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ELECTROCHIMICA ACTA · 2026 · IF 5.8

In-situ construction of a LiI@Li-Bi composite interlayer for stable Li|LATP interface in solid-state lithium batteries

Jiahao Fan,Mingdao Zhang,Li Song,Yachao Jin

BiI 3 drop-casting method is applied to prepare B-LATP electrolyte. • The addition of BiI 3 reduces interfacial resistance. • The addition of BiI 3 enhances the lithiophilicity of the material. • B-LATP achieves a critical current density of 3.7 mA cm −2 . NASICON-type Li 1.3 Al 0.3 Ti 1.7 (PO 4 ) 3 (LATP) solid-state electrolyte (SSE) is considered a promising candidate for solid-state lithium metal batteries (SLMB) due to its high room-temperature, Li-ion conductivity and superior air stability. However, its practical application is hindered by electro-chemo-mechanical degradation at the Li|LATP interface, including lithium dendrite penetration and poor physical contact. Rational interfacial design from a chemical compatibility synergistic perspective is therefore imperative. Herein, we report the in-situ construction of a multifunctional LiI@Li-Bi composite interlayer at the Li|LATP interface via a conversion reaction between a BiI 3 thin film and lithium metal. This tailored interlayer consists of electronically insulating LiI and a lithiophilic Li–Bi alloy. It effectively improves interfacial contact, reduces interfacial resistance, suppresses side reactions, and homogenizes Li-ion flux, thereby inhibiting dendrite growth. The Li|B-LATP|Li symmetric cell achieves a critical current density of 3.7 mA cm −2 and maintains stable cycling for over 600 h at 0.1 mA cm −2 . Furthermore, the LiFePO 4 |B-LATP|Li solid-state full cell exhibits stable cycling performance at 0.1 C and room temperature. These results highlight the critical role of rational Li|LATP interface design and provide a facile strategy for optimizing interfacial compatibility and addressing interfacial challenges in SLMBs. This simple method utilizes a conversion reaction between a BiI 3 thin film and Li metal to in-situ form a LiI@Li-Bi composite interlayer on LATP. The resulting interlayer improves interfacial contact, enhancing cycling stability of both symmetric and full cells. Download: Download high-res image (219KB) Download: Download full-size image

CAS / MDL: 7787-64-6
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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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INTERNATIONAL JOURNAL OF ENERGY RESEARCH · 2022 ·Vol. 46 ·期 14 ·19357-19367 · IF 4.672

A novel Nafion-Functionalized Polyethersulfone(PES)-based ion-permselective separator for high performance Li-O2 batteries using LiI as a redox mediator

Jiuqing Liu,Feifei Song,Junying He,Zikun Hong,Qihou Li,Ya Chen,Lishun Bai,Fanli Zeng,Chen Cheng,Zehao Chen

Summary Owing to its unparalleled theoretical energy density, the Li-O 2 batteries are thought to be one of the most promising energy storage systems, but its application is seriously hindered by its potential safety risks arising from the passivation and corrosion of lithium anode. To address these issues, it is an efficient way to develop functionalized separator that could prevent the migration of anions and macromolecules from cathode toward anode. Herein, a novel Nafion-functionalized polyethersulfone (PES)-based ion-permselective separator was prepared by using non-solvent induced phase separation (NIPS) method. The Nafion ensures a better physical strength of the composite separator, and further characterizations show that the obtained composite separator owns good ionic conductivity (0.52 mS cm −1 ), high lithium ion migration number (0.80), and better cyclic stability (120 cycles, 1000 mAh g −1 ). Consequently, the composite separator serves as an excellent candidate to solve the “shuttle effect” of redox mediators (RMs), the assembled Li-O 2 battery with composite separator adding LiI as RMs presents lower charge overpotential and longer cycle stability (170 cycles, 1000 mAh g −1 ).

研究领域: 材料科学 · 电化学
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CHEMICAL ENGINEERING JOURNAL · 2021 · IF 13.273

A bifunctional MnxCo3-xO4-decorated separator for efficient Li-LiI-O2 batteries: A novel strategy to promote redox coupling and inhibit redox shuttling

Dan Li,Ziye Kang,Hao Sun,Ying Wang,Haiming Xie,Jia Liu,Jiefang Zhu

Although redox mediator (RM) strategy can decrease the overpotential in Li-O 2 batteries by tuning the electrochemical formation/degradation of Li 2 O 2 from the circumscribed surface pathway to the solution one, the redox shuttling causes an unexpected RM degradation and a continuous deterioration of Li anode, finally leading to a poor cyclability. This work presents the first report detailing the development of a novel Mn x Co 3-x O 4 -decorated separator for Li-LiI-O 2 batteries. Benefiting from the promotion effect of Mn x Co 3-x O 4 nanocages on I − /I 3 − and I 3 − /I 2 redox coupling, the cell with as-prepared separator maintains a low charge potential of ~3.3 V till the death of cell cycling. In addition, as-prepared separator can efficiently restrain the redox shuttling, leading to an obvious improvement on cycling stability for the cell. Moreover, the contributions of LiI to the battery performance and the operation mechanism are systematically investigated. These results present a promising progress in the development of multi-functional separator materials for RM-involved Li-O 2 batteries and the new design of hybrid energy storage device.

研究领域: 材料科学 · 电化学 · 能源存储技术
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ACS Applied Materials & Interfaces · 2024 · IF 8.3

Synergistic Interfacial Optimization for High-Sulfur-Content All-Solid-State Lithium–Sulfur Batteries

BoSheng Zhao,Chang Zhou,Peng Chen,XuePing Gao

Improving the sulfur content in the cathode is essential for achieving high-energy-density all-solid-state lithium–sulfur batteries (ASSLSBs). However, the complex multiinterfaces, akin to the short wooden planks that consist of the cask, severely limit the performance of ASSLSBs with high sulfur content. Since singular approaches fail to optimize these interfaces simultaneously, we propose a synergistic approach using a dual-doped sulfide solid electrolyte (Y2S3 and LiI) and an SbSn alloy sulfur host in this work. The incorporation of Y2S3 in the solid electrolyte serves to improve the electrolyte–electrolyte interfaces and enhance the ionic conductivity, while the inclusion of LiI helps stabilize the electrolyte–anode interface and suppress dendrite formation. Meanwhile, the SbSn alloy sulfur host facilitates the transfer of Li+ at the electrolyte–cathode interfaces. Consequently, the solid–solid interfaces are significantly improved, leading to impressive specific capacities in ASSLSBs with high sulfur content (>44% in the cathode composite) at room temperature (1163.5 mAh g–1) and at 60 °C (1408.7 mAh g–1) during the 50th cycle at 0.05C. This work presents a promising strategy for achieving practical high-performance ASSLSBs.

研究领域: 材料科学 · 电化学 · 能源存储
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Nature Communications · 2024 ·Vol. 15 ·期 1 ·1-14 · IF 14.7

Deciphering the critical role of interstitial volume in glassy sulfide superionic conductors

Su Han,Zhong Yu,Wang Changhong,Liu Yu,Hu Yang,Li Jingru,Wang Minkang,Jiao Longan,Zhou Ningning,Xiao Bing,Wang Xiuli,Sun Xueliang,Tu Jiangping

Sulfide electrolytes represent a crucial category of superionic conductors for all-solid-state lithium metal batteries. Among sulfide electrolytes, glassy sulfide is highly promising due to its long-range disorder and grain-boundary-free nature. However, the lack of comprehension regarding glass formation chemistry has hindered their progress. Herein, we propose interstitial volume as the decisive factor influencing halogen dopant solubility within a glass matrix. We engineer a Li 3 PS 4 -Li 4 SiS 4 complex structure within the sulfide glassy network to facilitate the release of interstitial volume. Consequently, we increase the dissolution capacity of LiI to 40 mol% in 75Li 2 S-25P 2 S 5 glass. The synthesized glass exhibits one of the highest ionic conductivities among reported glass sulfides. Furthermore, we develop a glassy/crystalline composite electrolyte to mitigate the shortcomings of argyrodite-type sulfides by utilizing our synthesized glass as the filler. The composite electrolytes effectively mitigate Li intrusion. This work unveils a protocol for the dissolution of halogen dopants in glass electrolytes.

研究领域: 材料科学 · 电化学 · 电池技术
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