Guigan,Fatehi Pedram,Zhao Mengke,Wang Xiaofa,Shao Xinyi,Zhang Sufeng,Wu Ting
Replacing
petroleum-derived polyols with lignin in polyurethane
foams is essential for increasing renewable carbon utilization but
is hindered by lignin’s heterogeneity, poor solubility, and
limited reactivity. Here, we report a hydrogen-bond-engineered, eutectic-like
polyol platform based on polyethylene glycol (PEG) and salicylic acid
(SA), with ethylene carbonate (EC) as a cosolvent, enabling high lignin
incorporation in the polyurethane foam formulation while maintaining
its processability. Structural and thermal analyses confirm the formation
of a homogeneous amorphous system, in which EC disrupts intermolecular
interactions and enhances chain mobility, reducing the viscosity of
the foam formulation to industrially relevant levels (<5 Pa·s).
This platform enables the direct substitution of up to 80 wt % of
the petroleum-based polyol with kraft lignin, without chemical modification,
in the foam formulation. The resulting foams exhibit uniform closed-cell
morphology with reduced cell size (287 ± 154 μm), enhanced
network integration, improved compressive strength (0.26 MPa) and
hydrophobicity, and increased thermal stability. Notably, the foams
with a high lignin content demonstrate delayed heat penetration under
external heating conditions, which is associated with the formation
of stable closed-cell structures. This one-pot, room-temperature strategy
provides a promising pathway toward the scalable development of high-lignin
polyurethane foams with substantially increased renewable carbon content.
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Journal of Energy Chemistry
·
2026
·
IF 15.6
Wenrong Lv,Fei Pei,Minna Mao,Zhenyu Huang,Gaoce Han,Yi Zhang,Yu Huang,Aiqi He,Wenjie Lin,Qiang Gao,Yue Guo,Yunhui Huang,Yifei Yu
Understanding the structural evolution and failure mechanisms of electrodes is vital for advancing high-energy-density lithium batteries. However, real-time visualization of internal degradation processes under realistic conditions remains a major challenge. Here, we report an operando distributed strain imaging approach based on intrinsic Rayleigh backscattering to reveal the distinct stress evolution of Li-metal batteries (LMBs) with PVDF-based solid polymer electrolyte (SPE) and carbonate-based liquid electrolyte (LE). Distinct from conventional fiber Bragg grating (FBG)-based point strain monitoring, this distributed imaging method provides high spatiotemporal resolution and stress sensitivity, enabling non-destructive, full-area detection of interfacial inhomogeneity in lithium deposition beyond the reach of conventional electrochemical signals. Using this technique, we achieve continuous stress imaging over the full life cycle (>1600 h) in pouch-type LMBs, enabling life-cycle tracking of degradation evolution and uncovering an anomalous “V-shaped” stress trajectory during lithium deposition. Notably, NCM811|LE|Li batteries exhibit a maximum local strain of 441 µε after 120 h, more than twice that of NCM811|SPE|Li (164 µε). Large-area mapping further reveals that the PVDF-based SPE facilitates homogeneous Li + flux and uniform deposition. This Rayleigh-backscattering-enabled imaging offers a powerful diagnostic method for quantifying interfacial stress dynamics and real-time assessment of state of health in high-energy-density lithium batteries. Distributed Rayleigh-optical frequency domain reflectometry (OFDR) strain imaging reveals distinct chemo-mechanical degradation between NCM811|LE|Li and NCM811|SPE|Li pouch cells under industrial low stack pressure. Download: Download high-res image (201KB) Download: Download full-size image
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Nano-Micro Letters
·
2026
·
IF 38.5
Wenjing Zhang,Xiaoci Liang,Sixing Chen,Xiuquan Ma,Chen Chen,Songjia Han,Chuan Liu
High-density organic electrochemical transistor (OECT) arrays are essential for neuromorphic computing and bioelectronic interfaces, but progress has been limited by the low resolution of electrolyte patterning. Although conventional photolithography offers high feature resolution, it involves a fundamental trade-off among spatial resolution, ionic capacitance, and stability in the electrolyte. Here we report an ion compensation-assisted photolithography (ICAP) strategy that yields electrolyte micro-patterns combining high precision, high capacitance and high stability. A molecularly engineered electrolyte forms, under UV exposure, a physicochemical dual cross-linked network with strong solvent resistance and hydrophobicity, which suppresses swelling during both aqueous development and the subsequent ion-compensation step, preserving pattern fidelity. Ion compensation then restores and enhances the mobile-ion content, increasing areal capacitance. The resulting electrolytes achieve a record 2 μm resolution, 15.6 μF cm −2 capacitance, and strong thermal stability from − 50 to 200 °C. Integrated into OECTs, the ICAP-patterned electrolytes suppress crosstalk by 97.6% and boost on/off ratios by 325%, reducing parasitic coupling by more than 40 times compared to unpatterned arrays. The method is compatible with p -type and n -type organic semiconductors and inorganic oxides, providing a versatile route to scalable neuromorphic circuits and advanced bioelectronics.
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Nanoscale
·
2025
·
IF 5.1
Luo Zhang,Haodong Zhao,Donglai Xiao,Haibo Tian,Haibo Zhang,Xinghua Zhu,Dingyu Yang
Lithium-ion batteries (LIBs) have been widely applied in electric vehicles, smart grids, and other fields due to their high energy density and long cycle life. However, the flammability of conventional carbonate-based electrolytes poses significant safety risks and hinders the large-scale deployment of high-energy-density batteries. Herein, we propose a nonflammable carbonate-based local high-concentration electrolyte (LHCE) composed of lithium bis(trifluoromethanesulfonyl)imide (LiTFSI)/fluorinated ethylene carbonate (FEC)/1,1,2,2-tetrafluoroethyl-2,2,3,3-tetrafluoropropyl ether (TTE). This formulation replaces highly flammable conventional solvents with FEC and highly fluorinated TTE, substantially reducing fire hazards. The electrolyte exhibits an electrochemical window up to 5.5 V. Synergistic interactions between TFSI⁻ anions and FEC facilitate the formation of a robust, LiF-rich solid electrolyte interphase (SEI) on the graphite (Gr) anode and an effective cathode electrolyte interphase (CEI) on the high-voltage LiNi0.8Co0.1Mn0.1O2 (NCM811) cathode, suppressing structural degradation and transition metal dissolution. Consequently, the NCM811||Gr full battery using LHCE demonstrates superior cyclability, with a capacity loss below 8% over 200 cycles at a high cutoff voltage of 4.5 V and an average coulombic efficiency (CE) of 99.9%. This work provides a promising electrolyte design for stable and safe high-voltage LIBs, offering potential guidance for advanced battery systems.
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