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Advanced Energy and Sustainability Research · 2025 · IF 5.7

Electric and Temperature Field-Modulated Periodic Repair of the Electrode/Electrolyte Interface toward Long Cycle Stability of Low-Temperature Li-Ion Batteries

Zhenqiang Guo,Chengling Yang,Yu Fan,Yancai Zhang,Haolun Zou,Yukun Yan,Hongbin Zhang,Zhenhui Liu,Zinuo Chen,Sitong Peng,Ziyi Dang,Hengyi Li

This study tackles the poor low-temperature performance of lithium-ion batteries through a synergistic strategy that modulates electrode–electrolyte interfacial chemistry via coordinated temperature and electric field control. The research uncovers distinct interfacial evolution mechanisms: at −20 °C, strengthened solvent–Li + affinity causes solvation structure reorganization and interfacial deterioration, whereas at 25 °C, enhanced anion participation promotes formation of stable inorganic-rich interphases. Reduced electric field intensity further facilitates the construction of stable interfaces. Based on these findings, a variable-temperature constant-current cycling protocol with periodic room-temperature activation is developed. This approach effectively restores stable interfaces and substantially minimizes polarization, enabling commercial lithium iron phosphate (LFP) batteries to maintain nearly 100% initial capacity after 150 cycles at −20 °C—significantly surpassing conventional strategies (80.4% retention). Notably, this optimization method regulates interfacial chemistry through external field parameters without electrolyte formulation changes, demonstrating both theoretical innovation and engineering practicality. This work provides a novel paradigm for low-temperature battery design by decoupling interfacial regulation from material modification.

CAS / MDL: 372-48-5
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ACS Applied Energy Materials · 2023 · IF 6.4

Poly(Ether-Ester)-Based Solid Polymer Electrolytes with High Li-Ion Transference Number for High Voltage All-Solid-State Lithium Metal Batteries

Yang Chen,Yin Zhang,Jianda Niu,Hongli Xu,Zhixian Dong,Jinbao Xu,Caihong Lei

Considering the lower room temperature ionic conductivity, Li-ion transference number, and narrow electrochemical stability window in all-solid-state polymer electrolytes (ASSPEs)-based lithium metal batteries (LMBs), it is of particular necessity to find plausible strategies to accomplish these issues. In this paper, poly(ε-caprolactone-co-1,5-dioxepan-2-one) (PDCL)-based poly(ether-ester) ASSPEs have been successfully fabricated by the random ring-opening polymerization of cyclic CL and DXO. The PDCL-SPE exhibits a high ion conductivity of 3.54 × 10–5 S cm–1 at 30 °C with a high Li-ion transference number (0.62) and a superior electrochemical stability (5.1 V). FT-IR spectra confirm the synergistic effect of ether and carbonyl of ester from the main chain of PDCL, which is superior to the dissociation of lithium salts and facilitation the motivation of lithium ions. Furthermore, the assembled LiFePO4/PDCL-SPE/Li batteries displayed low interfacial resistance, Li dendrite suppression, high specific capacity, and excellent cyclic performance (capacity retention of 85% after 200 cycles at 0.1 C). The high-voltage LiNi0.5Co0.2Mn0.3O2/PDCL-SPE/Li batteries also exhibits good cycling performance and durability.

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CERAMICS INTERNATIONAL · 2023 · IF 5.2

Novel electrochemical sensing platform based on palygorskite nanorods/Super P Li carbon nanoparticles-graphitized carbon nanotubes nanocomposite for sensitive detection of niclosamide

Yunhang Liu,Qian Wang,Gan Zhu,Qiwen Ran,Fang Li,Meimei Guo,Guifang Wang,Hongyuan Zhao

We reported an one-pot ultrasonic-assisted method for the preparation of palygorskite nanorods/Super P Li carbon nanoparticles-graphitized carbon nanotubes (PNRs/SPCNPs-g-CNTs) nanocomposite, which was used to modify the glassy carbon electrode (GCE) for the fabrication of PNRs/SPCNPs-g-CNTs/GCE sensor. For the PNRs/SPCNPs-g-CNTs nanocomposite, PNRs with good stability presented large specific surface area and high adsorption, which promoted the enrichment of NA molecules on the electrode surface. SPCNPs with pearl chain-like nanostructure exhibited good electrical conductivity , and the combination of SPCNPs and g-CNTs with high graphitization degree formed an interconnected carbon conductive network with excellent electrical conductivity, which enhanced the charge transport efficiency. Moreover, the interconnected carbon conductive network of SPCNPs-g-CNTs not only promoted the dispersion degree of PNRs but also made up for the poor conductivity property of PNRs. When used for the detection of niclosamide (NA), an acceptable limit of detection (3.6 nM) was achieved at the PNRs/SPCNPs-g-CNTs/GCE sensor in linear NA concentration range of 0.01–10 μM. The PNRs/SPCNPs-g-CNTs/GCE sensor exhibited good reproducibility, repeatability, and anti-interference performance. For the practicability measurement, the fabricated sensor showed good practicability with satisfactory recoveries (97.0–102.7%) and low RSD values of 0.99–4.78% for the detection of NA in tap water and lake water samples.

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SEPARATION AND PURIFICATION TECHNOLOGY · 2022 · IF 9.136

A nanofiltration membrane with positively and negatively charged groups by grafted p-aminosalicylic acid-Fe(III) chelation for Li+/Mg2+ efficient separation

Yanghe Liu,Quan Li,Shenghuan Wang,Mengzhu Liang,Yanhong Ji,Zhenyu Cui,Mohammad Younas,Jianxin Li,Benqiao He

High-performance nanofiltration (NF) membrane plays a key role in Li + /Mg 2+ separation process. In this work, a new NF membrane with positively and negatively charged groups was prepared by grafting p-aminosalicylic acid (AS) onto the surface of polyamide (PA) membrane followed by chelation with Fe 3+ ions for Li + /Mg 2+ separation. The AS grafting (PA-g-AS) and Fe 3+ chelating (PA-g-AS-Fe) NF membranes had almost same surface and section structure and surface pore size as the PA membrane. But Zeta potential (about −8 mV at pH 7) of the obtained PA-g-AS-Fe membrane was improved in comparison with the PA and PA-g-AS NF (about −20 mV at pH 7) membranes due to Fe 3+ addition, suggesting that there were positively and negatively charged groups on the membrane surface. The PA-g-AS-Fe membrane showed a high Mg 2+ rejection of 97.7% and high Li + permeation (negative rejection of −87.6%); while a high Li + /Mg 2+ separation factor (S Li , Mg ) of about 81.5 was achieved, which is much higher than those for PA and PA-g-AS NF membranes and surpassed those of the results reported in literature. The fluxes of three membranes were about the same. The results demonstrated the NF membrane with positively and negatively charged groups was suitable for efficient separation of Li + /Mg 2+ and would have promising applications in recovery of lithium from brine.

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ACS Applied Materials & Interfaces · 2023 · IF 9.5

Fast Li+ Transport Polyurethane-Based Single-Ion Conducting Polymer Electrolyte with Sulfonamide Side chains in the Hard Segment for Lithium Metal Batteries

Naijie Wang,Xiangqun Chen,Qiu Sun,Ying Song,Tiezhu Xin

Single-ion conducting polymer electrolytes (SICPEs) are considered as one of the most promising candidates for achieving lithium metal batteries (LMBs). However, the application of traditional SICPEs is hindered by their low ionic conductivity and poor mechanical stability. Herein, a self-standing and flexible polyurethane-based single-ion conductor membrane was prepared via covalent tethering of the trifluoromethanesulfonamide anion to polyurethane, which was synthesized using a facile reaction of diisocyanates with poly(ethylene oxide) and 3,5-diaminobenzoic acid (or 3,5-dihydroxybenzoic acid). The polymer electrolyte exhibited excellent ionic conductivity, mechanical properties, lithium-ion transference number, thermal stability, and a broad electrochemical window because of the bulky anions and unique two-phase structures with lithium-ion nanochannels in the hard domains. Consequently, the plasticized electrolyte membrane showed exceptional stability and reliability in a Li||Li symmetric battery. The assembled LiFePO4||Li battery exhibited an outstanding capacity (∼180 mA h g–1), Coulombic efficiency (>96%), and capacity retention. This research provides a promising polymer electrolyte for high-performance LMBs.

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ACS Applied Energy Materials · 2022 · IF 6.959

Constructing a Strong-Affinity Elastic Network Binder Enabled by Tannic Acid as the Bifunctional Anchoring Agent for High-Performance Li–S Battery

Mingxiu Hou,Jianshun Feng,Fanghui Wang,Weiyu Wang,Zhenjiang Li,Jie Liu,Fengli Yu,Lei Wang

Lithium–sulfur (Li–S) batteries have been limited by their poor electrochemical performance due to the large volume change and severe shuttle effect during cycling. Binders serve as an essential role in sulfur electrodes and can stabilize the mechanical integrity of the electrode. It also has been demonstrated that designing strong-affinity binders is a feasible and facile method to suppress the shuttle effect. Therefore, in this work a strong-affinity elastic network binder is designed for high-performance Li–S battery coupling with tannic acid (TA) and polyurethane (PU). Firstly, the rich hydrogen bonds between TA and PU result in a mechanically robust network to keep the sulfur electrode from cracking in the cycling process. Secondly, the selected TA with abundant phenolic hydroxyl groups possesses strong adsorption capability toward polysulfides, which can efficiently restrain the shuttle effect. Hence, the cycling stability of Li–S batteries using P1T1 binder is significantly improved, maintaining the capacity of 602.5 mAh g–1 after 500 cycles at the current density of 0.5 C.

CAS / MDL: 7440-25-7 7704-34-9
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JOURNAL OF MEMBRANE SCIENCE · 2022 · IF 10.53

A low-overpotential, long-life, and “dendrite-free” lithium-O2 battery realized by integrating “iodide-redox-phobic” and “Li-ion-philic” membrane

Xiaohong Zou,Qian Lu,Cuie Wang,Sixuan She,Kaiming Liao,Ran Ran,Wei Zhou,Liang An,Zongping Shao

Before the practical application of the Li–O 2 battery (LOB), a critical issue regarding large overpotential upon charging (which causes irreversible side reactions and low energy efficiency) should be resolved. The utilization of redox mediators (RMs) which oxidatively decompose insulating discharge product, Li 2 O 2 , is one promising solution to address this issue. However, the soluble RMs can easily diffuse to and react with the Li metal anode (encountering Li dendrites is even worse). Here, a chemical self-assembly strategy is introduced into the fabrication of the iodide-redox-phobic and Li-ion-philic membrane for LOBs, in which the electronegative δ-MnO 2 layer is in-situ grown on commercial polyethylene (PE) membrane (MnO 2 @PE). The electronegative MnO 2 layer can simultaneously repel the shuttle of iodide species and regulate the uniform Li  +  deposition. Controlling cut-off capacity of 1000 mAh g −1 , iodide-redox-based LOB with MnO 2 @PE demonstrates low overpotentials (∼0.7 V vs. Li + /Li), dendrite-suppressing capability, as well as impressive long-term reversibility over 500 cycles (2000 h), which urges the LOB technology competitive among the next-generation rechargeable power systems.

CAS / MDL: 90076-65-6 10377-51-2
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Sustainable Energy & Fuels · 2022 ·Vol. 6 ·期 19 ·4520-4527 · IF 6.813

Enhancing the electrochemical performance of a micron-sized Ge anode through in situ surface composite flower-like Zn2GeO4 for Li-ion batteries

Jian Hao,Jun Bai,Jing Wang,Lu Xu,Junli Guo,Caixia Chi,Haihong Li

The large volume changes of Ge-based electrode result in poor electrochemical cycling and rate performance and are the important factors hampering the practical implementation of Ge-based materials in Li-ion batteries (LIBs). Here we fabricated a fascicular structure Ge/Zn2GeO4 (Ge/Zn2GeO4NFs) by an in situ growth of flower-like Zn2GeO4 on micron-sized Ge. In an EDTA/water solvent system, Zn2GeO4 were generated on the Ge substrate, and self-assembled into a flower-like structure through coordination and H-bonding. Benefiting from the improved structural stability and abundant transmission channels of lithium ions and electrons, the as-fabricated Ge/Zn2GeO4NFs anodes exhibited excellent cyclability and rate performance. At a current density of 0.2 A g−1, Ge/Zn2GeO4NFs delivered a high capacity of 1621 mA h g−1 with an initial coulombic efficiency of 62%, and even after the 200th cycle a capacity of 816 mA h g−1 could be maintained. Further, the Ge/Zn2GeO4NFs anode delivered excellent rate capabilities of 567 and 388 mA h g−1 at high current densities of 2 and 5 A g−1, which were superior to the micron-sized Ge electrode (133 mA h g−1 at 5 A g−1). The results show that the Zn2GeO4 nanoflower, which adheres on the micron Ge substrate inseparably, could buffer the volume change of Ge, enlarge the electrolyte contact area, provide continuous lithium-ion and electron pathways, and thus improve the lithium-storage performance of the micron-sized Ge electrodes. This synthesis strategy provides new ideas for the development of micron-sized anode materials for LIBs.

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Materials Today Energy · 2022 · IF 9.257

Fast Li+ transport pathways of quasi-solid-state electrolyte constructed by 3D MOF composite nanofibrous network for dendrite-free lithium metal battery

Maoshuai Sun,Ji Li,Haocheng Yuan,Xiaoyue Zeng,Jinle Lan,Yunhua Yu,Xiaoping Yang

Lithium metal batteries  with quasi-solid-state electrolytes are promising in the advanced energy storage system due to the high theoretical capacity and safety. Herein, a unique quasi-solid-state electrolyte (PUIE) containing 3D ion transport pathways based on UIO-66 has been constructed by a flexible process: electrospinning combined electrostatic spraying, followed by impregnation and roll press. In particular, UIO-66 with abundant Lewis acidic sites and channels enhances the ion transport and the restriction to anion in the electrolyte. The rationally designed PUIE-3 exhibits a high ionic conductivity of 1.08 mS/cm at 25 °C, a wide electrochemical window of 5.5 V, and a high Li + transference number of 0.52. On the basis of the regulating effect of UIO-66, the growth of Li dendrites is significantly restrained and the electrolyte exhibits long-life electrochemical stability with Li anode during the Li plating/stripping. In consequence, lithium metal batteries loaded with PUIE-3 exhibit remarkable cycling and rate performance. Our results indicate that rational design polymer nanofiber/metal-organic framework membranes offer a new avenue for developing high performance quasi-solid-state electrolytes.

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Journal of Energy Chemistry · 2022 · IF 13.599

Boosting the kinetics of PF6− into graphitic layers for the optimal cathode of dual-ion batteries: The rehearsal of pre-intercalating Li+

He Yang,Tingting Qin,Xinyan Zhou,Yu Feng,Zizhun Wang,Xin Ge,Nailin Yue,Dabing Li,Wei Zhang,Weitao Zheng

Large anions exhibit slow diffusion kinetics in graphite cathode of dual-ion batteries (DIBs); particularly at high current density, it suffers severely from the largely-reduced interlayer utilization of graphite cathode, which as a bottleneck limits the fast charge application of DIBs. To maximize interlayer utilization and achieve faster anion diffusion kinetics, a fast and uncrowded anion transport channel must be established. Herein, Li + was pre-intercalated into the graphite paper (GP) cathode to increase the interlayer spacing, and then hosted for the P F 6 - PF6- anion storage. Combined with theoretical calculation, it shows that the local interlayer spacing enlargement and the residual Li + reduce the anion intercalation energy and diffusion barrier, leading to better rate stability. The obtained GP with Li + pre-intercalation (GP-Li) electrode exhibits a discharge capacity of 23.1 mAh g −1 at a high current of 1300 mA g −1 . This work provides a facile method to efficiently improve the interlayer utilization of graphite cathode at large currents.

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ELECTROCHIMICA ACTA · 2022 · IF 7.336

Covalent S and Cl grafted porous carbon host realized via the one-step pyrolysis method results in boosted Li–O2 battery performances

Jie Li,Youcai Lu,Shiyu Ma,Zhongjun Li,Qingchao Liu

Li–O 2 battery has attracted wide attention because it can satisfy the need for a new energy storage system with high energy density. However, poor oxygen reduction (ORR)/oxygen evolution (OER) kinetics involving Li 2 O 2 formation/decomposition is a major obstacle to its development. By designing suitable cathode with desired structure and surface electronic states, the formation/morphology of Li 2 O 2 and the reaction kinetics of charge process can be efficiently optimized simultaneously. In this work, a novel sulfur (S) and chlorine (Cl) co-doped porous carbon (CSC) were synthesized by one-step pyrolysis strategy, and the amount of heterogeneous atoms could be flexibly controlled by different calcination temperatures . Experimental combined with theoretical calculations show that the content of C Cl bond plays an important role in the adsorption of intermediate LiO 2 , thus regulating the morphology of Li 2 O 2 and ultimately affecting the release of battery energy. The C S bond mainly acts on the dynamics of the ORR and OER processes, which has an important influence on improving the round-trip efficiency of the battery. Benefiting from the synergistic effect of heteroatoms , the electrochemical performances of the Li–O 2 battery, including round-trip efficiency, discharge capacity and cycling stability are greatly improved.

CAS / MDL: 54970-72-8 33454-82-9
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JOURNAL OF ALLOYS AND COMPOUNDS · 2022 · IF 6.371

Double-layered hollow carbon sphere with large interlayer space combined with Co-SnS cat. as efficient sulfur hosts for Li-S batteries

Haoxiang Zhong,Lingzhi Zhang

The low sulfur utilization and the serious shuttle effect of polysulfides severely hamper practical application of Li-S batteries. Herein, sulfur cathodes with the multi-functional structures, featured with double-layered hollow carbon sphere with up to 50 nm interlayer space (DLHC-50) in situ grown Co-SnS catalytic layer is designed and synthesized for lithium sulfur batteries. Co-SnS/DLHC-50 can encapsulate 72% sulfur, higher than 63% for Co-SnS/DLHC-20 due to the large interlayer spaces of DLHC-50. Meanwhile, polysulfides are also effectively restricted via physical entrapment from DLHC-50 as well as chemical binding between Co-SnS and polysulfides. Benefiting from the well-constructed host framework, Co-SnS/DLHC-50 @S shows higher specific capacity/capacity retention of 760.4 mA h g −1 /72.9% after 500 cycles at 0.5 C, than that of 546.5 mA h g −1 /62.2% and 668.9 mA h g −1 /62.2%, for DLHC-50 @S, and Co-SnS/DLHC-20 @S, respectively. In addition, the strategy can be also extended to prepare other metal oxides (sulfides)/DLHC-50 for wide applications. Therefore, this work demonstrates a promising route to combat some bottlenecks such as low sulfur utilization, and the shuttle effect of polysulfides for Li-S batteries.

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