NEW CARBON MATERIALS
·
2026
·Vol. 41
·期 1
·109-125
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IF 7.2
Yuanxiao Ji,Weiye Zhang,Jiarui Xue,Jiyuan Zhang,Yunping Ge,Nan Zhu,Ruibin Jiang,Zhibin Lei,Zonghuai Liu,Jie Sun
Despite their high theoretical capacity and energy density, lithium-sulfur (Li–S) batteries still face challenges such as soluble lithium polysulfides (LiPSs) shuttling and sluggish redox kinetics. In this work, we used a novel MoS 2 -Mo 2 C heterostructure anchored on a carbon sponge (CS) as a Li 2 S host to solve these problems. A simple hydrothermal process following carbothermal reduction was used to construct the MoS 2 -Mo 2 C heterostructure, enabling control of the phases and integration of MoS 2 and Mo 2 C. Structural characterization confirmed the coherent interface of the heterostructure with a precise orientation relationship between the two phases and their uniform distribution. An evaluation of the adsorption and catalytic performance of the material showed that it has an exceptional LiPSs adsorption capacity with faster conversion from Li 2 S 4 to Li 2 S 2 . Density functional theory calculations further confirmed these results. As a result, the cathode had a high initial discharge capacity of 693 mAh g −1 at 0.2 C and achieved stable cycling at 2 C for 500 cycles with a low decay rate of 0.107% per cycle. The heterostructure design, coupled with the macroporous CS framework, effectively prevented the shuttling and increased sulfur utilization, offering a promising way to produce practical high-energy-density Li–S batteries. Download: Download high-res image (95KB) Download: Download full-size image
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Journal of Materials Chemistry A
·
2022
·Vol. 10
·期 36
·18907-18915
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IF 14.511
Xuefan Zheng,Yuqi Wu,Cheng Li,Jinxue Peng,Wu Yang,Zhongwei Lv,Haoyue Zhong,Zhengliang Gong,Yong Yang
All-solid-state lithium–sulfur batteries (ASSLSBs) are promising candidates for the development of next-generation batteries with high energy density and improved safety. Nevertheless, the sluggish reaction kinetics of the S and Li2S cathode and the low active material content hinder the further development of ASSLSBs. Herein, a Co3O4@nitrogen-doped carbon (Co3O4@NC) nanocomposite is used as an electronically conductive additive to promote the conversion kinetics of S and Li2S in the solid sulfur cathode. With a high sulfur content of 50 wt% and sulfur loading of 4 mg cm−2, ASSLSBs with the S–Co3O4@NC–Li7P3S11 (S–CoNC–LPS) composite cathode exhibit a high specific capacity of 1313 mA h g−1 at 0.2 mA cm−2, as well as a reversible capacity of 1167 mA h g−1 after 100 charge/discharge cycles. Furthermore, the S–CoNC–LPS cathode also demonstrates a high areal capacity of 16.12 mA h cm−2, corresponding to a reversible capacity of 1343 mA h g−1, and good cycling stability even with an ultra-high sulfur loading of 12 mg cm−2. Such a superior electrochemical performance can be attributed to the fact that Co3O4@NC lowers the reaction energy barrier and promotes the interconversion of S and Li2S.
研究领域:
材料科学
·
电化学
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TRANSACTIONS OF TIANJIN UNIVERSITY
·
2025
·
IF 8.5
Jia Ke,Zhang Yanan,Zuo Rui,Lu Hongbing,Ji Kemeng,Chen Mingming
The sluggish bidirectional conversion rate between Li 2 S n (2 ≤ n ≤ 4) and Li 2 S, coupled with the uncontrolled deposition of Li 2 S, significantly impedes the realization of high-performance lithium–sulfur batteries (LSBs). In this study, a metal–organic framework was employed as a precursor for the synthesis of a CoO x –CeO 2− y /C (0 < x < 3/2, 0 < y < 1/2) heterojunction via pyrolysis, which was subsequently introduced onto the cathode side of the polypropylene (PP) separator in LSBs. The modification of CoO x –CeO 2− y /C enhances the kinetics of converting of Li 2 S n to Li 2 S during the discharge process. The Tafel slope for the Li 2 S deposition reaction is reduced to 52.1 mV/dec, representing a 56.6% decrease compared to LSBs with bare PP separator. Conversely, during the charging process, the modification lowers the energy barrier for the Li 2 S decomposition reaction, with the activation energy reduced to 6.12 kJ/mol, indicating a 70.3% decrease relative to LSBs with PP separator only. Consequently, more Li 2 S is promoted to undergo decomposition. The CoO x –CeO 2− y /C heterojunction facilitates uniform deposition of Li 2 S, featuring fine particles and a uniform distribution, after brief potentiostatic charging for decomposition, thereby effectively mitigating the deactivation of sulfur species. Thanks to the enhanced bidirectional conversion of lithium polysulfides (LiPS) facilitated by the CoO x –CeO 2− y /C modification layer, the (−)Li|CoO x –CeO 2− y /C@PP|S(+) coin cell maintains a Coulombic efficiency of 90.4% after 500 cycles at a current density of 1 C, exhibiting a low capacity-decay rate of only 0.081% per cycle, thereby demonstrating excellent long-cycle stability.
研究领域:
材料科学
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电化学
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ADVANCED FUNCTIONAL MATERIALS
·
2024
·
IF 18.5
Yaqi Hu,Yanchen Liu,Yang Lu,Zongliang Zhang,Siliang Liu,Fangbo He,Yang Liu,Yongle Chen,Fangyang Liu
All-solid-state lithium metal batteries (ASSLBs) offer an alternative route to safe and high energy density power sources. Sulfur-based cathodes with high theoretical specific capacity and low cost are crucial for advancing ASSLBs. However, the electronic insulation and sluggish kinetics of sulfide materials like Li 2 S severely limit battery performance. Herein, the strategy is proposed that a highly electronic conductive Li 2 S-NbSe 2 material enhances the electrochemical performance through bidirectional self-activation. The chemical interaction between Li 2 S and NbSe 2 induces NbSe 2-x S x and Li 2 Se derivatization, serving as the basis for activation. The carrier transport properties, chemical evolution and self-activation mechanism of Li 2 S-NbSe 2 during the oxidation–reduction process are revealed. The chemical activation of NbSe 2-x S x is explored to accelerate the electrochemical processes by modifying the conductivity of sulfur species and the conversion pathways without insulating Li 2 S and S aggregation. Therefore, ASSLBs using Li 2 S-NbSe 2 as cathode active material achieve an electrode-level energy density of 394 Wh kg −1 and a power density of 524 W kg −1 at 1 C (4.35 mA cm −2 ) and 25 °C. The capacity retention after 100 cycles at 0.5 C is ≈99.3% with almost no degradation. This work provides new options and insights for the rational design and development of chalcogenide cathode active materials for high-performance ASSLBs.
研究领域:
材料科学
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电化学
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Energy Technology
·
2020
·Vol. 8
·期 6
·2000023
·
IF 3.404
Huize Jiang,Yu Han,Hui Wang,Yuhao Zhu,Qingpeng Guo,Haolong Jiang,Chunman Zheng,Kai Xie
Compared with traditional lithium–sulfur batteries, all-solid-state lithium–sulfur batteries assembled with inorganic solid electrolytes can not only effectively eliminate the shuttle effect but also drastically improve the safety performance. Due to the low ionic conductivity of the active materials, the construction of the interface between the active materials and the solid electrolytes in the composite cathode is crucial to the performance of the battery. Herein, Li 2 S– Li 3 PS 4 (LPS) composite materials are prepared by the in situ growth of solid electrolytes on the surface of the active material Li 2 S through the method of liquid-phase shaking. After heat treatment at 320 °C for 1 h, the 45Li 2 S–55LPS-320 exhibits a high ionic conductivity of 1.11 × 10 −4 S cm −1 , much higher than that of commercial Li 2 S. Without additional electrolytes, the Li 2 S–LPS composite mixed with a conductive agent is directly used as the cathode material. The composite cathode with high active material Li 2 S, whose content is up to 50%, delivers a discharge specific capacity of 674.3 mAh g −1 after 30 cycles at a current density of 0.2 mA cm −2 at 60 °C, with Coulombic efficiency being 100%.
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Materials Today Energy
·
2022
·
IF 9.257
Yun Zhao,Hualin Ye,Huanyu Zhang,Dan Zhao,Limin Huang,Jim Yang Lee
Li–S batteries assembled without a lithium metal anode can significantly increase the battery specific energy and obviate the safety issue of excess Li metal in the battery. In this study we found that a black phosphorous (BP) modified cooper foil current collector could provide a beneficial anode solid-electrolyte-interface (SEI) to enable the charging and discharging of Li-metal free Li 2 S-based batteries at higher C rates. The BP modification is effective in several aspects: the lithiophilicity of BP reduces the energy barrier in Li metal deposition and stripping during battery charge and discharge. The reactions between BP and lithium polysulfides also form Li 7 PS 6 in the anode SEI layer. Since Li 7 PS 6 has a high ionic conductivity for Li + diffusion, the Li plating/stripping efficiency is improved. The synergy of the lithiophilicity of BP and a Li 7 PS 6 -rich anode interphase layer was demonstrated in Li-metal free Li 2 S batteries, where the capacity retention over 100 cycles is 64.8% at the 0.2 C rate. The findings here show that current collector modifications should attend to multiple functionalities in order to be effective for the Li-metal free Li 2 S batteries.
研究领域:
材料科学
·
能源存储与转换
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EcoMat
·
2023
·Vol. 5
·期 4
·e12327
·
IF 14.6
Zhan Wu,Wenkui Zhang,Yang Xia,Hui Huang,Yongping Gan,Xinping He,Xinhui Xia,Jun Zhang
Sulfide solid state electrolyte (SSE) possesses high ionic conductivity and great processability but suffers from narrow electrochemical window. Conversion sulfide cathode FeS 2 has higher specific capacity and moderate redox potential, making it appropriate toward sulfide SSE. However, the complex reaction pathway and capacity fading mechanism in FeS 2 are rarely studied, especially in all-solid-state lithium battery (ASSLB). Herein, argyrodite sulfide SSE is paired with FeS 2 to investigate the electrochemical reaction pathways and the capacity fade mechanism. Instead of single conversion reaction, an anionic redox driven reaction of FeS 2 is revealed. The oxidization of Li 2 S vanishes and large quantity of inactive Li 2 S accumulates to cause the interfacial deterioration, along with the stress concentration during cycling, which leads to the rapid capacity fade of FeS 2 . Finally, a simple strategy of slurry-coated composite electrode with highly conductive network is proposed to direct the uniform deposition of Li 2 S and alleviate the stress concentration.
研究领域:
材料科学
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电化学
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电池技术
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高影响因子
ACS Applied Materials & Interfaces
·
2026
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IF 7.8
Yingli Zhang,Hailong Zhu,Huaiyang Zuo,Yaqi Hou,Shumin Zheng,Shiming Yang,Jing Wang,Bao Wang
As a potential high-safety and high-energy-density technology, lithium sulfide has been extensively studied as a cathode material for lithium–sulfur batteries under room temperature conditions. However, limited by its intrinsic characteristics of low electronic conductivity and high activation energy barrier, conventional Li2S cathodes struggle to overcome the activation energy barrier at low temperatures, resulting in scarce research on their application below zero. Specifically, studies on operation at −20 °C are nearly nonexistent. Herein, a synergistic strategy combining molybdenum carbide support adsorption and cobalt metal catalysis is proposed for low-temperature performance investigation. Via a lithiation reaction, Li2S@MoC–Co nanocomposites are fabricated by in situ synthesizing Li2S nanoparticles, introducing MoC as the support, and incorporating Co metal. When assembled into batteries with Li2S@MoC–Co as the cathode and metallic lithium as the anode, the activation energy barrier is reduced to 2.41 V at room temperature, exhibiting excellent electrochemical performance. A high initial discharge capacity of 1100 mAh g–1 is achieved at 0.1 C, and a discharge capacity of 430 mAh g–1 is retained after 200 cycles at 0.5 C. Even at −20 °C, Li2S is almost fully activated during the first charging cycle, delivering a discharge capacity of 360 mAh g–1 at 0.05 C. Moreover, a capacity retention rate of 92% is maintained after 300 cycles at 0.5 C. This work realizes high output and high-capacity retention of Li2S at −20 °C, providing a new paradigm for the development of low-temperature Li2S-based batteries.
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PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Guo Wen Sun,Meng Jing Jin,Qian Yu Liu,Chao Yue Zhang,Jiang Long Pan,Yan Chun Wang,Xiu Ping Gao,Geng Zhi Sun,Xiao Jun Pan,Jin Yuan Zhou
Electric field from ferroelectric materials was often applied to energy-storage devices to enhance their electrochemical reaction kinetics via the electrostatic interaction. However, traditional ferroelectric materials are difficult to be used commercially for their insulation. Herein, we elucidate a novel strategy to introduce the electrostatic interaction by polarizing the polyvinylidene fluoride (PVDF) binder used in the C/S cathodes for lithium-sulfur batteries. In particular, we show both experimentally and theoretically how an external electric field from β -phase PVDF induces unprecedented performance and stabilities. Density functional theory calculation results indicate that the polarized topological β -phase PVDF possesses not only an strong built-in electric field and an improved conductance that benefits both the deposition of LiPSs and the transport of Li + ions, but also an enhanced adsorption capability to polysulfide ions. As a result, the specific capacity was improved by over 60 %, the rate capability (from 0.1 to 2.0 C) was enhanced by 138 %, and the capacity decay rate (1000 cycles at 1.0 C) largely decreases from 0.059 % to 0.038 % per cycle. Besides, the enhancement mechanism of Li 2 S deposition by electrostatic interaction has also been explored. This research would provide some new insight into the ferroelectric enhanced design of high-performance energy-storage devices.
研究领域:
材料科学
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电化学
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高影响因子
Nanoscale
·
2023
·Vol. 15
·期 37
·15318-15327
·
IF 6.7
Bo Zhou,Ting Li,Anjun Hu,Baihai Li,Runjing Li,Chuan Zhao,Nian Chen,Miao He,Jing Liu,Jianping Long
Minimizing the amount of metallic lithium (Li) to zero excess to achieve an anode-free configuration can help achieve safer, higher energy density, and more economical Li metal batteries. Nevertheless, removal of excess Li creates challenges for long-term cycling performance in Li metal batteries due to the lithiophobic copper foils as anodic current collectors. Here, we improve the long-term cycling performance of anode-free Li metal batteries by modifying the anode-free configuration. Specifically, a lithiophilic Au nanoparticle-anchored reduced graphene oxide (Au/rGO) film is used as an anodic modifier to reduce the Li nucleation overpotential and inhibit dendrite growth by forming a lithiophilic LixAu alloy and solid solution, which is convincingly evidenced by density functional theory calculations and experimentally. Meanwhile, the flexible rGO film can also act as a buffer layer to endure the volume expansion during repeated Li plating/stripping processes. In addition, the Au/rGO film promotes a homogeneous distribution of the electric field over the entire anodic surface, thus ensuring a uniform deposition of Li during the electrodeposition process, which is convincingly evidenced by finite element simulations. As expected, the Li||Au/rGO-Li half-cell shows a highly stable long-term cycling performance for at least 500 cycles at 0.5 mA cm−2 and 0.5 mA h cm−2. A Li2S-based anode-free full cell allows achieving a stable operation life of up to 200 cycles with a capacity retention of 63.3%. This work provides a simple and scalable fabrication method to achieve anode-free Li2S-based cells with high anodic interface stability and a long lifetime.
研究领域:
材料科学
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电化学
·
纳米技术
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DOI
PubMed
高影响因子
JOURNAL OF POWER SOURCES
·
2023
·
IF 9.2
Hongjiao Wang,Wenzhi Li,Lilin Wu,Bai Xue,Fang Wang,Zhongkuan Luo,Xianghua Zhang,Ping Fan,Laurent Calvez,Bo Fan
The solid/liquid Li-S battery shows promise in solving both the polysulfide “shuttle effect” in liquid batteries and the interfacial contact in all-solid-state batteries. However, increasing the interfacial stability of the electrolyte and the solid electrolyte remains a challenge in the solid/liquid batteries. In this work, a high ionic conductivity Li 3 PS 4 solution is synthesized using a nano-Li 2 S precursor, which is then utilized to form a solid electrolyte Li 3 PS 4 @Li 7 P 3 S 11 via dip-coating. The Li 3 PS 4 @Li 7 P 3 S 11 can form a dense protective interface Li 3 PS 4 -DME with the DOL/DME and DME electrolyte. This interface can prevent direct contact between the solid electrolyte and the electrolytes, efficiently inhibiting further solid electrolyte decomposition. The lithium symmetric battery with the solid electrolyte Li 3 PS 4 @Li 7 P 3 S 11 is cycled stably for 1000 h, at a current density of 0.38 mA cm −2 and a capacity of 1.51 mA h cm −2 . The Li-S battery with the solid electrolyte Li 3 PS 4 @Li 7 P 3 S 11 can cycle stably for 300 cycles at 0.2C with a capacity of 600 mA h g −1 remaining.
研究领域:
材料科学
·
电化学
·
能量存储
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高影响因子
Energy Storage Materials
·
2021
·
IF 17.789
Zhendong Li,Liyuan Huai,Shun Li,Mingming Ma,Kailin Luo,Yang Zhao,Deyu Wang,Xueliang Sun,Zhe Peng
Cycling lithium (Li) metal anode with a low negative/positive capacity (N/P) ratio is critical to build high-energy-density Li metal batteries (LMBs). Many strategies focusing on interfacial protection are limited to shallow conditions using excessive Li with a high negative/positive capacity (N/P) ratio > 50. Herein, we demonstrate a deeply enhanced charge transfer kinetic by a rational incorporation of nickel (Ni) seeds in the Li anodes with a tailored interfacial chemistry. The Ni seeds in the bulk Li anode not only act as well-dispersed nucleation sites to enable Ni-seeded growth of granular Li deposits, but also adsorb acetonitrile (AN) molecules when the Ni-seeded Li anodes are paired with an AN-based electrolyte using lithium bis-(fluorosulfonyl)imide as salt, forming a fast Li + conducting interphase with co-produced LiF, Li 3 N and Li 2 S components. These benefits conduct an exchange current density ~ 20 times higher than that of the bare Li in conventional carbonate electrolytes. Stable cycling of LMBs with a practical cathode loading (~ 5 mAh cm −2 ) and a low N/P capacity ratio of 2 is also demonstrated, showing the prominence of this remedy for developing high-energy-density LMBs.
研究领域:
材料科学
·
电化学
·
能源存储
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高影响因子
危险品化学品经营许可证（带存储）