SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Hongye Lv,Xuyong Tian,Haowei Feng,Chunlei Wang,Liying Wei,Xiuping Li,Haolong Xue,Changfa Xiao,Dawei Ji
In recent years, many researchers have focused on incorporating functional nanomaterials into thin-film composite (TFC) membranes to synthesize thin-film nanocomposite (TFNi) nanofiltration (NF) membranes with intermediate layers. The stability of the intermediate layer was very important for the TFNi NF membranes. This study constructed a unique structure of ZIF-8@CNTs-OH@PEI nanocomposite intermediate layers on the polysulfone (PSF) supporting membranes, where hydroxyl-functionalized carbon nanotubes (CNT-OH) captured 2-methylimidazole through its porous structure and hydrogen bonding with hydroxyl groups, enabling zeolitic imidazolate framework-8 (ZIF-8) to grow on CNT-OH. In addition, polyethylenimine (PEI) could act as the “adhesive” among ZIF-8 and CNT-OH due to the strong adhesion of hydrogen bonding with abundant –NH 2 groups. Thus, the nanocomposite particles could form a stable intermediate layer on the surface of PSF membrane. Furthermore, the positively charged PA/ZIF-8@CNTs-OH@PEI/PSF composite NF membranes with strong interlayer bonding were synthesized through further interfacial polymerization reactions on the intermediate layer. In particular, the synthesized nanocomposite suspension of ZIF-8@CNTs-OH@PEI address the particle aggregation and poor dispersibility. Moreover, the structure of intermediate layer features abundant voids, which can reduce the transmembrane resistance of water and enhance permeation performance. Compared to the PA/M−0 without the intermediate layer, the PA/M−30 exhibited a significantly improved flux of 70.6 L m -2 h −1 , that was 2.6 times higher compared to that for PA/M−0. Additionally, the optimized PA/ZIF-8@CNTs-OH@PEI/PSF composite NF membranes achieved Li + and Mg 2+ retention rates of −25.5 % and 95.2 %, respectively, with a Mg 2+ /Li + separation factor (SLi, Mg) equal to 29.9, which showed good long-term operational stability.
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高影响因子
ELECTROCHIMICA ACTA
·
2025
·
IF 5.6
Yaqin Ji,Wenjuan Yang,Jian Ma,Haoran Du,Xulai Yang,Zhenzhen Liu,Sheng Liang,Lingli Liu,Lei Hu,Xin Liang
It is a persistent goal for solid-state electrolytes to enhance their ionic conductivity while maintaining good mechanical strength to potentially inhibit lithium dendrites. In this work, we introduce garnet-type Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 (LLZTO) fillers and polyacrylonitrile (PAN) into thermoplastic polyurethane (TPU) to fabricate a composite solid-state electrolyte. The TPU matrix contains hard segments (−NH−COO−) that provide efficient mechanical support and soft segments (−O−) responsible for good flexibility and elasticity. When blended with PAN, hydrogen bonds form between the functional groups of PAN and TPU, establishing strong intermolecular connections that further enhance the structural/electrochemical stability of the electrolyte. A stable polymer/filler interface can be constructed through the ion-dipole coordination interaction between the metal ions at the LLZTO surface and the −CN groups of PAN. Benefiting from the intricate interactions among the PAN/TPU dual polymers and the LLZTO filler, the composite electrolyte exhibits not only exceptional flexibility (a tensile strain of 208%) and tensile strength (40 MPa), but also a good ionic conductivity of 2.33 × 10 −4 S cm⁻¹ at room temperature, a high oxidation potential of 4.48 V, and an excellent Li + transference number of 0.79. The Li||LiFePO 4 battery employing this composite solid-state electrolyte exhibits remarkable electrochemical stability, delivering an initial discharge capacity of 127.4 mAh g −1 at 0.3C and room temperature, and maintains a capacity retention of 91.9% after 600 cycles. This work provides a new electrolyte modification strategy for next-generation solid-state lithium metal batteries.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2025
·
IF 6.3
Xiang Li,Binbin Dan,Shixuan Li,Xiang Liu,Di Wang
The sluggish kinetics linked to CO 2 evolution reaction (CO 2 ER) processes, coupled with substantial electrode passivation, impose considerable constraints on the practical application of Li-CO 2 batteries. This study utilized ultrasound tech to enhance the synergistic modulation of defects and piezoelectric properties. By the concurrent creation of high-concentration oxygen vacancies (OVs) and the amplification of the inherent piezoelectric polarization field in BaTiO 3 material, the hysteresis of CO 2 ER processes and the occurrence of electrode passivation in Li-CO 2 batteries has been significantly improved. Further investigations reveal that high OV concentrations cause electronic structure reconstruction, leading to band gap contraction and Fermi energy level upshift, meanwhile, the augmented piezoelectric polarization field facilitates the directional migration of carriers, facilitating the growth of Li 2 CO 3 via the inherent electric field. Based on this synergistic mechanism, reversible decomposition of Li 2 CO 3 has been realized and Li-CO 2 cells with ultrasonic BTO cathode even exhibits a long cycle life of 375 cycles at the current density of 500 mA g −1 . This one-step physical field synergistic regulation of defect states in ferroelectric materials and their piezoelectric properties establishes a novel paradigm and mechanistic foundation for overcoming efficiency bottlenecks in piezoelectric catalytic systems and Li-CO 2 batteries.
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ACS Applied Energy Materials
·
2025
·
IF 5.5
Jiayin Li,Chenyu Wu,Yuxin Zheng,Wen Wen,Shuzhuo Bai,Qingqing Huang,Jintao Wu,Yalin Zhang,Chunyi Cai,Liyun Cao,Yijun Liu,Haibo Zhang,Hua Tan,Jianfeng Huang
Lithium carbon fluoride primary battery systems hold considerable promise for aerospace and deep-sea applications, yet they are limited by sluggish kinetics and low discharge plateaus. Incorporating high-conductivity materials such as carbon nanotubes is a key strategy to enhance charge migration; however, it is still difficult to use carbon nanotubes and other materials to catalyze the conversion reaction of CFx. Given this, the present work successfully fabricated a high-entropy alloy/carbon nanotube composite structure (CoCuFeZnNi/CNT) by loading a high-entropy alloy on the surface of carbon nanotubes and used it as a catalyst to effectively enhance the reaction kinetics of Li/CFx batteries. The CoCuFeZnNi/CNT catalyst exhibits a characteristic carbon nanotube structure with uniformly dispersed high-entropy alloy nanoparticles embedded within the tube walls. Its synergistic effect enhances the kinetic performance of the Li/CFx batteries. At 0.1 C, the specific capacity reaches 1113.6 mAh g–1, and the discharge voltage plateau is 2.455 V. Further analysis confirms that CoCuFeZnNi/CNT effectively accelerates the CFx conversion kinetics, facilitating rapid and uniform lithium fluoride nucleation and growth within the electrode structure. This provides a critical kinetic basis for maximizing the discharge capacity of CFx in a Li/CFx system. This research offers material solutions and theoretical support for the development of high-performance Li/CFx batteries.
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ADVANCED FUNCTIONAL MATERIALS
·
2025
·
IF 19
Jingbo Mu,Shimin Liao,Shengsheng Wang,Feng Xu,Bihai Su,Linlin Shi,Xiaojing Wang,Xuewei Hao,Zengcai Guo,Zhongkai Huang,Tian Tian
Achieving lithium-ion flux regulation in composite solid electrolytes (CSEs) remains a critical challenge for developing solid-state Li-metal batteries suppressing dendrite growth with high-voltage compatibility. Here, a new concept of Li⁺ transport gradient soft-rigid structure CSEs is introduced, which comprises a poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP) matrix integrated with acetate-functionalized cellulose nanocrystals (CNC-PVAc) and ZIF-8. This structure enables directed and fast Li⁺ conduction through low-tortuosity channels, significantly inhibiting lithium dendrite nucleation and growth. The electrochemical stability window of PHCF spans up to 4.82 V versus Li⁺/Li. Theoretical simulations reveal a synergistic intrinsic origin of the exceptional performance for this designed Li⁺ transport gradient soft-rigid structure CSEs. Consequently, the synthesized CSEs demonstrate high ionic conductivity (1.79 × 10 −4 S cm −1 ) and a notably high Li⁺ transference number (t Li⁺ ) of 0.79 at 60 °C. Corresponding all-solid-state LiFePO 4 ||Li and NCM811|| Li cells deliver impressive specific capacities of 163.78 (0.1C) and 190.67 mAh g −1 (0.5C) at 60 °C, respectively. This work presents a high-performance CSEs with intrinsic safety, providing valuable insights for novel design concept of solid-state batteries (SMBs).
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CHEMICAL ENGINEERING SCIENCE
·
2025
·
IF 4.3
Zhiyuan Yi,Kai Qu,Linlong Zhou,Qing Li,Zhi Xu
Metal-organic framework (MOF) glasses offer promising potential for membrane-based separations due to their excellent processability and structural versatility. However, their inherently disordered pore structures often lead to reduced porosity and limited ion transport performance. Here, we present a controlled unzipping polymer decomposition (CUPD) strategy for fabricating ZIF-62-based glass membrane featuring interconnected and negatively charged transport channels. Polystyrene sulfonic acid (PSS) is introduced as a sacrificial porogen during the melt-quenching process, wherein partial decomposition of its carbon backbone templates the formation of interconnected micropores. Simultaneously, the sulfonate groups stabilized by coordination with Zn sites, imparted negative surface charge to the channels, facilitating the selective ions transport. The optimized membrane fabricated by CUPD strategy achieves a Li + permeation rate of 0.64 mol m −2 h −1 , which is 60-fold higher than that of the pristine ZIF-62 glass membrane. This work provides a novel inspiration for constructing MOF-based membranes with interconnected channels with tunable property for advanced ion separation applications.
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ADVANCED MATERIALS
·
2024
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IF 27.4
Zhaofeng Zhuang,Junfeng Li,Haocheng Ji,Zhihong Piao,Xinru Wu,Guanjun Ji,Song Liu,Jun Ma,Di Tang,Nengzhan Zheng,Junxiong Wang,Guangmin Zhou
The direct recycling of cathode materials in lithium-ion batteries is important for environmental protection and resource conservation. The key regeneration processes are composition replenishment and atom rearrangement, both of which depend on the migration and diffusion of atoms. However, for the direct recycling of degraded LiNi 0.5 Co 0.2 Mn 0.3 O 2 (D-NCM523) cathode, the irreversible phase transitions that accumulate during the long-term cycles block the Li diffusion channels with a high diffusion energy barrier, making it difficult to fully repair the layered structure and resulting in rapid capacity decay. To address the challenge, fast Li replenishment channels are rebuilt to regulate the surface phase and effectively assist the regeneration process with a reduced energy barrier. This method reduces the amount of Li supplement by >75% and shortens the sintering time (only 2 h) to fully regenerate D-NCM523, compared to general direct recycling methods. The regenerated NCM523 (LCMB-NCM523) exhibits a satisfactory repaired specific capacity of 160 mAh g −1 and excellent cycling stability, retaining 78% of its capacity after 300 cycles. In addition, LCMB-NCM523 is recycled with improved thermal decomposition peak temperature and enables 200 cycles even at 60 °C, greatly improving safety. This work proposes a promising way for the large-scale direct regeneration of layered cathodes.
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Materials Today
·
2022
·
IF 26.943
Min Zhang,Kefan Zhou,Donghao Ma,Helin Wang,Xiaoyu Tang,Miao Bai,Fu Liu,Zhiqiao Wang,Yue Ma
The parasitic Li dendrite formation and retarded ion diffusion dynamics inhibit the deployment of solid-state batteries (SSBs) at high areal capacity loadings. Here, we present the modular design of the Li + percolating network by grafting the ionic-conductive polyether amine (PEA) at the multiple scales: the PEA modified zinc hydroxystannate (PEA@ZHS) (flame retardant units) and polyamide 6 (mechanical rigid units) are coherently introduced to optimize the PEO-based solid electrolyte (PX-PEA@ZHS) with the Young's modulus (3.41 GPa), ionic conductivity (4.29 × 10 −4 S cm −1 at 55 °C) and flame retardancy (22% reduction of heat release rate); on the other hand, PEA molecules are grafted onto the acetylene black additive to establish the dual conductive network, endowing two orders of magnitude increase of ionic conductivity for the high-compaction cathodes. The as-integrated symmetric cell exhibits a critical current density up to 0.8 mA cm −2 and cycling endurance for 1000 h at 0.2 mA cm −2 ; upon the SSBs assembly with the record high loading of LiFePO 4 (12.4 mg cm −2 ), the high-areal-capacity, cycling stability as well as the extreme temperature endurance till 110 °C are simultaneously realized, which inspire the rational design of commercially feasible, energy-dense, flame-resistance energy storage prototype.
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DOI
高影响因子
ADVANCED MATERIALS
·
2022
·Vol. 34
·期 40
·2201838
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IF 32.086
Guiru Sun,Rui Gao,Hailiang Jiao,Dan Luo,Yan Wang,Zexu Zhang,Wei Lu,Ming Feng,Zhongwei Chen
The major challenges for Li-O 2 batteries are sluggish reaction kinetics and large overpotentials due to the cathode passivation resulting from insulative and insoluble Li 2 O 2 . Here, a novel nanodot (ND)-modified electrolyte is designed by employing cobalt bis(trifluoromethylsulfonyl)imide (Co(TFSI) 2 ) as an electrolyte additive. The Co(TFSI) 2 additive can react with discharge intermediate LiO 2 and product Li 2 O 2 to form CoO NDs. The generated CoO NDs are well dispersed in electrolyte, which integrates both the high catalytic activity of solid catalyst and the good wettability of soluble catalyst. Under the catalytis of CoO NDs, Li 2 O 2 is produced and deposits on the cathode together with them. At the recharge process, these well dispersed CoO NDs help to decompose solid Li 2 O 2 at a lower overpotential. The Li-O 2 cells with Co(TFSI) 2 exhibit a long cycle life of 200 cycles at a current density of 200 mA g −1 under a cutoff capacity of 1000 mAh g −1 , as well as a superior reversibility associated with the Li 2 O 2 formation and decomposition. The study is expected to broaden the range of electrolyte additives and provide a new view to developing highly dispersed NDs-based catalysts for Li-O 2 batteries.
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高影响因子
Energy Storage Materials
·
2022
·
IF 20.831
Yiqiao Wang,Siyuan Pan,Yong Guo,Shichao Wu,Quan-Hong Yang
Li-O 2 batteries require catalysts to solve the problem of sluggish oxygen-related reaction kinetics. However, the solid catalysts and redox mediators are intrinsically deficient due to poor solid contacts and shuttle problems, respectively. Here, we report lithium phthalimide-N-oxyl (LiPINO) as a phase transfer catalyst (PTC) for promoting Li 2 O 2 formation and its reversible decomposition through the solution-phase reactions. The interaction between LiPINO and oxygen species in the electrolyte enables the high dissolution and stability of oxygen species, the fast charge transfer at liquid-solid interfaces and superior kinetics, and the suppressed side reactions. The efficient bidirectional catalytic activity and high stability of LiPINO capacitate batteries with a highly improved discharge capacity (11400 mAh g −1 ), a largely lowered charge potential (3.14 V) and an extended cycle life (more than 200 cycles) both in O 2 and air. Our understanding of the phase-transfer catalysis towards the Li-O 2 electrochemistry and the discovery of the PTC with superior activity and stability provide deep insights into the design of the most reliable catalysts for Li-O 2 batteries.
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高影响因子
Science Bulletin
·
2022
·
IF 20.577
Fangyuan Cheng,Xiaoyu Zhang,Peng Wei,Shixiong Sun,Yue Xu,Qing Li,Chun Fang,Jiantao Han,Yunhui Huang
The LiNi 0.8 Co 0.1 Mn 0.1 O 2 (Ni-rich NCM) cathode materials suffer from electrochemical performance degradation upon cycling due to detrimental cathode interface reactions and irreversible surface phase transition when operating at a high voltage (≥4.5 V). Herein, a traditional carbonate electrolyte with lithium difluoro(oxalato)borate (LiDFOB) and tris(trimethylsilyl)phosphate (TMSP) as dual additives that can preferentially oxidize and decompose to form a stable F, B and Si-rich cathode-electrolyte interphase (CEI) that effectively inhibits continual electrolyte decomposition, transition metal dissolves, surface phase transition and gas generation. In addition, TMSP also removes trace H 2 O/HF in the electrolyte to increase the electrolyte stability. Owing to the synergistic effect of LiDFOB and TMSP, the Li/LiNi 0.8 Co 0.1 Mn 0.1 O 2 half cells exhibit the capacity retention 76.3% after 500 cycles at a super high voltage of 4.7 V, the graphite/LiNi 0.8 Co 0.1 Mn 0.1 O 2 full cells exhibit high capacity retention of 82.8% after 500 cycles at 4.5 V, and Li/LiNi 0.8 Co 0.1 Mn 0.1 O 2 pouch cells exhibit high capacity retention 94% after 200 cycles at 4.5 V. This work is expected to provide an effective electrolyte optimizing strategy compatible with high energy density lithium-ion battery manufacturing systems.
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高影响因子
Energy Storage Materials
·
2025
·
IF 20.2
Ridong Hu,Chong Mao,Hao Zhuo,Xiaobing Dai,Lewen Yang,Xugang Shu,Yang Li,Zhanqiang Li,Wenhong Ruan,Fujie Yang,Xudong Chen
The precarious interfacial chemistry between the electrode and electrolyte is the determining step that restricts the long cycle life of Ni-rich-based Li-metal batteries. Here we show that the robust cathode electrolyte interphase (CEI) and solid electrolyte interphase (SEI) layers can be engineered by tuning the spatial linking structure of dipentacyclic anhydride (DPA) additives. Specifically, an inorganic-rich CEI/SEI layer induced by CBDA (a DPA featuring a quaternary ring spatial linking structure) exhibits superior Li + interfacial kinetics and an ultra-stable cycle performance, outperforming the other systems. As a result, the NCM811ǁLi cells containing CBDA show excellent long-term performances, even under high voltage, high load, and high charge-discharge current density, respectively. The coin-cell using a low-loading cathode exhibits 129 mAh g- 1 discharged capacity for over 200 cycles at a 6 C rate. Moreover, The high-loading cathode retains 80 % capacity after 312 cycles at 1.0 C. Furthermore, the NCM811ǁLi pouch cell demonstrated a capacity retention rate of 99.8 % after 50 cycles. Prolonged stable cycling for 900 cycles (93 % capacity retention) in an NCM811ǁGraphite pouch cell is enabled by CBDA. The DPA-based additives in this work offer a highly promising and feasible route to achieving a long-term and high-capacity lithium battery featuring a Ni-rich cathode.
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