Small Methods
·
2025
·
IF 9.1
Maoqiang Shen,Yang Liu,Xinyue Gao,Xuesen Liu,Yanhao Zhao,Linrui Hou,Changzhou Yuan
Typical shuttle effect of lithium polysulfides (LiPSs) and slow kinetics of redox reactions seriously hinder the potential application of lithium–sulfur batteries (LSBs). Herein, a titanium based ternary accordion heterostructure (i.e., TiC-TiN-TiO 2 ) is first fabricated through an acid-assisted eutectoid reaction of Ti 3 CN MXene obtained via efficiently gas-etching of Ti 3 AlCN MAX. The in situ crystal reconstruction not only creates functional sur/interface configuration but generates built-in electric field (BIEF) at the crystal interfaces, which induce interfacial charge redistribution and accelerate electronic/ionic conductions of the whole heterostructures. Besides, the well-defined functions of conductive TiC, adsorptive TiO 2 , and catalytic TiN enable the efficient fixation and conversion of LiPSs. Accordingly, LSBs assembled with the TiC-TiN-TiO 2 modified separators demonstrate a remarkable reversible capacity of 1185 mAh g −1 at 0.5 C, and an outstanding capacity retention of 778 mAh g −1 after 500 cycles with a decay rate of 0.078% per cycle. Moreover, excellent rate capability (838 mAh g −1 at 5 C) and superior cycling stability with high sulfur loading (3.7 mg cm −2 ) and low electrolyte/sulfur ratio (6.0 µL mg −1 ) are also achieved. More significantly, the eutectoid reaction of solid solution MXenes it devised here provides an innovative avenue to design functional hierarchical heterostructures for high-performance LSBs and beyond.
研究领域:
材料科学
·
能源存储
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DOI
PubMed
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2025
·
IF 2.5
Rong Li,ZhiHui Hao,Xiangwei Zhao,Huilin Zhou,Zhimin He,Qin Dong,Wei Hong,Xinglong Gou
Metal sulfides, such as SnS2, have been extensively studied as separator modifiers in lithium–sulfur batteries (LSBs) owing to their dual functionality in chemically anchoring lithium polysulfides (LiPSs) and catalytically facilitating redox reactions. Nevertheless, poor electrical conductivity and limited catalytic efficiency restrict their practical implementation for LiPS transformation kinetics. To address these issues, we prepared Mo-doped SnS2 (Mo–SnS2) nanosheets with sulfur vacancies through a rapid one-pot formamide-assisted method. The incorporation of Mo heteroatoms not only improves conductivity but also induces favorable sulfur vacancies, synergistically promoting both adsorption and electrocatalytic conversion of LiPSs. The Li–S cell with a Mo–SnS2 nanosheet-modified separator delivers a remarkable initial capacity of 1007.5 mAh g−1 at 1C, maintains 799.5 mAh g−1 after 600 cycles with a low fading ratio of 0.034% per cycle, and demonstrates a favorable rate performance of 591.9 mAh g−1 at 5C. This defect engineering strategy through heteroatom doping offers a promising approach to concurrently mitigate the polysulfide shuttle effect and enhance the reaction kinetics in sulfur-based energy storage systems.
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高影响因子
ACS Nano
·
2025
·
IF 16
Haohao Wang,Qinyu Qiao,Shuo Feng,Dong Cai,Peihang Li,Jinchen Jiang,Tao Yang,Huagui Nie,Jun Jiang,Shuo Yang,Zhi Yang
Catalysts are effective in mitigating slow sulfur redox reaction (SRR) kinetics in lithium–sulfur (Li–S) batteries. However, ideal battery performance has yet to be achieved under lean-electrolyte conditions due to the massive accumulation of lithium polysulfides in the electrolyte aggravating low ionic conductivity, increased electrolyte viscosity, and sluggish reaction kinetics. Inspired by the thrombolytic and microcirculation improvement functions of peptidyl nattokinase (NK) enzymes, herein, NK and its peptidyl mimicry enzyme (i.e., the serine (Ser)-histidine (His)-aspartate (Asp) triplet active center) are developed to boost lean-electrolyte SRR, featuring electronic axial stretching catalysis of Ser, strongly electronegative adsorption of Asp, and lithiophility of N-rich His synergistically catalyzing tandem sulfur conversions. After optimizing the catalyst formula by machine learning, the resultant Li–S batteries deliver impressive rate capacity (744 mAh g–1 at 5 C), durable cyclability at 0.5 C, and competitive areal capacity (8.87 mAh cm–2 under an electrolyte/sulfur ratio of 4 μL mg–1).
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高影响因子
ACS Nano
·
2025
·
IF 16
Chenzhi Ding,Yao Ding,Kao Wang,Zhaobo Zheng,Fang Liu,Xuyun Guo,Mohsen Tamtaji,Zhengtang Luo
Heterojunction engineering, serving as a key framework for building blocks between diverse functional materials, has emerged as a highly promising strategy to address the demand for efficient catalysts in lithium–sulfur (Li–S) batteries. However, achieving full matrix electronic control in the bulk phase is a bottleneck in regulating the electrochemical catalytic behavior of heterostructure catalysts. Herein, we report a “tube-in-tube” multifunctional catalyst that can strengthen the sulfur redox reaction (SRR) in Li–S batteries. Benefiting from a large-scale and oriented two-dimensional (2D) superlattice interface, the tailored heterostructure catalysts (MoSe2/MoS2@CNTs) show a “1 + 1 > 2” synergistic effect in lithium polysulfide (LiPSs) adsorption and catalytic conversion during SRR. In situ studies and theoretical results reveal that this 2D Moiré superlattice interface not only optimizes the adsorption of polysulfides but also moderates the overall electronic density of catalysts. Consequently, Li–S batteries assembled with MoSe2/MoS2@CNTs-PP as a modified separator deliver an outstanding discharge capacity of 1225 mAh g–1 at 0.2 C with a Ketjenblack/S cathode while maintaining a specific capacity of 870 mAh g–1 even at 5 C. Additionally, due to the inhibited “shuttle effect” by heterostructure catalysts, the modified separators exhibit a less capacity fading of 0.063% per cycle after 1000 cycles (1 C) even with a high sulfur loading (3.8 mg cm–2). This work focuses on designing an adsorption–catalysis synergistic interface within a full matrix of catalysts for Li–S chemistry and providing insights into the design of multifunctional catalysts for energy-storage systems based on the catalytic reaction, e.g., Zn–I2 and metal–air batteries, etc.
研究领域:
储能
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材料科学
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电化学
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纳米技术
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催化
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PubMed
高影响因子
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
·
2025
·Vol. 64
·期 27
·e202425601
·
IF 16.9
Yuemei Li,Shi-Yu Guo,Hongfei Gu,Bingyu Wang,Peiwu Su,Xiuming Zhang,Haoqing Zhang,Shuping Zhang,Fanzhi Yang,Jia Liu,Qing-An Chen,Jiatao Zhang
Visible light photoredox catalysis has become a rapidly emerging area owing to its potential of using sunlight to tame previously hard-to-harness radicals for organic synthesis. At present, such a blueprint faces a significant challenge, namely how to accomplish thermodynamically demanding reactions with sunlight encompassing a wide range of low-energy photons. Here, we report a new reaction framework to overcome this bottleneck through decoupling the thermodynamic limits of photoreduction from photoexcitation. This is fulfilled based on the construction of a heterogeneous photocatalyst Cu@CdS possessing in situ-formed surficial polysulfide species (including S 3 •− and S 4 2− ), which can efficiently harvest solar energy via plasmonic absorption of Cu while manifest sufficient redox potential for activating inert aryl bromides/chlorides enacted by excited polysulfides. We demonstrate that this designed material composes a potent photoredox catalyst for efficient aryl cross-coupling, borylation, hydrogenation, as well as Birch-type dearomatization reactions, with good recyclability and stability. In particular, when exclusively using natural sunlight as an energy source, the product yield can still reach up to 90%. Our findings introduce a straightforward yet viable way to progress toward the century-long dream of leveraging natural sunlight to produce structurally complex organic molecules, just like plants on Earth. Graphical Chemists have long aspired to construct complex organic compounds the way that plants do by harnessing natural sunlight as an energy source. This study presents an advancement toward this goal via synergistic exploitation of the plasmonic absorption of Cu and the unique redox potentials of excited polysulfide species (S 3 •− and S 4 2− ) on semiconductor surfaces to decouple the thermodynamic limits of photoreduction from photoexcitation.
研究领域:
光催化
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有机合成
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材料化学
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可再生能源
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物理化学
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DOI
PubMed
高影响因子
ACS Applied Polymer Materials
·
2024
·
IF 4.4
Yuanhao Shi,Dongxia Li,Xiangfeng Sun,Yuxin Xue,Zhiqi Li,Yulin Fu,Chongxian Luo,Qiong Lin,Xuefeng Gui,Kai Xu
Lithium–sulfur (Li–S) batteries, possessing substantial capacity, present a promising successor to current lithium-ion batteries, but the “shuttle effect” during cycling and deficient lithium-ion conductivity in Li–S batteries limit their practical applications. One potential remedy to these issues lies in the use of functional binders. In this study, building on the exceptional electrochemical stability of poly(vinylidene fluoride) (PVDF), we strategically grafted the cationic monomer 1-butyl-3-vinylimidazole with bis(trifluoromethanesulfonyl)imide (TFSI–) coordination from the chain of PVDF, thereby engineering the ionomer binder PVDF-g-(1-butyl-3-vinylimidazolium bis((trifluorompropyl)sulfonyl)imide) (BVIM). Density-functional theory (DFT) calculations affirmed that these cationic polymer branches, possessing a high binding energy with lithium polysulfides (LiPSs), are effective in trapping the LiPSs generated at the cathode. Moreover, while adsorbing LiPSs the TFSI– originally coordinated with the branched chain will be displaced, forming a dynamic small molecule pathway in the cathode that promotes lithium-ion conduction. As a result, Li–S batteries with BVIM binders deliver a persistent reversible capacity of 792.5 mAh g–1 over 250 cycles at a rate of 0.5C. Concurrently, at a high sulfur loading of 5.5 mg cm–2, a specific capacity of 3.3 mAh cm–2 was maintained after 50 cycles at 0.2C.
研究领域:
材料科学
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电化学
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DOI
高影响因子
ChemSusChem
·
2024
·
IF 7.5
Jiaqi Zhao,Zhanwei Xu,Yujiao Zhang,Jin QingZhu,Longhua Guo,Siyu Chen,Xuetao Shen,Jiayin Li,Zhi Li
The sluggish transition and shuttle of polysulfides (LiPS) significantly hinder the application and commercialization of Li-S batteries. Herein, carbon nanotubes (CNTs) supported 10 nm sized iron Hexadecafluorophthalocyanine (FePcF16/CNTs) are prepared using a solid synthesis approach. The well-exposed FePcF16 molecular improve the LiPS capture efficiency and redox kinetics by its central Fe-N4 units and F functional groups. The strong electron withdraw F groups significantly promote the conjugate effect and decrease the steric hindrance during mass migration procedure. Distribution of relaxation time (DRT) analysis shows that the Fe-N4 units exhibit strong affinity towards LiPS and the F groups further improve the Li+ diffusion rate in Li2S nucleation and oxidation procedure, accomplishing a porous surface on cathode. As a result, the FePcF16/CNTs separator exhibits a high initial capacity of 1136.2 mAh g-1 at 0.2 C, outstanding rate capacity of 624.9 mAh g-1 at 5 C and superior long-term stability at 2 C surviving 300 cycles with a low capacity decay of 0.43‰ per cycle.
研究领域:
材料科学
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电化学
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DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Shiwei Ge,Qian Zhao,Yaoyang Liu,Fangfang Wang,Guijuan Wei,Yu Liu,Bin Xu
Lithium–sulfur (Li–S) batteries are considered as promising energy storage systems due to the high energy density of 2600 W h kg–1. However, the practical application of Li–S batteries is hindered by the inadequate conductivity of sulfur and Li2S, as well as the shuttle effect caused by polysulfides during the charge–discharge process. Introducing a conductive interlayer between the cathode and the separator to physically resist polysulfides represents an effective and straightforward approach to mitigate the shuttle effect in Li–S batteries. In this paper, an ultrathin (<1 μm) 2D–2D MXene-LDH interlayer with high polysulfide adsorption ability was introduced to Li–S batteries. The synergistic effect between MXene and layered double hydroxide greatly improved the adsorption effect of the interlayers: the conductive Ti3C2Tx MXene chemically adsorbs polysulfides and promotes their fast transfer, and the NiCo-LDH alleviates the restack of MXene and facilitates Li+ diffusion. After inserting the MXene-LDH interlayer, the Li–S batteries exhibit an enhanced specific capacity of 1137.6 mA h g–1 at 0.1 C and retain 622.6 mA h g–1 after 100 cycles. The ultrathin 2D–2D interlayer offers a feasible way for the development of highly efficient and lightweight interlayers in Li–S batteries.
研究领域:
材料科学
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能源存储技术
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DOI
PubMed
高影响因子
ELECTROCHIMICA ACTA
·
2019
·
IF 5.383
Qifan Peng,Fan Yu,Weikun Wang,Anbang Wang,Feng Wang,Yaqin Huang
Lithium-sulfur (Li-S) battery has been regarded as one of the most promising next-generation energy storage systems, due to its high energy density and low cost. However, the dissolution of polysulfides to electrolyte and consequent “shuttle effect” still hinder the application of Li-S battery. Here, a polyethylenimine/fish-scale based porous carbon composite (PFPC) with abundant active sites and a relatively compact morphology is prepared by wet impregnation method. Modified separator with the PFPC coating significantly improves the rate capability and cycle stability of Li-S battery. The Li-S battery with the PFPC separator shows a reversible capacity of 638 mAh g −1 after stably cycling for 400 cycles at 1.0 C (1.0 C = 1675 mA g −1 ) with an ultralow capacity fading rate of 0.030% per cycle. The improved electrochemical performance of Li-S battery can be attributed to the synergistic effect of physical blocking and chemical adsorption of PFPC for polysulfides and the fast electron conduction between adsorbed polysulfides and conductive network. Moreover, the PFPC separator is ultralight with a mass loading of about 0.04 mg cm −2 . The good electrochemical performance, facile preparation method and light weight make the PFPC separator promising for the Li-S battery application.
研究领域:
材料科学
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电化学
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DOI
高影响因子
MACROMOLECULAR RAPID COMMUNICATIONS
·
2022
·Vol. 43
·期 19
·2200327
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IF 5.006
Zhuzuan Chen,Yuehai Peng,Zhuohong Yang,Yu Yang
Lithium–sulfur batteries (LSBs) represent a promising energy storage system due to the high theoretical energy density of the cathode; however, the high temperature and long-time drying required for electrode production result in high energy consumption and low efficiency. Ultraviolet (UV)-curing technology is an effective strategy to solve the abovementioned problems. However, carbon black and other conductive agents used in the production of the battery industry show strong absorption of UV light; thus, a single photoinitiator cannot absorb enough light intensity to realize initiation, limiting its application in the battery industry. In this work, the concept of full-band absorption is introduced into the manufacturing process of the LSB cathode to solve the abovementioned problems. The full-band absorption of photoinitiators in the UV band is successfully realized by combining the photoinitiators 2-benzyl-2-dimethylamino-1-(4-morpholinylphenyl)-1-butanone, 2-isopropyl thioxanthone, and bis (2,4,6-trimethyl benzoyl)-phenoxyphosphine. An ultraviolet in situ polymerized polyurethane acrylate (PUA) binder is successfully prepared by the combination of photoinitiators. PUA is used as the binder of LSBs and exhibits an excellent long-cycle performance of 1500 cycles with a low decay rate of 0.04% per cycle at 0.5 C. Thus, UV-curing technology provides a new prospect and possibility of industrialization for battery manufacturing.
研究领域:
材料科学
·
能源存储
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DOI
高影响因子
Journal of Materials Chemistry A
·
2019
·Vol. 7
·期 15
·9110-9119
·
IF 10.733
Xiao Xiang,Jing Yi Wu,Qing Xuan Shi,Qing Xia,Zhi Gang Xue,Xiao Lin Xie,Yun Sheng Ye
Nanostructured functional interlayers and separators have potential applications in high-performance lithium–sulfur (Li–S) batteries, due to their ability to suppress polysulfide (PS) shuttling. However, effective PS-trapping designs are usually accompanied by limited Li-ion diffusion, which becomes a key issue hindering practical application. Here, a nitrogen-functionalized 2D mesoporous silica nanoplate (FMSiNP) was used to construct a dense, lightweight (<0.2 mg cm−2) multi-functional interlayer using a simple casting approach, which effectively suppressed the PS shuttling, while facilitating Li+ diffusion. Being able to synergistically combine the merits of strong PS trapping with fast Li+ diffusion and excellent electrolyte wettability, Li–S batteries with FMSiNP coated-interlayers show improved PS utilization and retention. These batteries additionally show a superior cycling stability, capacity fading rate (0.038% per cycle at 1.0C over 1500 cycles), a high rate performance (discharge capacity of 574 mA h g−1 at 4.0C), low self-discharge behaviour and a high areal capacity (2.48 mA g cm−2 over 100 cycles), when using a pure sulfur/carbon black (CB) mixture as a cathode. This rational design for multi-functional interlayers provides a facile and effective strategy to create high energy density Li–S batteries for practical applications.
研究领域:
材料科学
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储能
·
纳米技术
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电化学
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电池技术
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Qing Xuan Shi,Hui Jie Pei,Na You,Jingyi Wu,Xiao Xiang,Qing Xia,Xiao Lin Xie,Shang Bin Jin,Yun Sheng Ye
The shuttling of polysulfides during discharging/charging processes is a major challenge that severely hinders the widespread use of lithium-sulfur batteries (LiSBs). Here, a group of scaled-up covalent triazine frameworks (CTFs) were explored under relatively mild reaction conditions to reduce reaction related interactions. Triazine shows good chemical compatibility with lithium polysulfide though its pyridinic and pyrrolic nitrogen groups, while hierarchical microporous structures interact physically as a blocking layer. Moreover, the dual chemical/physical functional CTFs act as an ionic sieves owing to their two-dimensional microporous structures that selectively sieve desired lithium ions, while effectively inhibiting soluble polysulfides reaching the lithium anode. As a result, the CTFs coated on commercial separator enhance battery performance, through improved active material utilization, high reversible specific capacity (1249 mA h g −1 at 0.5 C), an ideal rate performance of 802 mA h g −1 at 2 C, good cycling stability with a low capacity fade-rate of 0.052% per cycle over 800 cycles at 1 C, good anti-self-discharge behaviour and enhanced protection of the lithium anode.
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高影响因子
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