Facile Synthesis of Nitrogen-Doped Graphene-Like Active Carbon Materials for High Performance Lithium-Sulfur Battery

doi:10.13208/j.electrochem.200646

Abstract

Abstract:

Lithium-sulphur (Li-S) battery is regarded as a promising energy storage device because of its high theoretical capacity. However, the low S utilization and short cycling life limit the commercial applications. In this work, nitrogen-doped graphene-like carbon (NGC) materials were synthesized by simply pyrolyzing and carbonizing the mixture of melamine (C₃H₆N₆) and L-cysteine (C₃H₇NO₂S). The graphene-like structure in NGC effectively buffered the volume change of S during the discharge/charge process and improved the cycling stability. Meanwhile, nitrogen-containing functional groups in NGC facilitated the transportation of ions and suppressed the dissolution of polysulphide (PS), enabling a high utilization of S. As expected, the NGC-8 (the mass ratio of melamine and L-cysteine being 8:1)/PS cathode delivered a high initial discharge capacity of 1164.1 mAh·g^-1 at 0.2 C and still retained 909.4 mAh·g^-1 capacity after 400 cycles with a slow capacity decay rate of 0.05% per cycle. Even at as high as 2 C, a high-rate capacity of 820 mAh·g^-1 could be achieved.

Key words: lithium-sulphur battery, graphene-like carbon, volume change, cycling stability

CLC Number:

O646

MENG Quan-hua, DENG Wen-wen, LI Chang-ming. Facile Synthesis of Nitrogen-Doped Graphene-Like Active Carbon Materials for High Performance Lithium-Sulfur Battery[J]. Journal of Electrochemistry, 2020, 26(5): 740-749.

Figures/Tables 14

References 47

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Sample	BETSurface/ (cm²·g^-1)	Pore Volume/ (cc·g^-1)	XPS (at%)				Raman
Sample	BETSurface/ (cm²·g^-1)	Pore Volume/ (cc·g^-1)	C	O	N	S	ID/IG
NGC-2	130	0.604	84.72	4.76	10.42	0.11	1.28
NGC-4	161	0.827	84.81	5.19	9.92	0.09	1.37
NGC-8	304	1.016	83.51	6.37	9.99	0.12	1.51

Sample	Total N in sample/at%	Each N state in sample/at%
Sample	Total N in sample/at%	Pyridinc (398 eV)	Pyrrolic (398.8 eV)	Quaternary (400.8 eV)	Oxidized (402.9 eV)
NGC-2	10.42	2.18	2.37	4.02	1.85
NGC-4	9.92	2.73	2.26	4.66	0.27
NGC-8	9.99	2.28	2.14	4.51	1.06

Sample	Total O in sample/at%	Each O state in sample/at%
Sample	Total O in sample/at%	C=O(531.7 eV)	C-O(532.5 eV)	C-OH(533.6 eV)
NGC-2	4.76	0.12	3.16	1.48
NGC-4	5.19	0.56	2.77	1.86
NGC-8	6.37	2.72	1.67	1.98

Electrode	Before cycling	After cycling
Electrode	R_ct/Ω	R_ct/Ω	R_sf/Ω
NGC-8/PS	36.9	2.8	2.6
NGC-4/PS	39.2	3.1	2.4
NGC-2/PS	45.6	2.2	2.02

Cathode	Current density	Sulfur loading/（mg·cm^-2）	Cycle	Capacity/ （mAh·g^-1）	Reference
S-NPC/G	1 C	2.4	300	608	[40]
3DP-FDE	0.2 C	3	200	752	[41]
WSAC-8/S	1 C	1	200	800	[42]
rGO/PC/S	1 C	1.2	300	848	[43]
a-NOSPC/S	0.5 C	1.1	400	740	[44]
S-GO/MWCNT	0.2 C	1.5-2	400	670	[45]
rNGO/S	1 C	1.2	200	592	[46]
S/NDPC-1	1 C	1	500	541	[47]
NGC-8/PS	0.2 C	2	400	910	This work
NGC-8/PS	1 C	2	500	800	This work