Preparation of Nitrogen Doped Mesoporous Carbon Supported Cobalt Catalyst and Its Performance for Removal of CO in Hydrogen-Rich Gas

doi:10.12096/j.2096-4528.pgt.22142

Abstract

Abstract:

In order to effectively remove CO from hydrogen-rich gas, cobalt-based nano-particle catalyst supported on nitrogen-doped ordered mesoporous carbon was prepared and characterized by X-ray diffraction (XRD), Raman spectrum, X-ray photoelectron spectroscopy (XPS) and thermogravimetry-mass spectrometry (TG-MS). The effects of nitrogen doping on the self-reduction behavior of the catalyst and CO methanation reaction performance were studied. The characterization results show that the nitrogen atoms introduced into the mesoporous carbon skeleton are mainly used as the nucleation sites of cobalt oxide, which have a strong interaction with the oxide carrier, and greatly improve the dispersion of cobalt species. Thus, small nano-cobalt particles with uniform particle size are formed, which significantly promote self-reduction reaction and thereby improve the reduction degree of the catalyst. The catalyst evaluation results show that, compared with the mesoporous carbon carrier without doping, the CO removal efficiency of the catalyst doped by nitrogen is much higher.

Key words: fuel cell, nitrogen doping, mesoporous carbon, self-reduction, methanation, CO removal

CLC Number:

TK 09

Haiguang WANG, Yongfeng LIU, Jun ZHANG. Preparation of Nitrogen Doped Mesoporous Carbon Supported Cobalt Catalyst and Its Performance for Removal of CO in Hydrogen-Rich Gas[J]. Power Generation Technology, 2023, 44(3): 373-381.

Figures/Tables 10

Fig. 1 Thermogravimetry curve of cyanamide annealed in the argon atmosphere

Tab. 1 Results of nitrogen physisorption, elemental analysis and Raman analysis

样品	氮气物理吸附			元素质量分数/%				Raman分析
样品	S_BET/(m²/g)	V_t/(cm³/g)	D_pore/nm	N	C	H	其他	I_D/I_G
OMC	580.7	0.65	4.2	0	92.6	2.6	4.8	0.98
NMC	540.2	0.63	4.1	10.5	87.3	1.1	1.1	1.13

Fig. 2 Raman spectra and small-angle XRD patterns of as-calcined samples

Fig. 3 Nitrogen physical adsorption isothermal curve of catalyst

Tab. 2 Texture properties and cobalt particle size of catalysts

样品	氮气物理吸附			STEM		H₂化学吸附
样品	S_BET/(m²/g)	V_t/(cm³/g)	D_pore/nm	d(Co⁰)/nm	S²	分散度/%	d(Co⁰)/nm
15Co/OMC	494.3	0.58	4.1	19.4	3.24	5.9	16.4
15Co/NMC	460.2	0.55	4.0	6.7	0.21	16.0	6.0

Fig. 4 Co 2p XPS spectra of catalyst

Fig. 5 HAADF-STEM images of autoreduced samples

Fig. 6 Changes of TG, DTG curves and mass spectrometry CO signals of heat treatment

Fig. 7 Structural transformation of samples by in-situ XRD detection during annealing treatment

Tab. 3 CO methanation reaction performance of self-reduced samples

样品

初始CO

体积分数

CO转化率/%

残余CO

体积分数

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