ADVANCED FUNCTIONAL MATERIALS
·
2025
·Vol. 35
·期 44
·2509658
·
IF 19
Chaoqiang Tan,Zeyu Shen,Shichao Zhang,Zhijun Wu,Shengnan He,Hongge Pan,Hao Cheng,Yingying Lu
Sulfurized polyacrylonitrile (SPAN) recently emerges as a prospective cathode for lithium–sulfur (Li–S) batteries owing to its high S utilization, remarkable cycling stability, and liberty from shuttle effect. Despite weakly solvating ether electrolytes exhibiting simultaneously compatibility for SPAN cathode and lithium (Li) anode, they universally suffer from low ionic conductivity and narrow liquid-phase temperature range. However, conventional ether-based electrolytes with excellent ionic conductivity cannot realize reversible solid–solid conversion of SPAN cathode due to Li polysulfide intermediates (LiPSs) dissolving and shuttling. Here, a series of weakly solvating ethers are evaluated by selectively methylating dimethoxymethane (DMM) to fine-tune their solvation capability and liquid-phase temperature range. Enlightened from weakly solvating ether electrolytes, the contact ion pair (CIP)-dominated electrolyte is designed for satisfactory ionic conductivity of electrolyte and reversible solid–solid conversion of SPAN cathode over wide temperature range. The reinforcement mechanisms of the CIP-dominated electrolyte for the Li anode and SPAN cathode are comprehensively elucidated through experimental characterizations and molecular dynamics simulations. Based on the optimized electrolyte, Li||SPAN full cells can steadily operate over wide temperature range from −20 to 60 °C. Furthermore, the 120 mAh Li||SPAN pouch cell can exhibit 85.5% capacity retention after 45 cycles at 0.2 C.
研究领域:
电化学
·
能源材料
·
锂离子电池
·
电极界面化学
·
电解质工程
·
分子动力学模拟
✓ 已验证
产品关联
DOI
高影响因子
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.
✓ 已验证
产品关联
DOI
PubMed
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.
✓ 已验证
DOI
高影响因子
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.
✓ 已验证
DOI
高影响因子
DESALINATION
·
2026
·
IF 9.9
Chun-Xu Zhang,Yan-Yan Chen,Ren-Jie Fan,Yu-Xuan Sun,Xiaohu Wang,Fujun Xiong,Yong Wang,Mei-Ling Liu,Shi-Peng Sun,Weihong Xing
Electric field-assisted nanofiltration (ENF) has emerged as a promising technology for Mg 2+ /Li + separation from salt lake brines. However, integrating ENF process with widely used negatively charged membranes induces a non-uniform distribution of reconstructed positive charge. This leads to reduced separation efficiency under high feed concentrations due to charge shielding effects. To overcome this limitation, we developed a strategy employing a positively charged nanofiltration (NF) membrane under an applied electric field. This configuration facilitates both the dehydration of hydrated Li + and a more uniform distribution of positive charges on the membrane surface. The optimized system demonstrated a remarkable separation performance, achieving nearly 100% rejection of Mg 2+ and − 176% rejection of Li + . The separation factor ( S Li, Mg ) represents a 162-fold improvement over the system without an electric field. The ENF process successfully separated Mg 2+ and Li + even in real Yiliping salt lake brine. Furthermore, the permeate stream containing high-purity Li + enabled the production of battery-grade Li₂CO₃ with 99.9% purity. This study demonstrates a pragmatic and efficient approach for Mg 2+ /Li + separation, showcasing considerable promise for high-purity Li + extraction from salt lakes.
✓ 已验证
产品关联
DOI
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.
✓ 已验证
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
✓ 已验证
DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2026
·
IF 8.8
Yijing Zhang,Si Sun,Ming Wang,Yaling Han,Xuan Luo,Shenzhen Cong,Tao He,Huan Pang
Membranes featuring structural stability and precise ion selectivity are indispensable for efficient lithium recovery from magnesium-rich brines. Despite the promising potential of metal-organic framework (MOF) membranes in ion separation, the flexibility of aromatic linkers in conventional MOF structures often induces pore size fluctuations, which compromises size-based discrimination efficiency. Herein, defect-free Zr-Frustrated Trigonal-symmetry Rotor (Zr-FTR) membranes were fabricated on polyethylene terephthalate (PET) substrates via a counter-diffusion interfacial growth method. The Zr-FTR framework is constructed with bicyclopentane linkers, whose rigid geometric configuration and substantial torsional energy barriers ensure the retention of a fixed pore aperture (∼4.3 Å). This rigid confinement effect significantly suppresses transient pore expansion, enabling effective ion size sieving while retaining exceptional structural stability. The optimized Zr-FTR-24 membrane exhibits a high Li + permeability of 0.09 mol m −2 h −1 and a Li + /Mg 2+ selectivity of 235, with sustained performance stability over a 7-day continuous operation in mixed-ion solutions. This work establishes a novel design paradigm for suppressing linker dynamics in MOF membranes through rigid linker engineering, ultimately achieving structurally stable and size-exclusive ion transport.
✓ 已验证
产品关联
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.
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Energy Materials
·
2025
·
IF 5.5
Chenxin Diao,Xianhui Jiao,Jin Xu,Hui Zhan
Lithium/carbon fluoride (Li/CFx) primary batteries have attracted wide attention because of their high energy density. However, their application in high-power devices is severely hindered by the retarded reaction kinetics caused by lithium fluoride (LiF) accumulation and difficult desolvation, which is further intensified by low temperature. In this work, an electrolyte strategy has been proposed targeting the kinetic issues. The methyl acetate (MA) low-temperature solvent weakens the Li+ coordination and facilitates the Li+ desolvation, while crown ether provides a LiF removal effect through its complexing capability. After comprehensive optimization, the benzo-12-crown-4 (B12C4)- and MA-containing electrolyte significantly enhances the rate performance as well as low-temperature output of the CFx cathode, endowing it with excellent wide-temperature adaptability. This work not only greatly improves the electrochemical property of the CFx electrode but also provides an alternative electrolyte strategy for all-climate and high-power/energy Li/CFx cells.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
Advanced Science
·
2025
·
IF 14.1
Runhe He,Hao Liu,Qing Gao,Dong Cai,Kuikui Xiao,Yinhang Zhang,Xinmin Zhang,Xianyang Cheng,Yuhui Wang,Lixing Kang,Huagui Nie,Yatao Liu,Zhi Yang
Sulfurized polyacrylonitrile (SPAN) represents a highly promising cathode material for lithium–sulfur (Li–S) batteries, leveraging a solid-solid sulfur conversion mechanism. However, persistent interfacial side reactions and sluggish redox kinetics in SPAN cathodes compromise the electrochemical performance. Here, quaternized chitosan (QCS) is employed as a functional agent to stabilize the SPAN cathode electrolyte interphase (CEI). The positively charged quaternary ammonium groups selectively adsorb PF 6 – anions, modifying the Helmholtz layer structure and facilitating the formation of an anion-derived CEI enriched with LiF. Consequently, the SPAN@QCS-1.0% cathode delivers a high discharge capacity of 1499 mAh g −1 at 0.2 C, an outstanding rate capability of 902 mAh g −1 at 10 C, and a prolonged cycle life exceeding 1500 cycles at 1 C. Under practical conditions of high sulfur loading (12.0 mg cm −2 ) and lean electrolyte (E/S ratio = 5 µL mg −1 ), the SPAN cell achieves a high areal capacity of 17.1 mAh cm −2 , surpassing that of conventional lithium–ion batteries (≈4 mAh cm −2 ) by more than fourfold. Furthermore, a 0.9 Ah pouch-cell prototype demonstrates stable cycling for over 30 cycles. The interface strategy provides a facile and effective approach to developing high-performance SPAN-based Li–S batteries.
研究领域:
电化学
·
储能
·
材料科学
·
电池技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2025
·
IF 9
Yushuang Lin,Nan Li,Weihao Xue,Hong Chen,Zhiruo Zhang,Zhao Dai
Achieving precise pore size tuning in nanofiltration membranes for Mg 2+ /Li + separation remains challenging due to the similar hydrated radii of the ions and the lack of real-time monitoring for dynamic adjustments. In this study, we developed a novel pH-responsive color-changing nanofiltration membrane with tunable pore sizes, enabling real-time monitoring and enhanced separation efficiency. By incorporating γ-cyclodextrin during interfacial polymerization, we achieved angstrom-level pore size tuning and reduced pH sensitivity. The color response of the membrane enables dynamic adjustments to the feed solution pH, optimizing pore radii to ∼0.41 nm, leading to a separation factor of 35.5. Molecular dynamics simulations and weight cut-off experiments confirmed that γ-cyclodextrin enhanced pore uniformity, resulting in a denser, more efficient membrane. This innovative approach offers a flexible and precise solution for Mg 2+ /Li + separation, demonstrating high permeance (15.5 L m −2 h −1 bar −1 ) and potential for applications in seawater desalination, resource recovery, and industrial ion separation.
研究领域:
膜科学
·
分离技术
·
材料科学
·
化学工程
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子