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Journal of Materials Chemistry A · 2020 ·Vol. 8 ·期 15 ·7253-7260 · IF 11.301

Enveloping ultrathin Ti3C2 nanosheets on carbon fibers: a high-density sulfur loaded lithium–sulfur battery cathode with remarkable cycling stability

Ruiyi Gan,Na Yang,Qin Dong,Na Fu,Rui Wu,Cunpu Li,Qiang Liao,Jing Li,Zidong Wei

A Ti3C2@CF sulfur host material has been prepared by enveloping 3D carbon fibers (CFs) with isolated 2D ultrathin Ti3C2 nanosheets, which largely avoids the restacking of the nanosheets and significantly improves the exposure degree of the 2D surface. This material allows uniform thin-layer loading of sulfur at a high density of 4 mg cm−2 without loss of electrode conductivity. The Ti3C2 nanosheets form strong bonding with lithium polysulfides to inhibit shuttling. Also, the flexible enveloping Ti3C2 greatly enhances the ductility of CFs, which successfully withstands the stress and distortion caused by volume expansion, and thus avoids the pulverization of the cathode. The resulting Li–S battery exhibits remarkable cycling stability, a negligible capacity fading rate (0.06% per cycle over the first 200 cycles at 0.5C) and a greatly retained cycling capacity (626.0 mA h g−1 after 1000 cycles at 1C).

研究领域: 材料科学 · 能源存储
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APPLIED SURFACE SCIENCE · 2019 · IF 5.155

MOFs-derived nitrogen-doped carbon interwoven with carbon nanotubes for high sulfur content lithium–sulfur batteries

Maru Dessie Walle,Mengyuan Zhang,Ke Zeng,Yajuan Li,You-Nian Liu

Despite their high energy density , low-cost, and low environmental impacts compared with the current state-of-the-art lithium-ion batteries, lithium–sulfur (Li S) batteries still suffer from the low sulfur content, dissolution of polysulfides and capacity loss, which hinder their commercial application. To address these issues, nitrogen-doped cubic carbon (NC) interwoven with carbon nanotubes (CNT) host is introduced to achieve high sulfur content for lithium–sulfur batteries. The NC/CNT composites are derived from metal–organic frameworks (MOFs), which can physically confine sulfur, thus providing efficient sulfur loading. The sulfur content in the as-obtained S@NC/CNT composite is as high as 89 wt%, while the cathode membrane has a sulfur loading of 3.6 mg cm − 2 . In addition, the NC/CNT composite can obstruct the dissolution and outward diffusion of polysulfides . Impressively, under the high sulfur content and high sulfur loading conditions, the S@NC/CNT cell exhibits initial specific capacity of 1141 mA h g − 1 at the current rate of 0.5C (837.5 mA g − 1 ) and the capacity retains 674.4 mA h g − 1 after 120 cycles. The S@NC/CNT cathode also shows high areal capacity (4.1 mA h cm − 2 ). The NC/CNT composite derived from MOFs has great potential applications for high‑sulfur loading cathodes.

研究领域: 材料科学 · 能源存储
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JOURNAL OF ALLOYS AND COMPOUNDS · 2023 · IF 6.2

Cu2+ regulates high-performance Fe2O3 nanospheres (Fe1−xCuxO1.5-δ (x = 0.33, 0.4, 0.5)) sulfur loaded matrix to improve the electrochemical performance of lithium-sulfur batteries

Xiaoshi Lang,Ruiyin Ren,Xinxi Wang,Lan Li,Kedi Cai

Lithium-sulfur batteries are considered as promising energy storage systems owing to rather high theoretical specific capacity (1675 mAh.g −1 ) and low cost. Nevertheless, the practical prospect is always limited owing to some short-comings, such as sulfur insulation, volume alternation and shuttle effect. To solve these problems, Cu 2+ regulated Fe 2 O 3 nanospheres (Fe 1−x Cu x O 1.5-δ ) as high-performance matrixes for sulfur composite cathodes of lithium-sulfur batteries are constructed via a facile hydrothermal method . It indicates that Cu 2+ regulation can increase the lattice size and exhibit uniform nanospheres micromorphology with less serious agglomeration. Moreover, as sulfur loading material can realize the joint effect on the physical and chemical confinement and some dissociate excess Cu 2+ with sulfur also can directly compose some Cu-S structures, further stabilizing the structure of sulfur composite cathode. In addition, Fe 0.6 Cu 0.4 O 1.5-δ /S composite cathode with sulfur loading mass ratio to 1:3 has fast electrochemical reaction kinetics with the low charge transfer resistance (25.54 Ω) and the high lithium-ion transfer efficiency (D Li+ =2.59 ×10 −12 cm 2 ·s −1 ) and the initial specific discharge capacities and ideal capacity retention accompanied by a charge and discharge voltage platform with small fluctuation.

研究领域: 材料科学 · 能源存储技术
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Sustainable Energy & Fuels · 2018 ·Vol. 2 ·期 10 ·2197-2205 · IF 0

Porous 3D graphene-based biochar materials with high areal sulfur loading for lithium–sulfur batteries

Daoqing Liu,Qianwei Li,Jinbao Hou,Huazhang Zhao

The low electronic conductivity of sulfur and the high solubility of polysulfides seriously hinder the practical application of lithium–sulfur (Li–S) batteries. Therefore, the incorporation of sulfur into carbon-based materials is considered as a suitable solution. Here, a porous pomelo biochar/graphene composite (PBG) was prepared via a simple and green method combining hydrothermal carbonization and KOH activation. The obtained material was used as a host to encapsulate sulfur for the cathode of Li–S batteries, and the three-dimensional pore structure with enhanced conductivity is beneficial for the utilization of sulfur and absorption of soluble polysulfides. As a result, the PBG-S composite (63.3 wt% sulfur) delivered an initial discharge capacity of 1053 mA h g−1 at 0.1C (1C = 1675 mA g−1) and retained 418 mA h g−1 at 3C, even with a high sulfur loading of 4.0 mg cm−2. In addition, the performance of the composite was further improved by reducing the content of sulfur to an appropriate ratio in the PBG-S composite. The optimized PBG-S composite (48.6 wt% sulfur) exhibited a high initial discharge capacity of 1368 mA h g−1 at 0.1C and retained 638 mA h g−1 at 3C, and the discharge capacity remained as high as 664 mA h g−1 and 354 mA h g−1 even after the 200th and 600th cycles at 1C, respectively. The results indicated that PBG, with excellent electrochemical properties, is an ideal electrode material for lithium–sulfur batteries, and can also be prepared economically on an industrial scale.

CAS / MDL: 7440-44-0
研究领域: 材料科学 · 能源存储
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IONICS · 2020 ·Vol. 26 ·期 12 ·6035-6047 · IF 2.394

Effects of structural feature of biomass raw materials on carbon products as matrix in cathode of Li-S battery and its electrochemical performance

Yan Yinglin,Fan Chaojiang,Yang Yanyun,Xie Yigui,Cao Ye,Lin Jiaming,Zou Yiming,You Caiyin,Xu Yunhua,Yang Rong

In this study, three types of biomass with different structures were selected to synthesize carbon matrix in a cathode of Li-S battery. The influence of the structure of raw biomass on microstructure, sulfur-loading amount, and electrochemical performance was investigated in detail. The results demonstrated that the catkin-derived porous carbon (CPC) inherited the 1D-structured morphology and exhibited the highest specific surface area (2033.09 m 2 /g), the largest sulfur loading (53.72%), and the highest initial discharge specific capacity (1369.52 mA h g −1 ) under 0.1 C. Comparatively speaking, the wrinkled cloth-like sakura petal–derived porous carbon showed a better capacity (1218.14 mA h g −1 ) but poor cycling performance. And the 3D network structure of bamboo-derived porous carbon (BPC) exhibited a relatively high capacity retention. These results demonstrated that the structural feature of biomass raw materials plays an important role in the microstructure and electrochemical performance of the carbon products.

CAS / MDL: 90076-65-6 7704-34-9
研究领域: 材料科学 · 能源科学
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Journal of Energy Storage · 2023 · IF 9.4

Systematic insight of the behavior of LiNO3 additive in LiS batteries with gradient S loading

Yangyang Mao,Tianle Li,Siddig Abuelgasim,Xiaoqian Hao,Yupeng Xiao,Chongyang Li,Wenju Wang,Yuqian Li,Encai Bao

Previous studies revealed that LiNO 3 can enhance the cyclic stability of lithium‑sulfur (Li S) batteries by creating a solid electrolyte interface protecting the lithium electrode. However, this study investigated the effect of LiNO 3 and concentration in the electrolyte, first studied under low and high sulfur loading. It is confirmed that adding a small amount of LiNO 3 inhibits the shuttle effect phenomenon in Li S batteries, and the Coulombic efficiency was significantly improved. Appropriately increasing the concentration of LiNO 3 to 2 % could prolong the cycle life. However, when LiNO 3 is excessive, the rate and cycling performance decrease. The design of practical Li S batteries requires more research on the parameters of electrolyte additives under high‑sulfur-loading conditions. After gradient increasing the sulfur loading, the low concentration of LiNO 3 cannot play the best performance of the battery , so it is necessary to improve the concentration of LiNO 3 further. It is evident that adding LiNO 3 in Li S batteries has certain benefits, and the optimal amount of additive is related to the value of sulfur loading.

研究领域: 材料科学 · 电化学
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Journal of Energy Storage · 2024 · IF 8.9

Multifunction-balanced porous carbon and its application in sulfur-loading host and separator modification for lithium–sulfur batteries

Shengheng Nong,Dongyuan Huang,Yaoying Li,Ruoxi Yang,Jiawei Xie,Jia Li,Haifu Huang,Xianqing Liang,Guangxu Li,Zhiqiang Lan,Haizhen Liu,Dan Huang,Shuaikai Xu,Jin Guo,Wenzheng Zhou

Lithium–sulfur batteries have been researched extensively because of their high energy density and low price. However, the poor conductivity of sulfur, the shuttle effect of polysulfide, the slow redox kinetics of sulfur species, and the significant volume expansion and contraction during charging and discharging have hindered the commercial application of lithium–sulfur batteries. In this study, a simple, scalable, and cost-effective strategy was developed to control the balance of the porosity, specific surface area, graphitization , heteroatom co-doping, and polar-polar interactions of a biomass carbon source. With this strategy, multifunctional porous carbon materials with three-dimensional network structures were prepared to serve as sulfur-loading hosts with high specific surface area, strong adsorption activity, and good conductivity. Moreover, the optimal porous carbon material was directly coated on a commercial separator, and the modified separator was found to further improve the electrochemical performance of a lithium–sulfur battery . As a result, for the battery with GPCS-3 as cathode electrode and modified separator as separator, the initial discharge capacity at 1.0C is 926.2 mAh g −1 . After 300 cycles, the discharge capacity is 712.7 mAh g −1 , and the average capacity decay is only 0.077 % per cycle. Since the three-dimensional network structure material exhibits good performance as a sulfur-loading host as well as the ability to effectively modify a separator, this study provides a valuable strategy for the fabrication of high energy density lithium–sulfur batteries.

研究领域: 材料科学 · 能源存储与转换
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JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS · 2018 ·Vol. 29 ·期 13 ·11325-11335 · IF 2.324

Activated porous carbon materials with ultrahigh specific surface area derived from banana peels for high-performance lithium–sulfur batteries

Yan Yinglin,Wei Yiqi,Li Qiaole,Shi Mangmang,Zhao Chao,Chen Liping,Fan Chaojiang,Yang Rong,Xu Yunhua

A series of banana peels derived porous carbon (BPPC) materials were fabricated by pyrolysis carbonization with different numbers of KOH activation. The Brunauer–Emmett–Teller tests indicated the number of activation effectively improves the specific surface area and pore volume of the BPPC. Amongst, the BPPC-2 (activated twice) possesses ultrahigh specific surface area (2044.57 m 2  g −1 ) and large pore volume (2.40 cm 3  g −1 ) on account of the improved hierarchical porous microstructure. After S loading process, the resultant C/S composites were introduced as cathode material in Li–S batteries. The S/BPPC-2 composite cathode exhibited a higher initial specific capacity (1481.54 mAh g −1 at 0.1 C) and a better reversible capacity (351 mAh g −1 after 300 cycles at 1 C) than those of others. It also exhibited excellent high rate performance even at 5 C. The enhanced electrochemical performances were ascribed to the improved specific surface area and larger pore volume of the BPPC-2, which effectively facilitated the intimate contact between sulfur and the conductive matrix, accommodating severe volume change. Besides, the micro/mesopores provided high adsorption power to inhibit the dissolution of polysulfides. This research suggested that the activation number played a key role in improving the electrochemical performance of composite cathode in Li–S batteries.

CAS / MDL: 1310-58-3 7704-34-9
研究领域: 材料科学 · 能源存储
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ELECTROCHIMICA ACTA · 2024 · IF 5.5

Decoration on the inner surface of low-tortuosity microchannels derived from wood plate for highly stable lithium sulfur batteries

Yinglin Yan,Xingsheng Zhang,Wei Jing,Pufang Liu,Muze Song,Chaojiang Fan,Rongfu Xu,Yiming Zou,Wei Yu,Qijiu Deng,Xianhui Wang,Lisheng Zhong,Rong Yang,Yunhua Xu

The low-tortuosity microchannels of wood-based carbon matrix in free-standing cathodes for lithium sulfur batteries (LSBs) were a double-edged sword, which brought in both a high energy density due to a high sulfur loading and severe shuttle effect for poor cycling stability. Herein, a layer of cellulose aerogel extracted from the wood wall was coated on the inner surface of the low-tortuosity microchannels of the wood plate, which was further transformed into a hierarchical carbon matrix using in free-standing cathode for LSBs. The decorated cathode exhibited a maximal specific capacity of 1377.2 mAh g −1 due to the enhanced utilizing ratio of active materials and exceptional cycling stability even under a high current density (1 C) for more than 500 cycles. Furthermore, the decorated cathode maintained good cycling stability with a higher sulfur areal loading (6.3 mg cm −2 ). The cellulose-based carbon aerogel coated on the inner surface of low-tortuosity microchannels provided a large specific surface area. This decoration strategy not only provided physical restriction on polysulfides but also increased conversion sites for polysulfides, improving the cycling performance of the wood-based free-standing cathode of LSBs. This work provided a potential structural design strategy for the advanced free-standing cathode of LSBs.

研究领域: 材料科学 · 能源存储技术
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Advanced Energy Materials · 2025 · IF 26

In Situ Solid Electrolyte Ionic Pathway Formation in High Sulfur Loading Cathodes for High-Performance All-Solid-State Lithium–Sulfur Batteries

Yipeng Su,Shuaiyang Ren,Qiyuan Lin,Yi Su,Yitao Lin,Weining Jiang,Yuegang Zhang

All-solid-state lithium–sulfur batteries (ASSLSBs) are promising for next-generation energy storage. However, the limited ionic and electronic conductivities of sulfur-based cathodes make them difficult to realize high sulfur content and high areal loading. Herein, a facile approach of in situ solid electrolyte formation is used to build ionic pathways in high sulfur loading cathodes. A precursor of P₂S₅ is introduced into the interior space of sulfur-carbon secondary particles, and its in situ reaction with the discharge product Li₂S forms lithium phosphorus sulfide solid-state electrolyte that establishes 3D ionic pathways within the cathodes. This approach not only activates more active materials but also boosts the overall ionic conductivity of the cathodes. The optimized cathode with a sulfur loading of 4 mg cm −2 can achieve a high specific capacity of 1340 mAh g −1 (based on sulfur mass) with 89% capacity retention after 100 cycles at 0.1C (1C = 1675 mA g −1 ). Even with a higher sulfur loading of 8 mg cm −2 , the cathode still demonstrates a very high active materials utilization with an areal capacity of 9.2 mAh cm −2 . The simple and effective method to realize high-performance sulfur cathode with built-in solid electrolyte ionic pathways would be useful for the further development of practical ASSLSBs.

CAS / MDL: 1314-80-3
研究领域: 材料科学 · 能源存储技术
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ACS Nano · 2019 · IF 13.903

Triple-Layered Carbon-SiO2 Composite Membrane for High Energy Density and Long Cycling Li–S Batteries

Wei Kou,Xiangcun Li,Yang Liu,Xiaopeng Zhang,Shaoran Yang,Xiaobin Jiang,Gaohong He,Yan Dai,Wenji Zheng,Guihua Yu

Here we report a highly scalable yet flexible triple-layer structured porous C/SiO2 membrane via a facile phase inversion method for advancing Li–sulfur battery technology. As a multifunctional current-collector-free cathode, the conductive dense layer of the C/SiO2 membrane offers hierarchical macropores as an ideal sulfur host to alleviate the volume expansion of sulfur species and facilitate ion/electrolyte transport for fast kinetics, as well as spongelike pores to enable high sulfur loading. The triple-layer structured membrane cathode enables the filling of most sulfur species in the macropores and additional loading of a thin sulfur slurry on the membrane surface, which facilitates ion/electrolyte transport with faster kinetics than the conventional S/C slurry-based cathode. Furthermore, density functional theory simulations and visual adsorption measurements confirm the critical role of the doped SiO2 nanoparticles (∼10 nm) in the asymmetric C membrane in suppressing the shuttle effect of polysulfides via chemisorption and electrocatalysis. The rationally designed C/SiO2 membrane cathodes demonstrate long-term cycling stability of 300 cycles at a high sulfur loading of 2.8 mg cm–2 with a sulfur content of ∼75%. This scalable yet flexible self-supporting cathode design presents a useful strategy for realizing practical applications of high-performance Li–S batteries.

研究领域: 材料科学 · 能源存储
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ACS Nano · 2019 · IF 13.903

Adenine Derivative Host with Interlaced 2D Structure and Dual Lithiophilic–Sulfiphilic Sites to Enable High-Loading Li–S Batteries

Qingping Wu,Xuejun Zhou,Jun Xu,Fahai Cao,Chilin Li

How to simultaneously restrain the loss of active species and facilitate the conversion reaction under high S loading condition is the key to solve the commercialization of Li–S batteries. For this system, the availability of raw materials and simplicity (high efficiency) of synthetic strategies are also important factors. Herein, we propose an interlaced two-dimensional (2D) carbon material as advanced Li–S cathode host characterized by corrugated monolithic morphology and Co/N dopants as dual lithiophilic–sulfiphilic sites. This 2D structure is derived from a cheap biomass precursor, adenine, with bonding interaction with a MgCl2 hydrate template via a facile ionothermal method. It allows a homogeneous spatial distribution of S/Li2S deposits and strong adsorbability and enhanced conversion kinetics for polysulfides. Benefiting from the synergistic effects of corrugated 2D conductive matrix and embedded heteroatom/nanodot catalyst, the resultant sulfur cathode releases a high specific capacity of 1290.4 mA h g–1 at 0.2 C, small capacity fading rate of 0.029% per cycle over 600 cycles at 2 C, superior rate performance up to 20 C, and considerable areal capacity retention of 6.0 mA h cm–2 even under an ultrahigh sulfur loading up to 9.7 mg cm–2.

研究领域: 材料科学 · 能源存储
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