Preparation and visible light catalytic performance of N-doped C coated NaTaO3 composites
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摘要: 以五氯化钽(TaCl5)、乙酸钠为原料，三聚氰胺为N源，十六烷基三甲基溴化铵(CTAB)和聚乙烯吡咯烷酮(PVP)为表面活性剂，通过溶胶-凝胶法制备了N掺杂C包覆NaTaO3复合材料。采用XRD、TEM、XPS、UV-Vis DRS等对样品进行表征，以罗丹明B(RhB)溶液为目标降解物，测试了不同N比例掺杂的复合材料的吸附性能和光催化性能。结果表明，加入的CTAB和PVP经过N2保护的热处理后在NaTaO3周围形成超薄的碳膜，不仅限制NaTaO3粒径增长，而且提高复合材料对目标污染物的吸附性。N掺杂C包覆NaTaO3复合材料具备良好的可见光催化活性，其中三聚氰胺与TaCl5的摩尔比n为1.5时，制备的N掺杂C包覆NaTaO3复合材料可见光催化效率最高，暗中吸附80 min、可见光照8 h时，RhB的去除率为96.46%，其光催化反应过程符合准一级反应动力学规律。Abstract: The N-doped C coated NaTaO3 composite was prepared through sol-gel method by using tantalic chloride (TaCl5)
and sodium acetate as raw materials, melamine as N sources, cetyl trimethyl ammonium bromide (CTAB) and polyvinylpyrrolidone (PVP) as surfactant. The synthesized sample was characterized in detail by XRD, TEM, XPS and UV-Vis DRS. The dye rhodamine B (RhB) was used as a model contaminant to evaluate the adsorption and photocatalytic activity of N-doped carbon coated NaTaO3. The results indicate that CTAB and PVP form ultra-thin carbon film around NaTaO3, which not only limits the growth of NaTaO3 particles, but also improves the adsorbability to target pollutants. The composites with tripolynitrile amines to TaCl5 molar ratio n=1.5 have the best visible light catalytic performance and the removal ratio of RhB achieves 96.46% under dark adsorption for 80 min and irradiation for 8 h. The photodegradation of RhB is in accordance with the pseudo first order reduction kinetics model. -
Key words:
- coated composites /
- adsorption /
- light catalysis /
- visible-light /
- reaction kinetics
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图 1 不同三聚氰胺与TaCl5摩尔比(n)的N掺杂C包覆NaTaO3复合材料的XRD图谱
Figure 1. XRD patterns of N-doped C coated NaTaO3 composites with different molar ratios of tripolynitrile amines to TaCl5(n)
图 2 n=1.5的N掺杂C包覆NaTaO3复合材料的EDS图谱
Figure 2. EDS spectra of N-doped C coated NaTaO3 composites with n=1.5
图 3 N掺杂C包覆NaTaO3复合材料的TEM图像
Figure 3. TEM images of N-doped carbon coated NaTaO3 composites
图 4 不同三聚氰胺与TaCl5摩尔比(n)的N掺杂C包覆NaTaO3复合材料的XPS电子能谱
Figure 4. XPS electron spectra of of N-doped C coated NaTaO3 composites with different molar ratios of tripolynitrile amines to TaCl5(n)
图 5 n=1.5 N掺杂C包覆NaTaO3复合材料和纯NaTaO3的N 1s和C 1s的XPS能谱图
Figure 5. XPS electron spectra of N 1s and C 1s of N-doped carbon coated NaTaO3 composite with n=1.5 and pure NaTaO3
图 6 N掺杂C包覆NaTaO3复合材料紫外-可见漫反射光谱
Figure 6. UV-vis diffuse reflectance spectra of N-doped C coated NaTaO3 composites
图 7 N掺杂C包覆NaTaO3复合材料对罗丹明B(RhB)溶液的吸附动态曲线
Figure 7. Adsorption dynamic curves of rhodamine B(RhB) by N-doped C coated NaTaO3 composites
图 8 N掺杂C包覆NaTaO3复合材料的光催化性能
Figure 8. Photocatalytic performance of N-doped C coated NaTaO3 composites
图 9 N掺杂C包覆NaTaO3复合材料对RhB的光催化过程
Figure 9. Photocatalytic process of RhB by N-doped C coated NaTaO3 composites
图 10 N掺杂C包覆NaTaO3复合材料对RhB溶液的光降解准一级动力学曲线
Figure 10. Pseudo first-order kinetic curves of RhB photodegradation by N-doped C coated NaTaO3 composites
表 1 不同三聚氰胺与TaCl5摩尔比(n)的N掺杂C包覆NaTaO3复合材料的吸收带边波长λg和禁带宽度Eg
Table 1. Absorbing band edge wavelength λg and band gap Eg of of N-doped C coated NaTaO3 composites with different molar ratios of tripolynitrile amines to TaCl5(n)
Sample λg/nm Eg/eV n=0 317 3.91 n=0.5 318 3.90 n=1 320 3.88 n=1.5 388 3.20 n=2 392 3.16 
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表 2 N掺杂C包覆NaTaO3复合材料对RhB溶液光降解准一级动力学参数
Table 2. Pseudo first-order kinetic parameters of RhB photodegradation by N-doped C coated NaTaO3 composites
Parameters n=0 n=0.5 n=1 n=1.5 n=2 k/min−1 0.021 0.024 0.115 0.406 0.336 R2 0.991 0.974 0.995 0.996 0.996 Notes: k—Fit the kinetic constant; R2—Fitting correlation coefficient.
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