JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
·
2021
·
IF 8.067
Bo Yu,Fei Ma,Dongjiang Chen,Katam Srinivas,Xiaojuan Zhang,Xinqiang Wang,Bin Wang,Wanli Zhang,Zegao Wang,Weidong He,Yuanfu Chen
The shuttle effect of lithium polysulfides (LiPSs) and sluggish redox conversion significantly hinder practical implementation of lithium-sulfur batteries (LSBs). To overcome these issues, herein, we present MoP quantum dots anchored N, P-doped graphene (MPQ@G) as a multifunctional LSB cathode. The N, P-doped graphene layers serve as a conductive skeleton to support the MoP QDs which can accelerate the electron transfer, physically hinder the polysulfide migration and thus enhance the electrochemical performance. More importantly, as a polar and conductive catalyst, MoP QDs provide catalytically active sites for the conversion of LiPSs. As a result, the LSBs with MPQ@G/S cathodes deliver an elevated initial capacity of 1220.2 mAh g −1 at 0.2 C and remain 98.9% after rate cycles, signifying its exceptional cycling stability. Moreover, it displays a large capacity of 681.2 mAh g −1 even at a high rate of 1 C. The Li-S pouch cell also presents high specific capacities and preeminent cycling stabilities, confirming its great potential for high-rate applications. Density functional theory calculations demonstrate the improved absorptivity and redox conversion reversibility of LiPSs. This work provides an efficient strategy to improve composite with highly adsorptive and catalytic properties for high-performance Li-S batteries.
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DOI
高影响因子
ENERGY & FUELS
·
2020
·
IF 3.421
Yu Zhao,Zhoulu Wang,Xiliang Zhao,Xiaoyan Wang,Kwok-ho Lam,Fuming Chen,Lingzhi Zhao,Shaofeng Wang,Xianhua Hou
Lithium–sulfur (Li–S) batteries have been attracting great attention as promising rechargeable batteries because of their large specific capacity and high energy density. However, some technical problems still limit the commercialization value of Li–S batteries such as poor electrical conductivity, shuttle effects, and volume expansion. To overcome the aforementioned issues, N-doped carbon composites were synthesized via a one-step hydrothermal method. To obtain different N-doping configurations, a carbon precursor was annealed at different heating rates, resulting in different N-containing properties. The cell with the most content of pyridinic-N delivered the highest initial discharge capacity of ∼1121 mAh g–1, and the specific capacity still retained 605 mAh g–1 at 200 mA g–1 after 100 cycles. It was concluded that pyridinic-N has the most significant effect on immobilizing the soluble lithium polysulfides, which stabilized the cycle of Li–S batteries.
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DOI
高影响因子
Energy Storage Materials
·
2020
·
IF 16.28
Sha Li,Pan Xu,Muhammad Kashif Aslam,Changguo Chen,Arif Rashid,Gulian Wang,Li Zhang,Bingwei Mao
Li–S batteries have received unprecedented attention owing to their exceptionally high energy density and low cost. Nevertheless, the daunting challenges of insulating properties, soluble polysulfide shuttling, drastic volume change and sluggish polysulfide conversion kinetics, still hinder their application towards commercialization . Very recently, exciting progresses have been made on inorganic/organic polar hosts as either polysulfide immobilizers or polysulfide redox accelerators, targeting durable Li–S batteries. Herein, self-assembled NiCo 2 S 4 granules comprising secondary open-hole tubular structures are first devised as highly-efficient host materials for high-sulfur-loading and durable Li–S batteries. NiCo 2 S 4 hosts are featured with their large porosity, high electronic conductivity , rapid ion conduction, strong polysulfide immobilization capability and catalytic effect on polysulfide redox, thus greatly ameliorating the polysulfide-shuttle issue and accelerating the polysulfide conversion kinetics. Therefore, the NiCo 2 S 4 /S cathode shows a reversible capacity of 1387 mAh g −1 at 0.2C and retains a value of 543 mAh g −1 after 500 cycles at 2 C. Impressively, the NiCo 2 S 4 /S cathode with a sulfur loading of 8.9 mg cm −2 exhibits high areal capacity of 8.3 mAh cm −2 , low polarization and high cycling stability. Moreover, the as-derived soft-package battery with a 4.5 mg cm −2 sulfur loading can power 169 light-emitting diodes, verifying its great potential for practical application.
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DOI
高影响因子
ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Yu-Jiao Zhang,Zhen-Yu Xing,Wen-Peng Wang,Ning Gao,Jie Zhao,Wen-Ce Yue,Xue Li,Yi-Bo Gao,Sen Xin,Bao Li,Bao Wang
Lithium–sulfur batteries (LSBs) suffer from sluggish reaction kinetics of sulfur-containing species and loss of soluble polysulfides (PSs) during cycling, especially in the case of liquid electrolytes. Here, we improve the kinetics of sulfur species by decorating Mo2C nanoparticles on carbon nanotubes (CNTs) as the host for sulfur active mass. In addition, by use of gel polymer electrolytes (GPEs) derived from in situ polymerization of 1,3-dioxolane (DOL) to mitigate the diffusion of PSs and improve the stability of Li stripping/plating. As a result, the sulfur cathodes are endowed with enhanced initial specific capacity and suppressed dissolution of sulfur species. The cells with CNT/Mo2C/S cathodes and GPE exhibit excellent electrochemical performance. The anodes cycled with GPE show remarkably enhanced lithium plating-stripping behavior. Benefitting from the synergistic effect, LSBs with higher energy density and improved durability are obtained, demonstrating a new approach for developing high-performance quasi-solid-state Li metal batteries.
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DOI
PubMed
高影响因子
Nanoscale
·
2019
·Vol. 12
·期 2
·584-590
·
IF 6.97
Yining Fan,Feng Ma,Jiashun Liang,Xian Chen,Zhengpei Miao,Shuo Duan,Liang Wang,Tanyuan Wang,Jiantao Han,Ruiguo Cao,Shuhong Jiao,Qing Li
With high theoretical specific density, low cost, and non-toxicity, Li–S batteries are regarded as a promising candidate for next-generation energy storage systems. However, the shuttling of soluble Li polysulfides (LiPSs) results in self-discharge and rapid capacity degradation. Herein, nitrogen-doped hierarchical porous carbon with embedded highly dispersed vanadium (V)–Nx sites (V–N–C) is developed as a high-performance Li–S battery cathode for the first time. The metal–organic polymer supramolecule structure formed by the electrostatic/hydrogen bond interaction of chitosan–VO3− strongly stabilizes V to generate a high density of V–Nx/C sites. During the discharge/charge process, the unique V–Nx/C active sites can serve as efficient catalysts to accelerate the redox kinetics of LiPSs, while the hierarchical porous carbon structure of V–N–C benefits the diffusion/transfer of Li+/e− and suppresses the shuttling of LiPSs. As a result, the S/V–N–C composite delivers a high specific capacity of 1111.2 mA h g−1 at 0.5C and maintains 573.6 mA h g−1 at 5C with a low capacity decay rate of 0.087% per cycle (over 500 cycles at 1C). The rate performance of the developed V–N–C cathode in Li–S batteries is superior to that of most of the reported M–N–C and carbon material/metal compound composite electrodes.
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DOI
PubMed
高影响因子
Catalysis Science & Technology
·
2022
·Vol. 12
·期 17
·5408-5417
·
IF 6.177
Wenhua Li,Shule Zhang,Bo Peng,Qianqiao Chen,Qin Zhong
Typically, the more intrinsic defects of carbon materials are unfavorable to conductivity, while they are considered to be the active sites of carbon materials in the field of electrocatalysis. Therefore, seeking a balance between conductivity and active sites is the key to improve the catalytic performance of unadulterated carbon materials. Herein, the hierarchical porous carbon (HPC) prepared by the soft-templating approach is accurately adjusted via the facile hydrothermal method using H3BO3 and H3PO3 as structural modulators. The structural characterization indicates that both H3BO3 and H3PO3 reagents can drive the carbon catalyst to produce more intrinsic defects, and H3PO3 can reduce the amount of oxygen-containing groups in the carbon surface to improve conductivity. The structurally optimized HPC used as a counter electrode in polysulfide electrolytes exhibits a charge transfer resistance as low as 2.25 Ω, and the CdS/CdSe quantum dot sensitized solar cell (QDSSC) has a power conversion efficiency of 4.62%. These confirm that the reduction activity towards Sn2− ions in QDSSCs can be effectively improved by adjusting the degree of carbon defects. This report provides a new perspective on intrinsic defects for improving the electrocatalytic activity of the unadulterated carbon material.
研究领域:
材料科学
·
能源化学
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DOI
高影响因子
JOURNAL OF POWER SOURCES
·
2016
·
IF 6.333
Zhaoling Ma,Zhen Li,Kui Hu,Dongdong Liu,Jia Huo,Shuangyin Wang
The high-energy Li S battery suffers from poor cycling performance due to the shuttle effect of the polysulfides . Strategies must be adopted to suppress the diffusion of polysulfides into the electrolyte in Li S battery . In this work, for the first time, we adopt hydrophilic carbon paper anchored by hierarchically porous cobalt disulfides as the interlayer for capturing polysulfides through physical absorption and chemical bonding. Hierarchical pores can physically adsorb polysulfides, and moreover cobalt disulfide can trap the polysulfides by forming strong chemical interaction. The sulfur-graphene composite with a sulfur content of 70.5% delivers a high initial capacity of 1239.5 mAh g −1 at 0.2 C and retains a reversible capacity of 818 mAh g −1 after 200 cycles. In spite of a little capacity contribution by the insertion of lithium ions into cobalt disulfide for the initial cycles, it disappears in the subsequent cycling. Therefore, the as-developed porous transition metal disulfides on carbon paper as the interlayer could significantly enhance the cycling performance of Li S batteries.
研究领域:
材料科学
·
电化学
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DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2024
·
IF 5.8
Ni Wang,Wenbin Li,Guiqiang Cao,Ruixian Duan,Jingjie Pei,Penghui Luo,Jianhua Zhang,Jingjing Wang,Xifei Li
ABSTRACT The “shuttle effect” caused by polysulfide (LiPSs) dissolution and diffusion is a great challenge for sulfur (S) cathode in lithium-sulfur batteries (LSBs). Herein, we have successfully constructed Co/CoV 2 O 6 tandem catalytic heterostructure anchored by N-doped carbon (Co/CoV 2 O 6 /NC) via an impregnation-assisted pyriaolysis method. The “adsorption-transfer-conversion” tandem catalytic mechanism for LiPSs is realized by utilizing the three behaviors of the strong chemical adsorption of CoV 2 O 6 to LiPSs, the strong conversion of Co to LiPSs, and the transport effect of CoV 2 O 6 ←Co interfacial built-in electric field to polysulfide ions. This can effectively suppress the “shuttle effect” by separating the adsorption and conversion process of LiPSs at different active sites. The tandem catalytic characteristic coupled with the interfacial Co-N and V-N bonds among Co, CoV 2 O 6 and NC, the high electrical conductivities of metal Co and NC conducting network, the hierarchical porous structure of polyhedral framework, collectively endow Co/CoV 2 O 6 /NC@S cathode with strong structural stability, weak electrochemical polarization, good electrochemical reversibility and fast electrochemical kinetics. As a result, Co/CoV 2 O 6 /NC@S cathode presents the significantly enhanced electrochemical performance with a high capacity of 558.4 mAh g -1 at 0.2 C after 100 cycles and a low-capacity decay rate of 0.123% per cycle during 300 cycles at 1 C.
研究领域:
材料科学
·
电化学
·
能源存储
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DOI
高影响因子
NANOTECHNOLOGY
·
2023
·Vol. 34
·期 15
·155401
·
IF 3.5
Ruixian Duan,Xifei Li,Guiqiang Cao,Liping Chen,Jun Li,Qinting Jiang,Yanyan Cao,Jingjing Wang,Wenbin Li
The battery performance of sulfur cathode has obviously depended on the redox reaction kinetics of polysulfides upon cycling. Herein, an effective strategy was proposed to achieve the conversion from 2H (semiconductor phase) to 1T (metal phase) in hollow nano-flowered molybdenum selenide sphere (HFSMS) through crystal phase engineering. The HFSMS with different phase ratio was realized by regulating the proportion of reducing agents. Specifically, the 1T phase content can reach up to 60.8%, and then subsequently decreased to 59.1% with the further increase of the reducing agent. The as-prepared HFSMS with the 1T phase content of 60.8% showed a smallest Tafel slopes (49.99 and 79.65 mV/dec in reduction and oxidation process, respectively), fastest response time and highest response current (520 s, 0.459 mA in Li2S deposition test), which further exhibited excellent catalytic activity and faster reaction kinetics. This result was verified by electrochemical performance, which manifested as stable cycle life with only 0.112% capacity decay per cycle. It was found that the hollow structure can ensures a rich sulfur storage space, and effectually buffer the volume changes of the active substance. More importantly, the improved performance is attributed to the introduction of the 1T phase, which significantly improves the catalytic activity of MoSe2 with promoting the polysulfide conversion.
研究领域:
材料科学
·
电化学
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DOI
高影响因子
Chemical Science
·
2022
·Vol. 13
·期 21
·6224-6232
·
IF 9.969
Rui Xu,Hongan Tang,Yuanyuan Zhou,Fangzheng Wang,Hongrui Wang,Minhua Shao,Cunpu Li,Zidong Wei
The practical application of lithium–sulfur (Li–S) batteries is seriously hindered by severe lithium polysulfide (LiPS) shuttling and sluggish electrochemical conversions. Herein, the Co9S8/MoS2 heterojunction as a model cathode host material is employed to discuss the performance improvement strategy and elucidate the catalytic mechanism. The introduction of sulfur vacancies can harmonize the chemisorption of the heterojunction component. Also, sulfur vacancies induce the generation of radicals, which participate in a liquidus disproportionated reaction to reduce the accumulation of liquid LiPSs. To assess the conversion efficiency from liquid LiPSs to solid Li2S, a new descriptor calculated from basic cyclic voltammetry curves, nucleation transformation ratio, is proposed.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
RARE METALS
·
2026
·Vol. 45
·期 1
·e70176
·
IF 12.1
Mengchen Zhang,Xiaojing Zhang,Qingbing Xia,Long Jiang,Lingfeng Liu,Woying Li,Guoqiang Ma,Da Wang,Changyu Liu,Jianbo Jia,Junhui Zhou,Hao Chen,Chao Xing
en Lithium-sulfur batteries (LSBs) face sluggish sulfur reduction reaction kinetics and severe polysulfide shuttling issues, which significantly limit their performance. In this work, a multifunctional separator with a 3D porous framework featuring confined pore structures and selective adsorption capability is constructed to address these challenges. Within this separator, Lewis acid–base interactions between Ce-MOF-808 and lignosulfonate (SL) effectively regulate the Ce 4+ catalytic activity, thereby lowering the kinetic barrier and accelerating the conversion of short-chain polysulfides into insoluble Li 2 S during the liquid-solid transformation. Furthermore, SL prevents the accumulation of long-chain polysulfides near the Ce 4+ sites through localized electrostatic repulsion, avoiding catalyst poisoning and thereby maintaining continuous catalytic availability. These synergistic effects collectively enable long-lasting catalytic activity toward polysulfide conversion in LSBs, resulting in a fivefold enhancement in capacity and an impressively low capacity decay rate of just 0.033% per cycle over 500 cycles at 1C. This work underscores the transformative potential of Lewis acid–base interactions for enhancing sulfur redox kinetics and introduces a versatile methodology for designing advanced separators for LSBs. 摘要 zh 锂硫电池面临硫还原反应动力学缓慢和严重多硫化物穿梭问题,这显著限制了其性能。在本工作中,我们构建了一种具有受限孔结构和选择性吸附能力的三维多孔框架的多功能隔膜,以应对这些挑战。在该隔膜中,Ce-MOF-808与木质素磺酸盐之间的路易斯酸-碱相互作用有效调控了Ce 4+ 的催化活性,从而降低动力学障碍,加速液-固转化过程中短链多硫化物向不溶性Li 2 S的转化。此外,木质素磺酸钠通过局部静电排斥防止长链多硫化物在Ce 4+ 位点附近积累,从而避免了催化剂中毒,并维持连续的催化可用性。这些协同效应共同促使锂硫电池实现长效的多硫化物转化催化活性,使电池容量提高了五倍,并且在1C条件下经过500个循环后的容量衰减率极低,仅为每循环0.033%。这项工作强调了路易斯酸碱相互作用在增强硫氧化还原动力学方面的变革潜力,并引入了一种用于设计先进锂硫电池隔膜的多功能方法。
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产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
·
IF 8.128
Xiaoli Lu,Xinyi Zhou,Qin Yang,Xiaomin Huang,Qiaoji Zheng,Dunmin Lin,Yingze Song
Lithium–sulfur batteries (LSBs) have attracted much attention due to their high theoretical specific capacity, energy density and low cost. However, the commercial application of LSBs is hindered due to the lithium polysulfide (LiPS) shuttle as well as the sluggish reaction kinetics. Herein, cobalt selenide (Co 0.85 Se) nanowire arrays have been constructed on a carbon-modified separator by an in-situ electrodeposition technique without any other post-treatments such as coating with other ancillary materials. The introduced three-dimensional (3D) conductive carbon layer comprising of carbon nanotube (CNT) and acetylene black (AB) not only serves as the effective support for Co 0.85 Se (CS) but also builds a hierarchical structure to promote the e − transfer. The as-obtained CS-CNT/AB presents a strong anchoring effect on LiPSs and high electrocatalytic activity for sulfur reaction kinetics. As a result, the LSBs inserted with electrodeposition-enabled CS modified separator exhibit an outstanding rate capability (1560.4 mAh g −1 at 0.1 C) and relatively low capacity decay of only 0.068% per cycle over 500 cycles at 2.0 C. This study provides a promising strategy to realize the rational construction of high-efficiency and long-life LSBs.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）