Tuning Nitrogen Species and Content in Carbon Materials through Constructing Variable Structures for Supercapacitors

doi:10.15541/jim20200498

Abstract

Abstract:

Carbon materials are favorable for supercapacitors but suffer from insufficient capacitance. Heteroatom doping, especially nitrogen (N) doping, is an effective method to significantly improve the electrochemical performance, but it is still a big challenge to achieve high active nitrogen content in carbon materials. This work successfully tuned nitrogen species and content by interaction between Si-O-Si network and aluminum oxide. Besides, the structure of carbon materials varies from a coral-like network to three-dimensional structure by adjusting the precursor composition. Oxygen (O) in oxides bonds with N in carbon materials during the reaction, which makes it difficult to escape, achieving high nitrogen content of 5.29at% at 1000 ℃. On the other hand, the interaction empowers the carbon material with large pore volume of ~1.78 cm³·g^-1 and broad pore size distribution of 0.5-60 nm. Thus, the N-rich carbon material harvests high capacitance of 302 F·g^-1 at 1 A·g^-1 and excellent rate capability of 177 F·g^-1@120 A·g^-1. This unique nitrogen fixation method is a promising strategy for preparing high performance electrode materials of supercapacitors.

Key words: carbon material, nitrogen fixation, interaction, morphology design, supercapacitor

CLC Number:

O782

SUN Peng, ZHANG Shaoning, BI Hui, DONG Wujie, HUANG Fuqiang. Tuning Nitrogen Species and Content in Carbon Materials through Constructing Variable Structures for Supercapacitors[J]. Journal of Inorganic Materials, 2021, 36(7): 766-772.

Figures/Tables 18

References 23

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Sample	SSA /(m²·g^-1)	Pores volume /(cm³·g^-1)	N /at%	N-6 /at%	N-5 /at%
NC	440.78	0.07	1.42	0.21	0.03
SiO-NC	520.78	0.19	1.66	0.14	0.44
AlO-NC	980.35	0.68	3.52	0.78	1.75
SiAlO-NC	703.20	1.78	5.29	1.17	2.53

Sample	SSA /(m²·g^-1)	Pores volume /(cm³·g^-1)	N /at%	N-6 /at%	N-5 /at%
NC	440.78	0.07	1.42	0.21	0.03
SiO-NC	520.78	0.19	1.66	0.14	0.44
AlO-NC	980.35	0.68	3.52	0.78	1.75
SiAlO-NC	703.20	1.78	5.29	1.17	2.53

Sample	N/at%	N-6/at%	N-5/at%	N-Q/at%	Sample	N/at%	N-6/at%	N-5/at%	N-Q/at%
NC (900 ℃)	2.81	1.54	0.82	0.45	NC (1100 ℃)	0.61	0.03	0.32	0.26
SiAlO-NC (900 ℃)	8.27	3.65	3.00	1.62	SiAlO-NC (1100 ℃)	4.33	1.61	1.27	1.45

Sample	N/at%	N-6/at%	N-5/at%	N-Q/at%	Sample	N/at%	N-6/at%	N-5/at%	N-Q/at%
NC (900 ℃)	2.81	1.54	0.82	0.45	NC (1100 ℃)	0.61	0.03	0.32	0.26
SiAlO-NC (900 ℃)	8.27	3.65	3.00	1.62	SiAlO-NC (1100 ℃)	4.33	1.61	1.27	1.45

Carbon material	Specific capacitance /(F·g^-1)	Rate capability /(F·g^-1)	Cycling performance	Ref.
N-doped porous carbon	327 at 1 A·g^-1	200 at 20 A·g^-1	10000 cycles@100%	[2]
N/S co-doped porous carbon	272 at 1 A·g^-1	172 at 100 A·g^-1	5000 cycles at 5 A·g^-1@97.1%	[3]
N/O co-doped carbon	242 at 0.5 A·g^-1	132 at 20 A·g^-1	10000 cycles at 5 A·g^-1@97%	[4]
Graphene/N-rich carbon	229 at 1 A·g^-1	196 at 10 A·g^-1	10000 cycles at 2 A·g^-1@99.5%	[5]
N-doped carbon foam	280 at 1 A·g^-1	185 at 40 A·g^-1	10000 cycles at 5 A·g^-1@96.3%	[6]
N-doped tubular carbon	204 at 0.1 A·g^-1	173 at 10 A·g^-1	50000 cycles at 5 A·g^-1@91.5%	[7]
N-doped carbon microtube	309 at 1 A·g^-1	220 at 10 A·g^-1	10000 cycles at 1 A·g^-1@94%	[8]
N-doped porous carbon	292 at 1 A·g^-1	200 at 20 A·g^-1	10000 cycles at 1 A·g^-1@86%	[9]
N-doped carbon nanorod	271 at 0.5 A·g^-1	175 at 20 A·g^-1	10000 cycles at 5 A·g^-1@97%	[10]
3D porous carbon	261 at 0.5 A·g^-1	200 at 10 A·g^-1	5000 cycles at 1 A·g^-1@96%	[11]
N-doped porous carbon	250 at 1.0 A·g^-1	160 at 10 A·g^-1	3000 cycles at 1 A·g^-1@97.3%	[12]
N-doped carbon spheres	301 at 0.2 A·g^-1	210 at 5 A·g^-1	5000 cycles at 5 A·g^-1@100%	[13]
N-doped porous carbon	252 at 1.0 A·g^-1	189 at 15 A·g^-1	10000 cycles at 15 A·g^-1@94%	[14]
N-doped porous carbon	334 at 1.0 A·g^-1	215 at 20 A·g^-1	10000 cycles at 20 mV·s^-1@95.2%	[15]
3D graphene-like carbon	252 at 1.0 A·g^-1	168 at 50 A·g^-1	5000 cycles at 50 mV·s^-1@98%	[16]
SiAlO-NC	302 at 1 A·g^-1	218 at 20 A·g^-1	20000 cycles at 20 mV·s^-1@92%	This work
SiAlO-NC	302 at 1 A·g^-1	177 at 120 A·g^-1	20000 cycles at 20 mV·s^-1@92%	This work