Novel CO2 Adsorbent Prepared with ZSM-5/MCM-48 as Support: High Adsorption Property and Its Mechanism

doi:10.15541/jim20240403

Abstract

Abstract:

Adsorption by solid amine adsorbent is a promising technology for decarbonization of flue gas. However, adsorption properties of many solid amine adsorbents need to be enhanced, and it is necessary to further study the CO₂ adsorption mechanism. A novel CO₂ adsorbent with high capacity was obtained by grafting 3-aminopropyltriethoxysilane (APTES) on a micro-mesoporous composite molecular sieve ZSM-5/MCM-48 as the support, and then impregnated with tetraethylenepentamine (TEPA) or polyethyleneimine (PEI). The maximum adsorption capacity of APTES-ZSM-5/MCM-48-TEPA-60 (A-ZM-T60), loaded with 60% (in mass) TEPA, for CO₂ reaches 5.82 mmol·g^-1 at 60 ℃ in 15% (in volume) CO₂. Carbamate, alkyl ammonium carbamate and carbonate are generated during the chemical adsorption, which is dominant for CO₂ adsorption because of the reaction between CO₂ and amino groups on the adsorbent, simultaneously accompanied by weak physical adsorption. All above data confirm that these composites display an outstanding adsorption performance with a bright future for CO₂ capture from flue gas after desulfurization.

Key words: ZSM-5/MCM-48, amino-bifunctionalization, CO₂ capture, adsorption kinetics, adsorption mechanism

CLC Number:

TQ424

WEI Jianwen, ZHANG Lijuan, GENG Linlin, LI Yu, LIAO Lei, WANG Dunqiu. Novel CO₂ Adsorbent Prepared with ZSM-5/MCM-48 as Support: High Adsorption Property and Its Mechanism[J]. Journal of Inorganic Materials, 2025, 40(7): 833-839.

Figures/Tables 10

References 34

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Adsorbent	S_BET/ (m²·g^-1)	V_t/ (cm³·g^-1)	N₂ content/ (mmol·g^-1)	CO₂ adsorption capacity/ (mmol·g^-1)
A-ZM-1	237.0	0.52	4.97	1.71
A-ZM-T50	111.2	0.21	8.94	5.04
A-ZM-T60	13.0	0.04	11.89	5.82
A-ZM-T70	5.8	0.02	14.85	4.51
A-ZM-P50	91.5	0.20	8.52	3.53
A-ZM-P60	12.3	0.03	11.17	3.96
A-ZM-P70	-	-	14.06	3.05

Adsorbent	S_BET/ (m²·g^-1)	V_t/ (cm³·g^-1)	N₂ content/ (mmol·g^-1)	CO₂ adsorption capacity/ (mmol·g^-1)
A-ZM-1	237.0	0.52	4.97	1.71
A-ZM-T50	111.2	0.21	8.94	5.04
A-ZM-T60	13.0	0.04	11.89	5.82
A-ZM-T70	5.8	0.02	14.85	4.51
A-ZM-P50	91.5	0.20	8.52	3.53
A-ZM-P60	12.3	0.03	11.17	3.96
A-ZM-P70	-	-	14.06	3.05

Support	Modifier	Condition (CO₂, in volume)	CO₂ adsorption capacity/(mmol·g^-1)	Ref.
MCF	APTMS+PEI	75 ℃/10.5% CO₂	2.36	[25]
SBA-15	APTES+TEPA	75 ℃/20% CO₂	5.68	[26]
HNTS	APTES+PEI	50 ℃/50% CO₂	1.03	[27]
PE-SBA-15	APTES+TEPA	40 ℃/15% CO₂	5.50	[28]
PE-SBA-15	DT+TEPA	40 ℃/15% CO₂	4.20	[28]
Beta/KIT-6	APTMS+TEPA	60 ℃/15% CO₂	5.12	[29]
ZSM-5/MCM-48	APTES+TEPA	60 ℃/15% CO₂	5.82	This work

Support	Modifier	Condition (CO₂, in volume)	CO₂ adsorption capacity/(mmol·g^-1)	Ref.
MCF	APTMS+PEI	75 ℃/10.5% CO₂	2.36	[25]
SBA-15	APTES+TEPA	75 ℃/20% CO₂	5.68	[26]
HNTS	APTES+PEI	50 ℃/50% CO₂	1.03	[27]
PE-SBA-15	APTES+TEPA	40 ℃/15% CO₂	5.50	[28]
PE-SBA-15	DT+TEPA	40 ℃/15% CO₂	4.20	[28]
Beta/KIT-6	APTMS+TEPA	60 ℃/15% CO₂	5.12	[29]
ZSM-5/MCM-48	APTES+TEPA	60 ℃/15% CO₂	5.82	This work

Model	Kinetics parameter	30 ℃	45 ℃	60 ℃	75 ℃	90 ℃
Pseudo-first-order	q_e/(mmol·g^-1)	4.21	4.49	5.68	5.13	3.95
	k₁/min^-1	0.062	0.083	0.062	0.089	0.080
	R²	0.989	0.966	0.989	0.973	0.987
Pseudo-second-order	q_e/(mmol·g^-1)	4.83	5.06	5.70	6.51	4.48
	k₂/(g·mmol^-1·min^-1)	0.017	0.021	0.022	0.012	0.023
	R²	0.997	0.988	0.991	0.997	0.987
Avrami	q_e/(mmol·g^-1)	4.37	4.75	5.89	5.34	4.00
	k_A/min^-1	0.109	0.153	0.109	0.167	0.099
	n_A	0.776	0.696	0.776	0.704	0.901
	R²	0.998	0.991	0.998	0.990	0.998

Novel CO₂ Adsorbent Prepared with ZSM-5/MCM-48 as Support: High Adsorption Property and Its Mechanism

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