不同结构二元羧酸改性棉纤维铁配合物的制备和光催化性能

doi:10.7503/cjcu20190187

摘要/Abstract

摘要：

分别使用3种不同结构的二元羧酸[酒石酸(TA)、苹果酸(MA)和丁二酸(SA)]对棉纤维改性引入羧基并与Fe ³⁺离子反应制备羧酸改性棉纤维铁配合物, 考察了二元羧酸结构和浓度对改性棉纤维的羧基含量(Q_COOH)及其铁配合物的铁配合量(Q_Fe)的影响. 研究了3种羧酸改性棉纤维铁配合物作为有机染料氧化降解反应和Cr(Ⅵ)还原反应光催化剂的性能. 结果表明, 改性棉纤维的Q_COOH值随羧酸浓度的增加而增加. 不含羟基的SA比2种羟基羧酸TA和MA能给棉纤维引入更多羧基, 而2种羟基羧酸改性棉纤维铁配合物则具有更高的Q_Fe值. 3种羧酸改性棉纤维铁配合物对染料氧化降解反应和Cr(Ⅵ)还原反应都表现出显著的光催化作用, 且随其Q_Fe和辐射光强度的提高而增强. TA改性棉纤维铁配合物比其它2种配合物具有更高的光催化活性. 3种配合物不但能将Cr(Ⅵ)还原为Cr(Ⅲ)离子, 而且还能将其部分吸附去除, MA改性棉纤维铁配合物具有较高的铬离子去除效率.

关键词: 二元羧酸, 铁配合物, 光催化剂, 染料降解, 铬离子还原

Abstract:

Three dicarboxylic acids(DCAs), tartaric acid(TA), malic acid(MA) and succinic acd(SA), were used for the modification of cotton fiber to introduce carboxyl groups, respectively, which then coordinated with Fe ³⁺ ions to prepare the modified cotton fiber Fe complexes, Fe-DCA-Cotton. Effects of cha-racteristic structure and concentration of dicarboxylic acids on carboxyl group content(Q_COOH) of the modified cotton fiber and Fe content(Q_Fe) of the resulting Fe complexes were investigated. The catalytic activities of three Fe-DCA-cotton complexes as photocatalysts for the oxidative degradation of organic dye and Cr(Ⅵ) reduction were evaluated and compared. The results indicated that Q_COOH of the modified cotton fiber increased with concentration of carboxylic acid increasing. SA without hydroxyl group could give cotton fiber more carboxyl groups than the two hydroxyl dicarboxylic acids, TA and MA. However, the Fe complexes prepared with Fe ³⁺ ions and two hydroxyl dicarboxylic acids showed higher Q_Fevalues. The three Fe-DCA-cotton complexes exhibited significant photocatalytic performance for the oxidative degradation of organic dye and Cr(Ⅵ) reduction. Increasing Q_Fe and irradiation could enhance their catalytic activity. Fe-TA-cotton complex has a better photocatalytic activity than the two complexes. Besides, the three complexes could not only reduce Cr(Ⅵ) into Cr(Ⅲ) ion, but also partially remove it through adsorption effect. Fe-MA-cotton complex showed relatively high Cr removal efficiency.

Key words: Dicarboxylic acid, Fe complex, Photocatalyst, Dye degradation, Cr(Ⅵ) reduction

中图分类号:

O643.32

TrendMD:

甘露,董永春. 不同结构二元羧酸改性棉纤维铁配合物的制备和光催化性能. 高等学校化学学报, 2019, 40(10): 2205.

GAN Lu,DONG Yongchun. Photocatalytic Performance of Fe-complexes Prepared Using Cotton Fiber Modified with Different Dicarboxylic Acids ^†. Chem. J. Chinese Universities, 2019, 40(10): 2205.

图/表 11

Fig.1 Molecular structures of three DCAs

Scheme 1 Synthetic routes of Fe-DCA-Cotton

Fig.2 Effect of DCAs concentration on QCOOH value of DCA-Cotton

Fig.3 Relationship between QCOOH and QFe values of three Fe-DCA-Cotton

Fig.4 Intermolecular(A) and intramolecular(B—D) coordination of Fe3+ ions with DCA-Cotton

Fig.5 FTIR(A, B), XPS(C) and DRS(D) spectra of three Fe-DCA-Cotton

Fig.6 XRD patterns of cotton fiber(a), Fe-TA-Cotton(b), Fe-MA-Cotton(c) and Fe-SA-Cotton(d)

Fig.7 Effects of QFe value of Fe-DCA-Cotton on D30 and R30

Fig.8 Photocatalytic mechanism of Fe-DCA-Cotton for dye degradation and Cr(Ⅵ) reduction

Fig.9 Effect of irradiation on D50 and R50 with Fe-DCA-Cotton (A) Dye degradation; (B) Cr(Ⅵ) reduction.

Fig.10 Cr species removal performance of three Fe-DCA-Cotton samples(A) and XPS spectra of Cr2p on Fe-MA-Cotton before(a) and after(b) removal test(B)

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