ACS Applied Materials & Interfaces
·
2019
·
IF 8.456
Yun Zhao,Yimei Lai,Yuanyuan Zhang,Bin Ding,Jianyong Yu,Jianhua Yan
Li-metal anodes promise to build high-energy-storage systems, but they suffer from safety problems from severe dendrite growth. Here, we develop a thin and conformal hybrid ionic and electronic conducting metal-oxide nanofiber interface to stabilize Li-anodes without forming dendrites. The thin ionic-conductive Li0.33La0.56TiO3 (LLTO) nanofiber film is first fabricated by electrospinning followed by pyrolysis. After connecting with the electrolytes-wetted Li-metal anodes, due to the self-driven chemical reactions, LLTO is reduced, and a hybrid conducting interface is developed. The interface can act as a reservoir to redistribute the nonuniform Li-ion flux above the anode surface and reduce the driving force of dendrite formation by leveling electric potential distribution, enabling a stable Li plating-stripping with a low overpotential of 80 mV over 800 h at a high current of 5 mA/cm2. More practically, the Li-LiNi0.8Co0.15Al0.05O2 cells deliver a high capacity of 147 mA h/g at 1 C with a Coulombic efficiency of 99% over 150 cycles, offering prospects to achieve reliable Li-metal batteries.
研究领域:
储能
·
材料科学
·
电化学
·
纳米材料
·
电池技术
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DOI
高影响因子
Nature Chemistry
·
2026
·
IF 24.5
Chen Yawei,Huang Fanyang,Zhang Qiu,Zheng Lei,Li Ai-Min,Dong Dejian,Xia Kangxuan,Lee Taeyong,Zhang Weiran,Li Zheng,Zhang Xin,Zhao Chang-Xin,Chen Fu,Rao Jiancun,Gaskell Karen,Hu Enyuan,Wang Chunsheng
High-capacity anodes are desirable for high-energy lithium-ion batteries but suffer from limited cycle life due to large volume changes during cycling. The LiF-based solid–electrolyte interphase (SEI) has led to prolonged cycling stability. However, current LiF-forming electrolyte designs require anions to enter the Li + solvation sheath, which inherently reduces the electrolyte’s ionic conductivity, limiting both fast-charging and low-temperature performance. Here we develop solvent-bridged electrolytes composed of LiPF 6 dissolved in a cosolvent system comprising a bridging cyclic ether that solvates both PF 6 − and Li + to form a LiF-rich SEI, and a structural linear ether that governs the electrolyte liquid range. By mitigating direct Li + –anion interactions, the electrolytes maintain high ionic conductivity, enabling stable cycling of micrometre-sized silicon anodes under extreme conditions involving high rates (>4 C), low temperatures (down to −55 °C) and Li plating. Solvent-bridged electrolytes address the intrinsic trade-offs between LiF-rich SEI formation and electrolyte ionic conductivity, offering a promising approach for high-capacity anodes operating under demanding conditions.
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Energies
·
2026
·Vol. 19
·期 12
·2790
·
IF 3.9
Jin Liang,Xiaojin Liu,Weiye Ma,Zhiyi Pan,Zhiqiang Liu,Yuxin Liang,Wence Xu,Shengli Zhu,Zhonghui Gao
N-doped Li2ZrCl6−3xNxchloride solid electrolytes were synthesized via a mechanochemical method, and the effects of N incorporation on crystal structure, Li local environment, and Li+transport were systematically investigated. X-ray diffraction suggested that the main Li2ZrCl6-related diffraction features were largely retained, while N introduction induced partial structural evolution towardC2/m-related features. 7Li MAS NMR revealed that N incorporation sharpened Li resonance peaks. Among the series, Li2ZrCl5.7N0.1exhibited the highest room-temperature ionic conductivity of 1.15 mS cm−1, with the lowest activation energy of 0.237 eV, demonstrating a reduced Li+migration barrier. All-solid-state batteries incorporating Li2ZrCl5.7N0.1showed stable rate capability and long-term cycling, retaining 85.9% capacity after 500 cycles at 1C and 77.4% after 3000 cycles at 3C. These results suggest that appropriate N modification can tune the Li2ZrCl6-based structure and Li local environment, thereby improving Li+transport in all-solid-state lithium batteries. This work provides a feasible strategy for improving chloride-based solid electrolytes for next-generation energy storage.
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Nature Communications
·
2026
·
IF 18.1
Yang Sixie,Chang Bo,Wang Chang,Wang Yigang,Wen Zhang,Liu Yiwen,Zhou Haoshen,He Ping
The global shift to renewable energy has intensified demand for lithium-ion batteries. Conventional lithium sources and extraction methods—such as brine evaporation and ore roasting—are time- and resource-intensive, geographically constrained, and environmentally damaging, underscoring the need for more sustainable resources and extraction strategies. Here we report an electrodialysis-based approach for direct lithium carbonate extraction from seawater, using ambient carbon dioxide as the carbon source. The method integrates a solid-state lithium-conducting membrane with Li–air chemistry, enabling lithium enrichment and carbonate formation in a single step without added precipitants. The Li–air configuration imparts intrinsic ion selectivity via thermodynamically driven displacement reactions. Experimental results confirm the production of lithium carbonate (93.8% purity) with an applied voltage below 2 V, while reducing chemical input and energy consumption compared to conventional processes. This work has the potential to provide a low-impact route for accessing lithium resources and contributes to the sustainability of future battery supply chains.
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DOI
PubMed
高影响因子
JOURNAL OF NON-CRYSTALLINE SOLIDS
·
2026
·
IF 3.6
Beibei Pan,Yuanhao Ma,Jiawei Zhao,Caiyan Chen,Shuaishuai Liu,Yang Shen,Qiuju Zheng,Yuebo Hu
Li 0.5 La 0.5 TiO 3 (LLTO) is a promising solid-state electrolyte material due to its excellent chemical stability, wide electrochemical window, and relatively high ionic conductivity. This work aims to further improve the ionic conductivity of LLTO via modification with borophosphate glasses containing lithium halides. The underlying rationale is that the unique mixed network structure of borophosphate glass can provide additional pathways for lithium ion (Li + ) transport. Furthermore, the incorporation of halogenated borosilicate glass (especially LiI) is expected not only to supply extra Li + , but also to improve the solid electrolyte interface by filling the voids among LLTO pellets, thus enhancing the overall electrochemical performance. The results demonstrate that the sample with 2 wt.% Li 2 O-B 2 O 3 -P 2 O 5 -LiI (LBPI) glass achieves a favorable room temperature ionic conductivity of 1.03 × 10 –3 S·cm –1 , which is approximately double that of the pristine LLTO. Our findings confirm the synergistic modification effect of borophosphate glass and lithium halides in improving Li + transport and present a strategic approach for developing advanced solid-state electrolytes with satisfactory electrochemical performance.
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CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Yingchao Wang,Zhen Wang,Qiyang Lu,Qingxian Miao,Yonghao Ni,Liulian Huang,Lihui Chen,Zhiwei Lin,Yuxin Liu,Jianguo Li
Charged cellulose in nonwoven leads to nano-sized pores and high charged density of CNW. • Donnan exclusion and Debye-length-related electrostatic regulation facilitate Li+ transport and suppress Mg2+ in CNW. • CNW in FO delivers Li + permeation of 920 g·h −1 ·m −2 with Li + /Mg 2+ selectivity of 3.24. • CNW remains stable at wide pH, high salinity, and long-term operation. With the rapid growth of the lithium battery industry, global lithium demand continues to increase, making efficient and selective lithium extraction from salt lake brines increasingly important. In this context, the performance of ion-selective separation membranes is crucial, with surface charge and porous transport structure being widely recognized as key factors influencing separation efficiency. Herein, this study develops a scalable charged cellulose-inserted nonwoven composite membrane (CNW) by embedding charged cellulose molecules into a nonwoven fabric through a simple vacuum-assisted impregnation process. The CNW possesses interconnected porous transport pathways (porosity of 66%) and a negatively charged interface (zeta potential of −49 mV), which support the selective ion transport through the synergistic effects of Donnan exclusion and Debye-length-related electrostatic regulation. Under the optimal conditions, the permeation rates of Li + and Mg 2+ reach 920 and 284 g·h −1 ·m −2 , respectively, while the Li + /Mg 2+ selectivity of 3.24, approximately 3 times higher than that of the original cellulose membrane, under osmotically driven FO operation. Moreover, the membrane maintains stable separation performance and structural integrity during long-term operation. These findings demonstrate that the synergistic regulation of charged interfaces and porous transport pathways provides a promising strategy for scalable and sustainable lithium extraction from salt-lake brines. Download: Download high-res image (187KB) Download: Download full-size image
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高影响因子
Nature Communications
·
2026
·
IF 18.1
Chen Hao,Huang Jiawen,Peng Si-Hao,Liu Zhi-Hua,Zeng Zhi-Wei,Tang Pei-Jie,Liu Bo-Wen,Zeng Fu-Rong,Wang Yu-Zhong,Zhang Lin,Zhao Hai-Bo
Solid polymer electrolytes are important for lithium metal batteries, but their limited Li + transference efficiency hinders large-scale deployment. Here we report a Li⁺ shuttle bus strategy that immobilizes anions at one-dimensional charged interface, promotes lithium salt dissociation, and guides Li⁺ enrichment. The effect of Coulombic repulsion among densely coordinated Li⁺ species weakens solvation structure for Li + , achieving fast, collective and one-dimensional ion shuttling at the microscopic scale. Consequently, the designed solid polymer electrolyte exhibits a high ionic conductivity of 0.92 × 10 −3 S cm −1 at 28 °C. Li | |LiFePO 4 cells operate nearly 5000 cycles at 5 C and maintain 77% capacity after 900 cycles at −40 °C. Li | |LiNi 0.8 Co 0.1 Mn 0.1 O 2 pouch cell further realizes high specific energy (508 Wh kg −1 , 200 cycles, 95.2% retention). This work establishes a Li⁺ shuttle-bus strategy for constructing solid polymer electrolytes with fast-charging capability and wide-temperature adaptability, offering findings into the design of solid-state lithium metal batteries.
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DOI
高影响因子
Science Bulletin
·
2026
·
IF 20.7
Yuchun Liu,Tianqi Liu,Xinyun Wang,Jing Zhang,Xingwu Zhai,Tianchen Wei,Baichuan Zhu,Yuxin Xiao,Zhaorui Xin,Quan Zhang,Jing Peng,Chong Xiao,Min Zhou
Rechargeable Li–gas batteries, represented by Li–O 2 and Li–CO 2 systems, are promising for high-energy-density storage and gas-involved energy conversion, yet their operation is constrained by the trade-off between catalytic activity and structural durability of cathodes. Metastable defects such as stacking faults offer active sites for accelerating sluggish gas redox reactions, but readily undergo electrochemical stress-induced slip and structural collapse during cycling. Inspired by plant traumatic resinosis, we propose a site-specific self-protection strategy that exploits the intrinsic anisotropy of stacking faults to decouple catalytic reaction planes from orthogonal protective functional planes. On the reaction plane, over-coordinated dislocation sites amplify surface electrostatic potential differences and promote Li 2 CO 3 decomposition via nucleophilic/electrophilic interactions. On the functional plane, selective interactions with sulfur-containing electrolyte components induce in situ reconstruction of a multiphase inorganic–organic amorphous interphase, anchoring stacking faults without blocking catalytic sites. As a Li–CO 2 proof of concept, stacking-fault-rich molybdenum boride (MoB) delivers 90.13% average energy efficiency over 2500 h and stable operation at 150 °C for nearly 500 h. This work establishes a self-protection paradigm for stable metastable active structures and provides a universal interface design principle for durable Li–gas batteries. This work proposes a site-specific self-protection strategy, inspired by traumatic resinosis in plants, to stabilize highly active but fragile defect structures in Li–gas batteries. By spatially decoupling the catalytic and protective planes of stacking faults, a localized amorphous interphase forms in situ to suppress structural degradation without sacrificing catalytic activity. This strategy enables simultaneous optimization of activity and durability and offers a transferable design principle for stabilizing metastable active structures. 本研究针对锂气体电池中高活性缺陷结构易失稳的问题, 提出受植物创伤树脂化启发的“位点特异性自保护”策略。通过将堆垛层错的反应平面与保护功能平面空间解耦, 在保持催化活性的同时原位构筑局域非晶保护界面, 从而抑制结构滑移与破坏。该工作实现了活性与稳定性的协同优化, 并为亚稳活性结构的界面保护提供了新的可迁移设计思路. Download: Download high-res image (162KB) Download: Download full-size image
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JOURNAL OF CATALYSIS
·
2026
·
IF 6
Qiongyu Wang,Ziheng Zhang,Xilun Zhang,Hua Xie,Ling Jiang,Fei Chang
Catalytic alkyne semi-hydrogenation is a pivotal industrial transformation currently constrained by the limitations of existing heterogeneous catalysts: precious metals (e.g., Pd) face high costs, while non-precious alternatives (e.g., Ni, Cu, Fe) generally require harsh reaction conditions (100–200 °C, 10–40 bar H 2 ). To address these persistent challenges, we propose a novel strategy integrating alkali metal hydrides, serving simultaneously as hydrogen donors and anionic “ligands” into transition metal systems. Herein, we report a NiFe-LiH composite catalyst that enables efficient and highly selective liquid-phase semi-hydrogenation of alkynes—including aliphatic, aromatic, and heteroatom-substituted substrates under very mild conditions (25 °C, ≤3 bar H 2 ). Mechanistic investigations reveal that reactive hydride species (H − ) are integral to the hydrogenation catalysis. Critically, the formation of unique Li-Ni-Fe-H interfacial species facilitate synergistic interactions wherein anionic hydrides coordinate with transition metals, modulating their electronic states to simultaneously enhance catalytic activity and selectivity. This work demonstrates room-temperature activation and transformation of alkynes enabled by a catalytic Li-Ni-Fe-H system, offering a promising new pathway for developing efficient non-noble metal catalysts for selective hydrogenation reactions.
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DOI
高影响因子
INORGANIC CHEMISTRY
·
2026
·
IF 4.6
Jia Mohan,Yu Run,Zheng Hongwei,Zhang Qiaoxin,Yan Huacai,An Yifeng,Chen Hexuan,Nazir Atif,Wang Yonggang,Zou Ruqiang
Antifluorite oxides containing ordered tetrahedral voids
provide
a structurally flexible platform for Li-ion transport; however, experimentally
identifying and controlling the defect configurations that activate
these voids remains challenging. Here, Li-excess defect engineering
is demonstrated in orthorhombic Li 5 AlO 4 to regulate
its Li-ion transport behavior. High-resolution time-of-flight neutron
powder diffraction (TOF-NPD), combined with Rietveld refinement and
Fourier difference nuclear-density mapping, resolves the underlying
Li-related defect architecture. The refinement results reveal that
excess Li is accommodated through the coupled formation of Al/Li antisite
occupancy at the 2 a Wyckoff site and newly occupied
interstitial Li at the intrinsically vacant 2 b site,
accompanied by systematic lattice expansion and local structural relaxation.
BVSE-guided CI-NEB calculations reveal a multistep Li-ion migration
network, in which the three-dimensional bottleneck decreases from
0.43 eV in pristine Li 5 AlO 4 to 0.40 eV in the
coupled-defect model, while the local migration segments directly
involving the occupied 2 b site exhibit larger barrier
reductions. Consistently, electrochemical impedance spectroscopy shows
an increase in the room-temperature bulk ionic conductivity to 3.33
× 10 –7 S cm –1 for the Li-excess
sample. These findings establish an experimentally validated correlation
between Li-related defect chemistry and ion transport in Li 5 AlO 4 , providing guidance for defect-enabled transport
design in antifluorite oxide conductors.
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DOI
高影响因子
ACS Applied Materials & Interfaces
·
2025
·
IF 8.2
Bizhu Zheng,Hui Qian,Jiabao Ding,Chen Yuan,Ruixuan Zhang,Xiangsi Liu,Yuxuan Xiang
Unfavorable phase transformations and limited practical capacity remain significant challenges to the widespread application of layered oxides in sodium-ion batteries. Lithium doping has emerged as an effective strategy to suppress phase transformations and activate oxygen redox reactions. However, solid-state NMR reveals that Li+ gradually deintercalates from the bulk of the cathode during repeated cycles, ultimately compromising the efficacy of Li-doping. To address this, we introduce a straightforward yet effective approach involving the introduction of exogenous Li+ into the electrolyte, dynamically compensating for and mitigating undesired Li loss. Complementary solid-state NMR and XRD characterizations confirm that the exogenous Li+ preserves the bulk lithium content within the cathode, preventing structural degradation at both the long-range crystal structure and the local atomic environment. Additionally, interfacial characterization and electrochemical analysis demonstrate that exogenous Li+ optimizes the cathode-electrolyte interface and reduces interfacial impedance. As a result, the capacity retention of Na0.76Li0.1Ni0.23Mn0.67O2 improved significantly from 73.5% to 90.7% after 200 cycles. This study underscores the pivotal role of electrolytes in preserving the long-term effectiveness of structural modifications in the cathode, providing an approach to extending the cycling lifespan of high-performance sodium-ion batteries.
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高影响因子
Materials
·
2025
·Vol. 18
·期 10
·2373
·
IF 3.2
Jing Zhu,Xiyun Yang,Yongqiang Huang,Rongzheng Yao
With the depletion of solid lithium ore, extracting lithium from salt lake brine has become a critical focus for future endeavors. A four-step method was used to synthesize high-purity H1.6Mn1.6O4for extracting Li+. Porous cubic Mn2O3was hydrothermally synthesized with carbon spheres and surfactants as templates. Then, it was converted to LiMnO2by calcining with Li2CO3. After roasting and acid pickling, H1.6Mn1.6O4was successfully synthesized. The impacts of calcination temperature, Li/Mn molar ratio and glucose addition on LiMnO2composition, loss percentage of dissolved Mn in precursor, and the adsorption characteristics of the lithium ion sieve were studied. Glucose inhibited the formation of LiMn2O4and promoted the formation of pure LiMnO2. The resulting precursor without impurities showed porous structure. After acid pickling, H1.6Mn1.6O4showed a high-adsorption performance and excellent cycle performance. After five cycles, adsorption capacity remained above 30 mg/g, and the loss percentage of dissolved Mn stabilized at about 1%. The Li+–H+exchange conformed to pseudo-second-order adsorption dynamics and the Langmuir adsorption isotherm equation, indicating that the adsorption process can be classified as monolayer chemical adsorption.
研究领域:
材料科学
·
化学工程
·
环境科学
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高影响因子
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