Corresponding Author

Xue-ping GAO(xpgao@nankai.edu.cn)


Lithium-sulfur battery is one of the most promising secondary battery systems due to its super high theoretical gravimetric and volumetric energy densities (2600 Wh·kg-1 and 2800 Wh·L-1, respectively). However, the practical volumetric capacity of sulfur cathode is still unsatisfied due to the overuse of low-density host materials, such as carbon nanomaterials. Herein, commercial LiCoO2 with the high tap density of 2.94 g·cm-3 was used as the host material to build high density sulfur-based composite and compact electrode for increasing the volumetric capacity. Obviously, the tap density of the as-prepared S/LiCoO2 composite was 1.90 g·cm-3, larger than that of the conventional S/carbon composite (0.89 g·cm-3). Correspondingly, the pressed electrode density could be increased to 2.60 g·cm-3 by using the S/LiCoO2 composite. In particular, LiCoO2 showed an effective adsorption and electrocatalytic conversion toward soluble intermediate polysulfides, and facilitied to achieve the high utilization of sulfur and cycle stability. As expected, the S/LiCoO2 composite exhibited larger capacity and slower capacity decay rate at 0.1 C rate as compared with the S/carbon composite. Meanwhile, the polarization in discharge-charge processes was smaller for the S/LiCoO2 composite, showing the enhanced reaction kinetics by adopting LiCoO2 host. Therefore, the S/LiCoO2 composite showed superior rate capability and cycle performance at large current density. By virtue of the high tap density, the S/LiCoO2 composite delivered a larger volumetric capacity (1750.5 mAh·cm-3-composite), almost 2.2 times of the S/carbon composite (811.4 mAh·cm-3-composite). Furthermore, the volumetric capacity of the pressed S/LiCoO2 electrode could reach 1676.8 mAh·cm-3-electrode based on the electrode level, almost 2.5 times of the S/carbon electrode (676.5 mAh·cm-3-electrode). This work provides a feasible strategy to achieve the high volumetric capacity and energy density of cathode based on LiCoO2 as sulfur host, which provides reference for further developing high volumetric energy density cathode materials for lithium-sulfur battery.

Graphical Abstract


lithium-sulfur battery, sulfur cathode, metal oxides, volumetric capacity

Publication Date


Online Available Date


Revised Date


Received Date



[1] Seh Z W, Sun Y, Zhang Q, et al. Designing high-energy lithium-sulfur batteries[J]. Chemical Society Reviews, 2016,45(20):5605-5634.
URL pmid: 27460222

[2] Pang Q, Liang X, Kwok C Y, et al. Advances in lithium-sulfur batteries based on multifunctional cathodes and electrolytes[J]. Nature Energy, 2016,1(9):16132.

[3] Chen J H(陈加航), Yang H J(杨慧军), Guo C(郭城), et al. Current status and prospect of battery configuration in Li-S system[J]. Journal of Electrochemistry (电化学), 2019,25(1):3-16.

[4] Zhang Z, Kong L L, Liu S, et al. A high-efficiency sulfur/carbon composite based on 3D graphene nanosheet@carbon nanotube matrix as cathode for lithium-sulfur battery[J]. Advanced Energy Materials, 2017,7(11):1602543.

[5] Pang Q, Kundu D, Cuisinier M, et al. Surface-enhanced redox chemistry of polysulphides on a metallic and polar host for lithium-sulphur batteries[J]. Nature Communications, 2014,5:4759.
URL pmid: 25154399

[6] Park J, Yu B C, Park J S, et al. Tungsten disulfide catalysts supported on a carbon cloth interlayer for high performance Li-S battery[J]. Advanced Energy Materials, 2017,7(11):1602567.

[7] Wang W K(王维坤), Wang A B(王安邦), Jin C Q(金朝庆). Challenges on practicalization of lithium sulfur batteries[J]. Energy Storage Science and Technology (储能科学与技术), 2020,9(2):594-597.

[8] Yang X F, Li X, Adair K, et al. Structural design of lithium-sulfur batteries: from fundamental research to practical application[J]. Electrochemical Energy Reviews, 2018,1(3):239-293.

[9] Liu Y T, Han D D, Wang L, et al. NiCo2O4 nanofibers as carbon-free sulfur immobilizer to fabricate sulfur-based composite with high volumetric capacity for lithium-sulfur battery[J]. Advanced Energy Materials, 2019,9(11):1803477.

[10] Zhang B (张波), Liu J(刘佳), Liu X C(刘晓晨), Electrochemical properties of sulfur in different carbon support materials[J], Journal of Electrochemistry (电化学), 2019,25(6):749-756.

[11] Liang J(梁骥), Wen L(闻雷), Cheng H M(成会明), et al. Applications of carbon materials in electrochemical energy storage[J]. Journal of Electrochemistry (电化学), 2015,21(6):505-517.

[12] Liu Y T, Liu S, Li G R, et al. High volumetric energy density sulfur cathode with heavy and catalytic metal oxide host for lithium-sulfur battery[J]. Advanced Science, 2020,7(12):1903693.
URL pmid: 32596113

[13] Liang X, Hart C, Pang Q, et al. A highly efficient polysulfide mediator for lithium-sulfur batteries[J]. Nature Communications, 2015,6:5682.
doi: 10.1038/ncomms6682 URL pmid: 25562485

[14] Zheng C, Niu S Z, Lv W, et al. Propelling polysulfides transformation for high-rate and long-life lithium-sulfur batteries[J]. Nano Energy, 2017,33:306-312.

[15] Wang L, Song Y H, Zhang B H, et al. Spherical metal oxides with high tap density as sulfur host to enhance cathode volumetric capacity for lithium-sulfur battery[J]. ACS Applied Materials & Interfaces, 2020,12(5):5909-5019.
URL pmid: 31944646

[16] Pu J, Shen Z H, Zheng J X, et al. Multifunctional Co3S4@sulfur nanotubes for enhanced lithium-sulfur battery performance[J]. Nano Energy, 2017,37:7-14.

[17] Wang H T, Zhang Q F, Yao H B, et al. High electrochemical selectivity of edge versus terrace sites in two-dimensional layered MoS2 materials[J]. Nano Letters, 2014,14(12):7138-7144.
doi: 10.1021/nl503730c URL pmid: 25372985

[18] Zhou T H, Lv W, Li J, et al. Twinborn TiO2-TiN heterostructures enabling smooth trapping-diffusion-conversion of polysulfides towards ultralong life lithium-sulfur batteries[J]. Energy & Environmental Science, 2017,10(7):1694-1703.

[19] Sun Z H, Zhang J Q, Yin L C, et al. Conductive porous vanadium nitride/graphene composite as chemical anchor of polysulfides for lithium-sulfur batteries[J]. Nature Communications, 2017,8:14627.
URL pmid: 28256504

[20] Zhang Z, Wu D H, Zhou Z, et al. Sulfur/nickel ferrite composite as cathode with high-volumetric-capacity for lithium-sulfur battery[J]. Science China Materials, 2018,62(1):74-86.

[21] Liang X, Kwok C Y, Lodi-Marzano F, et al. Tuning transition metal oxide-sulfur interactions for long life lithium sulfur batteries: the “goldilocks” principle[J]. Advanced Energy Materials, 2016,6(6):1501636.

[22] Zhang L, Ji L W, Glans P A, et al. Electronic structure and chemical bonding of a graphene oxide-sulfur nanocomposite for use in superior performance lithium-sulfur cells[J]. Physical Chemistry Chemical Physics, 2012,14(39):13670-13675.
URL pmid: 22968125

[23] Zhou G M, Paek E, Hwang G S, et al. Long-life Li/polysulphide batteries with high sulphur loading enabled by lightweight three-dimensional nitrogen/sulphur-codoped graphene sponge[J]. Nature Communications, 2015,6:7760.
doi: 10.1038/ncomms8760 URL pmid: 26182892

[24] Zhou G M, Tian H Z, Jin Y, et al. Catalytic oxidation of Li2S on the surface of metal sulfides for Li-S batteries[J]. Proceedings of the National Academy of Sciences of the United States of America, 2017,114(5):840-845.
doi: 10.1073/pnas.1615837114 URL pmid: 28096362



To view the content in your browser, please download Adobe Reader or, alternately,
you may Download the file to your hard drive.

NOTE: The latest versions of Adobe Reader do not support viewing PDF files within Firefox on Mac OS and if you are using a modern (Intel) Mac, there is no official plugin for viewing PDF files within the browser window.