SCIENCE CHINA Materials, Volume 62, Issue 9: 1265-1274(2019) https://doi.org/10.1007/s40843-019-9430-0

Porous honeycomb-like C3N4/rGO composite as host for high performance Li-S batteries

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  • ReceivedJan 18, 2019
  • AcceptedApr 13, 2019
  • PublishedJun 4, 2019


Lithium-sulfur (Li-S) batteries have attracted extensive attention along with the urgent increasing demand for energy storage owing to the high theoretical specific capacity and energy density, abundant reserves and low cost of sulfur. However, the practical application of Li-S batteries is still impeded due to the low utilization of sulfur and serious shuttle-effect of lithium polysulfides (LiPSs). Here, we fabricated the porous honeycomb-like C3N4 (PHCN) through a hard template method. As a polar material, graphitic C3N4 has abundant nitrogen content (~58%), which can provide enough active sites to mitigate shuttle-effect, and then conductive reduced graphene oxide (rGO) was introduced to combine with PHCN to form PHCN/rGO composite in order to improve the utilization efficiency of sulfur. After sulfur loading, the PHCN/rGO/S cathode exhibited an initial discharge capacity of 1,061.1 mA h g−1 at 0.2 C and outstanding rate performance at high current density of 5 C (495.1 mA h g−1), and also retained 519 mA h g−1 after 400 cycles at 1 C. Even at high sulfur loading (4.3 mg cm−2), the capacity fade rate was only 0.16% per cycle at 0.5 C for 200 cycles. The above results demonstrate that the special design of PHCN/rGO composite as sulfur host has high potential application for Li-S rechargeable batteries.

Funded by

Chinese Academy of Sciences large apparatus United Fund(U1832187)

National Nature Science Foundation of China(21471091)

the Natural Science Foundation of Shandong Province(ZR2019MEM030)

Guangdong Province Science and Technology Plan Project for Public Welfare Fund and Ability Construction Project(2017A010104003)

the Fundamental Research Funds of Shandong University(2018JC022)

and Taishan Scholar Project of Shandong Province(ts201511004)


This work was supported by the Chinese Academy of Sciences Large Apparatus United Fund (U1832187), the National Natural Science Foundation of China (21471091), the Natural Science Foundation of Shandong Province (ZR2019MEM030), Guangdong Province Science and Technology Plan Project for Public Welfare Fund and Ability Construction Project (2017A010104003), the Fundamental Research Funds of Shandong University (2018JC022), and Taishan Scholar Project of Shandong Province (ts201511004).

Interest statement

The authors declare no conflict of interest.

Contributions statement

Xu L and Bai X conceived the idea. Bai X designed and performed the experiments, analyzed the results and wrote the manuscript. All authors discussed the results and commented on the manuscript.

Author information

Xiaomeng Bai got her Bachelor degree from Kunming University of Science and Technology. Now, she is a master student under the supervision of Prof. Liqiang Xu at the School of Chemistry and Chemical Engineering, Shandong University, China. Her research interests mainly focus on the design and preparation of host materials for lithium-sulfur batteries.

Liqiang Xu received his BSc degree in chemistry from Liaocheng University in 2000. In 2005, he received his PhD degree in inorganic chemistry from the University of Science and Technology of China. Then he worked at Shandong University, and from May 2012 to May 2013, he worked as a Research Fellow in Nanyang Technology University in Singapore. He is currently a professor at the School of Chemistry and Chemical Engineering, Shandong University, China. His research interests focus on energy related inorganic functional materials.


Supplementary information

Supporting data are available in the online version of the paper.


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  • Scheme 1

    Illustration of the fabrication process of porous honeycomb-like C3N4.

  • Figure 1

    (a) A typical TEM image of PHCN. (b, c) SEM images of PHCN. (d) A typical TEM image of PHCN/rGO. (e, f) SEM images of PHCN/rGO. (g) A typical TEM image of PHCN/rGO/S. (h) SEM image of PHCN/rGO/S. (i) A typical SEM image and the corresponding elemental mapping of PHCN/rGO/S.

  • Figure 2

    (a) XRD patterns of the PHCN and PHCN/rGO. (b) A typical TGA curve of PHCN/rGO/S. (c) N2 adsorption-desorption isotherm loop of PHCN/rGO and PHCN/rGO/S composites. (d) Pore size distribution of the PHCN/rGO.

  • Figure 3

    XPS spectra of PHCN/rGO. (a) Survey spectrum, (b) C 1s spectrum, (c) N 1s spectrum, and (d) O 1s spectrum.

  • Figure 4

    Electrochemical performances. (a) CV profiles of PHCN/rGO/S at a scan rate of 0.1 mV s−1. (b) Rate capability of PHCN/rGO/S. (c) Charge-discharge profiles of PHCN/rGO/S at 0.2 C. (d) Cycle performance of PHCN/rGO/S and rGO/S at 0.2 C. (e) Long cycle performance of PHCN/rGO/S at 0.5 C.

  • Figure 5

    Electrochemical performances. (a) Long cycle performance of PHCN/rGO/S and rGO/S at 1 C. (b) The electrochemical performances at 0.2 C with high sulfur mass loading of 3.1 mg cm−2. (c) The electrochemical performances at 0.5 C with high sulfur mass loading of 4.3 mg cm−2.

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