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CHEMICAL ENGINEERING JOURNAL · 2025 · IF 13.2

Poly(vinylidene fluoride)-based Janus separators with an ultrathin conductive layer for suppressing lithium dendrite growth

Ruiqi Che,Sha Cheng,Cheng Huang,Ming Liu,Zhongao Chen,Jin Han,Wen Chen,Pengchao Zhang

Lithium dendrites, growing during the charging and discharging processes, can pierce the separators and lead to internal short circuits, which is one of the main factors resulting in thermal runaway of lithium metal batteries (LMBs). In this work, we developed a poly(vinylidene fluoride) (PVDF)-based Janus separator with an ultrathin polypyrrole (PPy) layer towards efficiently suppressing lithium dendrite growth. The PPy layer with thickness of approximately 200 nm has Pyrrole-N with lone pairs of electrons, which can act as nucleation sites for lithium ions. As a result, lateral lithium deposition can be achieved on the anode, thus preventing the lithium dendrites from piercing the separators. Stable stripping/plating performance over extended cycling and a capacity retention rate of 76.8% after 1000 cycles have been achieved in the Janus PVDF/PPy separator-based Li//Li symmetric cells and Li//LiFePO 4 half cells, respectively. The development of Janus separators with conductive polymer layers presents a promising solution for improving the safety and electrochemical performance of LMBs.

CAS / MDL: 7727-54-0 109-97-7
研究领域: 材料科学 · 能源存储
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Small · 2022 ·Vol. 18 ·期 28 ·2202651 · IF 15.153

Interfacial Engineering of Binder-Free Janus Separator with Ultra-Thin Multifunctional Layer for Simultaneous Enhancement of Both Metallic Li Anode and Sulfur Cathode

Shuanglin Wu,Yingmei Yao,Xiaolin Nie,Zhifeng Yu,Yanting Yu,Fenglin Huang

Exploring a scalable strategy to fabricate a multifunctional separator is of great significance to overcome the challenges of lithium polysulfides (LiPSs) and dendritic growth in lithium-sulfur batteries (LSBs). Herein, a binder-free Janus separator is constructed by interfacial engineering. At the cathode interface, an ultra-thin covalent triazine piperazine film containing tailorable micropores and adsorption sites is decorated on polyacrylonitrile (PAN) membrane by in situ interfacial polymerization, building a triple barrier for LiPSs. The combination of steric hindrance and chemical adsorption reduces LiPS's migration by 81.85%. Meanwhile, at the anode interface, a fast-ionic conductor Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 (LLZTO) is created on the surface of PAN nanofiber by magnetron sputtering to suppress dendrite growth. Even though there is no binder between the ceramic layer and the fibrous separator, sputtering creates an inter-embedded structure that ensures no depowering after cycling. Furthermore, the PAN-based separator displays a high temperature tolerance of 180 °C. Consequently, the cell delivers a high capacity of 1287.9 mAh g −1 at 0.5 C and stable cycling performance with an ultra-low capacity decay rate of 0.059% per cycle over 500 cycles. This work provides a scalable strategy for functionalizing separators to tackle the challenges in LSBs, which is binder-free, stripping-free, and essentially thickening-free.

CAS / MDL: 108-77-0
研究领域: 材料科学 · 能源存储技术
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JOURNAL OF POWER SOURCES · 2022 · IF 9.794

All-in-one Janus separator for lithium–sulfur batteries with lithium polysulfide and dendrite growth suppressed at temperature gradient effect

Chen Chang,Chengyin Yang,Qiyue Wu,Xuyang Wang,Hui Nie,Xingping Zhou,Xiaolin Xie,Bingjoe Hwang,Yunsheng Ye

Designing an optimum separator configuration that can address severe lithium polysulfide (LiPS) shuttling and uncontrollable Li dendrite growth at the evaluated temperature is imperative for developing a high-performance, reliable, and safe Li–S battery (LSB). Herein, a promising LSB separator design is proposed, which consists of LiPS catalytic layer (LCL) and thermal conductive layer (TCL) fabricated by dual side filtrating the flower-like vanadium pentoxide (V 2 O 5 ) microspheres and aluminum oxide (Al 2 O 3 ) nanosheets , respectively. The LCL between the separator and S-cathode as combined LiPS trapper and catalyst significantly improves the redox reaction and sulfur utilization. At the anode/separator interface, the TCL uniforms Li-ion flux and thermal distribution to prevent undesirable Li dendrite growth under the temperature gradient ( TG ) effect. The Janus-type LCL-TCL separator with two parallel functions can achieve synchronous improvements in cathodic and anodic performance in LSB. Consequently, the LSB with Janus-type LCL-TCL separator exhibits excellent cycling stability with an ultralow capacity decay rate of 0.036% per cycle over 2000 cycles at 1C and superior rate capability up to 4C. The novel strategy can pave a new way to simultaneously tackle the limitations faced by anode and cathode in LSB.

研究领域: 材料科学 · 电化学 · 能源存储技术
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Journal of Energy Storage · 2025 · IF 9.8

High performance Janus separator based on microstructurally controllable halloysite nanotubes for zinc-ion batteries

Peijie Xu,Yuhang Yu,Beibei Du,Yongdan Cao,Donghui Sun,Zengchao Ji,Yifei Zhu,Yanyue Jia,Yang Liu,Zhao Cao

Zinc-ion batteries(ZIBs) are promising as the stationary energy storage owing to their inherent high safety, cost-effective, and environmental-friendly. Nevertheless, the notorious dendrite growth and water-induced side reactions on Zn anode significantly downgrade the long-lasting cycling stability and hinder the industrialization of ZIBs. Herein, a flux-homogenized Zn 2+ transport system based on a Janus separator is constructed. This Janus separator features bacterial cellulose (BC) layer on one side and roughened halloysite nanotubes/bacterial cellulose (RHNTs/BC) layer on the other side. The abundant surface hydroxyl groups, zincophilicity sites, and ionic transmission paths of RHNTs make them ideal for acting as an ion pump to accelerate the transportation of ions, contributing to the immensely improvement of the de-solvation process, zinc deposition, and the growth of Zn dendrites. As a result, the Zn/Zn symmetrical cell with Janus separator can achieve a stable cycle life of over 800 h at 4.40 mA cm −2 . More impressively, the full cell based on Janus separator enables excellent cycling stability. This study enriches the structurally controllable construction method of HNTs and provides the fundamental theories for the application of HNTs in the field of new high-efficiency mineral energy storage materials.

研究领域: 材料科学 · 能源存储技术
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2024 · IF 9.4

Engineering and construction of multi-functional Janus separator for high-stability Li-CO2 battery

Hangyu Li,Yang Gu,Xiaoyuan Zeng,Kai Ding,Haotian Tan,Peng Dong,Yanjia Zhang,Jie Xiao

Due to the high theoretical energy density, lithium-carbon dioxide (Li-CO 2 ) batteries provide unique advantages when using CO 2 to generate electricity. However, the issues with lithium dendrite generated by uneven deposition and quick cathode passivation continue to impede the development of Li-CO 2 batteries. In this work, a Janus separator with dual functionalities is created using an in-situ growth and hydrothermal technique. It can be used to expand the cathode to alleviate the quick passivation of the cathode, in addition to inhibiting the growth of lithium dendrite. On the one hand, as an ion transport framework, Prussian blue (PB) nanocubes formed in-situ on the anode side can control the uniform transport of Li-ions and prevent the proliferation of lithium dendrites. The Prussian blue and reduced graphene oxide composite material (PB-rGO) on the cathode side, on the other hand, can be employed as an extension of the cathode, which not only contains more discharge products but also encourages their decomposition, playing a self-cleaning role. Moreover, the Li||Li symmetrical battery with Janus separator exhibits a steady cycle life of more than 1700 h. Also, when applied to a Li-CO 2 battery, it demonstrates an extremely high discharge capacity of 12100 mAh g −1 and an exceptionally long cycle life of 3144 h.

研究领域: 材料科学 · 电化学 · 能源存储与转换
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Energy Storage Materials · 2022 · IF 20.831

Ti3C2Tx MXene as Janus separators for redox-enhanced electrochemical capacitors with reduced self-discharge

Wei Yang,Qiankun Han,Wenshi Li,Maosheng Wu,Jing Yao,Man Zhao,Xianmao Lu

Redox-enhanced electrochemical capacitors (redox ECs) are promising energy-storage devices with the potential to deliver both high power and energy performances, although overcoming the severe self-discharge remains a great challenge due to the shuttle effect of redox species such as I − /I 3 − ions introduced in the electrolytes for gaining additional capacities. Herein, we propose a cation-initiated self-assembly process of Ti 3 C 2 T x MXene nanosheets onto glass fiber membranes to form Janus separators that can mitigate the shuttling of I − /I 3 − ions in iodine-based redox ECs. The interlayer spacing of the MXene films can be controlled by selecting different cations such as imidazolium (C 4 mim + ), Mg 2+ , and Al 3+ , therefore the resulting Janus separators exhibit tailored nanochannels for ion sieving. Both molecular dynamic (MD) simulations and electrochemical tests indicate that C 4 mim + -intercalated MXene Janus separators (C 4 mim + -MXene) can block the diffusion of I 3 − ions while allowing the pass of other electrolyte ions. As a result, self-discharge caused by the shuttle effect can be much reduced in C 4 mim + -MXene-based redox ECs, which deliver voltage and energy retentions substantially higher than that of the cells using glass fiber membrane separators (voltage retention: 70% vs. 10%, energy retention: 51% vs. 6.5%) after 24-h open-circuit test.

研究领域: 材料科学 · 储能技术 · 电化学 · 纳米技术
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