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CHEMICAL ENGINEERING JOURNAL · 2022 · IF 16.744

Enabling the conventional TFSI-based electrolytes for high-performance Mg/Li hybrid batteries by Mg electrode interfacial regulation

Rupeng Zhang,Can Cui,Rang Xiao,L. Ruinan,Tiansheng Mu,Hua Huo,Yulin Ma,Geping Yin,Pengjian Zuo

The Mg-metal batteries (MMBs) as a forceful competitor for Li-metal batteries (LMBs) have the advantages of high-safety and high-volume energy density . Whereas, the MMBs still confronts two vital issues to be addressed, including the incompatibility of conventional TFSI-based electrolytes with the Mg electrode and the poor reversibility of the cathode. In this work, to satisfyingly settle the incompatibility, an artificial interphase was first pre-constructed by high-temperature displacement reaction of CuCl 2 and Mg metal, responsible for the faster charge-transfer rate and the lower Mg plating/stripping overpotential (∼0.2 V) in Mg symmetric cells. Regarding the Mg-Mo 6 S 8 full cells, to enhance the reversibility and rate performance, Mg/Li hybrid batteries were designed. Consequently, the Mg-Mo 6 S 8 battery can achieve excellent cycle stability and deliver a desirable capacity. Even as the current density increases to 1C, the battery still shows a desirable capacity of 92 mAh g −1 over 500 cycles.

研究领域: 材料科学 · 电化学
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Journal of Materials Chemistry A · 2024 ·Vol. 12 ·期 37 ·25407-25415 · IF 10.7

An artificial cathode-electrolyte interphase enabling one-step sulfur transition in polyethylene oxide-based solid-state lithium–sulfur batteries

Leicheng Zhang,Tianshuai Wang,Junjie Chen,Maochun Wu,Tianshou Zhao

All-solid-state lithium–sulfur (Li–S) batteries using polyethylene oxide (PEO)-based electrolytes hold the advantages of high theoretical energy density, cost-effectiveness, and high safety. However, the drawback of polysulfide dissolution in PEO results in a short battery lifespan. Here, we propose to construct an artificial cathode-electrolyte interphase (CEI) on the S cathode, which converts the S speciation pathway to a one-step solid transition, significantly mitigating the polysulfide migration in PEO. Surface analyses and theoretical calculations reveal the composition of the CEI and its effect on the reaction mechanism. As a result, the all-solid-state Li–S cell with the artificial CEI is able to deliver 873 mA h g−1 at 100 mA g−1 and maintain 739 mA h g−1 after 50 cycles, whereas the cell using the pristine S cathode retains only 364 mA h g−1. More remarkably, the artificial CEI enables the cell to achieve a high capacity retention rate of 83.1% at 300 mA g−1 over 200 cycles, demonstrating that our strategy of CEI manipulation effectively enhances the cycling reversibility of PEO-based solid-state Li–S batteries.

CAS / MDL: 1333-86-4
研究领域: 材料科学 · 电化学
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IONICS · 2025 · IF 2.6

Unlocking long-duration performance: MXene artificial interface for dendrite-free zinc-ion battery

Wu Mingjun,Li Junhao,Chen Weitao,Chen Junyang,Chen Xiaobo,Ru Qiang

The further advancement of high-performance zinc ion batteries (ZIBs) is restrained by inevitable metal dendrites in Zn anodes. Researchers actively pursue strategies to develop chemically stable, dendrite-free zinc anodes. Herein, we employ a zinc dendrite-inhibiting tactic by using highly conductive accordion-like V 2 CT x -MXene as robust artificial interface layers. Base on in-situ optical microscope, laser scanning confocal microscope and electrochemical analysis, the results confirm that the artificial interface can prevent direct contact between electrolyte and anode, which minimizes the chances of side reactions occurring. V 2 CT x -MXene@Zn electrode provides a stable Zn anode surface and facilitates homogeneous deposition of Zn ions. The V 2 CT x -MXene@Zn symmetric cell depicts the reinforced stability with over 2000 h life span at 0.5 mA cm −2 and 1.0 mAh cm −2 . The full batteries can work at 5 A g −1 up to 2000 cycles with a high-capacity retention of 86.64%. This work offers a controllable interface protection strategy to achieve long-duration and dendrite-free zinc-ion battery.

研究领域: 材料科学 · 电化学
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ADVANCED FUNCTIONAL MATERIALS · 2024 ·Vol. 34 ·期 39 ·2403222 · IF 18.5

3D Ternary Alloy Artificial Interphase Toward Ultra-Stable and Dendrite-Free Aqueous Zinc Batteries

Yan Xin,Jiayao Qi,Huanhuan Xie,Yunnian Ge,Zerui Wang,Fang Zhang,Bijiao He,Shuwei Wang,Huajun Tian

Rechargeable aqueous zinc-ion batteries (AZIBs) are one of the most promising post-lithium battery technologies due to their low cost, high safety, and environmental friendliness. However, their practical development is hindered by the issues of Zn metal anodes, including dendrite growth, passivation, hydrogen evolution and other side reactions. Herein, to circumvent these issues, a facile and universal alloy electrodeposition strategy is proposed to construct a 3D structured ternary Zn alloy artificial interphase layer on Zn foil as an anode for high-performance AZIBs. The density functional theory (DFT) theoretical calculations, in situ optical visualization and spectroscopic results validate that the zincophilic Zn─Sn─Bi@Zn ternary alloy anode with lower migration energy barrier and weak hydrogen adsorption sites can promote the uniform Zn deposition and suppress hydrogen evolution reactions. The Zn─Sn─Bi@Zn//NH 4 V 4 O 10 full cell demonstrates a high specific capacity 110.4 mAh g −1 even after 10 000 cycles at 5.0 A g −1 . Notably, the full cell with a high NH 4 V 4 O 10 cathode loading mass of ≈20.0 mg cm −2 maintains cyclic stability for 400 cycles. This work proposes an innovative Zn-based ternary alloy anode methodology as a design strategy for advanced AZIBs and beyond.

研究领域: 材料科学 · 电化学
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JOURNAL OF ALLOYS AND COMPOUNDS · 2019 · IF 4.175

Enhancing electrochemical performances of LiNi0.5Co0.2Mn0.3O2 cathode materials derived from NiF2 artificial interface at elevated voltage

Jishen Hao,Zhiyong Yu,Hanxing Liu,Wei Song,Jun Liu,Linghua Kong,Chuanhua Li

Herein, NiF 2 artificial interface was proposed for the first time to enhance the electrochemical performances of LiNi 0.5 Co 0.2 Mn 0.3 O 2 (NCM523) under 4.5 V. Scanning electron microscopy (SEM) and transmission electron microscopy (TEM) images verify NiF 2 layer is successfully constructed on the surface of NCM523. The 1.0 wt% NiF 2 -modified NCM523 delivers a much higher capacity retention (86.9%) than pristine sample (69.0%) after 100 cycles under 4.5 V at 30 °C, even exceeding pristine NCM523 under 4.2 V (82.2%). Beyond that, the cycling stability of NCM523 under 4.5 V at 55 °C is also visibly improved due to the NiF 2 protective layer. Electrochemical impedance spectroscopy analyses confirm that NiF 2 suppresses the increase of interface resistance and therefore makes for the interface kinetics behaviors during cycling. In addition, the measurements of SEM, TEM and XPS support that the inhibition of the SEI (solid electrolyte interphase) growth can be attributed to the restrained side reactions between electrolyte and NCM523 by NiF 2 artificial layer at 4.5 V.

CAS / MDL: 12125-01-8 13478-00-7
研究领域: 材料科学 · 电化学 · 电池技术
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JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY · 2023 · IF 10.9

Superior plating/stripping performance through constructing an artificial interphase layer on metallic Mg anode

Bangpeng Yang,Liuyan Xia,Rong Li,Guangsheng Huang,Shuangshuang Tan,Zhongting Wang,Baihua Qu,Jingfeng Wang,Fusheng Pan

Rechargeable magnesium batteries (RMBs) have attracted tremendous attention in energy storage applications in term of high abundance, high specific capacity and remarkable safety of metallic magnesium (Mg) anode. However, a serious passivation of Mg anode in the conventional electrolytes leads to extremely poor plating/stripping performance, further hindering its applications. Herein, we propose a convenient method to construct an artificial interphase layer on Mg anode by substitution and alloying reactions between SbCl 3 and Mg. This Sb-based artificial interphase layer containing mainly MgCl 2 and Mg 3 Sb 2 endows the significantly improved interfacial kinetics and electrochemical performance of Mg anode. The overpotential of Mg plating/stripping in conventional Mg(TFSI) 2 /DME electrolytes is vastly reduced from over 2 V to 0.25–0.3 V. Combining experiments and calculations, we demonstrate that under the uniform distribution of MgCl 2 and Mg 3 Sb 2 , an electric field with a favorable potential gradient is formed on the anode surface, which enables swift Mg 2+ migration. Meanwhile, this layer can inhibit the decomposition of electrolytes to protect anode. This work provides an in-depth exploration of the artificial solid-electrolyte interface (SEI) construction, and a more achievable and safe path to realize the application of metallic Mg anode in RMBs.

CAS / MDL: 10025-91-9 110-71-4
研究领域: 材料科学 · 电化学
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ACTA PHYSICO-CHIMICA SINICA · 2025 · IF 13.5

Phosphazene-based flame-retardant artificial interphase layer for lithium metal batteries

Caiyun Jin,Zexuan Wu,Guopeng Li,Zhan Luo,Nian-Wu Li

The rapid development of emerging fields such as electric vehicles, drones, and robotics has driven the demand for secondary batteries with higher energy density and enhanced safety. The lithium metal anode (LMA) is widely regarded as an ideal anode material for next-generation rechargeable batteries due to its high specific capacity (3860 mAh·g -1 ) and low redox potential (-3.04 V vs. standard hydrogen electrode). However, LMA faces significant challenges, primarily the uncontrollable growth of dendrites and its inherent propensity for thermal runaway. To address these issues, this study proposes a novel silsesquioxane-functionalized hexaphenoxycyclotriphosphazene (HPCTP)-based porous polymer (SHPP) artificial interphase layer, synthesized via Friedel-Crafts alkylation, to achieve highly stable LMA performance. N 2 adsorption/desorption analysis confirms that SHPP features a hierarchical nanoporous structure, with pores of approximately 0.5 and 0.6 nm that effectively restrict the mobility of PF 6 - anions. As a result, the Li-ion transference number increases from 0.29 in liquid electrolytes to 0.60, which helps suppress Li dendrite growth. Additionally, the rich nanoporous structure of SHPP significantly improves its wettability with the electrolyte. In situ thermogravimetric analysis coupled with Fourier transform infrared spectroscopy (TG-FTIR) reveals that SHPP decomposes at approximately 410 °C, generating phosphate radicals (PO•) that quench highly reactive hydroxyl (HO•) and oxygen (O•) radicals produced during the thermal decomposition of ester-based electrolytes, effectively mitigating thermal runaway risks. Thermal analysis and ignition tests confirm the outstanding thermal stability and flame-retardant properties of SHPP. Semi-in situ X-ray photoelectron spectroscopy (XPS) analysis indicates that the solid electrolyte interphase (SEI) on bare Li metal is predominantly organic and undergoes significant compositional fluctuations during cycling. In contrast, the SEI formed on SHPP-Li is enriched with Li phosphide (Li 3 P), which enhances ionic conductivity, and Li fluoride (LiF), which improves chemical stability, resulting in a compositionally stable SEI throughout cycling. SHPP not only facilitates interfacial Li-ion transport but also promotes the formation of a chemically robust interphase. In situ optical microscopy and semi-in situ field-emission scanning electron microscopy (FE-SEM) images demonstrate that the SHPP artificial interphase effectively suppresses Li dendrite growth, enabling uniform Li deposition. As a result, SHPP-Li||SHPP-Li symmetric cells exhibit stable cycling for 1,600 h at 0.5 mA·cm −2 and 0.5 mAh·cm −2 . Furthermore, SHPP-Li||LiNi 0.8 Co 0.1 Mn 0.1 O 2 full cells maintain a high capacity retention of 76.8% after 500 cycles at 1 C (1 C = 190 mA·g -1 ). This flame-retardant artificial interphase layer offers a promising strategy for designing dendrite-free and safe LMAs.

研究领域: 材料科学 · 能源存储
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CHEMICAL ENGINEERING JOURNAL · 2021 · IF 13.273

An artificial interphase enables the use of Mg(TFSI)2-based electrolytes in magnesium metal batteries

Rupeng Zhang,Can Cui,Ruinan Li,Yaqi Li,Chunyu Du,Yunzhi Gao,Hua Huo,Yulin Ma,Pengjian Zuo,Geping Yin

Due to the good safety and high energy density , rechargeable Mg-metal batteries (RMMBs) have been regarded as a potential competitor of Li-metal batteries (LMBs). However, the Mg(TFSI) 2 -based conventional electrolytes will cause large overpotential in reversible plating/stripping attributed to the high ion transport impedance of the electrolyte decomposition products. Here, an artificial interphase composed of amorphous (a-) MgCl 2 @polymer on the Mg-metal surface is prepared by in-situ chemical reaction of metallic Mg with H 3 PO 4 and SiCl 4 in sequence, and can effectively inhibit the electrolyte decomposition and facilitate Mg 2+ transport, which plays the role of solid electrolyte interface (SEI) on Mg anode. The Mg-Mg symmetrical cell with modified Mg electrode exhibits lower overpotential (~0.25 V) and interfacial impedance than bare Mg electrode in 0.5 M Mg(TFSI) 2 /DME electrolyte. The voltage hysteresis in the Mg-S and Mg-Mo 6 S 8 batteries with the modified Mg anode is greatly improved compared to bare Mg anode. This work provides a new idea for future applications of passivation-free Mg-metal anode technology in the MMBs based on conventional electrolytes.

研究领域: 材料科学 · 能源技术
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Journal of Materials Chemistry A · 2021 ·Vol. 9 ·期 19 ·11623-11631 · IF 12.732

Enabling stable and high-rate cycling of a Ni-rich layered oxide cathode for lithium-ion batteries by modification with an artificial Li+-conducting cathode-electrolyte interphase

Shixuan Wang,Alvin Dai,Yuliang Cao,Hanxi Yang,Amine Khalil,Jun Lu,Hui Li,Xinping Ai

Ni-rich LiNi0.8Co0.1Mn0.1O2 (NCM811) cathodes are investigated to realize high energy density Li ion batteries for long life electric vehicle applications. However, capacity decay and thermal instability due to cathode-electrolyte interfacial degradation remain challenges that require sophisticated surface stabilization methods to address. Here, we propose a strategy, for the first time, to form an artificial Li+-conducting cathode-electrolyte interphase (ALCEI) on the NCM811 cathode surface using a nucleophilic reaction between polysulfides and vinylene carbonate (VC). The as-formed ALCEI layer simultaneously protects the NCM particles from electrolyte corrosion and facilitates Li+ ion transport, thus enabling stable and high rate cycling of NCM811. As a result, the ALCEI-modified NCM811 cathode exhibits a high capacity (211.6 mA h g−1 at 0.1C), notable rate capability (134 mA h g−1 at 10C), and superior cycle stability (94.2% over 200 cycles at 1C). These results underscore the use of interfacial engineering in high voltage cathode material development and provide a feasible strategy for stabilizing Ni-rich cathode interfaces in practical Li ion battery applications.

研究领域: 材料科学 · 能源存储 · 化学工程
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2025 · IF 9.7

Fluorine-rich zincophilic covalent organic frameworks enabling anti-corrosion and uniform zinc deposition for aqueous zinc metal battery anodes

Yunyu Zhao,Yingjian Yu

Aqueous zinc metal batteries (AZMBs) are a promising alternative for next-generation secondary batteries owing to their high safety, low cost, and high electrical capacity. However, issues such as corrosion and dendrite growth on zinc anodes hinder the practical application of AZMBs. In this study, we developed two two-dimensional fluorine-rich covalent organic frameworks (COFs), TpFPa and TpFBD, as protective layers for the AZMB anode. The fluorine-rich hybrid interface composed of COFs@Zn and ZnF 2 , produced during Zn electroplating, promoted Zn 2+ dissolution and homogenized the Zn 2+ flux. These effects effectively inhibited side reactions and Zn dendrite growth. In addition, the uniform and dense COFs prevented direct contact between Zn and the electrolyte, which improved the corrosion resistance of the zinc anode. Thus, the symmetric cells assembled using COFs@Zn demonstrated a stable cycle performance of over 1680 h at 1 mA cm −2 @1 mAh cm −2 , which significantly surpassed the performance of bare zinc symmetric batteries. In addition, full cells protected by COFs maintained an ultra-long cycle stability of over 3500 cycles at 2 A g −1 . This strategy of developing a fluorinated artificial interface layer represents a promising approach for designing high-performance AZMBs.

CAS / MDL: 34374-88-4 364-13-6
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Journal of Energy Storage · 2025 · IF 9.8

3D tin whisker network enabling high-performance aqueous dendrite-free zinc anodes

Peigen Zhang,Tianyu Wang,Pei Ding,Feiyue Hu,Zhenglin Zou,Wei He,Vamsi Borra,Qinning Gao,Hanning Zhang,Jingwen Tang,Wei Zheng,ZhengMing Sun

Aqueous zinc-ion batteries (AZIBs) offer high safety, low cost, and environmental compatibility, yet their large-scale deployment is hindered by dendrite growth and severe side reactions arising from non-uniform Zn 2+ deposition. Constructing artificial interphase layers (AILs) to regulate Zn 2+ nucleation and growth has emerged as an effective strategy to mitigate these issues. One-dimensional (1D) Sn metal, featuring a high specific surface area, tunable structure, strong zinc affinity, and high hydrogen evolution overpotential, is an ideal candidate for interphase engineering. However, existing synthesis methods for 1D Sn, which rely on template-assisted electrodeposition, face challenges in scalability. In this work, Sn whiskers are synthesized via the mechanochemical decomposition of the Ti 2 SnC MAX phase and employed to construct a three-dimensional (3D) Sn whisker network as an artificial interphase layer on zinc anodes (Sn whisker@Zn). This continuous network effectively guides Zn 2+ migration and deposition, promotes preferential growth along the (002) crystal plane, reduces local current density, and suppresses dendrite formation. Simultaneously, it retards corrosion and inhibits the formation of by-products. Symmetric cells based on Sn whisker@Zn anodes exhibit exceptional cycling stability, sustaining over 1600 h of stable operation at 1 mA cm −2 with a capacity of 0.5 mAh cm −2 , and exceeding 1000 h at a high current density of 10 mA cm −2 . Moreover, the Sn whisker@Zn||NH 4 V 4 O 10 full cell retains 89.94 % of its capacity after 1400 cycles at 5 A g −1 , demonstrating strong application potential. This approach provides a scalable and effective strategy for developing durable zinc anodes, advancing the prospects of AZIBs in energy storage systems.

研究领域: 材料科学 · 电化学 · 能源存储 · 纳米材料 · 金属腐蚀与防护
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APPLIED SURFACE SCIENCE · 2023 · IF 6.7

Boosting adsorption and dissociation kinetics of magnesium-chloride ion pair via bismuth/indium-based artificial interface

Honghao Chu,Ning Yuan,Kun Zhang,Zhenfang Zhou,Kun Chao,Guicun Li,Zhonghua Zhang

The formation of passivating interphases on Mg-metal anode is impeding the wide employment of rechargeable Mg-metal batteries with less safety and cost concerns. Despite engineering artificial interlayers offers an efficient solution, it still falls short of expectation because of the compromised Mg plating/stripping performances in conventional electrolyte systems. In this work, a unique bismuth/indium-based artificial interface is introduced, which enables an exceptional reversibility (lowest nucleation overpotential of 189 mV than that (583 mV) of pristine Mg anode), high rate capability (a stable charge and discharge operation at 5.0 mA cm −2 without short circuit) and good temperature   tolerance (being cyclable over 10 °C and 50 °C) for the first time. This bismuth/indium-based artificial interface is constructed by facile displacement reactions between Bi(CF 3 SO 3 ) 3 /In(CF 3 SO 3 ) 3 and Mg. The dominant interphases, including Bi, In and BiO x species, can be controllably tailored via adjusting the relative ratio and concentration of Bi(CF 3 SO 3 ) 3 /In(CF 3 SO 3 ) 3 . Theoretical calculation results accompanied by electrochemical experiments indicate that kinetically favorable adsorption and dissociation processes of Mg-Cl ion pair on this interface, affording good magnesiophilic property and fast charge transfer kinetics, are responsible for the improved Mg-metal anode properties.

研究领域: 材料科学 · 电化学 · 能源存储
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