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CHEMICAL ENGINEERING JOURNAL · 2025 · IF 13.2

In situ FeF3 coating on FeNCN to stabilize discharged products Fe0 for enhanced loading and high-rate Na storage performance

Jiayin Li,Wen Wen,Shuzhuo Bai,Jing Zhang,Chenyu Wu,Jintao Wu,QingQing Huang,Yalin Zhang,Chunyi Cai,Liyun Cao,Yijun Liu,Haibo Zhang,Hua Tan,Jianfeng Huang

The instability of the interfacial structure during the synthesis of iron carbodiimide (FeNCN) leads to a decline in its electrochemical performance during cycling. By depositing FeF 3 particles on the surface of FeNCN, the in-situ transformation of this FeF 3 nanolayer into a FeF 2 nanolayer effectively utilizes the discharge product Fe 0 . This process constructs a mechanically stable sandwich-structured SEI film, thereby enhancing the stability of the FeNCN electrode interface. Consequently, the FeNCN electrode exhibits a capacity of 350.54 mAh g −1 after 2000 cycles at 2 A g −1 , with a capacity retention rate of 99.54 %. This strategy provides crucial theoretical and technical insights for regulating carbodiimide-based materials to achieve stable, long-cycle performance in electrode materials.

研究领域: 材料科学 · 电化学 · 纳米技术 · 储能
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ENERGY & FUELS · 2024 · IF 5.2

Improve High Voltage Resistance Performance of LiNi0.8Co0.1Mn0.1O2 Lithium Metal Batteries by Two Novel Aromatic Compound Electrolyte Additives

Jian Lv,Yiwen Wang,Zhuyu Wang,Danni Shen,Qinggong Jia

Ternary high-nickel oxide exhibits a relatively high working voltage compared with traditional lithium battery cathodes (LiFePO4, etc.). Consequently, it has been widely studied in recent years and is at the forefront of research on positive electrodes for power batteries. To achieve higher reversible capacity, it is often necessary to increase the battery operating voltage. However, there are many drawbacks to this method, such as surface cracking of the working electrode and serious side reactions with the electrolyte. The novel dual-additive combination in this work has the potential to significantly address the aforementioned issues. A composite polymer cathode–electrolyte interface (CEI) film is formed on the surface of the cathode due to two aromatic compound additives preoxidation. The stable CEI film not only improves the stability of the electrode but also suppresses solvent and hydrofluoric acid (HF) to effectively inhibit the side reaction on the cathode surface. Furthermore, these two additives can be readily reduced at the anode to form a solid electrolyte interface (SEI) membrane containing rich LiN&LiF, which effectively suppresses the formation of lithium dendrites. The battery capacity retention could be up to nearly 83% on the dual-additive electrolyte compared to the baseline electrolyte after 300 cycles. This work may provide more possibilities for future research on high-voltage lithium batteries.

CAS / MDL: 86-74-8 1072-63-5
研究领域: 材料科学 · 电化学 · 能源存储
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CHEMICAL ENGINEERING JOURNAL · 2021 · IF 13.273

Chemical interface engineering of solid garnet batteries for long-life and high-rate performance

Weilin Huang,Zhijie Bi,Ning Zhao,Qifu Sun,Xiangxin Guo

The solid garnet battery is viewed as one of the most attractive candidates for investigating the solid-state lithium batteries with high energy density and safety. However, the crucial interfacial problems between the solid electrolytes and the electrodes severely hinder the improvement of battery performance. In this work, the reactive intermediate layers are introduced in between the garnet electrolytes and the electrodes. On the anode side, the ether-based electrolyte layer is in-situ converted into a gradient solid-electrolyte-interphase (SEI) film with the organic-rich outer layer and the inorganic-rich (LiF and Li 3 N) inner layer, leading to the conductive contact and the homogeneous potential distribution. Consequently, the modified Li symmetric cells exhibit the dendrite-free Li plating/stripping at the remarkable current density as high as 2.1 mA cm −2 at 60 °C. On the cathode side, the ionically conducting species composed of solid-phase LiF and Li 3 N is in-situ formed through the decomposition of the 1-Butyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide-based ionic liquid layer, leading to the decreased interfacial resistance and enhanced Li + conduction. The resultant LiNi 0.6 Co 0.2 Mn 0.2 O 2 /Li batteries with the residual liquid-phase electrolytes at the solid-phase boundaries deliver the high discharge capacity of 162.4 mAh g −1 with the capacity retention of 87.6% after 100 cycles at 0.2C and 60 °C. This work demonstrates a useful strategy to make the ideal interfaces through the in-situ conversion reactions for construction of high-performance solid garnet batteries.

研究领域: 材料科学 · 电化学
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Small · 2024 · IF 13

Enabling Uniform and Stable Lithium-Ion Diffusion at the Ultrathin Artificial Solid-Electrolyte Interface in Siloxene Anodes

Tiantian Fang,Huibin Liu,Xinyu Luo,Mengru Sun,WenChao Peng,Yang Li,Fengbao Zhang,Xiaobin Fan

Constructing a stable and robust solid electrolyte interphase (SEI) has a decisive influence on the charge/discharge kinetics of lithium-ion batteries (LIBs), especially for silicon-based anodes which generate repeated destruction and regeneration of unstable SEI films. Herein, a facile way is proposed to fabricate an artificial SEI layer composed of lithiophilic chitosan on the surface of two-dimensional siloxene, which has aroused wide attention as an advanced anode for LIBs due to its special characteristics. The optimized chitosan-modified siloxene anode exhibits an excellent reversible cyclic stability of about 672.6 mAh g −1 at a current density of 1000 mA g −1 after 200 cycles and 139.9 mAh g −1 at 6000 mA g −1 for 1200 cycles. Further investigation shows that a stable and LiF-rich SEI film is formed and can effectively adhere to the surface during cycling, redistribute lithium-ion flux, and enable a relatively homogenous lithium-ion diffusion. This work provides constructive guidance for interface engineering strategy of nano-structured silicon anodes.

CAS / MDL: 64-19-7 9012-76-4
研究领域: 材料科学 · 电化学
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LANGMUIR · 2026 · IF 4.4

Roles of Anion and Cation Doping in g-C3N4 as Artificial SEI for Regulating Interfacial Zn2+ Deposition in Aqueous Zinc Metal Anodes

Xi Wang,Long Pan,Jilong Xu,Xu Dong,ZhengMing Sun,Dawei Sha,Jianning Ding

Aqueous zinc-ion batteries are promising for their inherent safety, low cost, and environmental friendliness. However, their performance is limited by dendrite growth, hydrogen evolution, and interfacial instability from uncontrolled Zn2+ deposition. Although graphitic carbon nitride (g-C3N4) has been explored as an artificial solid electrolyte interphase (ASEI), its limited active sites and sluggish Zn2+ transport restrict long-term stability. More importantly, the roles of different doping types in regulating interfacial Zn2+ behavior remain unclear. Herein, anion (O) and cation (K) are doped into g-C3N4 to construct model ASEI layers for elucidating their respective roles in interfacial regulation. Combined experimental characterizations and theoretical calculations reveal that cation doping (KCN) decreases Zn2+ diffusion barrier, thereby facilitating Zn2+ transport across the interphase. In contrast, anion doping (OCN) induces strong electrostatic interaction and enhances Zn2+ adsorption affinity, leading to improved zincophilicity and synergistically ion transport. These distinct interfacial interactions result in markedly different Zn deposition behaviors, where anion doping enables more uniform nucleation and suppressed dendrite growth. Consequently, the OCN@Zn anode exhibits enhanced cycling stability. This work clarifies the roles of anion and cation doping in regulating interfacial Zn2+ deposition from the perspectives of ion transport and interfacial nucleation, and provides mechanistic insights and design guidelines for constructing high-efficiency ASEI layers via heteroatom engineering.

CAS / MDL: 57-13-6
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Journal of Energy Chemistry · 2025 · IF 14.9

Dual-channel MOF enabling high-flux Li+ conduction and in situ LiI-rich SEI for high-performance solid-state lithium metal batteries

Xingxing Zhang,Weihao Shi,Qingmei Su,Zemin He,Liming Wang,Xinglong Deng,Dequn Zhao,Rui Yan,Jinqi Chen,Hongli Chen,Zongcheng Miao,Wenhuan Huang

Solid-state lithium metal batteries (SSLMBs) face critical challenges from dendrite growth and unstable interfaces. While composite polymer electrolytes (CPEs) offer promise, poor ionic conductivity (<10 −5 S cm −1 ), low Li + transference numbers ( t Li+ < 0.5), and inadequate interfacial stability limit practical application. Herein, we design a dual-channel metal-organic framework (MOF)-based CPEs that simultaneously regulate ion transport and construct a high-conductivity interphase. This MOF features two distinct channels. The one imposes spatial confinement (0.57 nm in pore size) to suppress anion migration (TFSI − ), while the other facilitates immobilizing TFSI − through iodine-mediated nucleophilic substitution. More importantly, the liberated I − reacts with Li + to in situ generate lithium iodide (LiI)-enhanced solid-electrolyte interphase (SEI), replacing insulating LiF-rich counterparts. This LiI-SEI exhibits superior ionic conductivity and homogenizes Li + flux to suppress dendrites. Integrated into a poly(vinylidene fluoride)-cohexafluoropropylene (PVDF-HFP) matrix, the MOF CPE achieves exceptional ionic conductivity (2.13×10 −4 S cm −1 ) and a high t Li+ of 0.95 (25 °C). Density functional theory and molecular dynamics calculations verify ion-regulation mechanisms. As a result, LiFePO 4 //Li cells retain 94.99% capacity after 800 cycles (1 C), while NCM811//Li cells demonstrate sustained stability over 200 cycles. This work provides valuable insights into the design of multifunctional MOF ionic conductors for high-performance SSLMBs.

研究领域: 材料科学 · 电化学 · 储能技术 · 纳米技术 · 固态电池
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Journal of Materials Chemistry A · 2023 ·Vol. 11 ·期 11 ·5636-5644 · IF 11.9

Tuning the LiF content in the SEI by engineering the molecular structures of porous organic polymers for solid-state lithium metal batteries

Shi Zhou,Yiting Zhu,Haoran Hu,Chenghan Li,Jie Jiang,Jianyu Huang,Biao Zhang

LiF, which is considered as a key component of the solid electrolyte interface (SEI), can promote the uniform deposition of lithium. However, excessive LiF will limit the transport of lithium ions (Li+) in the SEI, resulting in low coulombic efficiency and lithium dendrite growth. Regulating the LiF concentration in the SEI is challenging but critical to the development of solid-state lithium metal batteries (SSLMBs). Herein, we synthesized porous organic polymers (POPs) that can be flexibly modified at the molecular level. These modified POPs (denoted as POPs-X-FP, X = 2, 3, 4) are added into a PEO electrolyte as fillers to form composite solid electrolytes (denoted as CSE-X-FP, X = 2, 3, 4, respectively). CSE-X-FP have different catalytic decomposition capabilities of TFSI− anions in the electrolyte due to the different fluorine atom substitution positions on the benzene ring of the POPs. Consequently, the LiF concentration in the SEI can be optimized by tuning the fluorine atom substitution positions on the benzene rings of the POPs to boost the performance of PEO based ASSLMBs. Using the LiF optimized SEI, the LiFePO4(LFP)//CSE-4-FP//Li full cell delivered a long cycle life of 1200 cycles with an initial capacity of 160.7 mA h g−1 at 0.5C. This study provides a new strategy to regulate the LiF content in the SEI layer to boost the performance of SSLMBs.

研究领域: 材料科学 · 电化学
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ACS Applied Energy Materials · 2021 · IF 6.024

Dendrite-Free and Micron-Columnar Li Metal Deposited from LiNO3-Based Electrolytes

Jingjing Zhou,Jiahang Chen,Jun Yang,Yanna Nuli,Jiulin Wang

Rechargeable Li-metal anodes have received abundant attention for high-energy-density batteries. A solid electrolyte interphase (SEI) plays a significant role in regulating the Li+ deposition/stripping process. Aimed to solve detrimental Li deposition with a dendritic and mossy morphology, herein, dendrite-free columnar Li deposition in micron size is constructed via creatively adopting a LiNO3-based electrolyte even at a high current density (2 mA cm–2) and areal capacity (4 mAh cm–2). N-rich inorganic SEI (Li3N and LiNxOy) with superior Li+ conductivity is formed on Li deposition, which enables remarkable reversibility and high average Coulombic efficiency (CE) even over 240 cycles. A Li∥LiFePO4 cell delivers excellent cycling stability over 700 cycles with a capacity fading rate of merely 0.022% per cycle. This work provides a way to regulating columnar Li deposition via N-rich SEI coordination and developing electrolyte formulations for secondary Li-metal batteries.

研究领域: 材料科学 · 电化学
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Journal of Materials Chemistry A · 2025 · IF 9.5

Construction of a robust and high ion-conductivity SEI using a multifunctional additive to achieve high-rate and large-capacity lithium metal anodes

Jiaming Zhang,Hongxiang Kuai,Yike Liu,Zhenbiao Li,Pinjuan Zou,Jianhao Lin,Chuang Ji,Xunhui Xiong

Despite the ultrahigh theoretical capacity (3860 mAh g−1) and low redox potential (−3.04 V vs. SHE), Li metal anodes suffer from low coulombic efficiency and dendrite growth, especially in carbonate electrolytes due to their high polarity and reactivity. Herein, triethyl 2-fluoro-2-phosphonoacetate (TFPA) is proposed as an effective additive to construct a robust LiF/Li3PO4-rich solid electrolyte interphase (SEI), as confirmed by density functional theory (DFT) and and X-ray photoelectron spectroscopy (XPS). The LiF provides high interfacial energy while Li3PO4 ensures high ionic conductivity, enabling stable Li deposition. With 0.5 wt% TFPA, Li‖Li symmetric cells stably cycle for 600 h at 5.0 mA cm−2 and 5.0 mAh cm−2. Full cells using high-loading LiNi0.8Co0.1Mn0.1O2 or LiCoO2 cathodes and thin Li (50 µm, N/P = 3.0) also show markedly enhanced cycling and rate performance.

CAS / MDL: 2356-16-3
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CHEMICAL ENGINEERING JOURNAL · 2026 · IF 12.5

Fluorine functionalized MIL-101 endows polymer electrolyte with highly Li+ dissociation, Li+ transference number and stabilized SEI for high-rate lithium metal batteries

Kai Liu,Ziying Liu,Kaixiang Zhi,Chang Liu,Huarui Zhang,Zhenyuan Hu,Yunfeng Zhang,Fan Xia,Chen Li,Hansong Cheng

Fluorinated MOFs material F-MIL-101 simply synthesized by hydrothermal method. • A gel polymer electrolyte that can fully dissociate LiTFSI. • The t Li + tLi+ of FM-10 is 119% higher than M-10. • The FM-10 formed a LiF-rich SEI layer on the lithium anode. • LFP||Li cells achieve excellent rate and cycling characteristics. Development of an attractive inorganic filler plays a vital role in effectively enhancing the comprehensive performance of a polymer electrolyte. Herein, a fluorine-functionalized metal organic framework (fluorinated MIL-101, F-MIL-101) is intentionally designed as filler for fabricating a novel composite polymer electrolyte (FM-10). Spectroscopic analysis and density functional theory calculations reveal that F-MIL-101 exhibits high effective dissociation and transportation of Li + for LiTFSI salt. Notably, the F functional group hinders anion transport, thereby giving the FM-10 GPEs a high transfer number of 0.81 for a uniform deposition of Li + on the Li anode surface. Furthermore, the F group of F-MIL-101 is greatly favorable for the formation of a stable LiF-rich solid electrolyte interface (SEI) on the Li anode surface during cycling to hinder the uninterrupted reaction. Consequently, the FM-10 GPEs demonstrates an excellent stable Li anode with a long cycle-life of 600 h in Li||Li cell at 2 mA cm −2 . More importantly, the FM-10 GPEs assembled LiFePO 4 (LFP) || Li cell exhibited an initial discharge capacity of 120.5 mAh g −1 at a high 6C-rate and a retention of 98.68% after 300 cycles, implying that the F-MIL-101 filler shows great potential as a strategy for fast charging, long cycle life, and high safety SSLMBs.

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ACS Sustainable Chemistry & Engineering · 2024 · IF 7.1

High Charging Voltage Stable and Air Atmosphere Stable Li–O2 Batteries with an Electrolyte Based on Succinonitrile and In Situ Artificial SEI Construction

Zining Man,Hao Tian,Xingbao Zhu,Zhe Lü

One experiment in this study utilized the plasticizer succinonitrile and lithium salt LiTFSI to directly create an ionic liquid electrolyte, with an artificial solid electrolyte interface layer generated using fluoroethylene carbonate. The typical electrolyte exhibited an ionic conductivity of 10–3 S cm–1 at room temperature and an electrochemical window of up to 5.3 V based on electrochemical impedance spectroscopy and linear sweep voltammetry tests. This electrolyte system effectively addresses the issues of decomposition and deterioration of traditional organic electrolytes in Li–O2 batteries at high voltages (over 4.5 V), as well as the problem of direct oxidation of the anode caused by oxygen shuttling, thereby greatly improving the lifespan of Li–O2 batteries. Additionally, the electrolyte’s low volatility and flame retardancy allowed for reliable operation of the battery in an air atmosphere. A Li–O2 battery assembled with the novel electrolyte was capable of cycling in a pure oxygen atmosphere for more than 1000 cycles at a capacity density of 200 mA h g–1 and over 150 cycles at 500 mA h g–1. Even when connected to ambient air without an additional oxygen selective membrane (OSM), the battery can still cycle continuously for more than 350 and 150 cycles at these two kinds of capacity density.

CAS / MDL: 90076-65-6 114435-02-8
研究领域: 材料科学 · 电化学
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JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY · 2022 · IF 10.319

Difunctional NH2-modified MOF supporting plentiful ion channels and stable LiF-rich SEI construction via organocatalysis for all-solid-state lithium metal batteries

Xuanyi Zhou,Chenghan Li,Biao Zhang,Fenfen Huang,Pan Zhou,Xinming Wang,Zengsheng Ma

As an essential part of the performance improvement of lithium metal batteries, the acquisition of dense (LiF-rich solid electrolyte interphase (SEI)) has always been an urgent problem to be solved. Herein, we synthesized Zeolitic Imidazolate Frameworks (ZIFs) modified by two different functional groups (–NH 2 , –CH 3 ) and used them as the fillers of polyethylene oxide (PEO) composite solid electrolytes to explore the catalytic effect of groups on LiF generation at the Li/electrolytes interface. In a LiFePO 4 ||SPE||Li cell test, the PEO-ZIF-NH 2 with LiF-rich SEI exhibits enhanced cycling performance, which was 3.8 times longer than that of PEO-ZIF-CH 3 . The formation mechanism of LiF-rich SEI was investigated using first-principles calculation, revealing that ZIFs-NH 2 makes the C–F bond in TFSI – longer compared with ZIFs-CH 3 , which leads to easier breakage of the C–F bond and promoted the formation of LiF. The simple design idea of using organic catalysis to generate more stable SEI provides a new aspect for preparing high-performance lithium metal batteries.

研究领域: 材料科学 · 电化学 · 电池技术
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