ChemSusChem
·
2025
·
IF 6.6
Xinfeng Ma,Yiming Zhang,Wanlin Yang,Chengda Liu,Xin Wang,Yongzhu Fu
Organosulfur molecules are considered as highly promising cathode materials for lithium batteries due to their high theoretical specific capacities. However, their practical application is hindered due to the issues of the dissolution and shuttling of the discharge products as well as the electron/ion insulation. In this study, we synthesize abundant sulfur-vacancies niobium sulfide encapsulated by nitrogen-doped coral-shaped carbon (NbSx@N-CC) by an arc discharge method, and interweave it with carbon nanotubes (CNTs) to form an ideal host material for diphenyl tetrasulfide (PTS) as cathode in rechargeable lithium batteries. The NbSx@N-CC catalyst can accelerate the cathodic reaction kinetics, adsorb lithium polysulfides (LiPSs) to mitigate the shuttle effect, thus significantly improving the cycling performance. At the 0.5 C rate, the battery exhibits an initial discharge capacity of 520.7 mAh g−1, with a diminutive cycle capacity decay rate of 0.067% per cycle over 500 cycles. Even under the condition of high PTS loading (6.0 mg cm−2) and low electrolyte (5 μL mg−1), the Li-PTS battery can still maintain a capacity retention rate of 97% after stably cycling 150 times at 0.2 C rate. This work demonstrates that defect engineering is one of the effective approaches to address the challenges of lithium-organosulfur batteries.
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高影响因子
Advanced Science
·
2025
·
IF 14.1
Lili Liu,Chen Wang,Luxin Zhao,Yayun Xiao,Weiwei Fang,Lanling Zhao,Faxing Wang,Yuping Wu
The practical development of Li-O 2 batteries (LOBs) urgently needs to explore robust cathode catalysts to boost the sluggish Li 2 O 2 reaction kinetics and parasitic reactions despite their theoretically high specific energy. Profound understanding of the cathode properties and the battery performance is rather critical in developing rational-designed electrocatalysts. In this study, a Co-N x /Co (111) decorated N-doped hierarchical carbon framework (Co-N x /Co@NHCF) is proposed as an efficient cathode in LOBs. Spectroscopic analysis coupled with experimental results suggests that the Co-N x /Co (111) catalytic center can significantly reduce the battery overpotential, and meanwhile, the hierarchical carbon framework ensures rapid mass transportation and provides sufficient space to accommodate Li 2 O 2 deposition. Density functional theory calculations reveal that the incorporated Co (111) facet can effectively regulate the electronic distribution of N-carbon, optimize the adsorption of desirable intermediates, and eventually facilitate oxygen reduction reaction/oxygen evolution reaction kinetics. As expected, the Co-N x /Co@NHCF catalyzed LOBs deliver a high discharge/charge capacity of 6.15/ 6.22 mAh cm −2 with a columbic efficiency of 98.9%, along with a high rate cycling of 700 h at 0.3 mA cm −2 . This work provides valuable instruction for the rational design of efficient catalysts for high-performance LOBs via optimization of the crystal structure and the adsorption of intermediates.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Kaixin Ren,Tevin Li,Yun Shen,Guodong Li,Jinyu Yang,Shouyi Yuan,Xiaoli Dong,Fei Wang,Congxiao Wang,Junwei Lucas Bao,Yongyao Xia
Stable cycling of 4.5 V LiNi 0.8 Co 0.1 Mn 0.1 O 2 (NCM811) based Li metal batteries is a great challenge as both electrodes work at the extreme voltage. Ethereal electrolytes have been demonstrated to exhibit better stability towards Li metal anode. Unfortunately, their limited electrochemical windows hinder their application in high-voltage Li metal batteries. Herein, we take 1,2-dimethoxyethane molecules as a starting point to design a series of non-fluorinated linear ethereal solvents via either extending the ethylene glycol (EG) units in the backbones or the terminal alkyl group. Further theoretical calculation suggests that with the extension of the EG unit in the backbone, the Li + solvation energy increases, leading to the formation of solvent-separated ion pairs, while the extension of the terminal alkyl chain results in an ion-pair solvation structure due to the steric effect. Consequently, 1,2-dibutoxyethane (EDB) is selected as the solvent for high-voltage Li metal batteries. The 4.5 V Li || NCM811 cells can stably operate over 600 cycles with EDB electrolyte. Notably 1 Ah-level Li || NCM811 pouch cell demonstrates a long cycle life over 100 times, even with a low negative-to-positive capacity ratio of 1.2 and an electrolyte-to-cathode capacity of 2.8 g Ah −1 .
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JOURNAL OF MEMBRANE SCIENCE
·
2025
·
IF 9
Mengling Fang,Zhigang Ning,Jiao Tang,Qinggang Huang,Muhammad Junaid,Yiming Qian,Xuanlin Li,Xin Huang,Haizhou Xue,Jinglai Duan,Jie Liu,Huijin Yao
The escalating demand for lithium-ion batteries necessitates efficient extraction technologies for lithium-rich brines, where the formidable challenge lies in selectively separating Li + from ubiquitous Mg 2+ ions due to their similar sizes. This work addresses this critical separation bottleneck by engineering a high-performance positively charged nanofiltration membrane. We leverage ion-track technology to fabricate a polyethylene terephthalate (PET) substrate featuring vertically aligned, uniformly distributed nanochannels and a hydrophilic, carboxyl-functionalized surface. This optimized substrate facilitates the controlled interfacial polymerization of polyethyleneimine (PEI) and 1,3,5-benzenetricarbonyl chloride (TMC), resulting in a defect-free, robust polyamide selective layer with strong interfacial adhesion. The resultant PEI-TMC/PET-5 membrane exhibits exceptional separation performance, achieving a remarkably high water permeance of 7.6 L m −2 h −1 bar −1 coupled with an outstanding Mg 2+ /Li + separation factor of 29.6. Comprehensive analysis reveals that this superior selectivity stems from the synergistic interplay of the Donnan effect and dielectric exclusion: the membrane's strong positive surface charge electrostatically repels divalent Mg 2+ more effectively than monovalent Li + , while the dielectric discontinuity at the membrane-solution interface imposes significantly higher Born solvation energy and image charge forces on Mg 2+ due to its greater charge density. Critically, the membrane demonstrates notable long-term stability, maintaining 94.5 % Mg 2+ rejection and a stable permeance of 5.1 L m −2 h −1 bar −1 over 720 h of continuous filtration. Under simulated brine conditions (Mg 2+ /Li + = 80:1, 2000 ppm), it further sustains stable performance over two weeks of operation, with a S Li / Mg of 28.8. This study presents a rational substrate-to-active-layer design strategy, underpinned by fundamental insights into ion transport mechanisms, paving the way for scalable and energy-efficient membrane technologies for sustainable lithium extraction from high-magnesium brines.
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DESALINATION
·
2025
·
IF 9.8
Ping Li,Yuan Zhou,Chunxi Hai,Ying Cheng,Yu Tang,Yanxia Sun,Shengde Dong,Luxiang Ma,Xin He,Qi Xu
Nanofiltration (NF) membranes prepared by traditional interface polymerization (IP) have garnered widespread attention for Mg 2+ /Li + separation. However, traditional NF membranes, like thin film composite polyamide (PA) membranes, show inadequate selectivity and permeance. The regulation of monomer diffusion plays a crucial role in adjusting the structure of nanofiltration membranes and improving their separation performance. In this study, we introduced the co-solvent N , N -dimethylformamide (DMF) into the aqueous phase to efficiently modulate the IP process of polyethyleneimine (PEI) and Trimesoyl chloride (TMC) without additional steps. The DMF-induced activation of the PA layer resulted in a more uniform pore structure across the layers, and the optimized membrane (CAIP (4)) had a pure water permeance of 13.10 ± 1.01 L/m 2 hbar, which was approximately three times that of conventional nanofiltration membranes. Molecular dynamics (MD) simulations indicated that the co-solvent DMF reduced the surface tension and accelerated the diffusion rate of PEI monomers, which diffused through the pores of the PA layer to leave more unreacted positively charged amine groups on the membrane surface. Consequently, the membrane achieved efficient separation of magnesium and lithium while maintaining good water permeance. The MgCl 2 removal was 95.09 % ± 1.65 %, and the Li + /Mg 2+ selectivity was 21.05. This study elucidates the mechanisms by which aqueous cosolvents influence IP reactions and offers novel strategies for modulating membrane structures and separation characteristics. These advancements are crucial for enhancing the efficiency of magnesium‑lithium separation processes.
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ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Huixian Xie,Liping Tan,Zhuo Yao,Jiaxiang Cui,Xiaokai Ding,Zuhao Zhang,Dong Luo,Zhan Lin
Li-rich Mn-based layered oxides are proposed to be candidates for high-energy Li-ion batteries. However, their large-scale production is still hampered by poor rate capability and severe voltage decay. It was mainly attributed to the irreversible oxygen loss, which induces transition metal ion migration, electrolyte consumption, and structural evolution. Herein, we propose an effective strategy of phosphorylation, in which the phosphate ion is induced to remove the surface labile oxygen. It urges the Li2MnO3 component to transform to the spinel-like structure and promotes the anionic redox process, thus facilitating lithium-ion diffusion and improving structural stability. As a result, the Li2MnO3 component is more prone to be activated, with the capacity increased by 18% in comparison with the pristine one. It also exhibits a superior capacity retention of 86.1% after 150 extended cycles and better rate performance delivering a capacity of 148.1 mA h g–1 even at 10 C. The effective phosphorylation opens a new way to tune anion redox chemistry and obtain structurally stable materials.
研究领域:
材料科学
·
电化学
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高影响因子
Nanomaterials
·
2022
·Vol. 12
·期 5
·886
·
IF 5.719
Qianwen Jin,Yajing Yan,Chenchen Hu,Yongguang Zhang,Xi Wang,Chunyong Liang
The advantages of high energy density and low cost make lithium–sulfur batteries one of the most promising candidates for next-generation energy storage systems. However, the electrical insulativity of sulfur and the serious shuttle effect of lithium polysulfides (LiPSs) still impedes its further development. In this regard, a uniform hollow mesoporous Ni(OH)2@CNT microsphere was developed to address these issues. The SEM images show the Ni(OH)2delivers an average size of about 5 μm, which is composed of nanosheets. The designed Ni(OH)2@CNT contains transition metal cations and interlayer anions, featuring the unique 3D spheroidal flower structure, decent porosity, and large surface area, which is highly conducive to conversion systems and electrochemical energy storage. As a result, the as-fabricated Li-S battery delivers the reversible capacity of 652 mAh g−1after 400 cycles, demonstrating excellent capacity retention with a low average capacity loss of only 0.081% per cycle at 1 C. This work has shown that the Ni(OH)2@CNT sulfur host prepared by hydrothermal embraces delivers strong physical absorption as well as chemical affinity.Keywords:Li-S battery;carbon nanotube;nickel hydroxide;cathode
研究领域:
材料科学
·
电化学
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高影响因子
JOURNAL OF POWER SOURCES
·
2022
·
IF 9.794
Zhidong Hou,Mingwei Jiang,Yunjing Cao,Huanyan Liu,Yu Zhang,Jian-Gan Wang
Developing high-capacity anode materials based on metal sulfides is of great importance for building advanced lithium-ion batteries (LIBs). Herein, we demonstrate rational encapsulation of cobalt sulfide (CoS x ) nanoparticles into multichannel carbon nanofibers (CoS x /MCF) with substantially improved Li + reactivity and durability. The unique multichannel and conductive carbon scaffold not only affords boosted electron/Li + transportation pathways for fast redox reaction with CoS x , but also stabilizes the electrode structure by buffering the volume change of CoS x . Impressively, the CoS x /MCF composite could serve as flexible anodes to deliver a high reversible capacity of 737 mAh g −1 at 0.2 A g −1 after 100 cycles, superior rate capacity of 374 mAh g −1 at 5 A g −1 , and excellent operating stability over 1000 cycles. Practical feasibility is also demonstrated by a full cell based on the high-capacity CoS x /MCF anode and Li[Ni 0.8 Co 0.1 Mn 0.1 ]O 2 cathode. The present study may provide insights for the facile synthesis of advanced anode materials for high-performance LIBs.
研究领域:
材料科学
·
能源存储
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Progress in Natural Science-Materials International
·
2018
·
IF 2.572
Datong Zhang,Zhengping Ding,Shuai Zhao,Ying Yang,Yiming Feng,Lei Xiao,Ran Ji,Libao Chen,Weifeng Wei
Li 2 MnSiO 4 -based cathode materials possess reasonable work potentials and high theoretical capacities, while the practical energy/power densities are constrained by their inferior kinetics of Li + diffusion. In this work, the Pmn2 1 -structure Li 2 Fe x Mn 1-x SiO 4 /C materials were synthesized via a solvothermal method and evaluated as Li-ion cathode materials, with notable morphological evolutions and tunable crystallographic habits observed after solvothermal process. The Li 2 Fe 0.33 Mn 0.67 SiO 4 /C material delivers an initial reversible capacity of 250.2 mAh g −1 at 0.1 C (~ 1.51 Li + insertion/extraction, 1 C = 166 mA g −1 ), excellent high-rate capability (52.2 mAh g −1 at 5 C), and good long-term cyclability (64.6% after 196 cycles at 2 C). The enhanced electrochemical properties are attributed to the boosted ion/electron transports induced by preferred morphological and structural characteristics of Li 2 Fe 0.33 Mn 0.67 SiO 4 /C.
研究领域:
材料科学
·
电化学
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高影响因子
CERAMICS INTERNATIONAL
·
2017
·
IF 2.986
Junhao Zhang,Tingting Yu,Jiale Chen,Huili Liu,Dongqin Su,Zehua Tang,Jinfeng Xie,Lei Chen,Aihua Yuan,Qinghong Kong
Germanium-based materials possess promising potential as novel anode materials for high performance lithium-ion batteries (LIBs). However, the considerably huge volume change causes rapid capacity fade during the charge-discharge process. A simple strategy was devised to prepare porous GeO 2 nanoparticles via thermal decomposition of (Hbipy) 2 [Ge(C 2 O 4 ) 3 ]·2H 2 O in air atmosphere. As an anode material for LIBs, it shows superior electrochemical performance in comparison with commercial GeO 2 microparticles . The initial discharge capacity of porous GeO 2 nanoparticles is high to 2578.8 mA h/g, and it still retained 581.9 mA h/g after 100 cycles. Even at 2 A/g, a reversible discharge capacity of 184.2 mA h/g is yet obtained. The superior lithium storage performances should be chalked up to the positive synergism of nanoscale, porous structure and low crystalline nature, which effectively retard the huge volume change of GeO 2 and are beneficial for fast diffusion of lithium ions during cycling.
研究领域:
材料科学
·
能源存储
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高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Zhuo Chen,Qiming Wang,Shuai Bai,Xi Wang,Wenlie Lin,Yining Zhang
Pseudocapacitive material can achieve rapid charge and discharge response. In this study, a vanadium-based conductive network hydrate (Na 0.13 Mg 0.02 )V 2 O 5 ·0.98H 2 O (NMVO) was designed. The Na + and Mg 2+ in NMVO are sandwiched between two layers of vacancy-ordered prisms and monoclinic nanonetwork V 3 O 7 (VO 2 :V 2 O 5 = 1:1) to form a conductive network with a layer spacing of up to 11.67 Å, this structure facilitates rapid interlayer diffusion of cations and enhanced conductivity. Reduction-NMVO (r-NMVO) with hierarchical heterostructures was prepared via an in-situ electrochemical process to generate interlayer vanadium-based active sites (LiV 3 O 8 , LiV 2 O 5 , Na 3 V 3 O 8 , MgVO 3 ) with multi-electron reaction, which enhanced the generation of surface redox pseudocapacitance. The interlayer heterostructure is integrated with the core of the precursor V 3 O 7 to form an active site-rich conductive network with strong pulse impact resistance, which promotes the generation of intercalated pseudocapacitance and increases the cycle stability of the electrode. This intercalation-surface redox pseudocapacitive mechanism was confirmed by first-principles, in-situ, and ex-situ characterization analysis. The r-NMVO|Li battery still maintains a capacity of 95.5 % after 65,500 cycles at a current density of 50 A g −1 . These results contribute directly to the realization of stable, fast charge and discharge material design.
研究领域:
材料科学
·
电化学
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高影响因子
Journal of Energy Chemistry
·
2020
·
IF 7.216
Jianwen Feng,Huan Yi,Zhiwen Lei,Jun Wang,Hongbo Zeng,Yonghong Deng,Chaoyang Wang
Poor cycling performance caused by the shuttle effect of polysulfides is the main obstacle in the development of advanced lithium–sulfur (Li–S) batteries. Functional polymer binders with polar groups can effectively adsorb polysulfides chemically, thereby suppressing the shuttle effect. Herein, a robust three-dimensional crosslinked polymer network, which demonstrates excellent mechanical property and strong affinity for polysulfides , is prepared by the aldimine condensation and coordination reactions. The crosslinked chitosan sulfate network (CCSN) significantly enhances the cycling performance and rate capability of the sulfur cathode. The CCSN-based sulfur cathode exhibits a high initial discharge capacity of 824 mAh g −1 with only 0.082% average capacity loss per cycle at 1 C. At a high rate of 4 C, the cathode exhibits a high capacity retention of 84.8% after 300 cycles. Moreover, the CCSN-based sulfur cathode exhibits an excellent cycling performance at a high sulfur loading of 2.5 mg cm −2 , which indicates the excellent mechanical strength and binding performance of the CCSN binder for high-energy density Li–S batteries. This study demonstrates a viable approach for developing high-performance Li–S batteries for practical application.
研究领域:
材料科学
·
电化学
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高影响因子
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