Guanine-assisted N-doped ordered mesoporous carbons as efficient capacity decaying suppression materials for lithium-sulfur batteries

doi:10.1016/j.jmst.2021.06.016

Abstract

Abstract:

Lithium-sulfur (Li-S) batteries are considered promising next-generation energy storage devices due to their high weight capacities and theoretical energy densities, which are significantly higher than those of conventional lithium-ion batteries. However, the sulfur cathode presents two major drawbacks, specifically low specific capacity caused by the poor electrical conductivities of the active materials and fast capacity decay caused by polysulfide dissolution/shuttling. Herein, a high-rate and high-stability dendritic material consisting of N-doped ordered mesoporous carbons (NOMCs) was successfully synthesized via a facile and low-cost calcination method. The highly ordered mesoporous carbon skeleton limited the growth of the sulfur nanofiller within its channels and provided the necessary electrical contact with the insulating sulfur. Furthermore, N-doped heteroatoms presented strong binding sites for trapping polysulfide intermediates, achieving high electrochemical activity, which promoted polysulfide conversion reactions. As a result, the prepared NOMC-2/S cathode material with 1.2-1.5 mg cm^-2 of sulfur displayed excellent electrochemical performance with a high-rate capability of 460.5 mAh g^-1 at 1 C, a high specific capacity of 530.9 mAh g^-1 after 200 cycles at 0.1 C, and a decay rate of ∼0.19% per cycle.

Key words: Lithium-sulfur batteries, N-doped ordered mesoporous carbons, Electrochemistry

Riguang Cheng, Yanxun Guan, Yumei Luo, Chenchen Zhang, Sheng Wei, Mengmeng Zhao, Qi Lin, Hao Li, Shiyou Zheng, Federico Rosei, Lixian Sun, Fen Xu, Hongge Pan. Guanine-assisted N-doped ordered mesoporous carbons as efficient capacity decaying suppression materials for lithium-sulfur batteries[J]. J. Mater. Sci. Technol., 2022, 101: 155-164.

Figures/Tables 9

Fig. 1. Schematic showing the fabrication procedure of the NOMCs/S composites.

Fig. 2. SEM images of NOMC-0 (a), NOMC-2 (b, c), NOMC-2/S (d), TEM image of NOMC-2 (e), HRTEM image of NOMC-2 (f), and elemental mapping of C, N, and S (g).

Fig. 3. Small-angle (a) and wide-angle (b) XRD patterns of NOMC-0, NOMC-1, NOMC-2, NOMC-3, NOMC-2/S and sulfur samples; N2 adsorption-desorption isotherms (c) and pore size distribution (d) of NOMC-0, NOMC-1, NOMC-2, and NOMC-3, the overall XPS spectrum of NOMC-1, NOMC-2, and NOMC-3 (e) and the N 1s spectrum of NOMC-2 (f), Raman spectra (g), and TGA plots (h) of NOMC-2/S.

Table 1 NOMCs parameters of nitrogen adsorption-desorption, Raman spectroscopy and nitrogen content.

Sample	Specific surface area (m²/g)	Pore size (nm)	Pore volume (cm³/g)	I_D/I_G^a	N (at%)
NOMC-0	1275	4.04	1.11	1.06	0.0
NOMC-1	1044	3.56	1.05	0.98	4.8
NOMC-2	1021	3.76	0.99	1.04	8.3
NOMC-3	837	3.73	0.78	1.02	13.6

Fig. 4. In situ XRD data collected at different discharge states (a) and recharge states (b), photo of the NOMC-0, NOMC-1, NOMC-2, NOMC-3, and Li2S6 samples after adsorption ability tests (c).

Fig. 5. Electrochemical performance of the NOMC-0/S, NOMC-1/S, NOMC-2/S, and NOMC-3/S cathodes, showing the rate performance at various current densities (a), the CV of NOMC-2/S at 0.1 mV s-1 (b), electrochemical impedance spectroscopy before cycling (c), and the first discharge/charge profiles at 0.1 C (d).

Fig. 6. Cycling performance at 0.1 C (a) and the cycling and Coulombic efficiency at 0.5 C (b) of the NOMC-0/S, NOMC-1/S, NOMC-2/S, and NOMC-3/S cathodes, long-term cycling performance of NOMC-0/S and NOMC-2/S at 1 C (c), and the NOMC-2/S electrode with 3.5 and 5 mg cm-2 mass loadings (d).

Fig. 7. Optical photographs of the NOMC-0/S and NOMC-2/S lithium anodes and separators (a), SEM images of the pristine lithium anode (b), lithium surface of NOMC-2/S (c), NOMC-2/S (d) electrode after 100 cycles.

Table 2 Comparison of electrochemical performance with different nitrogen content of Li-S batteries in this work (1 C = 1675 mAh g-1).

Materials	Sulfurcontent (%)	Nitrogencontent (at%)	Current density (C)	Initial discharge capacity(mAh g^-1)	Cycle life	Capacity fadingrate (%/cycle)	Ref.
Melamine-derived N-doped porous carbon	60	20.4	1	895	100	0.28	[45]
Polyurethane-derived N-doped mesoporous carbons	75	7.18	2	910	100	0.44	[60]
Dopamine-derived N-Doped hollow carbon spheres	62	1.61	0.5	838.7	100	0.39	[61]
Ammonia-derived N-doped nanocarbon	65	1.76	1	937	100	0.31	[59]
Dicyandiamide N-derived doped graphene/polyaniline	52.5	—	0.5	1227	100	0.43	[62]
Coffee grounds-derived O and N Co-Doped Porous Carbon	48	—	0.2	1150	100	0.47	[63]
Silk Cocoon-derived N-doped Porous Carbon Nanosheets	56	1.9	0.5	876	100	0.32	[64]
Guanine-derived N-doped ordered mesoporous carbons	60.5	8.3	0.5	638.3	100	0.25	our work

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