Coordination Kinetics of Different Carboxylic Fiber with Fe3+ and Catalytic Degradation Performance of Their Fe3+ Complexes†

doi:10.7503/cjcu20140037

Abstract

Abstract:

Three carboxylic fibers including alginate fiber, polyacrylic acid grafted polypropylene and polyte-trafluoroethylene fibers(PAA-g-PP and PAA-g-PTFE) with similar carboxyl contents were coordinated with Fe³⁺, respectively to prepare the different Fe(Ⅲ)-carboxylic fiber complexes. The coordinating kinetics of three carboxylic fibers with Fe³⁺ was compared, and the effecting factors were also examined. And the catalytic performance of three Fe(Ⅲ)-carboxylic fiber complexes was then evaluated as the heterogeneous Fenton catalysts in the dye degradation in water. The results indicated that within the observed temperature and concentration range, the coordination of carboxylic fiber with Fe³⁺showed better agreement with Langmuir isotherm equation and Lagergren second order equation. Increasing Fe³⁺initial concentration led to a low coordination rate constant. Higher temperature increased the Fe content of the resulting complexes. Alginate fiber reacted more easily with than PAA-g-PP and PAA-g-PTFE at the same conditions. Moreover, their coordination rate constants and Fe contents were ranked as follow: alginate fiber >PAA-g-PP >PAA-g-PTFE. Three Fe(Ⅲ)-carboxylic fiber complexes acted as the heterogeneous Fenton catalysts for dye degradation. UV irradiation could more significantly enhance the catalytic capacity of the complexes than visible irradiation. Fe(Ⅲ)-alginate fiber complex has a higher catalytic performance than the other Fe(Ⅲ)-carboxylic fiber complexes with similar Fe content, which is in relation to the big difference in coordinating structure and surface property between them.

Key words: Alginate fibers, Carboxyl group, Ferric ion, Coordination, Catalysis, Dye degradation, Coordination kinetics

CLC Number:

O643.32

TrendMD:

LI Bing, DONG Yongchun. Coordination Kinetics of Different Carboxylic Fiber with Fe³⁺ and Catalytic Degradation Performance of Their Fe³⁺ Complexes^†[J]. Chem. J. Chinese Universities, 2014, 35(8): 1761.

Figures/Tables 15

Table 1 ACOOH values and surface properties of three carboxylic fibers

Carboxylic fiber	A_COOH/(mmol·g^-1)	Specific surface area/(m²·g^-1)	Water contact angle/(°)
Alginate fiber	2.23	0.286	48.3
PAA-g-PP	2.27	0.251	85.8
PAA-g-PTFE	2.35	0.178	91.1

Fig.1 Isothermal adsorption curves of Fe3+ onto alginate(A), PAA-g-PP(B) and PAA-g-PTFE fibers(C) Temperature/℃: a. 20; b. 35; c. 50.

Table 2 Parameters and equations for Langmuir adsorption isothermals of Fe3+ onto three carboxylic fibers

Fiber	Temperature/℃	Linear regression equation	k_L/(L·mmol^-1)	Q_m/(mmol·g^-1)	r²
Alginate fiber	50	Q_e=0.4389c_e/(1+0.1389c_e)	0.1389	3.16	0.9877
	35	Q_e=0.2708c_e/(1+0.1231c_e)	0.1231	2.20	0.9856
	20	Q_e=0.1158c_e/(1+1.1007c_e)	0.1007	1.15	0.9898
PAA-g-PP	50	Q_e=0.1400c_e/(1+0.0625c_e)	0.0625	2.24	0.9862
	35	Q_e=0.0705c_e/(1+0.0538c_e)	0.0538	1.31	0.9933
	20	Q_e=0.0367c_e/(1+0.00448c_e)	0.0448	0.82	0.9861
PAA-g-PTFE	50	Q_e=0.1195c_e/(1+0.0561c_e)	0.0561	2.13	0.9930
	35	Q_e=0.0489c_e/(1+0.0457c_e)	0.0457	1.07	0.9962
	20	Q_e=0.0212c_e/(1+0.0365c_e)	0.0365	0.58	0.9876

Table 3 Parameters and equations for Freundlich adsorption isothermals of Fe3+ onto three carboxylic fibers

Fiber	Temperature/℃	Linear regression equation	n	k_F	r²
Alginate fiber	50	Q_e=0.8929 $c e 0.2688$	3.720	0.8929	0.9258
	35	Q_e=0.6090 $c e 0.2705$	3.697	0.6090	0.9579
	20	Q_e=0.3050 $c e 0.2724$	3.671	0.3050	0.9733
PAA-g-PP	50	Q_e=0.3707 $c e 0.3754$	2.664	0.3707	0.9710
	35	Q_e=0.1998 $c e 0.3765$	2.656	0.1998	0.9530
	20	Q_e=0.1051 $c e 0.4065$	2.460	0.1051	0.9464
PAA-g-PTFE	50	Q_e=0.3103 $c e 0.3899$	2.565	0.3103	0.9682
	35	Q_e=0.0137 $c e 0.4078$	2.452	0.1376	0.9750
	20	Q_e=0.0640 $c e 0.4244$	2.356	0.0640	0.9465

Table 3 Parameters and equations for Freundlich adsorption isothermals of Fe3+ onto three carboxylic fibers

Fiber	Temperature/℃	Linear regression equation	n	k_F	r²
Alginate fiber	50	Q_e=0.8929 $c e 0.2688$	3.720	0.8929	0.9258
	35	Q_e=0.6090 $c e 0.2705$	3.697	0.6090	0.9579
	20	Q_e=0.3050 $c e 0.2724$	3.671	0.3050	0.9733
PAA-g-PP	50	Q_e=0.3707 $c e 0.3754$	2.664	0.3707	0.9710
	35	Q_e=0.1998 $c e 0.3765$	2.656	0.1998	0.9530
	20	Q_e=0.1051 $c e 0.4065$	2.460	0.1051	0.9464
PAA-g-PTFE	50	Q_e=0.3103 $c e 0.3899$	2.565	0.3103	0.9682
	35	Q_e=0.0137 $c e 0.4078$	2.452	0.1376	0.9750
	20	Q_e=0.0640 $c e 0.4244$	2.356	0.0640	0.9465

Fig.2 Intermolecular(A) and intramolecular(B) coordination of Fe(Ⅲ) ion with fibrous ligands

Fig.3 Coordination kinetics curves at different initial concentrations of Fe3+ on alginate(A), PAA-g-PP(B) and PAA-g-PTFE fibers(C) Initial concentration of Fe3+/(mmol·L-1): a. 30; b. 60; c. 90; d. 120.

Fig.4 Simulation curves of Lagergren pseudo first-order equation plots on alginate(A), PAA-g-PP(B) and PAA-g-PTFE fibers(C) Initial concentration of Fe3+/(mmol·L-1): a. 30; b. 60; c. 90; d. 120.

Table 4 Results from linear regression of Lagergren pseudo first-order equation plots

Fiber	c₀/(mmol ·L^-1)	Rate equation	k₁	r²
Alginate fiber	30	ln(1-F)=-0.0628t	0.0628	0.9807
	60	ln(1-F)=-0.0517t	0.0517	0.9833
	90	ln(1-F)=-0.0417t	0.0417	0.9907
	120	ln(1-F)=-0.0387t	0.0387	0.9852
PAA-g-PP	30	ln(1-F)=-0.0437t	0.0437	0.9916
	60	ln(1-F)=-0.0353t	0.0353	0.9940
	90	ln(1-F)=-0.0336t	0.0336	0.9975
	120	ln(1-F)=-0.0316t	0.0316	0.9962
PAA-g-PTFE	30	ln(1-F)=-0.0380t	0.0380	0.9967
	60	ln(1-F)=-0.0223t	0.0323	0.9989
	90	ln(1-F)=-0.0305t	0.0305	0.9989
	120	ln(1-F)=-0.0281t	0.0281	0.9984

Fig.5 Simulation curves of Lagergren pseudo second-order equation plots on alginate(A), PAA-g-PP(B) and PAA-g-PTFE fibers(C) Initial concentration of Fe3+/(mmol·L-1): a. 30; b. 60; c. 90; d. 120.

Table 5 Results from linear regression of Lagergren pseudo second-order equation plots

Fiber	c₀/(mmol·L^-1)	Rate equation	k₂	Q_e/(mmol·g^-1)	r²
Alginatefiber	30	t/Q_t=2.470+t/2.28	0.0781	2.28	0.9985
	60	t/Q_t=2.943+t/2.64	0.0487	2.64	0.9991
	90	t/Q_t=2.979+t/3.04	0.0364	3.04	0.9986
	120	t/Q_t=3.096+t/3.32	0.0293	3.32	0.9985
PAA-g-PP	30	t/Q_t=8.941+t/1.37	0.0598	1.37	0.9947
	60	t/Q_t=9.936+t/1.80	0.0311	1.80	0.9983
	90	t/Q_t=9.020+t/2.09	0.0255	2.09	0.9970
	120	t/Q_t=9.898+t/2.42	0.0173	2.42	0.9976
PAA-g-PTFE	30	t/Q_t=12.665+t/1.40	0.0404	1.40	0.9962
	60	t/Q_t=12.726+t/1.71	0.0268	1.71	0.9968
	90	t/Q_t=11.838+t/2.01	0.0209	2.01	0.9986
	120	t/Q_t=11.628+t/2.29	0.0164	2.29	0.9984

Fig.6 Simulation curves of intra-particle diffusion equation plots on alginate(A), PAA-g-PP(B) and PAA-g-PTFE(C) fibers Initial concentration of Fe3+/(mmol·L-1): a. 30; b. 60; c. 90; d. 120.

Table 6 Results from linear regression of intra-particle diffusion equation plots

Fiber	c₀/(mmol·L^-1)	Rate equation	k_p	r²
Alginate fiber	30	Q_t=0.3121t^1/2	0.3121	0.9486
	60	Q_t=0.3414t^1/2	0.3415	0.9597
	90	Q_t=0.3428t^1/2	0.3428	0.9787
	120	Q_t=0.3637t^1/2	0.3637	0.9771
PAA-g-PP	30	Q_t=0.1816t^1/2	0.1816	0.9692
	60	Q_t=0.2176t^1/2	0.2176	0.9861
	90	Q_t=0.2436t^1/2	0.2436	0.9957
	120	Q_t=0.2693t^1/2	0.2693	0.9983
PAA-g-PTFE	30	Q_t=0.1767t^1/2	0.1767	0.9943
	60	Q_t=0.2008t^1/2	0.2008	0.9952
	90	Q_t=0.2287t^1/2	0.2287	0.9991
	120	Q_t=0.2466t^1/2	0.2466	0.9995

Table 7 Q values and surface properties of three carboxylic fiber-Fe(Ⅲ) complexes

Complex	Q/(mmol·g^-1)	Specific surface area/(m²·g^-1)	Water contact angle/(°)
Fe-ALG	2.32	0.248	82.1
Fe-PAA-g-PP	2.37	0.263	100.3
Fe-PAA-g-PTFE	2.29	0.151	104.6

Fig.7 Decoloration rate and mineralization of RR 195 in the presence of different complexes (A) D90 values under different irradiation; (B—D) UV-Vis spectra and TOCR(%) of dye degradation with Fe-ALG(B), Fe-PAA-g-PP(C) and Fe-PAA-g-PTFE(D), respectively. (B—D) t/min: a. 0; b. 10; c. 25; d. 40; e. 55; f. 70.

Fig.8 UV-Vis spectra of Fe-ALG(a), Fe-PAA-g-PP(b) and Fe-PAA-g-PTFE complexes(c)

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Coordination Kinetics of Different Carboxylic Fiber with Fe³⁺ and Catalytic Degradation Performance of Their Fe³⁺ Complexes^†

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