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CHEMICAL ENGINEERING JOURNAL · 2022 · IF 16.744

Nanofiltration membrane with crown ether as exclusive Li+ transport channels achieving efficient extraction of lithium from salt lake brine

Hongwei Li,Ying Wang,Tingyu Li,Xiang-Kui Ren,Jixiao Wang,Zhi Wang,Song Zhao

Lithium extraction from salt lake brines with high Mg 2+ /Li + ratios represents an effective alternative for tackling the scarcity of lithium resources. In this work, nanofiltration (NF) membrane with exclusive Li + transport channels was designed and prepared through facile interfacial polymerization, in which polyethyleneimine (PEI) bonded with 15-crown-5 ether (15C5) through hydrogen interaction was selected as the aqueous monomer ( [email protected] ) and reacted with trimesoyl chloride (TMC). The channels generated by 15C5 molecules could facilitate Li + transport owing to their affinity to Li + . Molecular dynamics simulation was conducted to further confirm the Li + transport through [email protected] membrane with exclusive Li + transport channels provided by 15C5. The [email protected] membrane displayed a permeability of 8.0 L·m −2 ·h −1 ·bar −1 and stable separation factor ( S Li,Mg ) of 14, which could reduce Mg 2+ /Li + mass ratio of a simulated brine from 20 to 1.7. Furthermore, a three-stage NF process was designed and performed using a [email protected] membrane to separate a simulated salt lake brine, containing multiple ions and Mg 2+ /Li + mass ratio of 50. After the treatment, the ultimate permeate solution of the third stage contained 24 ppm of Li + and 2.7 ppm of Mg 2+ with Mg 2+ /Li + mass ratio of 0.1. Therefore, this process could be applied to obtain Li 2 CO 3 products with high purity. Our investigation highlights the highly efficient Mg 2+ /Li + separation through NF membranes with exclusive Li + transport channels, potentially applicable to lithium extraction from salt lake brines with high Mg 2+ /Li + mass ratios.

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Advanced Science · 2021 ·Vol. 8 ·期 9 ·2003887 · IF 16.806

In Situ Polymerization Permeated Three-Dimensional Li+-Percolated Porous Oxide Ceramic Framework Boosting All Solid-State Lithium Metal Battery

Yiyuan Yan,Jiangwei Ju,Shanmu Dong,Yantao Wang,Lang Huang,Longfei Cui,Feng Jiang,Qinglei Wang,Yanfen Zhang,Guanglei Cui

Solid-state lithium battery promises highly safe electrochemical energy storage. Conductivity of solid electrolyte and compatibility of electrolyte/electrode interface are two keys to dominate the electrochemical performance of all solid-state battery. By in situ polymerizing poly(ethylene glycol) methyl ether acrylate within self-supported three-dimensional porous Li 1.3 Al 0.3 Ti 1.7 (PO 4 ) 3 framework, the as-assembled solid-state battery employing 4.5 V LiNi 0.8 Mn 0.1 Co 0.1 O 2 cathode and Li metal anode demonstrates a high Coulombic efficiency exceeding 99% at room temperature. Solid-state nuclear magnetic resonance results reveal that Li + migrates fast along the continuous Li 1.3 Al 0.3 Ti 1.7 (PO 4 ) 3 phase and Li 1.3 Al 0.3 Ti 1.7 (PO 4 ) 3 /polymer interfacial phase to generate a fantastic conductivity of 2.0 × 10 −4 S cm −1 at room temperature, which is 56 times higher than that of pristine poly(ethylene glycol) methyl ether acrylate. Meanwhile, the in situ polymerized poly(ethylene glycol) methyl ether acrylate can not only integrate the loose interfacial contact but also protect Li 1.3 Al 0.3 Ti 1.7 (PO 4 ) 3 from being reduced by lithium metal. As a consequence of the compatible solid-solid contact, the interfacial resistance decreases significantly by a factor of 40 times, resolving the notorious interfacial issue effectively. The integrated strategy proposed by this work can thereby guide both the preparation of highly conductive solid electrolyte and compatible interface design to boost practical high energy density all solid-state lithium metal battery.

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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2025 · IF 8.3

Optical field modulation for enhanced ORR and OER activity in Li–O2 batteries based on 2D porous Co3O4 nanosheets

Daming Yang,Yingyue Zhang,Jiaqi Sun,Xinyu Zhang,Ze Gao,Qilong Sun,Tong Wu,Wei Lu,Guiru Sun,Ming Feng

The photo-assisted strategy is viewed as a promising method to improve the ORR and OER performance of Li–O 2 batteries. Nevertheless, designing a photocatalyst that ensures wide light absorption and minimizes the recombination of photoinduced electrons and holes is still a notable challenge. In this study, 2D porous Co 3 O 4 nanosheets are synthesized as photocatalysts for photo-assisted Li–O 2 batteries. Their unique structure improves surface area, facilitates O 2 transport, and stores discharge products. Equally, the Co 3 O 4 nanosheets exhibit strong light responsiveness and photocatalytic activity. Upon optical field, photoinduced electrons and holes are successfully separated on Co 3 O 4 nanosheets, which promotes the formation and decomposition of Li 2 O 2 , respectively. Li–O 2 cells using Co 3 O 4 nanosheets display a low overpotential of 0.15 V and good cycling stability under optical field. These findings highlight the potential of Co 3 O 4 nanosheets as photocatalysts for photo-assisted Li–O 2 batteries, providing a foundation for future energy storage advancements.

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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS · 2024 · IF 4.9

ZIF-derived "cocoon"-like in-situ Zn/N-doped carbon as high-capacity anodes for Li/Na-ion batteries

Fengzhou Yuan,Zhe Chen,Huan Zhang,Yachao Jin,Li Song,Mingdao Zhang

Owing to the unique structure and physicochemical properties, including high specific surface area , self-doped N atoms, open pore structure and good chemical stability, zeolitic imidazolate frameworks (ZIFs) and their derivatives have been widely used in the field of energy storage. Here, a new type of "cocoon"-like Zn/N doped ZIF-derived porous carbon (Zn@N-C-800) is synthesized as an anode for lithium-ion batteries (LIBs) and sodium ion batteries (SIBs) through a one-step carbonization process using a novel Zn-ZIF as the precursor. In Zn@N-C-800, the "cocoon"-like disordered carbon skeleton is conducive to electrolyte infiltration, while the Zn/N doping can provide additional active sites for ion storage. Benefiting from these unique structural characteristics, Zn@N-C-800 achieves excellent electrochemical performances as anode for both LIBs and SIBs: an ultrahigh rate capability of 352 mAh g −1 can be delivered at 12.8 A g −1 for LIBs; an outstanding long-term cycling stability (312 mAh g −1 at 1 A g −1 after 2000 cycles) can be achieved for SIBs. This paper provides new ideas for the design and preparation of high-performance anodes for LIBs and SIBs.

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eScience · 2025 · IF 36.6

In situ fabrication of ether-in-gel electrolyte enables long-cycle Li–air batteries over a wide temperature range

Qingxu Zhang,Yaohui Huang,Honghao Hu,Chao Ma,Yifan Zhong,Pingli Wu,Wei Lv,Fujun Li,Xizheng Liu

Practical application of lithium–air batteries (LABs) is hindered by volatile liquid electrolytes, which compromise cycling stability at both high and low temperatures. Herein, we propose an in situ strategy for the fabrication of an ether-in-gel electrolyte to enhance their performance. LiN(CH 3 ) 2 (LDA), formed from metallic Li and N,N-dimethylformamide, binds with TEGDME (G4) to create an LDA(G4) 2 matrix that confines liquid G4 and traces of DMF, forming a gel electrolyte. The strong Li + -O/N interaction between LDA and G4 enables high superoxide solubility and high intrinsic thermal stability. LABs with the gel electrolyte exhibit over 1250 h stability (>50 days) in ambient air with high energy efficiency of over 70% and maintain stable cycles (540 h at 55 °C and 800 hours at −20 °C) without significant capacity decay. This work paves the way for design of new ether-in-gel electrolytes for high-energy batteries under all climate conditions.

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APPLIED SURFACE SCIENCE · 2025 · IF 6.9

Amorphous FePx nanoparticles embedded in N, P-codoped carbon nanofibers for high capacity and long cycle Li-ion batteries

Xuxu Wang,Wenbo Wang,Jinhui Li,Shuang Gao,Ping Nie,Fen Yao,Limin Chang

Transition metal phosphides (TMPs) are ideal anodes for lithium-ion batteries (LIBs) due to their high theoretical specific capacity and suitable lithiation potential. However, transition metal phosphides suffer from the shortcomings of large volume change and low electrical conductivity, resulting in poor rate performance and short cycle life. In this paper, nanofibers consisting of amorphous FeP x nanoparticles and N, P-codoped carbon substrate are synthesized by electrospinning and in-situ phosphidation to address these challenges. The amorphous structure with no grain boundary and isotropy can provide more Li + transport channels and Li + storage sites. Moreover, the N, P-codoped carbon substrate can effectively improve the electronic conductivity of the electrodes and the structural robustness of the nanofibers. Due to the unique structure and composition, the FeP x /C nanofibers exhibit excellent electrochemical performance when used as anodes for LIBs (stable cycling over 2200 cycles at 1 A g −1 ). It is suggested that the large pseudo-capacitance and fast Li + diffusion resulting from the amorphous structure are important reasons for the excellent electrochemical performance of FeP x /C nanofibers. This work provides a new idea to optimize the electrochemical performance of TMPs, which is expected to be used in other conversion anode materials.

CAS / MDL: 7705-08-0 83-86-3
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CHEMICAL ENGINEERING JOURNAL · 2025 · IF 13.2

A prelithiation pathway with high-release efficiency and self-enhanced interface chemistry to achieve stable Li-ion full cells

Jiabao Lai,Jiao You,Jianhui Zhu,Ming Yang,Yanyi Wang,Shengkui Zhong,Hongwei Mi,Chuanxin He,Dingtao Ma,Peixin Zhang

First-cycle irreversible lithium loss critically limits lithium-ion battery capacity. This study proposes the design of unique cathode prelithiation material, carbon sphere-composited lithium squarate (FSL-CS). Among them, the three-dimensional conductive network fabricated through chemical precipitation significantly enhances both electronic conductivity and structural stability. Electrochemical characterization reveals that FSL-CS delivers a compensation capacity of 390.8 mAh·g −1 during initial charging, achieving 92 % efficiency in lithium release, which have high-release efficiency. Compared to unmodified one, the composite demonstrates reduced kinetic barriers with a lowered delithiation plateau voltage of 3.97 V (vs. 4.16 V for pristine material). In situ/ex situ analyses confirm the carbon sphere composite strategy establishes self-enhanced interface chemistry. This optimizes interfacial charge transfer, boosting the Li + diffusion coefficient by an order of magnitude and continuously inducing in-situ formation of a gradient organic-inorganic composite cathode electrolyte interphase. Full-cell evaluations show that NCM811||Graphite batteries with 5 % FSL-CS maintain 87.3 % capacity retention after 400 cycles at 1C, while pouch cells retain 70.2 % capacity after 1000 cycles. Theoretical calculation reveals that FSL-CS exhibits a lower lithium migration energy barrier (0.65 eV) compared to conventional Li 2 NiO 2 (1.00 eV). This work provides new design principles for stable organic prelithiation systems featuring high-release efficiency, self-enhanced interfaces, and low-voltage operation.

CAS / MDL: 2892-51-5 554-13-2
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DESALINATION · 2025 · IF 9.8

Mussel-inspired surface engineering for LiMn1.9Cr0.1O4@carbon cloth electrodes for high-selectivity membrane capacitive Li-extraction from old brine

Xiaomeng Tan,Chengping Li,Guiying Tian,Minrui Wang,Lujie Zhang,Yifang Gao,Qixuan Ma,Yiming Xiao,Lei Zhang,Na Tang

Membrane capacitive Li-extraction technology (MCLiE) emerges as a highly promising technology for extracting lithium from saline brines, catering to the surging demand for lithium resources. In this study, a positively charged polymeric membrane consisting of dopamine-polyethyleneimine is adhered to the surface of LiMn 1.9 Cr 0.1 O 4 @carbon cloth (LMC@CC/DA-PEI) via surface engineering strategy, which is then employed as a flexible electrode for Li-extraction assembled in the membrane capacitive deionization (MCDI) system. Experimental results confirm that the old brine from West Taijinar with high Li content and low Mg/Li ratio is proper for practical Li-extraction, and the initial discharge/absorption capacities of LMC@CC/DA-PEI-0.5 electrode are 105.9 mAh·g −1 /27.4 mg·g −1 . Following 200 cycles, capacity retentions of bare LMC@CC and LMC@CC/DA-PEI-0.5 are 43.40 % (13.5 mg·g −1 ) and 59.77 % (16.4 mg·g −1 ), respectively. Therefore, surface incorporation of DA-PEI mitigates structural degradation of LMC and stabilizes long-cycle (de)lithiation of Mn-based electrodes. Moreover, the high Li + selectivity (α Li/Mg  = 156.7) is due to the spinel lattice of the LMC in combination with the electrostatic repulsion of the positively charged DA-PEI layer. Considering the strict environmental protection requirements and abundant new energy power supply in salt-lake areas, the assembled MCDI system with the DA-PEI-assisted LMC@CC electrode holds great potential for yielding enhanced Li + selectivity in the lithium recovery from old brine.

CAS / MDL: 1310-66-3
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Energy Storage Materials · 2025 · IF 20.2

Precise Ni/Co separation from spent Li-Ion batteries: Revealing the pivotal role of H2O in deep eutectic solvents

Xingyu Hu,Hui Shi,Yilei Zheng,Penghui Shao,Liming Yang,Xubiao Luo

The sustainable recovery of valuable metals from end-of-life lithium-ion batteries (LIBs) has become essential for relieving the supply-demand contradiction of key resources. However, the high similarity in physicochemical properties of transition metals poses a fundamental challenge for the selective recycling. Here we proposed a facile strategy for defining the demarcation line of precipitation/dissolution behavior for precise Ni/Co separation. A malonic acid-based deep eutectic solvent (DES) is developed, emphasizing the H 2 O-mediated competitive coordination and differentiated solubility. We discovered the distinctive formation of [Ni(H 2 O) 6 ] 2+ and [CoCl 4 ] 2- in the DES-20 % H 2 O system. Furthermore, the K sp differences of the Ni-complex and Co-complex in the C 3 H 2 O 4 2- -rich environment was effectively magnified. These significant differences synergistically enable the generation of C 3 H 2 NiO 4 ·2H 2 O precipitation (∼ 99.9 % purity), achieving a remarkable Ni/Co separation factor of 125, which guarantees sequential separation of all metals. This universal methodology along with in-depth mechanism understanding provides a guideline toward value-added recovery of LIBs.

CAS / MDL: 110-94-1 144-62-7
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Batteries-Basel · 2025 ·Vol. 11 ·期 9 ·334 · IF 4.8

In Situ Engineered Plastic–Crystal Interlayers Enable Li-Rich Cathodes in PVDF-HFP-Based All-Solid-State Polymer Batteries

Fei Zhou,Jinwei Tan,Feixiang Wang,Meiling Sun

All-solid-state lithium batteries (ASSLBs) employing Li-rich layered oxide (LLO) cathodes are regarded as promising next-generation energy storage systems owing to their outstanding energy density and intrinsic safety. Polymer-in-salt solid electrolytes (PISSEs) offer advantages such as high room-temperature ionic conductivity, enhanced Li anode interfacial compatibility, and low processing costs; however, their practical deployment is hindered by poor oxidative stability especially under high-voltage conditions. In this study, we report the rational design of a bilayer electrolyte architecture featuring an in situ solidified LiClO4-doped succinonitrile (LiClO4–SN) plastic–crystal interlayer between a Li1.2Mn0.6Ni0.2O2(LMNO) cathode and a poly (vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP)-based PISSE. This PISSE/SN–LiClO4configuration exhibits a wide electrochemical stability window up to 4.7 V vs. Li+/Li and delivers a high ionic conductivity of 5.68 × 10−4S cm−1at 25 °C. The solidified LiClO4-SN layer serves as an effective physical barrier, shielding the PVDF-HFP matrix from direct interfacial contact with LMNO and thereby suppressing its oxidative decomposition at elevated potentials. As a result, the bilayer polymer-based cells with the LMNO cathode demonstrate an initial discharge capacity of ∼206 mAh g−1at 0.05 C and exhibit good cycling stability with 85.7% capacity retention after 100 cycles at 0.5 C under a high cut-off voltage of 4.6 V. This work not only provides a promising strategy to enhance the compatibility of PVDF-HFP-based electrolytes with high-voltage cathodes through the facile in situ solidification of plastic interlayers but also promotes the application of LMNO cathode material in high-energy ASSLBs.

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ADVANCED MATERIALS · 2024 ·Vol. 36 ·期 25 ·2400656 · IF 27.4

The Potential Regulation of Working Anode for Long-Term Zero-Volt Storage at 37 °C in Li-Ion Batteries

Hanchen Wang,Yingtian Liu,Mingze Jiang,Yu-Xing Yao,Chunhua Hu,Chong Yan,Qiang Zhang,Luming Li

The advanced lithium-ion batteries that can tolerate zero-volt storage (ZVS) are in high demand for implantable medical devices and spacecraft. However, ZVS can raise the anode potential, leading to Cu current collector dissolution and solid-electrolyte interphase (SEI) degradation, especially at 37 °C. In this contribution, by quantitatively regulating the dosage of Li 6 CoO 4 cathode additives, controllable potential of the working anode under abusive-discharge conditions is demonstrated. The addition of Li 6 CoO 4 keeps zero-crossing potential (ZCP) and the potential of ZVS below 2.0 V (vs Li/Li + ) for LiCoO 2 |mesocarbon microbead cells at 37 °C. The capacity retention ratio (CRR) increases from 69.1% and 35.9% to 98.6% and 90.8% after 10 and 20 days of ZVS, respectively. The Cu dissolution and SEI degradation are effectively suppressed, while the over-lithiated cathode exhibits high reversible capacity after ZVS. The limiting conditions of long-term ZVS are further explored and a corresponding guide map is designed. When quantitatively regulating ZCP and the potential in ZVS, Cu dissolution, SEI degradation, and irreversible conversion of the cathode constitute the limiting conditions. This contribution designs the most reasonable potential range for ZVS protection at 37 °C, and realizes the best CRR record through precise potential regulation for the first time.

CAS / MDL: 1307-96-6 12057-24-8
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ADVANCED MATERIALS · 2024 ·Vol. 36 ·期 27 ·2403078 · IF 27.4

Super-Ionic Conductor Soft Filler Promotes Li+ Transport in Integrated Cathode–Electrolyte for Solid-State Battery at Room Temperature

Binbin Yang,Chenglong Deng,Nan Chen,Fengling Zhang,Kaikai Hu,Boshun Gui,Liyuan Zhao,Feng Wu,Renjie Chen

Composite polymer solid electrolytes (CPEs), possessing good rigid flexible, are expected to be used in solid-state lithium-metal batteries. The integration of fillers into polymer matrices emerges as a dominant strategy to improve Li + transport and form a Li + -conducting electrode–electrolyte interface. However, challenges arise as traditional fillers: 1) inorganic fillers, characterized by high interfacial energy, induce agglomeration; 2) organic fillers, with elevated crystallinity, impede intrinsic ionic conductivity, both severely hindering Li + migration. Here, a concept of super-ionic conductor soft filler, utilizing a Li + conductivity nanocellulose (Li-NC) as a model, is introduced which exhibits super-ionic conductivity. Li-NC anchors anions, and enhances Li + transport speed, and assists in the integration of cathode–electrolyte electrodes for room temperature solid-state batteries. The tough dual-channel Li + transport electrolyte (TDCT) with Li-NC and polyvinylidene fluoride (PVDF) demonstrates a high Li + transfer number (0.79) due to the synergistic coordination mechanism in Li + transport. Integrated electrodes’ design enables stable performance in LiNi 0.5 Co 0.2 Mn 0.3 O 2 |Li cells, with 720 cycles at 0.5 C, and 88.8% capacity retention. Furthermore, the lifespan of Li|TDCT|Li cells over 4000 h and Li-rich Li 1.2 Ni 0.13 Co 0.13 Mn 0.54 O 2 |Li cells exhibits excellent performance, proving the practical application potential of soft filler for high energy density solid-state lithium-metal batteries at room temperature.

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