Preparation and photocatalytic performance of montmorillonite-BiVO4/BiOIO3 composite
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摘要: 本文以十六烷基三甲基溴化铵改性蒙脱土、BiVO4及BiOIO3前驱体为原料，水热法制备了改性蒙脱土负载BiVO4/BiOIO3的复合材料(MMT- BiVO4/BiOIO3)。相比BiOIO3，UV-vis DRS显示复合材料的吸收边缘红移至可见光区，200~800 nm区域的吸光强度增强；40%MMT-65% BiVO4/BiOIO3位于579 nm附近的荧光强度低于BiVO4、BiOIO3的，其电化学阻抗圆弧半径最小，表明构建的II型BiVO4/BiOIO3异质结降低了光生载流子的复合率。同时，阳离子表面活性剂修饰的蒙脱土可静电吸引光生电子，载流子的分离率进一步提高，有利于光催化反应。模拟可见光降解酸性品红(AF)的实验中，光照60 min，40%MMT-65% BiVO4/BiOIO3对AF的降解率为97.7%，拟一级动力学反应速率常数为
0.0532 min−1，h+、${\text{•}}\text{O}_{2}^{-} $光降解反应的活性基团。此外，复合材料对结晶紫(CV)、亚甲基蓝(MB)、孔雀石绿(MG)等阳离子染料的吸附性能极佳，光降解甲基橙(MO)、罗丹明B(RhB)、盐酸四环素(TC)效果较好。-
关键词:
- 有机改性蒙脱土 /
- BiVO4/BiOIO3 /
- 模拟可见光 /
- 光降解
Abstract: Montmorillonite supported BiVO4/BiOIO3 composites (MMT-BiVO4/BiOIO3) were prepared by hydrothermal method using hexadecyl trimethyl ammonium bromide modified montmorillonite, BiVO4 and precursor of BiOIO3 as raw material. Compared to BiOIO3, the absorption edge of composite materials occur red shift to visible light region and absorption intensity is enhanced located near 579 nm is lower than that of BiVO4 or BiOIO3. Its half circular diameter is the smallest in electrochemical impedance spectra. These results indicate that the recombination rate of photo generated carriers is reduced by constructing II-scheme BiVO4/BiOIO3 heterojunction. Meanwhile, the electrostatic attraction between modified montmorillonite and photogenerated electron further improve the separation rate of photo generated charge carriers and is beneficial for photocatalytic reactions. In the experiment of simulating visible light degradation of acid fuchsin (AF), the degradation rate of AF is 97.7% with 60 min by 40% MMT-65% BiVO4/BiOIO3 as photocatalysts. The pseudo-first-order rate constant is0.0532 min−1 and the active species are h+, ${\text{•}}\text{O}_{2}^{-} $ in photodegradation reaction. As well as, the composite has excellent adsorption performance for cationic dyes, such as crystal violet (CV), methylene blue (MB) and malachite green (MG). The photodegradation effect on methyl orange (MO), Rhodamine B (RhB) and tetracycline hydrochloride (TC) is more effective. -
图 1 MMT(CTAB)、BiVO4、BiOIO3、65% BiVO4/BiOIO3和 40% MMT-65%BV/BO的XRD谱
Figure 1. 图 Fig. 1 XRD patterns of MMT(CTAB), BiVO4, BiOIO3, 65% BiVO4/BiOIO3 and 40% MMT-65%BV/BO
MMT—Montmorillonite; CTAB—Hexadecyltrimethyl ammonium bromide
图 2 BiVO4 (a)、BiOIO3 (b)、65% BiVO4/BiOIO3 (c)和40% MMT-65%BV/BO (d)的扫描电镜图片；40% MMT- 65%BV/BO (e, f, g, h)的透射电镜图片
Figure 2. SEM patterns of BiVO4 (a), BiOIO3 (b), 65% BiVO4/BiOIO3 (c) and 40% MMT-65%BV/BO (d). TEM patterns of 40% MMT-65%BV/BO (e, f, g, h)
图 3 不同BiVO4/BiOIO3材料的N2吸附-脱附等温线
Figure 3. N2 adsorption-desorption isotherms of different BiVO4/BiOIO3 materials
图 4 不同BiVO4/BiOIO3样品的紫外-可见漫反射光谱(a)及对应的禁带宽度(b)
Figure 4. UV-Vis diffuse reflectance spectra of several different BiVO4/BiOIO3 samples (a) and corresponding band gap widths of different samples (b)
α −Absorption coefficient; hv−Photon energy
图 5 不同BiVO4/BiOIO3材料的光致发光光谱
Figure 5. Photoluminescence spectrum of different BiVO4/BiOIO3 materials
图 7 不同BiVO4/BiOIO3样品对AF的光催化活性
Figure 7. Photocatalytic activity of different BiVO4/BiOIO3 samples to AF
图 8 不同MMT含量的MMT-65%BV/BO对AF的光降解(a)及相应的表观速率常数k(b)
Figure 8. The photodegradation of AF with different contents of MMT in MMT-65%BV/BO (a) and the associated apparent reaction rate constants k (b)
图 9 40% MMT-65%BV/BO对有机污染物的光催化降解 (a)及相应的表观速率常数k(b)
Figure 9. Photocatalytic degradation of organic pollutants by 40% MMT-65%BV/BO (a) and the associated apparent reaction rate constants k (b)
MO-Methyl orange; AF-Acid fuchsin; RhB-Rhodamine B; CV-Crystal violet; MB-Methylene blue; MG-Malachite green; TC-Tetracycline hydrochloride
图 10 40% MMT-65%BV/BO光催化循环实验
Figure 10. Photocatalysis cycle experiment by 40% MMT-65%BV/BO
图 11 40% MMT-65%BV/BO光催化剂使用前后XRD
Figure 11. XRD analysis before and after the use by 40% MMT-65%BV/BO photocatalysts
图 12 不同捕获剂对40% MMT-65%BV/BO光催化降解AF的影响
Figure 12. Effect of different trapping agents on the photocatalytic degradation of AF by 40% MMT-65%BV/BO
EDTA-2Na—Ethylenediamine tetraacetic acid disodium salt; IPA—Isopropyl alcohol
图 13 40% MMT-65%BV/BO光催化降解AF可能机制
Figure 13. The proposed mechanism of the photocatalytic degradation of AF by 40% MMT-65%BV/BO
表 1 BiVO4/BiOIO3复合材料的命名
Table 1. Naming of BiVO4/BiOIO3 composites
Sample Mass of BiVO4 /g Mass ratio of BiVO4
to BiOIO3/wt%35% BiVO4/BiOIO3 0.162 35 45% BiVO4/BiOIO3 0.208 45 55% BiVO4/BiOIO3 0.255 55 65% BiVO4/BiOIO3 0.301 65 
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表 2 蒙脱土- 65%BiVO4/BiOIO3复合材料的命名
Table 2. Naming of MMT-65%BiVO4/BiOIO3 composites
Sample Mass of MMT /g Mass ratio of MMT
to 65%BV/BO/wt%10% MMT-65%BV/BO 0.076 10 20% MMT-65%BV/BO 0.153 20 30% MMT-65%BV/BO 0.229 30 40% MMT-65%BV/BO 0.306 40
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表 3 不同材料的比表面积、孔容及孔径
Table 3. Specific surface area, pore volume and pore diameter of different materials
Sample Specific
surface
area /(m2.g−1)Pore
volume/
(cm3.g−1)Pore
diameter/
nmBiVO4 0.803 0.012 2.674 BiOIO3 15.706 0.100 3.140 65% BiVO4/BiOIO3 3.2337 0.024 2.849 40%MMT-65%BV/BO 8.357 0.034 3.896
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