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Energy Storage: A Dual‐Function Na2SO4 Template Directed Formation of Cathode Materials with a High Content of Sulfur Nanodots for Lithium–Sulfur Batteries (Small 27/2017)
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Chong Luo Wei Lv Yaqian Deng Guangmin Zhou Zheng‐Ze Pan Shuzhang Niu Baohua Li Feiyu Kang Quan‐Hong Yang 《Small (Weinheim an der Bergstrasse, Germany)》2017,13(27)
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Long‐Life Lithium–Sulfur Batteries with a Bifunctional Cathode Substrate Configured with Boron Carbide Nanowires
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Liu Luo Sheng‐Heng Chung Hooman Yaghoobnejad Asl Arumugam Manthiram 《Advanced materials (Deerfield Beach, Fla.)》2018,30(39)
Developing high‐energy‐density lithium–sulfur (Li–S) batteries relies on the design of electrode substrates that can host a high sulfur loading and still attain high electrochemical utilization. Herein, a new bifunctional cathode substrate configured with boron‐carbide nanowires in situ grown on carbon nanofibers (B4C@CNF) is established through a facile catalyst‐assisted process. The B4C nanowires acting as chemical‐anchoring centers provide strong polysulfide adsorptivity, as validated by experimental data and first‐principle calculations. Meanwhile, the catalytic effect of B4C also accelerates the redox kinetics of polysulfide conversion, contributing to enhanced rate capability. As a result, a remarkable capacity retention of 80% after 500 cycles as well as stable cyclability at 4C rate is accomplished with the cells employing B4C@CNF as a cathode substrate for sulfur. Moreover, the B4C@CNF substrate enables the cathode to achieve both high sulfur content (70 wt%) and sulfur loading (10.3 mg cm?2), delivering a superb areal capacity of 9 mAh cm?2. Additionally, Li–S pouch cells fabricated with the B4C@CNF substrate are able to host a high sulfur mass of 200 mg per cathode and deliver a high discharge capacity of 125 mAh after 50 cycles. 相似文献
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Yolk–Shelled C@Fe3O4 Nanoboxes as Efficient Sulfur Hosts for High‐Performance Lithium–Sulfur Batteries
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Jiarui He Liu Luo Yuanfu Chen Arumugam Manthiram 《Advanced materials (Deerfield Beach, Fla.)》2017,29(34)
Owing to the high theoretical specific capacity (1675 mA h g?1) and low cost, lithium–sulfur (Li–S) batteries offer advantages for next‐generation energy storage. However, the polysulfide dissolution and low electronic conductivity of sulfur cathodes limit the practical application of Li–S batteries. To address such issues, well‐designed yolk–shelled carbon@Fe3O4 (YSC@Fe3O4) nanoboxes as highly efficient sulfur hosts for Li–S batteries are reported here. With both physical entrapment by carbon shells and strong chemical interaction with Fe3O4 cores, this unique architecture immobilizes the active material and inhibits diffusion of the polysulfide intermediates. Moreover, due to their high conductivity, the carbon shells and the polar Fe3O4 cores facilitate fast electron/ion transport and promote continuous reactivation of the active material during the charge/discharge process, resulting in improved electrochemical utilization and reversibility. With these merits, the S/YSC@Fe3O4 cathodes support high sulfur content (80 wt%) and loading (5.5 mg cm?2) and deliver high specific capacity, excellent rate capacity, and long cycling stability. This work provides a new perspective to design a carbon/metal‐oxide‐based yolk–shelled framework as a high sulfur‐loading host for advanced Li–S batteries with superior electrochemical properties. 相似文献
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Kezhong Lv Pengfei Wang Chao Wang Zihan Shen Zhenda Lu Huigang Zhang Mingbo Zheng Ping He Haoshen Zhou 《Small (Weinheim an der Bergstrasse, Germany)》2020,16(22)
Lithium–sulfur batteries, as one of promising next‐generation energy storage devices, hold great potential to meet the demands of electric vehicles and grids due to their high specific energy. However, the sluggish kinetics and the inevitable “shuttle effect” severely limit the practical application of this technology. Recently, design of composite cathode with effective catalysts has been reported as an essential way to overcome these issues. In this work, oxygen‐deficient ferric oxide (Fe2O3?x), prepared by lithiothermic reduction, is used as a low‐cost and effective cathodic catalyst. By introducing a small amount of Fe2O3?x into the cathode, the battery can deliver a high capacity of 512 mAh g?1 over 500 cycles at 4 C, with a capacity fade rate of 0.049% per cycle. In addition, a self‐supporting porous S@KB/Fe2O3?x cathode with a high sulfur loading of 12.73 mg cm?2 is prepared by freeze‐drying, which can achieve a high areal capacity of 12.24 mAh cm?2 at 0.05 C. Both the calculative and experimental results demonstrate that the Fe2O3?x has a strong adsorption toward soluble polysulfides and can accelerate their subsequent conversion to insoluble products. As a result, this work provides a low‐cost and effective catalyst candidate for the practical application of lithium–sulfur batteries. 相似文献
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Atomic Interlamellar Ion Path in High Sulfur Content Lithium‐Montmorillonite Host Enables High‐Rate and Stable Lithium–Sulfur Battery
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Wei Chen Tianyu Lei Weiqiang Lv Yin Hu Yichao Yan Yu Jiao Weidong He Zhenghan Li Chenglin Yan Jie Xiong 《Advanced materials (Deerfield Beach, Fla.)》2018,30(40)
Fast lithium ion transport with a high current density is critical for thick sulfur cathodes, stemming mainly from the difficulties in creating effective lithium ion pathways in high sulfur content electrodes. To develop a high‐rate cathode for lithium–sulfur (Li–S) batteries, extenuation of the lithium ion diffusion barrier in thick electrodes is potentially straightforward. Here, a phyllosilicate material with a large interlamellar distance is demonstrated in high‐rate cathodes as high sulfur loading. The interlayer space (≈1.396 nm) incorporated into a low lithium ion diffusion barrier (0.155 eV) significantly facilitates lithium ion diffusion within the entire sulfur cathode, and gives rise to remarkable nearly sulfur loading‐independent cell performances. When combined with 80% sulfur contents, the electrodes achieve a high capacity of 865 mAh g?1 at 1 mA cm?2 and a retention of 345 mAh g?1 at a high discharging/charging rate of 15 mA cm?2, with a sulfur loading up to 4 mg. This strategy represents a major advance in high‐rate Li–S batteries via the construction of fast ions transfer paths toward real‐life applications, and contributes to the research community for the fundamental mechanism study of loading‐independent electrode systems. 相似文献
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Chen‐Yu Chen Hong‐Jie Peng Ting‐Zheng Hou Pei‐Yan Zhai Bo‐Quan Li Cheng Tang Wancheng Zhu Jia‐Qi Huang Qiang Zhang 《Advanced materials (Deerfield Beach, Fla.)》2017,29(23)
The reversible formation of chemical bonds has potential for tuning multi‐electron redox reactions in emerging energy‐storage applications, such as lithium?sulfur batteries. The dissolution of polysulfide intermediates, however, results in severe shuttle effect and sluggish electrochemical kinetics. In this study, quinonoid imine is proposed to anchor polysulfides and to facilitate the formation of Li2S2/Li2S through the reversible chemical transition between protonated state (? NH+ ?) and deprotonated state (? N?). When serving as the sulfur host, the quinonoid imine‐doped graphene affords a very tiny shuttle current of 2.60 × 10?4 mA cm?2, a rapid redox reaction of polysulfide, and therefore improved sulfur utilization and enhanced rate performance. A high areal specific capacity of 3.72 mAh cm?2 is achieved at 5.50 mA cm?2 on the quinonoid imine‐doped graphene based electrode with a high sulfur loading of 3.3 mg cm?2. This strategy sheds a new light on the organic redox mediators for reversible modulation of electrochemical reactions. 相似文献
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A Flexible Nanostructured Paper of a Reduced Graphene Oxide–Sulfur Composite for High‐Performance Lithium–Sulfur Batteries with Unconventional Configurations
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Jun Cao Chen Chen Qing Zhao Ning Zhang Qiongqiong Lu Xinyu Wang Zhiqiang Niu Jun Chen 《Advanced materials (Deerfield Beach, Fla.)》2016,28(43):9629-9636
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Design Principles for Heteroatom‐Doped Nanocarbon to Achieve Strong Anchoring of Polysulfides for Lithium–Sulfur Batteries
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Ting‐Zheng Hou Xiang Chen Hong‐Jie Peng Jia‐Qi Huang Bo‐Quan Li Qiang Zhang Bo Li 《Small (Weinheim an der Bergstrasse, Germany)》2016,12(24):3283-3291
Lithium–sulfur (Li–S) batteries have been intensively concerned to fulfill the urgent demands of high capacity energy storage. One of the major unsolved issues is the complex diffusion of lithium polysulfide intermediates, which in combination with the subsequent paradox reactions is known as the shuttle effect. Nanocarbon with homogeneous nonpolar surface served as scaffolding materials in sulfur cathode basically cannot afford a sufficient binding and confining effect to maintain lithium polysulfides within the cathode. Herein, a systematical density functional theory calculation of various heteroatoms‐doped nanocarbon materials is conducted to elaborate the mechanism and guide the future screening and rational design of Li–S cathode for better performance. It is proved that the chemical modification using N or O dopant significantly enhances the interaction between the carbon hosts and the polysulfide guests via dipole–dipole electrostatic interaction and thereby effectively prevents shuttle of polysulfides, allowing high capacity and high coulombic efficiency. By contrast, the introduction of B, F, S, P, and Cl monodopants into carbon matrix is unsatisfactory. To achieve the strong‐couple effect toward Li2Sx, the principles for rational design of doped carbon scaffolds in Li–S batteries to achieve a strong electrostatic dipole–dipole interaction are proposed. An implicit volcano plot is obtained to describe the dependence of binding energies on electronegativity of dopants. Moreover, the codoping strategy is predicted to achieve even stronger interfacial interaction to trap lithium polysulfides. 相似文献
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Yanfang Zhu Shun Wang Zongcheng Miao Yong Liu Shu‐Lei Chou 《Small (Weinheim an der Bergstrasse, Germany)》2018,14(40)
Lithium–sulfur (Li–S) batteries are considered as promising candidates for energy storage systems owing to their high theoretical capacity and high energy density. The application of Li–S batteries is hindered by several obstacles, however, including the shuttle effect, poor electrical conductivity, and the severe volume expansion of sulfur. The traditional method is to integrate sulfur with carbon materials. But the interaction between polysulfide intermediates and carbon is only weak physical adsorption, which easily leads to the escape of species from the framework (shuttle effect) of the material causing capacity loss. Recently, however, there has been a trend for the introduction of novel non‐carbon materials as sulfur hosts based on the strong chemisorption. This review highlights recent research progress on novel non‐carbon sulfur hosts based on strong chemisorption, in Li–S batteries. In comparison with carbon‐based sulfur hosts, most non‐carbon sulfur hosts have been demonstrated to be polar host materials that could efficiently adsorb polysulfide via strong chemisorption, mitigating their dissolution. The intrinsic mechanism associated with the role of non‐carbon‐based host materials in improving the performance of Li–S batteries is discussed. 相似文献
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Li‐Ping Lv Chao‐Fei Guo Weiwei Sun Yong Wang 《Small (Weinheim an der Bergstrasse, Germany)》2019,15(3)
In this work, hydroxyl‐functionalized Mo2C‐based MXene nanosheets are synthesized by facilely removing the Sn layer of Mo2SnC. The hydroxyl‐functionalized surface of Mo2C suppresses the shuttle effect of lithium polysulfides (LiPSs) through strong interaction between Mo atoms on the MXenes surface and LiPSs. Carbon nanotubes (CNTs) are further introduced into Mo2C phase to enlarge the specific surface area of the composite, improve its electronic conductivity, and alleviate the volume change during discharging/charging. The strong surface‐bound sulfur in the hierarchical Mo2C‐CNTs host can lead to a superior electrochemical performance in lithium–sulfur batteries. A large reversible capacity of ≈925 mAh g ? 1 is observed after 250 cycles at a current density of 0.1 C (1 C = 1675 mAh g?1) with good rate capability. Notably, the electrodes with high loading amounts of sulfur can also deliver good electrochemical performances, i.e., initial reversible capacities of ≈1314 mAh g?1 (2.4 mAh cm?2), ≈1068 mAh g?1 (3.7 mAh cm?2), and ≈959 mAh g?1 (5.3 mAh cm?2) at various areal loading amounts of sulfur (1.8, 3.5, and 5.6 mg cm?2) are also observed, respectively. 相似文献
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A Praline‐Like Flexible Interlayer with Highly Mounted Polysulfide Anchors for Lithium–Sulfur Batteries
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Teng Zhao Yusheng Ye Cheng‐Yen Lao Giorgio Divitini Paul R. Coxon Xiaoyu Peng Xiong He Hyun‐Kyung Kim Kai Xi Caterina Ducati Renjie Chen Yingjun Liu Seeram Ramakrishna Ramachandran Vasant Kumar 《Small (Weinheim an der Bergstrasse, Germany)》2017,13(40)
The development of lithium–sulfur (Li–S) batteries is dogged by the rapid capacity decay arising from polysulfide dissolution and diffusion in organic electrolytes. To solve this critical issue, a praline‐like flexible interlayer consisting of high‐loading titanium oxide (TiO2) nanoparticles and relatively long carbon nanofibers is fabricated. TiO2 nanoparticles with a size gradient occupy both the external and internal of carbon fiber and serve as anchors that allow the chemical adsorption of polysulfides through a conductive nanoarchitecture. The porous conductive carbon backbone helps in the physical absorption of polysulfides and provides redox reaction sites to allow the polysulfides to be reused. More importantly, it offers enough mechanical strength to support a high load TiO2 nanoparticle (79 wt%) that maximizes their chemical role, and can accommodate the large volume changes. Significant enhancement in cycle stability and rate capability is achieved for a readily available sulfur/multi‐walled carbon nanotube composite cathode simply by incorporating this hierarchically nanostructured interlayer. The design and synthesis of interlayers by in situ integration of metal oxides and carbon fibers via a simple route offers the potential to advance Li–S batteries for practical applications in the future. 相似文献
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Batteries: A Graphene–Pure‐Sulfur Sandwich Structure for Ultrafast,Long‐Life Lithium–Sulfur Batteries (Adv. Mater. 4/2014)
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Guangmin Zhou Songfeng Pei Lu Li Da‐Wei Wang Shaogang Wang Kun Huang Li‐Chang Yin Feng Li Hui‐Ming Cheng 《Advanced materials (Deerfield Beach, Fla.)》2014,26(4):664-664
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Ruiqing Liu Zhiwei Liu Wenhui Liu Yuejiao Liu Xiujing Lin Yi Li Pan Li Zhendong Huang Xiaomiao Feng Leshu Yu Dan Wang Yanwen Ma Wei Huang 《Small (Weinheim an der Bergstrasse, Germany)》2019,15(29)
Metal organic frameworks (MOFs)‐derived porous carbon is proposed as a promising candidate to develop novel, tailorable structures as polysulfides immobilizers for lithium–sulfur batteries because of their high‐efficiency electron conductive networks, open ion channels, and abundant central ions that can store a large amount of sulfur and trap the easily soluble polysulfides. However, most central ions in MOFs‐derived carbon framework are encapsulated in the carbon matrix so that their exposures as active sites to adsorb polysulfides are limited. To resolve this issue, highly dispersed TiO2 nanoparticles are anchored into the cobalt‐containing carbon polyhedras that are converted from ZIF‐67. Such a type of TiO2 and Co nanoparticles‐decorated carbon polyhedras (C? Co/TiO2) provide more exposed active sites and much stronger chemical trapping for polysulfides, hence improving the sulfur utilization and enhancing reaction kinetics of sulfur‐containing cathode simultaneously. The sulfur‐containing carbon polyhedras decorated with TiO2 nanoparticles (S@C? Co/TiO2) show a significantly improved cycling stability and rate capability, and deliver a discharge capacity of 32.9% higher than that of TiO2‐free S@C? Co cathode at 837.5 mA g?1 after 200 cycles. 相似文献
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Linlin Zhang Daobin Liu Zahir Muhammad Fang Wan Wei Xie Yijing Wang Li Song Zhiqiang Niu Jun Chen 《Advanced materials (Deerfield Beach, Fla.)》2019,31(40)
Lithium–sulfur (Li–S) batteries have arousing interest because of their high theoretical energy density. However, they often suffer from sluggish conversion of lithium polysulfides (LiPS) during the charge/discharge process. Single nickel (Ni) atoms on nitrogen‐doped graphene (Ni@NG) with Ni–N4 structure are prepared and introduced to modify the separators of Li–S batteries. The oxidized Ni sites of the Ni–N4 structure act as polysulfide traps, efficiently accommodating polysulfide ion electrons by forming strong Sx 2????Ni? N bonding. Additionally, charge transfer between the LiPS and oxidized Ni sites endows the LiPS on Ni@NG with low free energy and decomposition energy barrier in an electrochemical process, accelerating the kinetic conversion of LiPS during the charge/discharge process. Furthermore, the large binding energy of LiPS on Ni@NG also shows its ability to immobilize the LiPS and further suppresses the undesirable shuttle effect. Therefore, a Li–S battery based on a Ni@NG modified separator exhibits excellent rate performance and stable cycling life with only 0.06% capacity decay per cycle. It affords fresh insights for developing single‐atom catalysts to accelerate the kinetic conversion of LiPS for highly stable Li–S batteries. 相似文献